NONEQUILIBRIUM STATISTICAL SPECIAL SYSTEMS SPECIALSECTION: SECTION: Persistence in nonequilibrium systems Satya N. Majumdar Department of Theoretical Physics, Tata Institute of Fundamental Research, Homi Bhabha Road, Mumbai 400 005, India This is a brief review of recent theoretical efforts to understand persistence in nonequilibrium systems. THE problem of persistence in spatially extended nonequilibrium systems has recently generated a lot of interest both theoretically1–7 and experimentally8–10. Persistence is simply the probability that the local value of the fluctuating nonequilibrium field does not change sign up to time t. It has been studied in various systems, including several models undergoing phase separation1–4,11–15, the simple diffusion equation with random initial conditions5,6, several reaction diffusion systems in both pure16 and disordered17 environments, fluctuating interfaces18–20, Lotka–Volterra models of population dynamics21, and granular media22. The precise definition of persistence is as follows. Let φ(x, t) be a nonequilibrium field fluctuating in space and time according to some dynamics. For example, it could represent the coarsening spin field in the Ising model after being quenched to low temperature from an initial high temperature. It could also be simply a diffusing field starting from random initial configuration or the height of a fluctuating interface. Persistence is simply the probability P0(t) that at a fixed point in space, the quantity sgn[φ(x, t) – 〈φ(x, t)〉] does not change up to time t. In all the examples mentioned above this probability decays as a power law P0(t) ~ t–θ at late times, where the persistence exponent θ is usually nontrivial. In this article, we review some recent theoretical efforts in calculating this nontrivial exponent in various models and also mention some recent experiments that measured this exponent. The plan of the paper is as follows. We first discuss the persistence in very simple single variable systems. This makes the ground for later study of persistence in more complex many-body systems. Next, we consider many-body systems such as the Ising model and discuss where the complexity is coming from. We follow it up with the calculation of this exponent for a simpler manybody system namely diffusion equation and see that even in this simple case, the exponent θ is nontrivial. Next, we show that all these examples can be viewed within the general framework of the ‘zero crossing’ problem of a Gaussian stationary process (GSP). We review the new results obtained for this general Gaussian problem in various special cases. Finally, we mention the emerging new directions towards different generalizations of persistence. We start with a very simple system namely the onedimensional Brownian walker. Let φ(t) represent the position of a 1-D Brownian walker at time t. This is a single-body system in the sense that the field φhas no x dependence but only t dependence. The position of the walker evolves as, dφ = η(t ), dt (1) where η(t) is a white noise with zero mean and delta correlated, 〈φ(t)φ(t′)〉 = δ(t – t′). Then persistence P0(t) is simply the probability that φ(t) does not change sign up to time t, i.e. the walker does not cross the origin up to time t. This problem can be very easily solved exactly by writing down the corresponding Fokker–Planck equation with an absorbing boundary condition at the origin23. The persistence decays as P0(t) ~ t–1/2 and hence θ = 1/2. The important point to note here is that the exact calculation is possible here due to the Markovian nature of the process in eq. (1). Note that φ evolves according to a first order equation in time, i.e. to know φ(t), we just need the value of φ(t – ∆t) but not on the previous history. This is precisely the definition of a Markov process. In order to make contact with the general framework to be developed in this article, we now solve the same process by a different method. We note from eq. (1) that η(t) is a Gaussian noise and eq. (1) is linear in φ. Hence, φ is also a Gaussian process with zero mean and a two-time correlator, 〈φ(t)φ(t′)〉 = min(t, t') obtained by integrating eq. (1). We recall that a Gaussian process can be completely characterized by just the two-time correlator. Any higher order correlator can be simply calculated by using Wick’s theorem. Since min(t, t′) depends on both time t and t′ and not just on their difference |t – t′|, clearly φ is a Gaussian non-stationary process. From the technical point of view, stationary processes are often preferable to non-stationary processes. Fortunately there turns out to be a simple transformation by which one can convert this nonstationary process into a stationary one. It turns out that this transformation is more general and will work even for more complicated examples to follow. Therefore we illustrate it in detail for the Brownian walker problem in the following paragraph. The transformation works as follows. Consider first the normalized process, X (t ) = φ(t ) / 〈φ2 (t )〉Then, X(t) is also . e-mail: satya@theory.tifr.res.in 370 t ′) / (tt′ ) . CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS a Gaussian process with zero mean and its two-time correlator is given by, 〈X(t)X(t′)〉 = min(t, Now we define a new ‘time’ variable, T = log(t). Then, in this new time variable T, the two-time correlator becomes, 〈X(T )X(T ′)〉 = exp(– |T – T ′|/2) and hence is stationary in T. 1 3 Thus, the persistence problem reduces to calculating the 2 2 probability P0(T ) of no zero crossing of X(T ), a GSP characterized by its two-time correlator, 〈X(T )X(T ′)〉 = exp(– |T – T ′|/2). 3 One could, of course, ask the same question for an 2 arbitrary GSP with a given correlator 〈X(T )X(T ′)〉 = f (|T – T ′|) [in case of Brownian motion, f (T ) = exp(– T / 2)]. This general zero crossing problem of a GSP has been studied by mathematicians for a long time24. Few results are known exactly. For example, it is known that if f (T ) < 1/T for large T, then P0(T ) ~ exp(–µT ) for large T. Exact result is known only for Markov GSP which are characterized by purely exponential correlator, f (T ) = exp(–λT ). In that case, P0(T ) = (2/π) sin–1 [exp(–λT )] (ref. 24). Our example of Brownian motion corresponds to the case when λ= 1/2 and therefore the persistence P0(T ) ~ exp(– T/2) for large T. Reverting to the original time using T = log(t), we recover the result, P0(t) ~ t– 1/2 . Thus the inverse of the decay rate in T becomes the power law exponent in t by virtue of this ‘log–time’ transformation. Note that when the correlator f (T ) is different from pure exponential, the process is nonMarkovian and in that case no general answer is known. Having described the simplest one-body Markov process, we now consider another one-body process which however is non-Markovian. Let φ(t) (still independent of x) now represent the position of a particle undergoing random acceleration, d2φ dt 2 = η( t), (2) where η(t) is a white noise as before. What is the probability P0(t) that the particle does not cross zero up to time t? This problem was first proposed in the review article by Wang and Uhlenbeck25 way back in 1945 and it got solved only very recently in 1992, first by Sinai26, followed by Burkhardt27 by a different method. The answer is, P0(t) ~ t–1/4 for large t and the persistence exponent is θ = 1/4. Thus even for this apparently simple looking problem, the calculation of θ is nontrivial. This nontriviality can be traced back to the fact that this process is nonMarkovian. Note that eq. (2) is a second order equation and to know φ(t + ∆t), we need to know its values at two previous points φ(t) and φ(t – ∆t). Thus, it depends on two previous steps as opposed to just the previous step as in eq. (1). Hence it is a non-Markovian process. We notice that eq. (2) is still linear and hence φ(t) is still a Gaussian process with a non-stationary correlator. However, using the same T = log(t) transformation as defined in the previous paragraph, we can convert this to CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 the zero crossing problem in time T of a GSP with correlator, f (T ) = exp(–T/2) – exp(– 3T/2). Note that this is different from pure exponential and hence is nonMarkovian. We also notice another important point: It is not correct to just consider the asymptotic form of f (T ) ~ exp(–T/2) and conclude that the exponent is therefore 1/2. The fact that the exponent is exactly 1/4, reflects that the ‘no zero crossing’ probability P0(T ) depends very crucially on the full functional form of f (T ) and not just on its asymptotic form. This example thus illustrates the history dependence of the exponent θ which makes its calculation nontrivial. Having discussed the single particle system, let us now turn to many body systems where the field φ(x, t) now has x dependence also. The first example that was studied is when φ(x, t) represents the spin field of one-dimensional Ising model undergoing zero temperature coarsening dynamics, starting from a random high temperature configuration. Let us consider for simplicity a discrete lattice where φ(i, t) = ± 1 representing Ising spins. One starts from a random initial configuration of these spins. The zero temperature dynamics proceeds as follows: at every step, a spin is chosen at random and its value is updated to that of one of its neighbours chosen at random and then time is incremented by ∆t and one keeps repeating this process. Then persistence is simply the probability that a given spin (say at site i ) does not flip up to time t. Even in one dimension, the calculation of P0(t) is quite nontrivial. Derrida et al.2 solved this problem exactly and found P0(t) ~ t–θ for large t with θ = 3/8. They also generalized this to q-state Potts model in 1-D and found an exact formula, θ(q) = – + [cos–1 {(2 – q)/ q}]2 for all q. This calculation however cannot be easily extended to d = 2 which is more relevant from an experimental point of 2 view. Early numerical results indicated that the18 exponent θ 2 π ~ 0.22 (ref. 2 3) for d = 2 Ising model evolving with zero temperature spin flip dynamics. It was therefore important to have a theory in d = 2 which, if not exact, at least could give approximate results. We will discuss later about our efforts towards such an approximate theory of Ising model in higher dimensions. But before that let us try to understand the main difficulties that one encounters in general in manybody systems. In a many-body system, if one sits at a particular point x in space and monitors the local field φ(x, t) there as a function of t, how would this ‘effective’ stochastic process (as a function of time only) look like? If one knows enough properties of this single site process as a function of time, then the next step is to ask what is the probability that this stochastic process viewed from x as a function of t, does not change sign up to time t. So, the general strategy involves two steps: first, one has to solve the underlying many-body dynamics to find out what the ‘effective’ single site process looks like and second, given this single site process, what is its no zero crossing probability. 371 SPECIAL SECTION: Before discussing the higher dimensional Ising model where both of these steps are quite hard, let us discuss a simple example (which however is quite abundant in nature), namely the diffusion equation. This is a many-body system but at least the first step of the two-step strategy can be carried out exactly and quite simply. The second step cannot be carried out exactly even for this simple example, but one can obtain very good approximate results. Let φ(x, t) (which depends on both x and t) denote field that is evolving via the simple diffusion equation, ∂φ = ∇ 2 φ. ∂t (3) This equation is deterministic and the only randomness is in the initial condition φ(x, 0) which can be chosen as a Gaussian random variable with zero mean. For example, φ(x, t) could simply represent the density fluctuation, φ(x, t) = ρ(x, t) – 〈ρ〉 of a diffusing gas. The persistence, as usual, is simply the probability that φ(x, t) at some x does not change sign up to time t. This classical diffusion equation is so simple that it came as a surprise to find that even in this case, the persistence P0(t) ~ t–θ numerically with nontrivial θ ≈ 0.1207, 0.1875, 0.2380 in d = 1, 2 and 3, respectively. In the light of our previous discussion, it is however easy to see why one would expect a nontrivial answer even in this simple case. Since the diffusion equation (3) is linear, the field φ(x, t) at a fixed point x as a function of t is clearly a Gaussian process with zero mean and is simply given by ρ ρ the solution of eq. (3), φ(x, t) = ∫ d dx′ G( x − x ′, t)φ(x′, 0), ρ where G( x , t) = (4πt)–d/2 exp[– x2/4t] is the Green's function in d. Note that by solving eq. (3), we have already reduced the many-body diffusion problem to an ‘effective’ singlesite Gaussian process in time t at fixed x. This therefore completes the first step of the two-step strategy mentioned earlier exactly. Now we turn to the second step, namely the ‘no zero crossing’ probability of this single-site Gaussian process. The two-time correlator of this can be easily computed from above and turns out to be non-stationary as in the examples specified by eqs (1) and (2). However by using the T = log(t) transformation as before, the normalized field reduces to a GSP in time T with correlator, 〈X(T1)X(T2)〉 = [sech(T/2)]d/2, where T = |T1–T2|. Thus, once again, we are back to the general problem of the zero crossing of a GSP, this time with a correlator f(T) = [sech(T/2)]d/2 which is very different from pure exponential form and hence is non Markovian. The persistence, P0(T ) will still decay as P0(T ) ~ exp(– θT ) ~ t–θ for large T (since f (T ) decays faster than 1/T for large T ) but clearly with a nontrivial exponent. Since persistence in all the examples that we have discussed so far (except the Ising model) reduces to the zero crossing probability of a GSP with correlator f (T ) [where f (T ) of course varies from problem to problem], let us now discuss some general properties of such a process. 372 It turns out that a lot of information can already be inferred by examining the short-time properties of the correlator f (T ). In case of Brownian motion, we found f(T) = exp(–T/2) ~ 1 – T/2 + O(T2) for small T. For the random acceleration problem, f (T ) = exp(– T/2) – exp(– 3T/2) ~ 1 – 3T 2/8 + O(T 3) for small T and for the diffusion problem, f (T ) = [sech(T/2)]d/2 ~ 1 – T2 3 α + O(T ) as T → 0. In general f (T ) = 1 – aT + . . . for small T, where 0 < α ≤ 2 (ref. 24). It turns out that processes for which α= 2 are ‘smooth’ in the sense that the density of zero crossings ρ is finite, i.e. the number of zero crossings of the process in a given time T scales linearly with T. Indeed there exists an exact formula due to Rice28, ρ = when α= 2. However, for α< 2, f″ (0) does not exist and this formula breaks down. It turns out that the density is infinite for α< 2 and once the process crosses zero, it immediately crosses many times and then makes a long excursion before crossing the zero again. In other words, the zero’s are not uniformly distributed over a given interval and in general the set of zeros has a fractal structure.29 Let us first consider ‘smooth’ processes with α= 2 such as random acceleration or the diffusion problem. It turns out that for such processes, one can make very good progress in calculating the persistence exponent θ. The first approach consists of using an ‘independent interval approximation’ (IIA)5. Consider the ‘effective’ single-site process φ(T ) as a function of the ‘log–time’ T = log(t). As a first step, one introduces the ‘clipped’ variable σ= sgn(φ), which changes sign at the zeros of φ(T ). Given that φ(T ) is a Gaussian process, it is easy to compute the correlator, A(T ) = 〈σ(0)σ(T )〉 = sin–1 [ f (T )], π2where f (T ) is the correlator of φ(T ). Since the ‘clipped’ process σ(T ) can take values ± 1 only, one can express A(T ) as, A(T ) = ∞ ∑ ( −1) n Pn (T ), (4) n= 0 where Pn(T ) is the probability that the interval T contains n zeros of φ(T ). So far, there is no approximation. The strategy next is to use the following approximation, Pn (T ) = 〈T 〉 −1 ∫ dT1 ∫ 2 dT 2 Λ T T 0 T1 ∫T T n −1 dT n × Q (Tn ) P (T2 − T1 ) Λ P(Tn − Tn −1 ) Q (T − Tn ), (5) where P(T ) is the distribution of intervals between two successive zeros and Q(T ) is the probability that an interval of size T to the right or left of a zero contains no further zeros. Clearly, P(T ) = – Q′(T ). 〈T 〉 = 1/ρ is the mean interval size. We have made the IIA by writing the joint distribution of n successive zero-crossing intervals as the product of the distribution of single intervals. The rest is straightforward5. By taking the Laplace transform of the ~ above equations, one finally obtains, P (s) = [2 – F (s)]/F (s), where CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 3 2 1 2 NONEQUILIBRIUM STATISTICAL SYSTEMS 1 ~ F (s ) = 1 + s[1 − s A( s )], 2ρ (6) ~ where the Laplace transform A (s) of A(T ) can be easily computed knowing f (T ). The expectation that the persistence, P0(T ) and hence the interval distribution, P(T ) ~ ~ exp(– θT ) for large T, suggests a simple pole in the P (s) at s = – θ. The exponent θ is therefore given by the first zero on the negative s axis of the function, F (s ) = 1 + 1 s 2ρ 2s ∞ −1 1 − ∫0 d T exp( − sT ) sin [ f (T )] . π (7) For the diffusion equation, f(T) = [sech(T/2)]d/2 and ρ= We then get the IIA estimates of θ = 0.1203, 0.1862 and 0.2358 in d = 1, 2 and 3 respectively, which should be compared with the simulation values, 0.1207 ± 0.0005, 0.1875 ± 0.0010 and 0.2380 ± 0.0015. For the random acceleration problem, f(T) = exp(–T/2) – exp(– 3T/2) and ρ = /2π and we get, d/8θπiia2=. 0.2647 which can be compared with its exact value, θ = 1/4. Though the IIA approach produces excellent results when compared to numerical simulations, it cannot however be systematically improved. For this purpose, we turn to the 3 1 6 ‘series expansion’ approach which can be improved 3 2 2 systematically order by order. The idea is to consider the generating function, P( p , t ) = by Bendat30. We have computed the third moment as well6. For example, for 2-D diffusion equation, we get the series, θ( p = 1 − ε) = P0 (T ) = 2∫ where Pn(t) is the probability of n zero crossings in time t of the ‘effective’ single-site process. For p = 0, P(0, t) is the usual persistence, decaying as t–θ(0) as usual. Note that we have used θ(0) instead of the usual notation θ, because it turns out 6 that for general p, P(p, t) ~ t–θ (p) for large t, where θ(p) depends continuously on p for ‘smooth’ Gaussian processes. This has been checked numerically as well as within IIA approach6. Note that for p = 1, P(1, t) = 1 implying θ(1) = 0. For smooth Gaussian processes, one can then derive an exact series expansion of θ(p) near p = 1. Writing p n = exp(n log p) and expanding the exponential, we then obtain an expansion in terms of moments of n, the number of zero crossings, ∞ (log p ) r r (9) 〈n 〉 c , r ! r =1 r where 〈n 〉 c are the cumulants of the moments. Using p = 1 – ε, we express the right hand side as a series in powers of ε. Fortunately, the computation of the moments of n is relatively straightforward, though tedious for higher moments. We have already mentioned the result of Rice for the first moment. The second moment 〈n 2〉 was computed CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 φ >0 D φ(τ) exp[ − S ] ∫ D φ(τ) exp[ − S ] = Z1 , Z0 (11) (8) n= 0 log P ( p , t ) = ∑ (10) Keeping terms up to second order and putting ε = 1 (in the same spirit as ε expansion in critical phenomena) gives, θ(0) = (π+ 4)/4π2 = 0.180899. . ., just 3.5% below the simulation value, θsim = 0.1875 ± 0.001. Thus, this gives us a systematic series expansion approach for calculating the persistence exponent for any smooth Gaussian process. Note that both the above approaches (IIA and series expansion) are valid only for ‘smooth’ Gaussian processes (α= 2) with finite density ρ of zero crossings. What about the nonsmooth processes where 0 < α< 2, where such approaches fail? Even the Markov process, for which f (T ) = exp(– λT ) is a non-smooth process with α= 1. However, for the Markov case, one knows that the persistence exponent θ = λ exactly. One expects therefore that for Gaussian processes which may be non-smooth but ‘close’ to a Markov process, it may be possible to compute θ by perturbing around the Markov result. In order to achieve this, we note that the persistence P0(T ) in stationary time T, can be written formally4 as the ratio of two path integrals, ∞ ∑ p n Pn ( t), 1 1 2 1 3 ε+ 2 − ε + O (ε ) . 2π 4π π where Z1 denotes the total weight of all paths which never crossed zero, i.e. paths restricted to either positive or negative (which accounts for the factor 2) side of φ= 0 and Z0 denotes the weight of all paths completely unrestricted. 1 T T Here S = φ(τ1 ) G (τ1 − τ2 ) φ(τ2 ) d τ1 dτ 2 2 ∫0 ∫0 is the ‘action’ with G(τ1–τ2) being the inverse matrix of the Gaussian correlator f (τ1–τ2). Since P0(T ) is expected to decay as exp(– θT ) for large T, we get, 1 log P0 (T ). T →∞ T θ = − lim (12) If we now interpret the time T as inverse temperature β, then θ = E1 – E0, where E1 and E0 are respectively the ground states of two ‘quantum’ problems, one with a ‘hard’ wall at the origin and the other without the wall. For concreteness, first consider the Markov process, f (T ) = exp(– λ|T |). In this case, it is easy to see that S is the action of a harmonic oscillator with frequency λ. The ground state energy, E0 = λ/2 for an unrestricted oscillator with frequency λ. Whereas, for an oscillator with a ‘hard’ wall at the origin, it is well known that E1 = 3λ/2. This then reproduces the Markovian result, θ = E1 – E0 = λ. For processes close to Markov process, such that f (T ) = exp(– λT ) + ε f1(T ), where ε is small, it is then straightforward to 373 SPECIAL SECTION: λT ) + ε f1(T ), where ε is small, it is then straightforward to carry out a perturbation expansion around the harmonic oscillator action in orders of ε (ref. 4). The exponent θ, to order ε, can be expressed as, 2λ ∞ θ = λ1 − ε f1 (T )[1 − exp( − 2λT )] −3 / 2 dT . ∫ π 0 (13) At this point, we go back momentarily to the zero temperature Glauber dynamics of Ising model. Note that the spin at a site in the Ising model takes values either 1 or – 1 at any given time. Therefore, one really cannot consider the single-site process s(t) as a Gaussian process. However, one can make a useful approximation in order to make contact with the Gaussian processes discussed so far. This is achieved by the so-called Gaussian closure approximation, first used by Mazenko31 in the context of phase ordering kinetics. The idea is to write, s(t) = sgn[φ(t)], where φ(t) now is assumed to be Gaussian. This is clearly an approximation. However, for phase ordering kinetics with nonconserved order parameter, this approximation has been quite accurate31. Note that within this approximation, the persistence or no flipping probability of the Ising spin s(t) is same as the no zero crossing probability of the underlying Gaussian process φ(t). Assuming φ(t) to be a Gaussian process, one can compute its two-point non-stationary correlator self-consistently. Then, using the same ‘log–time’ transformation (with T = log(t)) mentioned earlier, one can evaluate the corresponding stationary correlator f (T ). We are thus back to the general problem of zero crossing of a GSP even for the Ising case, though only approximately. In 1-D, the correlator f (T ) of the underlying process can be computed exactly, f (T ) = 2 /(1 + exp( 2 | T |(ref. )) 4) and in higher dimensions, it can be obtained numerically as the solution of a closed differential equation. By expanding around, T = 0, we find that in all dimensions, α= 1 and hence they represent non-smooth processes with infinite density of zero crossings. Hence, we cannot use IIA or series expansion result for θ. Also due to the lack of a small parameter, we cannot think of this process as ‘close’ to a Markov process and hence cannot use the perturbation result. However, since θ = E1 – E0 quite generally and since α= 1, we can use a variational approximation to estimate E1 and E0. We use as trial Hamiltonian that of a harmonic oscillator whose frequency λ is our tunable variational parameter4. We just mention the results here, the details can be found in Majumdar and Sire, and Sire et al.4. For example, in d = 1, we find θ ≈ 0.35 compared to the exact result θ = 3/8. In d = 2 and 3, we find θ ≈ 0.195 and 0.156. The exponent in 2-D has recently been measured experimentally9 in a liquid crystal system which has an effective Glauber dynamics and is in good agreement with our variational prediction. So far we have been discussing about the persistence of 374 a single spin in the Ising model11. This can be immediately generalized to the persistence of ‘global’ order parameter in the Ising model. For example, what is the probability that the total magnetization (sum of all the spins) does not change sign up to time t in the Ising model? It turns out that when quenched to zero temperature, this probability also decays as a power law with an exponent θg that is different from the single spin persistence exponent θ. For example, in 1-D, θg = 1/4 exactly11 as opposed to θ = 3/8 (ref. 2). A natural interpolation between the local and global persistence can be established via introducing the idea of ‘block’ persistence. The ‘block’ persistence is the probability p l(t) that a block of size l does not flip up to time t. As l increases from 0 to ∞, the exponent crosses over from its ‘local’ value θ to its ‘global’ value θg. When quenched to the critical temperature Tc of the Ising model, the local persistence decays exponentially with time due to the flips induced by thermal fluctuations but the ‘global’ persistence still decays algebraically, ~ t −θ c , where the exponent θc is a new non-equilibrium critical exponent11. It has been computed in mean field theory, in the n →∞ limit of the O(n) model, to first order in ε = 4 – d expansion11. Recently this epsilon expansion has been carried out to order ε 2 (ref. 12). Recently, the persistence of a single spin has also been generalized to persistence of ‘patterns’ in the zero temperature dynamics of 1-D Ising or more generally q-state Potts model. For example, the survival probability of a given ‘domain’ was found to decay algebraically in time as t −θ d where the q-dependent exponent θd(2) ≈ 0.126 (ref. (ref.~ 14), 14) for q = 2 (Ising case), different from θ = 3/8 and θ0 = 1/4. Also, the probability that a ‘domain’ wall has not encountered any other domain wall up to time t was found to decay as with yet another~ new t −θ1 exponent θ1(q), where θ1(2) = 1/2 and θ1(3) ≈ 0.72 (ref. 15). Thus, it seems that there is a whole hierarchy of nontrivial exponents associated with the decay of persistence of different patterns in phase ordering systems. Another direction of generalization has been to investigate the ‘residence time’ distribution, whose limiting behaviour determines the persistence exponent32. Consider the effective single-site stochastic process φ(t) discussed in this paper. Let r(t) denote the fraction of time the process φ(t) is positive (or negative) within time window [0, t]. The distribution f (r, t) of the random variable r is the residence time distribution. In the limits r → 0 or r → 1, this distribution is proportional to usual persistence. However, the full function f (r, t) obviously gives more detailed information about the process than its limiting behaviours. This quantity has been studied extensively for diffusion equation32,33, Ising model34, Le’vy processes35, interface models20 and generalized Gaussian Markov processes36. The various persistence probabilities in pure systems have recently been generalized to systems with disorder17. For example, what is the probability that a random walker in a random environment (such as in Sinai model) does not CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS cross the origin? Analytical predictions for the persistence in disordered environment have been made recently based on an asymptotically exact renormalization group approach17. Another important application of some of these persistence ideas, experimentally somewhat more relevant perhaps, is in the area of interface fluctuations18,19. The persistence in Gaussian interfaces such as the Edwards– Wilkinson model, the problem can again be mapped to a general GSP but with a non-Markovian correlator18. In this case, several upper and lower bounds have been obtained analytically18. For nonlinear interfaces of KPZ types, one has to mostly resort to numerical means19. The study of history dependence via persistence has provided some deeper insights into the problems of interface fluctuations19,20. On the experimental side, the persistence exponent has been measured in systems with breath figures8, soap bubbles10 and twisted nematic liquid crystal exhibiting planar Glauber dynamics9. It has also been noted recently37 that persistence exponent for diffusion equation may possibly be measured in dense spin-polarized noble gases (Helium-3 and Xenon-129) using NMR spectroscopy and imaging38. In these systems, the polarization acts like a diffusing field. With some modifications these systems may possibly also be used to measure the persistence of ‘patterns’ discussed in this paper. In conclusion, persistence is an interesting and challenging problem with many applications in the area of nonequilibrium statistical physics. Some aspects of the problem have been understood recently as reviewed here. But there still exist many questions and emerging new directions open to more theoretical and experimental efforts. 1. Derrida, B., Bray, A. J. and Godrèche, C., J. Phys. A, 1994, 27, L357; Stauffer, D., J. Phys. A, 1994, 27, 5029; Krapivsky, P. L., Ben-Naim, E. and Redner, S., Phys. Rev. E, 1994, 50, 2474. 2. Derrida, B., Hakim, V. and Pasquier, V., Phys. Rev. Lett., 1995, 75, 751 and J. Stat. Phys., 1996, 85, 763. 3. Bray, A. J., Derrida, B., and Godrèche, C., Europhys. Lett., 1994, 27, 175. 4. Majumdar, S. N. and Sire, C., Phys. Rev. Lett., 1996, 77, 1420; Sire, C., Majumdar, S. N. and Rudinger, A., Phys. Rev. E., condmat/9810136, (to appear). 5. Majumdar, S. N., Sire, C., Bray, A. J. and Cornell, S. J., Phys. Rev. Lett., 1996, 77, 2867; Derrida, B., Hakim, V. and Zeitak, R., ibid., 2871. 6. Majumdar, S. N. and Bray, A. J., Phys. Rev. Lett., 1998, 81, 2626. 7. Watson, A., Science, 1996, 274, 919. 8. Marcos-Martin, M., Beysens, D., Bouchaud, J-P, Godrèche, C. and Yekutieli, I., Physica, 1995, D214, 396. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 9. Yurke, B., Pargellis, A. N., Majumdar, S. N. and Sire, C., Phys. Rev. E, 1997, 56, R40. 10. Tam, W. Y., Zeitak, R., Szeto, K. Y. and Stavans, J., Phys. Rev. Lett., 1997, 78, 1588. 11. Majumdar, S. N., Bray, A. J., Cornell, S. J. and Sire, C., Phys. Rev. Lett., 1996, 77, 3704. 12. Oerding, K., Cornell, S. J. and Bray, A. J., Phys. Rev. E, 1997, 56, R25; Oerding, K. and van Wijland, F ., J. Phys. A, 1998, 31, 7011. 13. Cueille, S. and Sire, C., J. Phys. A, 1997, 30, L791; Euro. Phys. J. B, 1999, 7, 111. 14. Krapivsky, P. L. and Ben-Naim, E., Phys. Rev. E, 1998, 56, 3788. 15. Majumdar, S. N. and Cornell, S. J., Phys. Rev. E, 1998, 57, 3757. 16. Cardy, J., J. Phys. A, 1995, 28, L19; Ben-Naim, E., Phys. Rev. E, 1996, 53, 1566; Howard, M., J. Phys. A, 1996, 29, 3437; Monthus, C., Phys. Rev. E, 1996, 54, 4844. 17. Fisher, D. S., Le Doussal, P. and Monthus, C., Phys. Rev. Lett., 1998, 80, 3539; cond-mat/9811300; Le Doussal, P. and Monthus, C., cond-mat/9901306, (to appear). 18. Krug, J., Kallabis, H., Majumdar, S. N., Cornell, S. J., Bray, A. J. and Sire, C., Phys. Rev. E, 1997, 56, 2702. 19. Kallabis, H. and Krug, J., cond-mat/9809241, (to appear). 20. Toroczkai, Z., Newman, T. J. and Das Sarma, S., cond-mat/ 9810359, (to appear). 21. Frachebourg, L., Krapivsky, P. L. and Ben-Naim, E., Phys. Rev. Lett., 1996, 77, 2125; Phys. Rev. E, 1996, 54, 6186. 22. Swift, M. R. and Bray, A. J., cond-mat/9811422, (to appear). 23. Feller, W., Introduction to Probability Theory and its Applications, Wiley, New York, 3rd edn, 1968, vol. 1. 24. Slepian, D., Bell Syst. Tech. J., 1962, 41, 463. 25. Wang, M. C. and Uhlenbeck, G. E., Rev. Mod. Phys., 1945, 17, 323. 26. Sinai, Y. G., Theor. Math. Phys., 1992, 90, 219. 27. Burkhardt, T . W., J. Phys. A, 1993, 26, L1157. 28. Rice, S. O., Bell Syst. Tech. J., 1944, 23, 282; 1945, 24, 46. 29. Kac, M., SIAM Rev., 1962, 4, 1; Blake, I. F. and Lindsey, W. C., IEEE Trans. Inf. Theory, 1973, 19, 295. 30. Bendat J. S., Principles and Applications of Random Noise Theory, Wiley, New York, 1958. 31. Mazenko, G. F., Phys. Rev. Lett., 1989, 63, 1605. 32. Dornic, I. and Godrèche, C., J. Phys. A, 1998, 31, 5413. 33. Newman, T. J. and Toroczkai, Z., Phys. Rev. E, 1998, 58, R2685. 34. Drouffe , J-M. and Godrèche, C., cond-mat/9808153, (to appear). 35. Baldassarri, A., Bouchaud, J. P., Dornic, I. and Godrèche, C., cond-mat/9805212, (to appear). 36. Dhar, A. and Majumdar, S. N., Phys. Rev. E., condmat/9902004, (to appear). 37. Walsworth , R. L. (private communication). 38. Tseng, C. H., Peled, S., Nascimben, L., Oteiza, E., Walsworth, R. L. and Jolesz, F. A., J. Magn. Reson., Ser. B, (to appear). ACKNOWLEDGEMENTS. I thank my collaborators C. Sire, A. J. Bray, S. J. Cornell, J. Krug, H. Kallabis, B. Yurke, A. Pargellis and A. Dhar. I also thank D. Dhar for many valuable suggestions and discussions. I am grateful to M. Barma, B. Derrida and C. Godrèche for useful discussions and to CNRS, Universite’ Paul Sabatier for hospitality where the whole series of work began. 375 SPECIAL SECTION: Kinetics of phase ordering Sanjay Puri School of Physical Sciences, Jawaharlal Nehru University, New Delhi 110 067, India We briefly review our current understanding of phase ordering kinetics, viz. the far-from-equilibrium evolution of a homogeneous two-phase mixture which has been rendered thermodynamically unstable by a rapid change in parameters. In particular, we emphasize the large number of unsolved problems in this area. THERE now exists a good understanding of phase transitions in physical systems. It has long been known that a particular physical system (e.g. water) can exist in more than one phase (e.g. vapour, liquid or solid) depending upon values of external parameters (e.g. pressure, temperature). In statistical physics, one formulates microscopic or macroscopic models for such systems, which have different states as free-energy minima in different regions of the phase diagram. Calculations with these models are not necessarily straightforward but there are few conceptual hurdles left in understanding the static aspects of phase transitions. Recent attention has turned to the dynamics of phase transitions, and this article provides an overview of a particularly important problem in this area. We will consider the evolution of a homogeneous two-phase mixture which has been rendered thermodynamically unstable by a sudden change in parameters. The evolution of the homogeneous system towards its new equilibrium state is referred to as ‘phase ordering dynamics’ and has been the subject of intense experimental, numerical and theoretical investigation1. In this article, we focus upon the successes and outstanding challenges of research in this area. This article is organized as follows. There are two prototypical problems of phase ordering dynamics. The ordering of a ferromagnet or evolution with a nonconserved order parameter is discussed first. The phase separation of a binary mixture or evolution with a conserved order parameter is discussed next. Then, we briefly discuss future directions for studies of phase ordering dynamics. H = −J ∑ Si S j 〈 i, j〉 − h∑ Si , S i = ± 1, (1) i where S i is the z-component of the spin at site i. We consider the simplest case of a two-state spin so that S i = ± 1 in dimensionless units. In eq. (1), J(> 0) is the strength of the exchange interaction which makes it energetically preferable for neighbouring spins to align parallel; and h is a magnetic field pointing along the zdirection. The notation Σ refers to a sum over nearest〈 i, j 〉 neighbour pairs. The Ising model in eq. (1) has been a paradigm for understanding phase transitions in a ferromagnet. With minimal effort (using mean-field theory2), we can obtain qualitative features of the phase diagram. Figure 1 shows the spontaneous magnetization M as a function of temperature T for a ferromagnet in zero magnetic field (h = 0). Of course, various behaviours around the critical point (T = Tc , h c = 0) are not captured correctly in meanfield theory, but that will not concern us here. We are interested in the following dynamical problem. A disordered ferromagnet at temperature TI > Tc is rapidly cooled to a temperature TF < Tc . Clearly, the ferromagnet would now be in equilibrium in a spontaneously-magnetized state, with spins pointing either ‘up’ or ‘down’. This is our first prototypical phase ordering problem, i.e. the far-fromequilibrium evolution of the disordered initial condition to the ordered final state. The appropriate order parameter Case with nonconserved order parameter Consider a ferromagnet, which is an assembly of atoms with residual spin angular momentum. Due to an exchange interaction, spins at neighbouring sites tend to align parallel to each other. This is encapsulated in the simple Ising Hamiltonian defined on a lattice: e-mail: puri@jnuniv.ernet.in 376 Figure 1. Spontaneous magnetization M as a function of temperature T for a ferromagnet in zero field (h = 0). We consider temperature quenches from TI > Tc to TF < Tc at time t = 0. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS which labels the state of the system is the spontaneous magnetization, which takes a value 0 in the disordered state; and ± M0 in the ordered state. There is no constraint on the evolution of the order parameter with time – hence, this evolution is referred to as the case with nonconserved order parameter. To obtain a dynamical model for this evolution, we again consider the Ising model. Unfortunately, this model has no intrinsic dynamics, as is seen by constructing the appropriate Poisson bracket. This problem is circumvented by introducing a stochastic kinetics, which is presumed to result from thermal fluctuations of a heat-bath at temperature T. The simplest nonconserved kinetics is the so-called Glauber spin-flip kinetics, where a randomlychosen spin is flipped as S i → – S i. The change in configuration is accepted with a probability which must satisfy the detailed balance condition3. This condition ensures that the system evolves towards statistical equilibrium. The Ising model, in conjunction with Glauber spin-flip kinetics, constitutes a reasonable microscopic model for phase ordering dynamics with a nonconserved order parameter. We can obtain an equivalent model at the macroscopic ρ level, in terms of a continuum magnetization field ψ( r , t ). This field is obtained by coarse-graining the microscopic ρ spins, with r and t being space and time variables. The appropriate dynamical equation for nonconserved ordering is the time-dependent Ginzburg–Landau (TDGL) equation or Model A (ref. 4): ρ ρ ∂ψ( r , t) δF [ψ( r , t )] ρ = −L + σ( r , t ), ρ ∂t δψ( r , t ) (2) where L is an Onsager coefficient. The free-energy ρ functional F [ψ(r , t)] is usually taken to be of the form: ρ ρ a ρ b ρ F [ψ( r , t )] = ∫ d r ψ(r , t ) 2 + ψ( r , t ) 4 4 2 ρ ρ K ρ − h ψ( r , t ) + [ ∇ψ( r , t )] 2 , 2 (3) where a ∝ (T – Tc ), b, h and K are phenomenological ρ constants. The Gaussian white noise σ(r , t) in eq. (2) must be chosen to satisfy the fluctuation–dissipation relation. Eq. (2) can be interpreted in either of two ways. Firstly, it can be thought of as a generalized Newton’s equation in the overdamped limit with ψ as ‘coordinates’; F [ψ] as the ‘potential’; and L–1 as the ‘friction constant’. Secondly, at a more formal level, it can be obtained from a master equation formulation for the Ising model with spin-flip kinetics3. Though all our statements are in the context of an ordering ferromagnet, it should be stressed that the above modelling is applicable to a wide range of physical systems, with appropriate changes in nomenclature and/or generalizations of the Hamiltonian or free-energy functional. Furthermore, in most phase ordering problems, thermal CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 noise is asymptotically irrelevant and the ordering dynamics is governed by a zero-temperature fixed point. At an intuitive level, this can be understood as follows. Essentially, thermal fluctuations affect only the interfaces between domains and have no effect on the bulk domain structure. However, the interfacial structure is asymptotically irrelevant in comparison with the growing domain length scale. Thus, thermal noise does not alter the asymptotic behaviour of phase ordering systems. Equations (2) and (3) are the starting points for most analytical studies of this problem, which have been reviewed by Bray1. Essentially, theoretical approaches assume that there are well-defined domains of ‘up’ and ‘down’ phases, with sharp interfaces between them. The dynamical evolution of these interfaces is governed by the local curvature. This interface-dynamics formulation was used by Ohta et al.5 (OJK) to obtain (a) the growth law for the characteristic domain size L(t) ~ t1/2; and (b) the dynamical-scaling form for the time-dependent correlation function ρ ρ ρ ρ r G ( r , t) = 〈ψ( R, t )ψ( R + r , t) 〉 ≡ g . L (t ) (4) In eq. (4), the angular brackets denote an average over initial conditions and thermal fluctuations; and g(x) is a time-independent master function, which characterizes the domain morphology of the evolving system. In physical terms, the dynamical-scaling property reflects the fact that the coarsening morphology is self-similar in time. Thus, the only change with time is in the scale of the morphology. The experimentally relevant quantity inρ ordering systems is the structure factor which is S (the k , t ), Fourier transform ρ of G (r , t). Scattering experiments on phase ordering systems give an amplitude proportional to the structure factor. An important extension of the OJK result is due to Oono and Puri6, who incorporated the nonuniversal effects of nonzero interfacial thickness into the analytical form for the correlation function. This extension was of considerable experimental and numerical relevance because the nonzero interfacial thickness has a severe impact on the tail of the structure factor. ρ The vector version of the TDGL equation, with ψ(r , t) ρ ρ replaced by an n-component vector ψ(r , t), is also of great experimental relevance. For example, the n = 2 case (dynamical XY model) is relevant in the ordering of superconductors, superfluids and liquid crystals. The n = 3 case (dynamical Heisenberg model) is also of relevance in the ordering of liquid crystals; and even in the evolution dynamics of the early universe!! Bray and Puri7 and (independently) Toyoki8 have used a defect-dynamics approach to solve the ordering problem for the ncomponent TDGL equation in d-dimensional space for arbitrary n and d (with n ≤ d). They have demonstrated that the characteristic length scale L(t) ~ t1/2 in this case also. 377 Σ SPECIAL SECTION: i Furthermore, they also obtained an explicit scaling form for the correlation function. The analytical results of Bray and Puri7 and Toyoki8 have stimulated much experimental and numerical work. We should stress that the case with n > d is unusual in that there are no topological defects, and it is not possible to characterize the evolution of the system in terms of the annealing of ‘defects’. To date, there are no general analytical results available for the case of the n-component TDGL equation with n > d. Thus, it would be fair to say that we have a good understanding of phase ordering dynamics in the nonconserved case. However, we should stress that the defect-dynamics approach discussed above is essentially mean-field like and valid only when d → ∞. There are important corrections in the finite-dimensional case, which we do not yet clearly understand. Nevertheless, most researchers in this area would agree that the nonconserved problem is ‘well understood’. Perhaps this optimistic evaluation is a result of comparison with the rather bleak picture which emerges when we consider the dynamics of phase separation. Case with conserved order parameter Consider next a binary mixture of atoms A and B, with similar atoms attracting and dissimilar atoms repelling each other. This is a fairly ubiquitous situation in metallurgy and materials science. Again, we assume that the system is defined on a lattice, whose sites are occupied by either Aor B-atoms; and there are NA(NB) atoms of A(B). We further assume that there are only nearest-neighbour interactions, as in the case of a ferromagnet. Then, we can formulate a Hamiltonian for the binary mixture as follows: H = εAA ∑ niA n Aj + εBB ∑ niB n Bj 〈 i, j 〉 + ε AB ∑ 〈 i, j 〉 〈i , j 〉 ( n iA n Bj + n iB n Aj ), (5) where we have introduced occupation-number variables n αi = 1 or 0, depending on whether or not a site i is occupied by an α-atom. The quantities εAA and εBB (both less than 0) refer to the attractive energy of an A–A and B–B pair, respectively. The quantity εAB (> 0) refers to the repulsive energy of an A–B pair. It is straightforward to transform the Hamiltonian in eq. (5) into the Ising model by introducing spin variables S i = + 1 or – 1 if site i is occupied by A or B, respectively. Clearly, n Ai = (1 + S i)/2 and n Bi = (1 – S i)/2, which transforms the Hamiltonian in eq. (5) into the Ising Hamiltonian of eq. (1) (ref. 2). Again, it is simple to perform a mean-field calculation with this Hamiltonian but one has to work in a ‘fixed-magnetization’ ensemble, as S i = NA – NB is fixed by the composition of the mixture. The phase diagram for a 378 symmetric binary mixture is shown in Figure 2. There is a high-temperature disordered phase, where A and B are homogeneously mixed; and a low-temperature ordered phase, where A and B prefer to phase separate. The corresponding dynamical problem considers a homogeneous binary mixture in the one-phase region, which is rendered thermodynamically unstable by a rapid quench below the coexistence curve. This is our second prototypical phase ordering problem and pictures of the resultant evolution will be shown later. The appropriate order parameter in this case is the local density difference ρ ρ ρ ρ ψ( r , t) =ρA ( r , t) – ρB ( r , t) , where ρα ( r , t) denotes the ρ density of species α at point r at time t. In contrast to the ordering dynamics of the ferromagnet, the order parameter evolution in this case must satisfy a local conservation constraint as phase separation proceeds by the diffusion of A- and B-atoms. Hence, this evolution is said to be characterized by a conserved order parameter. Typically, the coarsening dynamics proceeds via the slow process of evaporation of A-rich (or B-rich) domains; diffusion of this material through domains rich in the other component B (or A); and condensation on A-rich (or B-rich) domains elsewhere. A reasonable microscopic model for phase separation associates a suitable stochastic kinetic process with the Ising model, as before. The simplest conserved kinetics is the Kawasaki spin-exchange process, which interchanges spins at neighbouring sites. This simple model has been the basis of Monte Carlo (MC) simulations of phase separation dynamics. We can also formulate a phenomenological model for the ρ dynamical evolution of the order parameter ψ( r , t ), which is the local density difference of the two species. The freeenergy functional in eq. (3) is still reasonable as it corresponds to a coarse-grained description of the Ising model. Currents are set up in the phase-separating system ρ due to gradients in the chemical potential µ( r , t) as follows: ρ ρ ρ ρ ρ ρ J ( r , t ) = − M (ψ)∇ µ(r , t ) + η( r , t) ρ ρ δF [ψ( r , t )] ρ ρ = − M (ψ)∇ ρ + η( r , t) . δψ( r , t) (6) In eq. (6), M(ψ) is the mobility and we have introduced a ρ ρ vector Gaussian white noise η( r , t) , which models thermal fluctuations in the current. The evolution of the order parameter is obtained from the continuity equation as (7) CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 ∂ψ( r , t) ∂t ρ = −∇ ⋅ J ( r , t) ρ ρ ρ δF [ψ( r , t )] ρ ρ ρ = −∇ ⋅ M (ψ) ∇ ρ − ∇ ⋅ η( r , t) . δψ( r , t) SYSTEMS NONEQUILIBRIUM STATISTICAL Equation (7) is well known in the literature as the Cahn– Hilliard–Cook (CHC) equation (or Model B (ref. 4)) and describes phase separation in binary mixtures when hydrodynamic effects are not relevant, e.g. binary alloys. For binary fluid mixtures, hydrodynamic effects play a crucial role and eq. (7) has to be coupled with the Navier– Stokes equation for the fluid velocity field – the extended model is described by the Kawasaki equations and is referred to as Model H (ref. 4). There have been numerous experimental studies of phase separation in binary alloys and binary fluid mixtures1,9,10. These studies found that there is a growing characteristic domain length scale L(t), which asymptotically exhibits a power-law behaviour in time, i.e. L(t) ~ tφ, where φ is the growth exponent. The value of the exponent is φ= 1/3 for binary alloys9; and φ= 1 for binary fluids10. These experiments have also investigated the scaling form for the structure factor and its various features, which we do not enumerate here. There have also been many numerical studies of phase separation in binary mixtures (alloys or fluids) and these are in agreement with the experimental results quoted above. The most extensive simulations to date are due to Shinozaki and Oono11, who used the coarse-grained Cell Dynamical System models developed earlier by Oono and Puri12. However, it is not the purpose of this article to review the numerous experimental and numerical results in this field. Rather, we would like to focus on the current analytical understanding of the phase separation problem. It is relatively easy to analytically obtain the growth exponents for phase-separating binary alloys and fluids1. However, there has been only limited progress in developing a good theory for the scaling form of the correlation function or Figure 2. Phase diagram of a binary mixture AB in the (c, T )plane, where c refers to the concentration of (say) A. We consider quenches from the one-phase (disordered) region to the two-phase (ordered) region. There are two different possibilities for the evolution of the system. If A and B are present in approximately equal proportions (cf. quench labelled as ‘u’), the system is spontaneously unstable and segregates via ‘spinodal decomposition’. If one of the components is present in a much larger fraction (cf. quench labelled as ‘m’), the mixture separates via ‘nucleation and growth’ of critical droplets. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 structure factor. Typically, approaches based on interface dynamics have not worked well in the conserved case because of the long-range correlations between movements of interfaces. Sadly enough, the most complete analytical work in this context is still the classic work of Lifshitz and Slyozov13, who considered the limiting case of phase separation in binary alloys when one of the components is present in a vanishingly small fraction. Therefore, unlike the nonconserved case, there remain many challenging analytical problems in understanding domain growth in the conserved case!! We understand various limiting behaviours of the scaled structure factor for the conserved problem, but there is still no comprehensive theory which gives the entire structure factor. Future directions We have discussed in some detail the two prototypical problems of phase ordering dynamics, viz. the nonconserved and conserved cases. These two simple problems provide the launch-pad for a range of further studies, as we will briefly elucidate here. Recall that the earlier discussions were in the context of pure and isotropic systems. Of course, real experimental systems are neither pure nor isotropic. Recent research in this area has attempted to incorporate and study various experimentally relevant effects in phase ordering systems. In what follows, we discuss some of these recent directions. Phase ordering systems typically contain disorder, either quenched or annealed. Quenched (or immobile) disorder is in the form of large impurities, which act as pinning centres for domain interfaces. Thus, the coarsening of domains is driven by a curvature-reduction mechanism only for a transient period. This is followed by a crossover to a regime in which domains can grow only by thermally-activated hopping over disorder traps. The presence of quenched disorder drastically changes the nature of the asymptotic domain growth law, but does not appreciably alter the domain morphology of the evolving system14. Domain growth with quenched disorder has received considerable attention in the literature and there are still many issues to be clarified in this context. Another class of important problems concerns the role of annealed (or mobile) disorder. Let us consider two particularly important classes of annealed disorder, viz. surfactants and vacancies. Surfactants are amphiphilic molecules which reduce the surface tension between two immiscible fluids (e.g. oil and water) and promote mixing. Consider a phase-separating binary fluid with a small concentration of surfactants. (This would constitute a ternary or three-component mixture.) Typically, the surfactants migrate rapidly to interfacial regions – diminishing the surface tension and, thereby, the drive to segregate. Thus, a binary fluid with surfactants can exhibit a range of fascinating meso-scale structures15. Vacancies in binary alloys also play a similar role as surfactants16. However, we should stress that phase separation in binary 379 SPECIAL SECTION: should stress that phase separation in binary alloys is mediated by vacancies rather than direct A–B interchanges. Therefore, vacancies are necessary for the phase separation of binary alloys and are not just a complicating feature in the phase diagram!! At a coarse-grained level, phase ordering in ternary mixtures is described in terms of coupled dynamical equations for two conserved order parameters, referred to as Model D (ref. 4). We could also consider the problem of ordering of a ferromagnet with vacancies and this would be described by coupled dynamical equations for one nonconserved order parameter (i.e. spontaneous magnetization) and one conserved order parameter (i.e. atom-vacancy density-difference field). These equations are referred to as Model C in the classification of Hohenberg and Halperin4. Next, we consider the role of anisotropies in phase ordering systems. Many interesting physical situations give rise to anisotropic phase ordering dynamics. Thus, anisotropy can result from external fields, e.g. originating from a surface with a preferential attraction for one of the components of a phase-separating binary mixture. We have studied the fascinating dynamical interplay of two timedependent phenomena in this problem, viz. dynamics of surface wetting by the preferred component; and dynamics of phase separation in the bulk17. Figure 3 shows an example of a numerical simulation of ‘surface-directed phase separation’. Anisotropies in phase ordering systems can result from internal fields also. In our earlier discussion, we have referred to phase separation in binary alloys as a realization of the CHC equation. This is a gross over-simplification of the actual situation. In real binary alloys, strain fields are invariably set up at interfaces between A-rich and B-rich domains due to lattice parameter mismatches. These longranged strain fields strongly affect the intermediate and late stages of phase separation in binary alloys, inducing Figure 3. Dynamics of phase separation of a binary mixture AB in the presence of a surface with a preferential attraction for one of the components (say, A). These evolution pictures were obtained from the numerical solution of a 2-dimensional version of the appropriate dynamical equations (Puri and Frisch17 ). The surface is located at Z = 0; and the system size was LX × LZ ≡ 400 × 300. We show snapshots for dimensionless times 30, 90, 900 and 9000. The A-rich and B-rich regions are denoted by black and white, respectively. There are three distinct regions: (i) the bulk region (Z large), where one has usual bulk phase separation; (ii) the surface region (Z ~ – 0), where there is a growing wetting layer; and (iii) the region between the bulk and surface regions, which is of maximum interest to us in the present context. 380 CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS various anisotropies18. The examples quoted above merely constitute the tip of the iceberg. There are a large number of experimentally relevant effects in phase ordering systems (e.g. gravity, viscoelasticity, shear flows, chemical reactions, etc.), which are presently being investigated by various groups worldwide. As yet, we do not even have a comprehensive experimental or numerical understanding of the asymptotic behaviour of phase ordering dynamics in most of the above situations – leave alone an analytical understanding. The field of phase ordering dynamics continues to be a fascinating realization of far-from-equilibrium statistical mechanics, and promises to be so for many years to come. 1. For reviews, see Binder, K., in Materials Science and Technology: Phase Transformations of Materials (eds Cahn, R. W., Haasen, P. and Kramer, E. J.) VCH, Weinheim, 1991, vol. 5, p. 405; Bray, A. J., Adv. Phys., 1994, 43, 357. 2. Plischke, M. and Bergersen, B., Equilibrium Statistical Physics, Prentice–Hall, New Jersey, 1989. 3. Kawasaki, K., in Phase Transitions and Critical Phenomena (eds Domb, C. and Green, M. S.), Academic Press, New York, 1972, vol. 2, p. 443 and references therein. 4. Hohenberg, P. C. and Halperin, B. I., Rev. Mod. Phys., 1977, 49, 435. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 5. Ohta, T., Jasnow, D. and Kawasaki, K., Phys. Rev. Lett., 1982, 49, 1223. 6. Oono, Y. and Puri, S., Mod. Phys. Lett. B, 1988, 2, 861. 7. Bray, A. J. and Puri, S., Phys. Rev. Lett., 1991, 67, 2670. 8. Toyoki, H., Phys. Rev. B, 1992, 45, 1965. 9. For example, see Gaulin, B. D., Spooner, S. and Morii, Y., Phys. Rev. Lett., 1987, 59, 668; Malik, A., Sandy, A. R., Lurio, L. B., Stephenson, G. B., Mochrie, S. G. J., McNulty, I. and Sutton, M., Phys. Rev. Lett., 1998, 81, 5832. 10. For example, see Wong, N. C. and Knobler, C. M., Phys. Rev. A, 1981, 24, 3205; Tanaka, H., J. Chem. Phys., 1996, 105, 10099. 11. Shinozaki, A. and Oono, Y., Phys. Rev. E, 1993, 48, 2622. 12. Oono, Y. and Puri, S., Phys. Rev. Lett., 1987, 58, 836; Phys. Rev. A, 1988, 38, 434; Puri, S. and Oono, Y., Phys. Rev. A, 1988, 38, 1542. 13. Lifshitz, I. M. and Slyozov, V. V., J. Phys. Chem. Solids, 1961, 19, 35. 14. Puri, S., Chowdhury, D. and Parekh, N., J. Phys. A, 1991, 24, L1087; Gyure, M. F., Harrington, S. T., Strilka, R. and Stanley, H. E., Phys. Rev. E, 1995, 52, 4632. 15. For reviews, see Chowdhury, D., J. Phys. Condens. Matter, 1994, 6, 2435; Kawakatsu, T., Kawasaki, K., Furusaka, M., Okabayashi, H. and Kanaya, T., J. Phys. Condens. Matter, 1994, 6, 6385. 16. Puri, S., Phys. Rev. E, 1997, 55, 1752; Puri, S. and Sharma, R., Phys. Rev. E, 1998, 57, 1873. 17. For a review of experimental results, see Krausch, G., Mater. Sci. Eng. Rep., 1995, R14, 1; For a review of modelling and numerical simulations, see Puri, S. and Frisch, H. L., J. Phys. Condens. Matter, 1997, 9, 2109. 18. Onuki, A. and Nishimori, H., Phys. Rev. B, 1991, 43, 13649; Sagui, C., Somoza, A. M. and Desai, R. C., Phys. Rev. E, 1994, 50, 4865. 381 SPECIAL SECTION: Arrested states of solids Madan Rao*† and Surajit Sengupta**,§ *Raman Research Institute, C.V. Raman Avenue, Sadashivanagar, Bangalore 560 080, India **Material Science Division, Indira Gandhi Center for Atomic Research, Kalpakkam 603 102, India § Current address: Institut für Physik, Johannes Gutenberg Universität Mainz, 55099 Mainz, Germany Solids produced as a result of a fast quench across a freezing or a structural transition get stuck in long-lived metastable configurations of distinct morphology, sensitively dependent on the processing history. Martensites are particularly well-studied examples of nonequilibrium solid–solid transformations. Since there are some excellent reviews on the subject, we shall, in this brief article, mainly present our viewpoint. Nonequilibrium structures in solids What determines the final microstructure of a solid under changes of temperature or pressure? This is a complex issue, since a rigid solid finds it difficult to flow along its free energy landscape to settle into a unique equilibrium configuration. Solids often get stuck in long-lived metastable or jammed states because the energy barriers that need to be surmounted in order to get unstuck are much larger than kBT. Such nonequilibrium solid structures may be obtained either by quenching from the liquid phase across a freezing transition (see Caroli et al.1 for a comprehensive review), or by cooling from the solid phase across a structural transition. Unlike the former, nonequilibrium structures resulting from structural transformations do not seem to have attracted much attention amongst physicists, apart from Barsch et al.2 and Gooding et al.3, possibly because the microstructures and mechanical properties obtained appear nongeneric and sensitively dependent on details of processing history. Metallurgical studies have however classified some of the more generic nonequilibrium microstructures obtained in solid (parent/austenite)–solid (product/ferrite) transformations depending on the kind of shape change and the mobility of atoms. To cite a few: • Martensites are the result of solid state transformations involving shear and no atomic transport. Martensites occur in a wide variety of alloys, polymeric solids and ceramics, and exhibit very distinct plate-like structures built from twinned variants of the product. • Bainites are similar to martensites, but in addition possess a small concentration of impurities (e.g. carbon in iron) which diffuse and preferentially dissolve in the † On leave of absence from Intitute of Mathematical Sciences, CIT Campus, Taramani, Chennai 600 113, India. *For correspondence. (e-mail: madan@rri.ernet.in) 382 parent phase. • Widmanstätten ferrites result from structural transformations involving shape changes and are accompanied by short-range atomic diffusion. • Pearlites are an eutectic mixture of bcc Fe and the carbide consisting of alternating stripes. • Amorphous alloys, a result of a fast quench, typically possess some short range ordering of atoms. • Polycrystalline materials of the product phase are a result of a slower quench across a structural transition and display macroscopic regions of ordered configurations of atoms separated by grain boundaries. That the morphology of a solid depends on the detailed dynamics across a solid–solid transformation, has been recognized by metallurgists who routinely use time– temperature–transformation (TTT) diagrams to determine heat treatment schedules. The TTT diagram is a family of curves parametrized by a fraction δ of transformed product. Each curve is a plot of the time required to obtain δ versus temperature of the quench (Figure 1). The TTT curves for an alloy of fixed composition may be viewed as a ‘kinetic phase diagram’. For example, starting from a hot alloy at Figure 1. TTT curves 11 for steel AISI 1090 (0.84%C + 0.60% Mn). A: austenite (fcc), F: ferrite (bcc), C: carbide (Fe3 C). Curves correspond to 0, 50 and 100% transformation. Below a temperature Ms, the metastable martensite (M) is formed – the transformation curves for martensites are horizontal. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS t = 0 equilibrated above the transition temperature (upper left corner) one could, depending on the quench rate (obtained from the slope of a line T(t)), avoid the nose of the curve and go directly into the martensitic region or obtain a mixture of ferrite and carbide when cooled slowly. It appears from these studies that several qualitative features of the kinetics and morphology of microstructures are common to a wide variety of materials. This would suggest that there must be a set of general principles underlying such nonequilibrium solid–solid transformations. Since most of the microstructures exhibit features at length scales ranging from 100 Å to 100 µm, it seems reasonable to describe the phenomenon at the mesoscopic scale, wherein the solid is treated as a continuum. Such a coarse-grained description would ignore atomic details and instead involve effective continuum theories based on symmetry principles, conservation laws and broken symmetry. Let us state the general problem in its simplest context. Consider a solid state phase diagram exhibiting two different equilibrium crystalline phases separated by a first order boundary (Figure 2). An adiabatically slow quench from Tin → Tfin across the phase boundary in which the cooling rate is so small that at any instant the solid is in equilibrium corresponding to the instantaneous temperature would clearly result in an equilibrium final product at Tfin. On the other hand, an instantaneous quench would result in a metastable product bearing some specific relation to the parent phase. The task is to develop a nonequilibrium theory of solid state transformations which would relate the nature of the final arrested state and the dynamics leading to it to the type of structural change, the quench rate and the mobility of atoms. In this article, we concentrate on the dynamical and structural features of a class of solid–solid transformations called Martensites. Because of its commercial importance, martensitic transformations are a well-studied field in metallurgy and materials science. Several classic review articles and books discuss various aspects of martensites in great detail4. The growing literature on the subject is a clear indication that the dynamics of solid state transformations is still not well understood. We would like to take this opportunity to present, for discussion and criticism, our point of view on this very complex area of nonequilibrium physics 5,6. We next review the phenomenology of martensites and highlight generic features that need to be explained by a nonequilibrium theory of solid state transformations. nucleates a grain of the ferrite which grows isotropically, leading to a polycrystalline bcc solid. A faster quench from Tin > Tc to Tfin < Ms < Tc (where Ms: martensite start temperature) instead produces a rapidly transformed metastable phase called the martensite, preempting the formation of the equilibrium ferrite. It is believed that martensites form by a process of heterogeneous nucleation. On nucleation, martensite ‘plates’ grow radially with a constant front velocity ~ 105 cm/s, comparable to the speed of sound. Since the transformation is not accompanied by the diffusion of atoms, either in the parent or the product, it is called a diffusionless transformation. Electron microscopy reveals that each plate consists of an alternating array of twinned or slipped bcc regions of size ≈ 100 Å. Such martensites are called acicular martensites. The plates grow to a size of approximately 1 µm before they collide with other plates and stop. Most often the nucleation of plates is athermal; the amount of martensite nucleated at any temperature is independent of time. This implies that there is always some retained fcc, partitioned by martensite plates. Optical micrographs reveal that the jammed plates lie along specific directions known as habit planes. Martensites, characterized by such a configuration of jammed plates, are long lived since the elastic energy barriers for reorganization are much larger than kBT. A theoretical analysis of the dynamics of the martensitic transformation in Fe–C is complicated by the fact that the deformation is 3-dimensional (Bain strain) with 3 twin variants of the bcc phase. Alloys like In–Tl, In–Pb and Mn– Fe however, offer the simplest examples of martensitic transformations having only two twin variants. In–Tl alloys undergo a tetragonal to orthorhombic transformation when cooled below 72°C (ref. 2). The orthorhombic phase can be obtained from the tetragonal phase by a two-dimensional deformation, essentially a square to rhombus transition. Experiments indicate that all along the kinetic pathway, the local configurations can be obtained from a twodimensional deformation of the tetragonal cell. This would imply that the movement of atoms is strongly anisotropic and confined to the ab-plane. Thus as far as the physics of this transformation is concerned, the ab-planes are in perfect registry (no variation of the strain along the c-axis). In the next two sections we shall discuss our work on the dynamics of the square to a rhombus transformation in 2-dimensions using a molecular dynamics simulation and a coarse-grained mode coupling theory. Phenomenology of martensites One of the most studied alloys undergoing martensitic transformations is iron–carbon4. As the temperature is reduced, Fe with less than 0.02%C undergoes an equilibrium structural transition (Figure 2) from fcc (austenite) to bcc (ferrite) at Tc = 910°C. An adiabatic cooling across Tc CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 Figure 2. Phase diagram of Fe–C (weight per cent of C < 0.02%). Ms is the martensite start temperature. 383 SPECIAL SECTION: Molecular dynamics simulation of solid–solid transformations Our aim in this will be to study the simplest molecular dynamics (MD) simulation of the square to rhombus transformation. We would like to use the simulation results to construct the complete set of coarse grained variables needed in a continuum description of the dynamics of solid state tranformations. We carry out the MD simulation in the constant NVT ensemble using a Nosé–Hoover thermostat (N = 12000)7. Our MD simulation is to be thought of as a ‘coarsegrained’ MD simulation, where the effective potential is a result of a complicated many-body interaction. One part of the interaction is a purely repulsive two-body potential V2(rij) = v 2/r1i 2j , where rij is the distance between particles i and j. The two-body interaction favours a triangular lattice ground state. In addition, triplets of particles interact via a short-range three-body potential V3(ri, rj, rk ) = v 3w(rij, rjk, rik) [sin2 (4θijk) + sin2 (4θjki) + sin2 (4θkij)], where w(r) is a smooth short-range function and θijk is the bond angle at j between particles (ijk). Since V3 is minimized when θijk = 0 or π/2, the three-body term favours a square lattice ground state. Thus at sufficiently low temperatures, we can induce a square to triangular lattice transformation by tuning v 3. The phase diagram in the T – v 3 plane is shown in Figure 3. We define elastic variables, coarse-grained over a spatial block of size ξ and a time interval τ, from the instantaneous positions u of the particles. These include the deformation tensor ∂u i/∂xk , the full nonlinear strain εij, and the vacancy field φ= ρ – ρ (ρ = coarse-grained local density, ρ = average density). We have kept track of the time dependence of these coarse-grained fields during the MD simulation. Consider two ‘quench’ scenarios – a high and low temperature quench (upper and lower arrows in Figure 3 respectively) across the phase boundary. In both cases the solid is initially at equilibrium in the square phase. The high temperature quench across the phase boundary, induces a homogeneous nucleation (i.e. strain inhomogeneities created by thermal fluctuations are sufficient to induce critical nucleation) and growth of a triangular region. The product nucleus grows isotropically with the size R ~ t1/2. A plot of the vacancy/interstitial fields shows that, at these temperatures they diffuse fast to their equilibrium value (vacancy diffusion obeys an Arrenhius form Dv = D0 exp (– A/kBT ), where A is an activation energy, and so is larger at higher temperatures). The final morphology is a polycrystalline triangular solid. The low temperature quench on the other hand, needs defects (either vacancies or dislocations) to seed nucleation in an appreciable time. This heterogeneous nucleation initiates an embryo of triangular phase, which grows anisotropically along specific directions (Figure 4). Two aspects are immediately apparent, the growing nucleus is twinned and the front velocities are high. Indeed, the velocity of the front is a constant and roughly half the velocity of longitudinal sound. A plot of the vacancy/interstitial field shows a high concentration at the parent–product interface. The vacancy field now diffuses very slowly and so appears to get stuck to the interface over the time scale of the simulation. If we force the vacancies and interstitials to annihilate each other, then the anisotropic twinned nucleus changes in the course of time to an isotropic untwinned one! Therefore the lessons from the MD simulation are: (i) There are two scenarios of nucleation of a product in a parent depending on the temperature of quench. The product grows via homogeneous nucleation at high T, and via heterogeneous nucleation at low T. (ii) The complete set of slow variables necessary to describe the nucleation of solid–solid transformations should include the strain tensor and defects (vacancies and dislocations) which are generated at the parent–product interface at the onset of nucleation. (iii) The relaxation times of these defects dictate the final morphology. At high temperatures the defects relax fast and the grains grow isotropically with a diffusive front. The final morphology is a polycrystalline triangular solid. At low temperatures, the interfacial defects (vacancies) created by the nucleating grain relax slowly and get stuck at the parent–product interface. The grains grow anisotropically along specific directions. The critical nucleus is twinned and the front grows ballistically (with a velocity comparable to the sound speed). The final morphology is a twinned martensite. Mode coupling theory of solid–solid transformations v3 Figure 3. T–v 3 phase diagram from the MD simulations showing the freezing and structural transitions. The upper and lower arrows correspond to the high and low temperature quenches, respectively. 384 CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS Figure 4. MD snapshot of (a) the nucleating grain at some intermediate time initiated by the low temperature quench across the square– triangle transition. The dark (white) region is the triangular (square) phase, respectively. Notice that the nucleus is twinned and highly anisotropic. (b) The vacancy (white)/interstitial (black) density profile at the same time as a. Notice that the vacancies and interstitials are well separated and cluster around the parent–product interface. Armed with the lessons from the MD simulation, let us now construct a continuum elastic theory of solid-state nucleation. The analysis follows in part the theories of Krumhansl et al.2, but has important points of departure. The procedure is to define a coarse grained free energy functional in terms of all the relevant ‘slow’ variables. From the simulation results, we found that every configuration is described in terms of the local (nonsingular) strain field εij, the vacancy field φ, and singular defect fields like the dislocation density b ij. These variables are essentially related to the phase and amplitudes of the density wave describing the solid {ρG }. It is clear from the simulation that the strain tensor, defined with respect to the ideal parent, gets to be of O(1) in the interfacial region between the parent and the product. Thus we need to use the full nonlinear strain tensor εij = (∂iu j + ∂ju i + ∂iu k ∂ju k )/2. Further, since the strain is inhomogeneous during the nucleation process, the free energy functional should have derivatives of the strain tensor ∂k εij (this has unfortunately been termed ‘nonlocal strain’ by some authors). In general, the form of the free energy functional can be very complicated, but in the context of the square-torhombus transformation, the free energy density may be approximated by a simple form, f = c(∇ε)2 + ε2 – aε4 + ε6 + χvφ2 + χd b 2 + k d bε, (1) where ε is the nonzero component of the strain CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 corresponding to the transformation between a square and a rhombus, φ is the vacancy field and b is the (scalar) dislocation density. The tuning parameter a induces a transition from a square (described by ε = 0) to a rhombus (ε = ± e0). Starting with ε = 0 corresponding to the equilibrium square parent phase at a temperature T > Tc , we quench across the structural transition. The initial configuration of ε is now metastable at this lower temperature, and would decay towards the true equilibrium configuration by nucleating a small ‘droplet’ of the product. As we saw in the last section, as soon as a droplet of the product appears embedded in the parent matrix, atomic mismatch at the parent–product interface gives rise to interfacial defects like vacancies and dislocations. Let us confine ourselves to solids for which the energy cost of producing dislocations is prohibitively large. This would imply that the interfacial defects consist of only vacancies and interstitials. The dynamics of nucleation now written in terms of ε, g (the conserved momentum density) and vacancy φare complicated5. For the present purpose, all we need to realize is that φ couples to the strain and is diffusive with a diffusion coefficient Dv depending on temperature. As in the MD simulation, we find that the morphology and growth of the droplet of the product depends critically on the diffusion of these vacancies. If the temperature of quench is high, φdiffuses to zero before the critical nucleus 385 SPECIAL SECTION: size is attained and the nucleus eventually grows into an equilibrium (or polycrystalline) triangular solid. In this case, the nucleus grows isotropically with R ~ t1/2. However, a quench to lower temperatures results in a low vacancy diffusion coefficient. In the limit Dv → 0, the φ-field remains frozen at the moving parent–product interface. In this case, a constrained variational calculation of the morphology of the nucleus shows that it is energetically favourable to form a twinned martensite rather than a uniform triangular structure. The growth of the twinned nucleus is not isotropic, but along habit planes. Lastly, the growth along the longer direction is ballistic with a velocity proportional to (χv)1/2 (of the order of the sound velocity). All these results are consistent with the results of the previous section and with martensite phenomenology. Let us try and understand in more physical terms, why the growing nucleus might want to form twins. As soon as a droplet of the triangular phase of dimension L is nucleated, it creates vacancies at the parent–product interface. The free energy of such an inclusion is F = Fbulk + Fpp + Fφ. The first term is simply the bulk free energy gain equal to ∆FL2, where ∆F is the free energy difference between the square and triangular phases. The next two terms are interfacial terms. Fpp is the elastic contribution to the parent–product interface coming from the gradient terms in the free energy density eq. (1), and is equal to 4σppL, where σpp is the surface tension at the parent–product interface. Fφ is the contribution from the interfacial vacancy field glued to the parent–product interface and is proportional to φ2 ~ L2 (since the atomic mismatch should scale with the amount of parent–product interface). This last contribution dominates at large L setting a prohibitive price to the growth of the triangular nucleus. The solid gets around this by nucleating a twin with a strain opposite to the one initially nucleated, thereby reducing φ. Indeed for an equal size twin, φ→ 0 on the average, and leads to a much lower interfacial energy Fφ ~ L. However, the solid now pays the price of having created an additional twin interface whose energy cost is Ftw = σtwL. Considering now an (in general) anisotropic inclusion of length L, width W consisting of N twins, the free energy calculation goes as F = ∆FLW + σpp(L + W) + σtw NW + β(L/N)2Ν, (2) where the last term is the vacancy contribution. Minimization with respect to N gives L/N ~ W1/2, a relation that is well known for 2-dimensional martensites like In–Tl. Our next task is to solve the coupled dynamical equations with appropriate initial conditions numerically, to obtain the full morphology phase diagram as a function of the type of structural change, the parameters entering the free energy functional and kinetic parameters like Dv. It should be mentioned that our theory takes off from the 386 theories of Krumhansl et al.2, in that we write the elastic energy in terms of the nonlinear strain tensor and its derivatives. In addition, we have shown that the process of creating a solid nucleus in a parent generates interfacial defects which evolve in time. The importance of defects has been stressed by a few metallurgists8. We note also that the parent–product interface is studded with an array of vacancies with a separation equal to the twin size. This implies that the strain decays exponentially from the interface over a distance of order L/N. This has been called ‘fringing field’2. They obtain this by imposing boundary conditions on the parent–product interface, whereas here it appears dynamically. Patterning in solid–solid tranformations: Growth and arrest So far we have discussed the nucleation and growth of single grains. This description is clearly valid at very early times, for as time progresses the grains grow to a size of approximately 1 µm and start colliding, whereupon in most alloys they stop. Optical micrographs of acicular martensites reveal that the jammed plates lie along habit planes that criss-cross and partition the surrounding fcc (parent) matrix. Can we quantify the patterning seen in martensite aggregates over a scale of a millimeter? A useful measure is the size distribution of the martensite grains embedded in a given volume of the parent. The appropriate (but difficult!) calculation at this stage would be the analogue of a Becker– Döring theory for nucleation in solids. In the absence of such a theory, we shall take a phenomenological approach. Clearly the size distribution P(l, t) depends on the spatiotemporal distribution I of nucleation sites and the growth velocity v. We have analysed the problem explicitly in a simple 2-dimensional context. Since the nucleating martensitic grains are highly anisotropic and grow along certain directions with a uniform velocity, a good approximation is to treat the grains as lines or rays. These rays (lines) emanate from nucleation sites along certain directions, and grow with a constant velocity v. The rays stop on meeting other rays and eventually after a time T, the 2-dimensional space is fragmented by N colliding rays. The size distribution of rays, expressed in terms of a scaling variable y = y(I, v), has two geometrical limits – the Γ -fixed point (at y = 0) and the L-fixed point (at y = ∞). The Γ -fixed point corresponds to the limit where the rays nucleate simultaneously with a uniform spatial distribution. The stationary distribution P(l) is a Gamma distribution with an exponentially decaying tail. The L-fixed point, corresponds to the limit where the rays are nucleated sequentially in time (and uniformly in space) and grow with infinite velocity. By mapping on to a multifragmentation problem, Ben Naim and Krapivsky9 were able to derive the exact asymptotic form for the moments of P(l) at the L-fixed point. The distribution CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS function P(l) has a multiscaling form, characterized by its moments 〈lq〉 ~ N –µ(q), where µ(q) = (q + 2 – (q 2 + 4)1/2)/2. At intermediate values of the scaling variable y, there is a smooth crossover from the Γ -fixed point to the L-fixed point with a kinematical crossover function and crossover exponents. The emergence of scale invariant microstructures in martensites as arising out of a competition between the nucleation rate and growth is a novel feature well worth experimental investigation. There have been similar suggestions in the literature, but as far as we know there have been no direct visualization studies of the microstructure of acicular martensites using optical micrographs. Recent acoustic emission experiments10 on the thermoelastic reversible martensite Cu–Zn–Al, may be argued to provide indirect support of the above claim5, but the theory of acoustic emission in martensites is not understood well enough to make such an assertion with any confidence. Open questions We hope this short review makes clear how far we are in our understanding of the dynamics of solid–solid transformations. A deeper understanding of the field will only come about with systematic experiments on carefully selected systems. For instance, a crucial feature of our nonequilibrium theory of martensitic transformations is the existence of a dynamical interfacial defect field. In conventional Fe based alloys, the martensitic front grows incredibly fast, making it difficult to test this using in situ transmission electron microscopy. Colloidal solutions of polysterene spheres (polyballs) however, are excellent systems for studying materials properties. Polyballs exhibiting fcc → bcc structural transitions have been seen to undergo twinned martensitic transformations. The length and time scales associated with colloids are large, making it comfortable to study these systems using light scattering and optical microscopy. In this article we have focused on a small part of the dynamics of solid state transformations, namely the dynamics and morphology of martensites. Even so our presentation here is far from complete and there are crucial unresolved questions that we need to address. Let us list the issues as they appear following a nucleation event. The physics of heterogeneous nucleation in solids is very poorly understood. For instance, it appears from our simulations that the morphology of the growing nucleus depends on the nature of the defects seeding the nucleation process (e.g. vacancies, dislocations and grain boundaries). In addition, several martensitic transformations are associated with correlated nucleation events and autocatalysis. Though these features are not central to the CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 issue of martensites, such a study would lead to a better understanding of the origins of athermal, isothermal and burst nucleation. This in conjunction with a ‘Becker–Döring theory’ for multiple martensite grains would be a first step towards the computation of TTT curves. We still do not understand the details of the dynamics of twinning and how subsequent twins are added to the growing nucleus. Moreover, the structure and dynamics of the parent–product interface and of the defects embedded in it have not been clearly analysed. It would be desirable to have a more complete theory which displays a morphology phase diagram (for a single nucleus) given the type of structural transition and the kinetic, thermal and elastic parameters. Certain new directions immediately suggest themselves. For instance, the role of carbon in interstitial alloys like Fe– C leading to the formation of bainites; the coupling of the strain to an external stress and the shape memory effect; tweed phases and pre-martensitic phenomena (role of quenched impurities). The study of the dynamics of solid–solid transformations and the resulting long-lived morphologies lies at the intersection of metallurgy, materials science and nonequilibrium statistical mechanics. The diversity of phenomena makes this an extremely challenging area of nonequilibrium physics. 1. Caroli, B., Caroli, C. and Roulet, B., in Solids Far from Equilibrium (ed. Godreche, C.), Cambridge University Press, 1992. 2. Barsch, G. R. and Krumhansl, J. A., Phys. Rev. Lett., 1974, 37, 9328; Barsch, G. R., Horovitz, B. and Krumhansl, J. A., Phys. Rev. Lett., 1987, 59, 1251. 3. Bales, G. S. and Gooding, R. J., Phys. Rev. Lett., 1991, 67, 3412; Reed, A. C. E. and Gooding, R. J., Phys. Rev., 1994, B50, 3588; van Zyl, B. P. and Gooding, R. J., http://xxx.lanl.gov/archive/cond-mat/9602109. 4. Roitburd, A., in Solid State Physics (eds Seitz and Turnbull), Academic Press, NY, 1958; Nishiyama, Z., Martensitic Transformation, Academic Press, NY, 1978; Kachaturyan, A. G., Theory of Structural Transformations in Solids, Wiley, NY, 1983; Martensite (eds Olson, G. B. and Owen, W. S.), ASM International, The Materials Information Society, 1992. 5. Rao, M. and Sengupta, S., Phys. Rev. Lett., 1997, 78, 2168; Rao, M. and Sengupta, S., lanl e-print: cond-mat/9709022; Rao, M. and Sengupta, S., IMSc preprint, 1998. 6. Rao, M., Sengupta, S. and Sahu, H. K., Phys. Rev. Lett., 1995, 75, 2164; Rao, M. and Sengupta, S., Phys. Rev. Lett., 1996, 76, 3235; Rao, M. and Sengupta, S., Physica A, 1996, 224, 403. 7. Sengupta, S. and Rao, M., to be published. 8. Olson, G. B. and Cohen, M., Acta Metall., 1979, 27, 1907; Olson, G. B., Acta Metall., 1981, 29, 1475; Christian, J. W., Metall. Trans. A, 1982, 13, 509. 9. Ben Naim, E. and Krapivsky, P., Phys. Rev. Lett., 1996, 76, 3235. 10. Vives, E. et al., Phys. Rev. Lett., 1994, 72, 1694. 11. Metals Handbook, ASM, Ohio, 9th edition, vol. 4, 1981. ACKNOWLEDGEMENT. We thank Yashodhan Hatwalne for a critical reading of the manuscript. 387 SPECIAL SECTION: Sandpile models of self-organized criticality S. S. Manna Laboratoire de Physique et Mecanique des Milieux Heterogenes, École Supérieure de Physique et de Chimie Industrielles, 10 rue Vauquelin, 75231 Paris Cedex 05, France and Satyendra Nath Bose National Centre for Basic Sciences, Block-JD, Sector-III, Salt Lake, Calcutta 700 091, India Self-organized criticality is the emergence of long-ranged spatio-temporal correlations in non-equilibrium steady states of slowly driven systems without fine tuning of any control parameter. Sandpiles were proposed as prototypical examples of self-organized criticality. However, only some of the laboratory experiments looking for the evidence of criticality in sandpiles have reported a positive outcome. On the other hand, a large number of theoretical models have been constructed that do show the existence of such a critical state. We discuss here some of the theoretical models as well as some experiments. THE concept of self-organized criticality (SOC) was introduced by Bak, Tang and Wiesenfeld (BTW) in 1987 (ref. 1). It says that there is a certain class of systems in nature whose members become critical under their own dynamical evolutions. An external agency drives the system by injecting some mass (in other examples, it could be the slope, energy or even local voids) into it. This starts a transport process within the system: Whenever the mass at some local region becomes too large, it is distributed to the neighbourhood by using some local relaxation rules. Globally, mass is transported by many such successive local relaxation events. In the language of sandpiles, these together constitute a burst of activity called an avalanche. If we start with an initial uncritical state, initially most of the avalanches are small, but the range of sizes of avalanches grows with time. After a long time, the system arrives at a critical state, in which the avalanches extend over all length and time scales. Customarily, critical states have measure zero in the phase space. However, with self-organizing dynamics, the system finds these states in polynomial times, irrespective of the initial state2–4. BTW used the example of a sandpile to illustrate their ideas about SOC. If a sandpile is formed on a horizontal circular base with any arbitrary initial distribution of sand grains, a sandpile of fixed conical shape (steady state) is formed by slowly adding sand grains one after another (external drive). The surface of the sandpile in the steady state, on the average, makes a constant angle known as the angle of repose, with the horizontal plane. Addition of each sand grain results in some activity on the surface of the pile: an avalanche of sand mass follows, which propagates on the surface of the sandpile. Avalanches are of many different sizes and BTW argued that they would have a e-mail: manna@boson.bose.res.in 388 power law distribution in the steady state. There are also some other naturally occurring phenomena which are considered to be examples of SOC. Slow creeping of tectonic plates against each other results in intermittent burst of stress release during earthquakes. The energy released is known to follow power law distributions as described by the well-known Gutenberg–Richter Law5. The phenomenon of earthquakes is being studied using SOC models6. River networks have been found to have fractal properties. Water flow causes erosion in river beds, which in turn changes the flow distribution in the network. It has been argued that the evolution of river pattern is a selforganized dynamical process7. Propagation of forest fires8 and biological evolution processes9 have also been suggested to be examples of SOC. Laboratory experiments on sandpiles, however, have not always found evidence of criticality in sandpiles. In the first experiment, the granular material was kept in a semicircular drum which was slowly rotated about the horizontal axis, thus slowly tilting the free surface of the pile. Grains fell vertically downward and were allowed to pass through the plates of a capacitor. Power spectrum analysis of the time series for the fluctuating capacitance however showed a broad peak, contrary to the expectation of a power law decay, from the SOC theory10. In a second experiment, sand was slowly dropped on to a horizontal circular disc, to form a conical pile in the steady state. On further addition of sand, avalanches were created on the surface of the pile, and the outflow statistics was recorded. The size of the avalanche was measured by the amount of sand mass that dropped out of the system. It was observed that the avalanche size distribution obeys a scaling behaviour for small piles. For large piles, however, scaling did not work very well. It was suggested that SOC behaviour is seen only for small sizes, and very large systems would not show SOC11. Another experiment used a pile of rice between two vertical glass plates separated by a small gap. Rice grains were slowly dropped on to the pile. Due to the anisotropy of grains, various packing configurations were observed. In the steady state, avalanches of moving rice grains refreshed the surface repeatedly. SOC behaviour was observed for grains of large aspect ratio, but not for the less elongated grains12. Theoretically, however, a large number of models have been proposed and studied. Most of these models study the system using cellular automata where discrete or CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS continuous variables are used for the heights of sand columns. Among them, the Abelian Sandpile Model (ASM) is the most popular1,13. Other models of SOC have been studied but will not be discussed here. These include the Zhang model which has modified rules for sandpile evolution14, a model for Abelian distributed processors and other stochastic rule models15, the Eulerian Walkers model16 and the Takayasu aggregation model17. In the ASM, we associate a non-negative integer variable h representing the height of the ‘sand column’ with every lattice site on a d-dimensional lattice (in general on any connected graph). One often starts with an arbitrary initial distribution of heights. Grains are added one at a time at randomly selected sites The O :sand h O →column h O + 1. at any arbitrary site i becomes unstable when h i exceeds a previously selected threshold value h c for the stability. Without loss of generality, one usually chooses h c = 2d –1. An unstable sand column always topples. In a toppling, the height is reduced as: h i → h i –2d and all the 2d neighbouring sites {j} gain a unit sand grain each: h j → h j + 1. This toppling may make some of the neighbouring sites unstable. Consequently, these sites will topple again, possibly making further neighbours unstable. In this way a cascade of topplings propagates, which finally terminates when all sites in the system become stable (Figure 1). One waits until this avalanche stops before adding the next grain. This is equivalent to assuming that the rate of adding sand is much slower than the natural rate of relaxation of the system. The wide separation of the ‘time scale of drive’ and ‘time scale of relaxation’ is common in many models of SOC. For instance, in earthquakes, the drive is the slow tectonic movement of continental plates, which occurs over a time scale of centuries, while the actual stress relaxation occurs in quakes, whose duration is only a few seconds. This separation of time scales is usually considered to be a defining characteristic of SOC. However, Dhar has argued that the wide separation of time scales should not be considered as a necessary condition for SOC in general4. Finally, the system must have an outlet, through which the grains go out of the system, which is absolutely necessary to attain a steady state. Most popularly, the outlet is chosen as the (d –1)-dimensional surface of a ddimensional hypercubic system. The beauty of the ASM is that the final stable height configuration of the system is independent of the sequence in which sand grains are added to the system to reach this stable configuration13. On a stable configuration C, if two grains are added, first at i and then at j, the resulting stable configuration C′ is exactly the same in case the grains were added first at j and then at i. In other sandpile models, where the stability of a sand column depends on the local slope or the local Laplacian, the dynamics is not Abelian, since toppling of one unstable site may convert another unstable site to a stable site (Figure 2). Many such rules have been studied in the literature18,19. An avalanche is a cascade of topplings of a number of sites created on the addition of a sand grain. The strength of an avalanche in general, is a measure of the effect of the external perturbation created due to the addition of the sand grain. Quantitatively, the strength of an avalanche is estimated in four different ways: (i) size (s): the total number topplings in the avalanche, (ii) area (a): the number of distinct sites which toppled, (iii) life-time (t): the duration of the avalanche, and (iv) radius (r): the maximum distance of a toppled site from the origin. These four different quantities are not independent and are related to each other by scaling laws. Between any two measures x, y ∈{s, a, t, r} one can define a mutual dependence as: 〈y〉 ~ xγ . These exponents are related to one another, e.g. γts = γtr γrs. For the ASM, it can be proved that the avalanche clusters cannot have any holes. It has been shown that γrs = 2 in two-dimensions. It has also been proved that γr t = 5/4 (ref. 21). A better way to estimate the γtx exponents is to average over the intermediate values of the size, area and radius at every intermediate time step during the growth of the avalanche. Quite generally, the finite size scaling form for the probability distribution function for any measure x ∈{s, a, t, r} is taken to be: xy Figure 2. Example to show that a directed slope model is nonAbelian. Two slopes are measured from any site (i, j) as h(i, j) – h(i, j + 1) and h(i, j) – h(i + 1, j + 1). If either of them is greater than Figure 1. Avalanche of the from Abelian Sandpile 1, two grains are transferred (i, j) and areModel, given generated one each on to a(i, j3+× 1) 3 and square lattice. graina is dropped a stable (i + 1, j + 1). AOnsand dropping grain on the on initial configuration site. two Thedifferent avalanche created has size configuration, at we the see central that finally height configuration sresult = 6, area a= 6, different life-time sequences t =24 and the r =20 . . due to two of radius topplings CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 389 SPECIAL SECTION: P(x) ~ x–τ x f x (x/Lσx). The exponent σx determines the variation of the cut-off of the quantity x with the system size L. Alternatively, sometimes it is helpful to consider the cumulative σx probability distribution F (x) = ∫xL P(x) dx which varies as x1–τ x . However, in the case of τx = 1, the variation should be in the form F (x) = C – log(x). Between any two measures, scaling relations like γxy = (τx –1)/(τy –1) exist. Recently, the scaling assumptions for the avalanche sizes have been questioned. It has been argued that there actually exists a multifractal distribution instead22. Numerical estimation for the exponents has yielded scattered values. For example estimates of the exponent τs range from 1.20 (ref. 18) to 1.27 (ref. 23) and 1.29 (ref. 24). We will now look into the structure of avalanches in more detail. A site i can topple more than once in the same avalanche. The set of its neighbouring sites {j}, can be divided into two subsets. Except at the origin O, where a grain is added from the outside, for a toppling, the site i must receive some grains from some of the neighbouring sites {j1} to exceed the threshold h c . These sites must have toppled before the site i. When the site i topples, it loses 2d grains to the neighbours, by giving back the grains it has received from {j1}, and also donating grains to the other neighbours {j2}. Some of these neighbours may topple later, which returns grains to the site i and its height h i is raised. The following possibilities may arise: (i) some sites of {j2} may not topple at all; then the site i will never re-topple and is a singly toppled site on the surface of the avalanche. (ii) all sites in {j2} topple, but no site in {j1} topples again; then i will be a singly toppled site, surrounded by singly toppled sites. (iii) all sites in {j2} topple, and some sites of {j1} retopple; then i will remain a singly toppled site, adjacent to the doubly toppled sites. (iv) all sites in {j2} topple, and all sites of {j1} re-topple; then the site i must be a doubly toppled site. This implies that the set of at least doubly toppled sites must be surrounded by the set of singly toppled sites. Arguing in a similar way will reveal that sites which toppled at least n times, must be a subset and also are surrounded by the set of sites which toppled at least (n –1) times. Finally, there will be a central region in the avalanche, where all sites have toppled a maximum of m times. The origin of the avalanche O where the sand grain was dropped, must be a site in this maximum toppled zone. Also, the origin must be at the boundary of this mth zone, since otherwise it should have toppled (m + 1) times25. Using this idea, we see that the boundary sites on any arbitrary system can topple at most once in any arbitrary number of avalanches. Similar restrictions are true for inner sites also. A (2n + 1) × (2n + 1) square lattice can be divided into (n + 1) subsets which are concentric squares. Sites on the mth such square from the boundary can topple at most m times, whereas the central site cannot topple more than n 390 times in any avalanche. Avalanches can also be decomposed in a different way, using Waves of Toppling. Suppose, on a stable configuration C a sand grain is added at the site O. The site is toppled once, but is not allowed to topple for the second time, till all other sites become stable. This is called the first wave. It may happen that after the first wave, the site O is stable; in that case the avalanche has terminated. If the O is still unstable, it is toppled for the second time and all other sites are allowed to become stable again; this is called the second wave, and so on. It was shown, that in a sample where all waves occur with equal weights, the probability of occurrence of a wave of area a is D(a) ~ 1/a (ref. 26). It is known that the stable height configurations in ASM are of two types: Recurrent configurations appear only in the steady state with uniform probabilities, whereas Transient configurations occur in the steady state with zero probability. Since long-range correlations appear only in the steady states, it implies that the recurrent configurations are correlated. This correlation is manifested by the fact that certain clusters of connected sites with some specific distributions of heights never appear in any recurrent configuration. Such clusters are called the forbidden subconfigurations. It is easy to show that two zero heights at the neighbouring sites: (0–0) or, an unit height with two zero heights at its two sides: (0–1–0) never occur in the steady state. There are also many more forbidden sub-configurations of bigger sizes. An L × L lattice is a graph, which has all the sites and all the nearest neighbour edges (bonds). A Spanning tree is a connected sub-graph having all sites but no loops. Therefore, between any pair of sites there exists an unique path through a sequence of bonds. There can be many possible Spanning trees on a lattice. These trees have interesting statistics in a sample where they are equally likely. Suppose we randomly select such a tree and then randomly select one of the unoccupied bonds and occupy it, it forms a loop of length l . It has been shown that these loops have the length distribution D(l ) ~ l –8/5. Similarly, if a bond of a Spanning tree is randomly selected and deleted, then it divides into two fragments. The sizes of the two fragments generated follow a probability distribution D(a) ~ a –11/8 (ref. 27). It was also shown that every recurrent configuration of the ASM on an arbitrary lattice has a one-to-one correspondence to a random Spanning tree graph on the same lattice. Therefore, there are exactly the same number of distinct Spanning trees as the number of recurrent ASM configurations on any arbitrary lattice21. Given a stable height configuration, there exists an unique prescription to obtain the equivalent Spanning tree. This is called the Burning method21. A fire front, initially at every site outside the boundary, gradually penetrates (burns) into the system using a deterministic rule. The paths of the fire front constitute the Spanning tree. A fully burnt system is recurrent, otherwise it is transient (Figure 3). CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS Suppose, addition of a grain at the site O of a stable recurrent configuration C, leads to another stable configuration C′. Is it possible to get back the configuration C knowing C′ and the position of O ? This is done by Inverse toppling28. Since C′ is recurrent, a corresponding Spanning tree ST(C′) exists. Now, one grain at O is taken out from C′ and the configuration C″ = C′ – δO j is obtained. This means on ST(C′), one bond is deleted at O and it is divided into two fragments. Therefore one cannot burn the configuration C″completely since the resulting tree has a hole consisting of at least the sites of the smaller fragment. This implies that C″ has a forbidden sub-configuration (F1) a b c Figure 3. a, An example of the height distribution in a recurrent configuration C ′ on a 24 × 24 square lattice. This configuration is obtained by dropping a grain a some previous configuration C at the encircled site; b, The spanning tree representation of the configuration C ′; c, A new configuration C ″ is obtained by taking out one grain at the encircled site from the configuration C ′. A spanning tree cannot be obtained for C ″. The bonds of the spanning tree corresonding to the forbidden sub-configuration in C ″ are shown by the thin lines. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 391 SPECIAL SECTION: of equal size and C″ is not recurrent. On (F1), one runs the inverse toppling process: 4 grains are added to each site i, and one grain each is taken out from all its neighbours {j}. The cluster of f1 sites in F1 is called the first inverse avalanche. The lattice is burnt again. If it still has a forbidden sub-configuration (F2), another inverse toppling process is executed, and is called the second inverse avalanche. The size of the avalanche is: s = f1 + f2 + f3 + . . ., and f1 is related to the maximum toppled zone of the avalanche. From the statistics of random spanning trees27 it is clear that f1 should have the same statistics of the two fragments of the tree generated on deleting one bond. Therefore, the maximum toppled zone also has a power law distribution of the size, D(a) ~ a –11/8. Sandpile models with stochastic evolution rules have also been studied. The simplest of these is a two-state sandpile model. A stable configuration of this system consists of sites, either vacant or occupied by at most one grain. If there are two or more grains at a site at the same time we say there is a collision. In this case, all grains at that site are moved. Each grain chooses a randomly selected site from the neighbours and is moved to that site. The avalanche size is the total number of collisions in an avalanche. From the numerical simulations, the distribution of avalanche sizes is found to follow a power law, characterized by an exponent τs ≈ 1.27 (ref. 29). This twostate model has a nontrivial dynamics even in onedimension30. Recently, it has been shown that instead of moving all grains, if only two grains are moved randomly leaving others at the site, the dynamics is Abelian31. Some other stochastic models also have nontrivial critical behaviour in one dimension. To model the dynamics of rice piles, Christensen et al.32 studied the following slope model. On a one-dimensional lattice of length L, non-negative integer variable h i represents the height of the sand column at the site i. The local slope zi = h i – h i + 1 is defined, maintaining zero height on the right boundary. Grains are added only at the left boundary i = 1. Addition of one grain h i → h i + 1 implies an increase in the slope zi → zi + 1. If at any site, the local slope exceeeds a pre-assigned threshold value zci , one grain is transferred from the column at i to the column at (i + 1). This implies a change in the local slope as: zi → zi – 2 and zi ± 1 → zi ± 1+ 1. The thresholds of the instability zci are dynamical variables and are randomly chosen between 1 and 2 in each toppling. Numerically, the avalanche sizes are found to follow a power law distribution with an exponent τs ≈ 1.55 and the cutoff exponent was found to be σs ≈ 2.25. This model is referred as the Oslo model. Addition of one grain at a time, and allowing the system to relax to its stable state, implies a zero rate of driving of the system. What happens when the driving rate is finite? Corral and Paczuski studied the Oslo model in the situation of nonzero flow rate. Grains were added at a rate r, i.e. at every (1/r) time updates, one grain is dropped at the left boundary i = 1. They observed a dynamical transition 392 separating intermittent and continuous flows33. Many different versions of the sandpile model have been studied. However the precise classification of various models in different universality classes in terms of their critical exponents is not yet available and still attracts much attention18,19. Exact values of the critical exponents of the most widely studied ASM are still not known in twodimensions. Some effort has also been made towards the analytical calculation of avalanche size exponents34–36. Numerical studies for these exponents are found to give scattered values. On the other hand, the two-state sandpile model is believed to be better behaved and there is good agreement of numerical values of its exponents by different investigators. However, whether the ASM and the twostate model belong to the same universality class or not is still an unsettled question37. If a real sandpile is to be modelled in terms of any of these sandpile models or their modifications, it must be a slope model, rather than a height model. However, not much work has been done to study the slope models of sandpiles18,19. Another old question is whether the conservation of the grain number in the toppling rules is a necessary condition to obtain a critical state. It has been shown already that too much non-conservation leads to avalanches of characteristic sizes36. However, if grains are taken out of the system slowly, the system is found to be critical in some situations. A non-conservative version of the ASM with directional bias shows a mean field type critical behaviour39. Therefore, the detailed role of the conservation of the grain numbers during the topplings is still an open question. 1. Bak, P., Tang, C. and Wiesenfeld, K., Phys. Rev. Lett., 1987, 59, 381; Phys. Rev. A, 1988, 38, 364. 2. Bak, P., How Nature Works: The Science of Self-Organized Criticality, Copernicus, New York, 1996. 3. Jensen, H. J., Self-Organized Criticality, Cambridge University Press, 1998. 4. Dhar, D., Physica A, 1999, 263, 4. 5. Gutenberg, B. and Richter, C. F., Ann. Geophys., 1956, 9, 1. 6. Bak, P. and Tang, C., J. Geophys. Res., 1989, 94, 15635; Carlson, J. M. and Langer, J. S., Phys. Rev. Lett., 1989, 62, 2632; Sornette, A. and Sornette, D., Europhys. Lett., 1989, 9, 197; Olami, Z., Feder, H. J. S. and Christensen, K., Phys. Rev. Lett., 1992, 68, 1244. 7. Takayasu, H. and Inaoka, H., Phys. Rev. Lett., 1992, 68, 966; Rinaldo, A., Rodriguez-Iturbe, I., Rigon, R., Ijjasz-Vasquez, E. and Bras, R. L., Phys. Rev. Lett., 1993, 70, 822; Manna, S. S. and Subramanian, B., Phys. Rev. Lett., 1996, 76, 3460. 8. Bak, P. and Chen, K., Physica D, 1989, 38, 5; Drossel B. and Schwabl, F., Phys. Rev. Lett., 1992, 69, 1629; Drossel, B., Clar, S. and Schwabl, F., ibid. 1993, 71, 3739; Grassberger, P., J. Phys. A, 1993, 26, 2081. 9. Bak, P. and Sneppen, K., 1993, 71, 4083. 10. Jaeger, H. M., Liu C-H and Nagel, S. R., Phys. Rev. Lett., 1989, 62, 40. 11. Held, G. A., Solina II, D. H., Keane, D. T., Haag, W. J., Horn, P. M. and Grinstein, G., Phys. Rev. Lett., 1990, 65, 1120. 12. Frette, V., Christensen, K., Malte-Sorensen, A., Feder, J., Josang, T. and Meakin, P., Nature, 1996, 379, 49. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS 13. 14. 15. 16. 17. 18. 19. 20. 21. 22. 23. 24. 25. 26. 27. 28. 29. 30. Dhar, D., Phys. Rev. Lett., 1990, 64, 1613. Zhang, Y.C., Phys. Rev. Lett., 1989, 63, 470. Dhar, D., Physica A, 1999, 263, 4. Priezzhenv, V. B., Dhar, A., Krishnamurthy, S. and Dhar, D., Phys. Rev. Lett., 1996, 77, 5079. Takayasu, H., Phys. Rev. Lett., 1989, 63, 2563; Takayasu, H., Nishikawa, I. and Tasaki, H., Phys. Rev. A, 1988, 37, 3110. Manna, S. S., Physica A, 1991, 179, 249. Kadanoff, L. P., Nagel, S. R., Wu L. and Zhou, S., Phys. Rev. A, 1989, 39, 6524. Manna, S. S., preprint, 1999, (to appear). Majumdar, S. N. and Dhar, D., Physica A, 1992, 185, 129. Tebaldi, C., Menech, M. D. and Stella, A. L., cond-mat/9903270 (to appear). Chessa, A., Stanley, H. E., Vespignani, A. and Zapperi, S., Phys. Rev. E, 1999, 59, R12. Lubeck, S. and Usadel, K. D., Phys. Rev. E, 1997, 55, 4095. Grassberger, G-M P. and Manna, S. S., J. Phys. (France), 1990, 51, 1077. Ivashkevich, E. V., Ktitarev, D. V. and Priezzhev, V. B., Physica A, 1994, 209, 347; J. Phys. A, 1994, 27, L585. Manna, S. S., Dhar, D. and Majumdar, S. N., Phys. Rev. A, 1992, 46, R4471. Dhar, D. and Manna, S. S., Phys. Rev. E, 1994, 49, 2684,. Manna, S. S., J. Phys. A, 1992, 24, L363. Priezzhev, V. B. and Sneppen, K., Phys. Rev. E, 1998, 58, CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 6959,. 31. Dhar, D., Proceedings of Statphys-Calcutta III, Physica A., (to appear). 32. Christensen, K., Corral, A., Frette, V., Feder, J. and Jossang, T., Phys. Rev. Lett., 1996, 77, 107. 33. Corral, A. and Paczuski, M., cond-mat preprint 9903157, (to appear). 34. Priezzhev, V. B., Ktitarev, D. V. and Ivashkevitch, E. V., Phys. Rev. Lett., 1996, 76, 2093. 35. Paczuski, M. and Boettcher, S., cond-mat/9705174, (to appear). 36. Ktitarev, D. V. and Priezzhev, V. B., Phys. Rev. E, 1998, 58, 2883,. 37. Vespignani, A., Zapperi, S. and Pietronero, L., Phys. Rev. Lett., 1994, 72, 1690; Phys. Rev. E, 1995, 51, 1711; Ben-Hur, A. and Biham, O., Phys. Rev. E, 1996, 53, R1317; Nakanishi, H. and Sneppen, K., Phys. Rev. E, 1997, 55, 4012. 38. Manna, S. S., Kiss, L. B. and Kertesz, J., J. Stat. Phys., 1990, 61, 923. 39. Manna, S. S., Chakrabarti, A. and Cafiero, R., preprint, (to appear). ACKNOWLEDGEMENTS. We thank D. Dhar for a critical reading of the manuscript and for useful comments. 393 SPECIAL SECTION: Nonequilibrium growth problems Sutapa Mukherji* and Somendra M. Bhattacharjee†§ *Department of Physics and Meteorology, Indian Institute of Technology, Kharagpur 721 302, India † Institute of Physics, Bhubaneswar 751 005, India We discuss the features of nonequilibrium growth problems, their scaling description and their differences from equilibrium problems. The emphasis is on the Kardar–Parisi–Zhang equation and the renormalization group point of view. Some of the recent developments along these lines are mentioned. HOW to characterize the degree of roughness of a surface as it grows and how the roughness varies in time have evolved into an important topic due to diverse interests in physics, biology, chemistry and in technological applications. One crucial aspect of these nonequilibrium growth processes is the scale invariance of surface fluctuations similar to the scale invariance observed in equilibrium critical point phenomena. Although different kinds of growths may be governed by distinct natural processes, they share a common feature that the surface, crudely speaking, looks similar under any magnification and at various times. This nonequilibrium generalization of scaling involving space and time (called ‘dynamic scaling’) makes this subject of growth problems important in statistical mechanics. Growth problems are both of near-equilibrium and nonequilibrium varieties. Therefore, they provide us with a fertile ground to study the differences and the extra features that might emerge in a nonequilibrium situation1,2. Take for example the case of crystal growth. In equilibrium, entropic contributions generally lead to a rough or fluctuating surface, an effect called thermal roughening, but, for crystals, because of the lattice periodicity a roughening transition from a smooth to rough surface occurs at some temperature. The nature of the growth of a crystal close to equilibrium expectedly depends on whether the surface is smooth or rough. One can also think of a crystal growth process which is far away from equilibrium by subjecting it to an external drive, for instance by random deposition of particles on the surface. The roughening that occurs in the nonequilibrium case is called kinetic roughening. Is the nature of the surface any different in kinetic roughening? Crystals are definitely not the only example of growth processes; some other examples of such nonequilibrium growths would be the growth of bacterial colonies in a petri dish, sedimentation of colloids in a drop, the formation of clouds in the upper atmosphere, and so on. Note the large variation of length scales of these problems. § For correspondence. (e-mail: somen@polymer.iopb.res.in) 394 In many such examples, it is difficult if not impossible to think of an equilibrium counterpart. Scale invariance in interface fluctuations implies that fluctuations look statistically the same when viewed at different length scales. A quantitative measure of the height fluctuation (height measured from an arbitrary base) is provided by the correlation function C(x, t) = 〈[h(x + x0, t + t0) – h(x0, t0)]2〉, (1) where x and t denote the d-dimensional coordinate on the substrate and time, respectively. The averaging in eq. (1) is over all x0, and, by definition, C(x, t) is independent of the choice of the arbitrary base. In simple language, scale invariance then means that when the system is, say, amplified by a scaling x → bx and t → b zt, the height fluctuations reveal the same features as the original, up to an overall scale factor. Quantitatively, there exists a generalized scaling C(x, t) = b –2χC(bx, b zt), (2) where b is a scale factor, and χ and z are known as the roughening and dynamic exponents which are also universal. As a direct consequence of eq. (2), a scaling form for C(x, t) can be obtained by choosing b = 1/x C(x, t) = x2χ Ĉ (t/xz), (3) a form that also explains the origin of the name ‘dynamic exponent’ for z. The power law behaviour (as opposed to say exponential decay) of the correlation function implies absence of any scale, neither in space nor in time. All the underlying length scales required to define the problem dropped out of the leading behaviour in eq. (3). Such a scale invariance is one of the most important features of equilibrium phase transitions and is observed when a parameter, say the temperature, approaches its critical value. However, here there is no special tuning parameter; the scale invariance appears from the interplay of competing processes which in the simplest case can be the surface tension and noise present due to inherent randomness in the growth. There can be, of course, more complex events like a phase transition between surfaces with different roughness but scale invariance (not only of the correlation function but of any physical quantity) is generically preserved in all these surfaces. It is worth emphasizing the enormous simplification that CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS occurs in the scaling description. It is only a very few quantities that define the asymptotic behaviour of the system. Consequently, the idea of studying the universal aspects of growth processes is to classify and characterize the various universality classes as determined by the exponents, e.g. χ and z, the scaling function and if necessary certain other important universal quantities. At this point, it might be helpful to compare the equilibrium and nonequilibrium cases again. In equilibrium, thanks to thermal energy (or ‘random kicks’ from a heat reservoir), all configurations of a system are accessible and do occur, but no net flow of probability between any two states is expected (called ‘detailed balance’). Consequently, the knowledge of the states (and the energies) of a system allows one to obtain the thermodynamic free energy by summing over the Boltzmann factors exp(– E/kBT ), where E is the energy of the state, T the temperature and kB is the Boltzmann constant. In a nonequilibrium situation, either or both of the above two conditions may be violated, and the framework of predicting the properties of a system from free energy is not necessarily available. A dynamic formulation is needed. By assigning a time-dependent probability for the system to be in a configuration at a particular time, one may study the time evolution of the probability. The equilibrium problem can be viewed from a dynamical point also. This description must give back the Boltzmann distribution in the infinite time steady state limit. This is the Fokker–Planck approach. The probabilistic description comes from the ensemble picture where identical copies of the same system exchange energy with the bath independently. An alternative approach which finds easy generalization to the nonequilibrium cases is the Langevin approach where one describes the time evolution of the degrees of freedom, in our example h(x, t), taking care of the random exchange of energy by a noise. The dynamics we would consider is dissipative so that the system in absence of any noise would tend to a steady state. However, for it to reach the equilibrium Boltzmann distribution in the presence of noise, it is clear that the noise must satisfy certain conditions (Einstein relation) connecting it to the system parameters. The nonequilibrium case does not have any thermodynamic free energy as a guiding light and therefore, there is no requirement to reach the Boltzmann distribution. In the Langevin approach, the noise term can be completely independent. In the equilibrium case, the Langevin equation will be determined by the Hamiltonian or the free energy of the system, but for nonequilibrium cases there might be terms which cannot be obtained from Hamiltonians. Since for t → ∞, the probability distribution for equilibrium cases attains the Boltzmann distribution, the roughness exponent χ is determined even in dynamics by the stationary state while the details of the dynamics is encoded in the dynamic exponent z. In other words, the two exponents χ and z are independent quantities. In the nonequilibrium case, there is no compulsion to reach any predetermined stationary state CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 and therefore the surface roughness is related to the growth, i.e. χ and z need not be independent. We see below that there is in fact a specific relation connecting these two exponents. The existence of scale invariance and universal exponents implies that as far as the exponents are concerned, the theory should be insensitive to the microscopic details, or, in other words, one may integrate out all the small length scale features. The universal exponents come out as an output of this process of coarse graining of say the Langevin equation, followed by a length rescaling that brings the system back to its original form. The new system will however have different values of the parameters and one can study the flow of these parameters in the long length and time scale limit. This is the basic idea behind the renormalization group (RG). In this approach, the importance of an interaction or a term is judged not by its numerical value but by its relevance. One may start with any physically possible process in dynamics and see how it appears as the length scale or resolution changes. For large length scales, one is left only with the relevant terms that grow with length, and marginal terms that do not change; the irrelevant terms or interactions that decay with length scale automatically drop out from the theory. The exponents are determined at the fixed points of the flows in the parameter space. These fixed points, which remain invariant under renormalization, characterize the macroscopic or asymptotic behaviour of the system. Clearly from this viewpoint of RG, one can explain why the microscopic details can be ignored and how the idea of ‘universality’ emerges. All systems whose dynamical behaviour would flow to the same fixed point under RG transformation will have identical scaling behaviour. The various universality classes can then be associated with the various fixed points of RG transformations, and phase transitions or criticality with unstable fixed points or special flows in the parameter space. An RG approach therefore seems rather natural and well suited for studying any scale invariant phenomena in general, and growth problems in particular. Quite expectedly, the modern approach to growth problems is based on these views of RG. For a quantitative discussion, we consider two simple equations that, from the historical point of view, played a crucial role in the development of the subject in the last two decades. A simple Langevin equation describing the dynamics of a surface is the Edwards–Wilkinson (EW) equation3 ∂h = ν∇ 2 h + η( x, t), ∂t (4) where x represents in general the coordinate on the ddimensional substrate. ν is the coefficient of the diffusion term trying to smoothen the surface and η is the Langevin noise which tries to roughen the surface3. One may add a constant current c to the right hand side, but by going over to a moving frame of reference (h → h + ct) one recovers eq. 395 SPECIAL SECTION: (4). The noise here is chosen to have zero mean and shortrange correlation as 〈η(x, t)η(x′,t′)〉 = 2Dδ(x –x′) δ(t – t′). One of the important assumptions in this equation is that the surface is single-valued and there are no overhangs. One can solve eq. (4) exactly just by taking the Fourier transform and obtain the exponents χ = (2 –d)/2 and z = 2. That the dynamic exponent z is 2 follows from the simple fact that the equation involves a first derivative in time but a second derivative in space. The surface is logarithmically rough at d = 2. For d > 2, fluctuations in the height are bounded and such a surface is more or less flat, better called ‘asymptotically flat’. From the growth equation one can also derive the stationary probability distribution for the height h(x) which takes the form of a Boltzmann factor P(h(x)) ∝ exp[– (ν/D)∫(∇h)2d dx] resembling an equilibrium system at a temperature given by D = kBT. This is the Einstein relation that noise should satisfy to recover equilibrium probability distribution. Conversely, given a hamiltonian of the form ∫(∇h)2d dx, the equilibrium dynamics will be given by eq. (4) with D determined by the temperature. Nevertheless, if we do not ascribe any thermal meaning to D, eq. (4) is good enough to describe a nonequilibrium dynamic process as well. Such a nonequilibrium growth will have many similarities with equilibrium processes, differing only in the origin of the noise, e.g. the expected symmetry h → – h, with 〈h〉 = 0 in equilibrium will be preserved in the nonequilibrium case also. The growing Ĉ surface with a correlation C(x, t) = | x |(2 – d)/2 (t/| x |2) will be similar in both cases for d > 2. A genuine nonequilibrium process will involve breaking the up-down symmetry which in equilibrium follows from detailed balance. It should therefore be represented by a term involving even powers of h. We already saw that a constant current (zeroth power) does not add anything new. Since the origin in space or time or the position of the basal plane should not matter, the first possible term is (∇h)2. By looking at the geometry of a rough surface, it is easy to see that such a term implies a lateral growth that would happen if a deposited particle sticks to the first particle it touches on the surface. One gets the Kardar–Parisi–Zhang (KPZ) equation4 ∂h λ = ν∇ 2 h + (∇ h ) 2 + η(x , t ) . ∂t 2 (5) As a consequence of its mapping to the noisy Burger’s equation, to the statistical mechanics of directed polymer in a random medium and other equilibrium and nonequilibrium systems, the KPZ equation has become a model of quite widespread interest in statistical mechanics. Though we focus on growth problems in this paper, the KPZ equation is also applicable in erosion processes. Taking cue from the development in understanding the growth phenomenon through the KPZ equation, a vast class of simulational and analytical models have evolved to 396 explain different experimentally observed growth processes. Diverse technical tools ranging from simulations with various dynamical rules to different versions of RG techniques, mode coupling theory, transfer matrix techniques, and scaling arguments have been employed to understand kinetic roughening. In this review we attempt to provide an overview of this phenomenon of roughening of a growing surface. It is almost beyond the scope of this review to describe in detail various models and their experimental relevance. Rather, we focus our attention on a few examples which may broadly represent a few different routes along which research has continued. The plan of this article is as follows. In the next section we focus on the KPZ equation and its RG description. We also point out the connection of the KPZ equation to some other problems of physics. Next, a more generalized growth mechanism involving nonlocal interactions is presented. Finally, the progress in understanding the roughening and super roughening transitions which appear in a very distinct class of models involving lattice pinning potential is presented. KPZ equation and more Let us first look at the origin of the various terms in eqs (4) and (5). In both the equations, the noise term represents random deposition, the fluctuation around the steady value. As already mentioned, a steady current can be removed from the equation by going over to a moving frame. The term involving second derivative of h can represent either of the two processes. It could be a surface tension controlled diffusion process, in which a particle comes to the surface and then does a random walk on the surface to settle at the minimum height position, thereby smoothening the surface. An alternative interpretation would be that there is desorption from the surface and the process is proportional to the chemical potential gradient. The chemical potential of the particles on the surface cannot depend on h or gradient of h because it is independent of the arbitrary base or its tilt. The chemical potential then is related to the second derivative of h. This also has a geometric meaning that ∇2h is related to the local curvature. The larger the curvature, the higher is the chance to desorb because of a lesser number of neighbours. In the KPZ equation, the nonlinear term represents lateral growth. The diffusion-like term can then be thought of either (a) as an alternative that a particle coming to the surface instead of sticking to the first particle it touches, deposits on the surface and then diffuses, or (b) as a random deposition process with desorption. In either case, the noise term tends to roughen the surface, the diffusion term, of whatever origin, smoothens it while the nonlinear term leads to a laterally growing surface. Even if the smoothening linear term is not present, RG or the scaling argument indicates that such a term is generated on a large length scale. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS The KPZ equation has a special symmetry not present in the EW case. This is the tilt symmetry (often called Galilean invariance – a misnomer, though, in this context). If we tilt the surface by a small angle, then with a reparametrization h′ = h +ε· x and x = x + λεt′ and t = t′, the equation remains invariant for small ε. This transformation depends only on λ, the coefficient of the nonlinear term and fails for λ= 0. Since this tilt symmetry is to be maintained no matter at what lengthscale we look at, λmust be an RG invariant. Let us now perform a length rescaling analysis. Under a change of scale as x → bx, t → b zt and h → b χh, KPZ equation transforms as b χ–z ∂h λ = νb χ–2∇2h + b 2χ–2(∇h)2 + b –d/2–z/2η, ∂t 2 (6) where the noise correlation has been used to obtain the scaling of the noise term. Therefore under this scale transformation different parameters scale as ν → b z–2ν, D → b z–d–2χD and λ→ b χ+z–2λ. For λ= 0, the equation remains invariant provided z = 2 and χ = (2 – d)/2. These are just the exponents one expects from the EW model. (Such surfaces with anisotropic scaling in different directions like x and h are called self-affine.) Though we cannot predict the exponents from eq. (6) when λ≠ 0, it does tell us that a small nonlinearity added to the EW equation scales with a scaling dimension χ + z – 2. This term is always relevant in one-dimension, because it scales like b 1/2. This type of scaling argument also shows that no other integral powers of derivatives of h need be considered in eq. (5) as they are all irrelevant, except (∂h/∂x)3 at d = 1, which, however, detailed analysis shows to be marginally irrelevant. Based on this analysis, we reach an important conclusion that the nonequilibrium behaviour in onedimension, and in fact for any dimension below two, would be distinctly different from the equilibrium behaviour. For dimensions greater than two, EW or equilibrium surfaces, as already mentioned, are asymptotically flat with χ = 0, z = 2, and so, a small nonlinearity is irrelevant because it will decay with b. In other words, the growth in higher dimensions for small λ would be very similar to equilibrium problems because the EW model is stable with respect to a small perturbation with nonlinearity. The simple scaling argument does not tell us if the nature of the surface changes for large λfor d > 2, but an RG analysis shows that it does change. That the nonequilibrium growth is always different in lower dimensions and in higher dimensions (greater than two), and that there will be a dynamic phase transition from an equilibrium-like to a genuine nonequilibrium behaviour, explains the source of excitement in this minimal KPZ equation, in the last two decades. If the nonlinear parameter λ is to remain an invariant, i.e. independent of b in eq. (6), then χ + z = 2, a relation which need not be satisfied by the equilibrium growth. It is this relation connecting the two exponents of the scaling function of eq. (2) that distinguishes nonequilibrium growth CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 from equilibrium, the former requiring one less exponent than the latter. We wonder if such an exponent relation is generally true for all nonequilibrium systems. Though we are far away from a complete understanding of all the nuances and details of the KPZ equation, the RG analysis has been very successful in identifying different phases, nature of phase transitions, and, in certain cases, relevant exponents. In brief, the various results obtained from RG analysis are as follows. In one-dimension and for d < 2, even a small nonlinearity, as already mentioned, being relevant in the RG sense, leads to new values of roughening and dynamic exponents, and is characterized by a RG fixed point. Beyond d = 2, there is a phase transition demarcating two different types of surfaces. A small nonlinearity is irrelevant around EW model and the surface is almost flat with χ = 0 and z = 2. A strong nonlinear growth, however, drives the system to a different phase with rougher surface where χ ≠ 0. Several aspects of this phase transition can be studied from RG but the strong λregime is still out of reach, because of the absence of any RG fixed point. The KPZ equation in d = 1 has distinct nonequilibrium behaviour, and the scaling behaviour is the same no matter how small or large λ is. More peculiar is the existence of a stationary probability distribution of the height in onedimension which is the same as for the linear EW model. This is not just an accident but a consequence of certain subtle relations valid only in one-dimension. We do not go into those issues here. The same stationary distribution implies that the nonlinearity does not affect the stationary state solution, and χ = 1/2. The two models, however, differ in the dynamic exponent which, in the case of KPZ growth, has to satisfy χ + z = 2. This leads to an exact answer z = 3/2. Its significance can be grasped if we compare various known cases. For ballistic motion, distance goes linearly with time so that the dynamic exponent is z = 1 while for diffusive motion or in quantum mechanics (e.g. a nonrelativistic free quantum particle), z = 2 as is also the case for EW. Here is an example where the nonequilibrium nature of the problem leads to a completely new exponent connecting the scaling of space and that of time. Dynamic renormalization group analysis A dynamic RG analysis is a more general approach applicable for dynamics which e.g. may be governed by the Langevin equation for the appropriate dynamical variable. For our problem, it is easier to work in Fourier coordinates q, and ωconjugate to space and time. Long distance, long time implies q → 0 and ω→ 0, and q can be taken as the inverse wavelength at which the height variable is probed. The magnitude of wave vector q varies from 0 to Λ, where the upper cutoff is determined by the underlying microscopic length scale like lattice spacing or size of particles, etc. In the Fourier space, different Fourier modes in the linear EW model get decoupled so that each h(q, ω) for each (q, ω) behaves independently. It is this decoupling that allows the 397 SPECIAL SECTION: simple rescaling analysis of eq. (6) or dimensional analysis to give the correct exponents. For the KPZ equation, the nonlinear term couples heights of various wavelengths and therefore any attempt to integrate out the large (q, ω) modes will affect h with low values of (q, ω). This mixing is taken into account in the RG analysis which is implemented in a perturbative way. One thinks of the noise and the nonlinear term as disturbances affecting the EW-like surface. If we know the response of such a surface to a localized disturbance we may recover the full response by summing over the disturbances at all the points and times. However, this disturbance from the nonlinear term itself depends on the height, requiring an iterative approach that generates successively a series of terms. By averaging over the noise, one then can compute any physical quantity. At this stage only degrees of freedom with q in a small shell e–lΛ < q < Λ is integrated out. In real space this corresponds to integrating out the small scale fluctuation. The contribution from this integration over the shell is absorbed by redefining the various parameters ν, λ and D. These are the coupling constants for a similar equation as eq. (5) but with a smaller cutoff Λe–l. A subsequent rescaling then restores the original cutoff to Λ. Following this procedure, the flow equations for different parameters ν, D, and λ can be obtained5. Using the exponent relation predicted from the Galilean invariance and the RG invariance of ν, the flow equations for all the parameters can be combined into a single flow equation for λ2 = λ2D/ν3 (with Λ = 1). This is the only dimensionless parameter that can be constructed from λ, ν, D, and Λ, and it is always easier to work with dimensionless quantities. Its recursion relation is dλ 2 − d 2d − 3 3 = λ + Kd λ , dl 2 4d (7) where Kd is the surface area of a d-dimensional sphere divided by (2π)d. The invariance of ν under the RG 2−d transformation implies z = 2 – Kd λ 2 4 d , and the Galilean invariance provides the value of χ = 2 – z once the value of z is known. To be noted here is that the dynamic exponent is different from 2 by a term that depends on λ coming from the renormalization effects. A few very important features are apparent from eq. (7). From the fixed point requirement dλ /dl = 0, we find that at d = 1, there is a stable fixed point λ2 = 2/K1. At this fixed point z = 3/2 and χ = 1/2 supporting the results predicted from the symmetry analysis. At d = 2, the coupling is marginally relevant, indicating a strong coupling phase not accessible in a perturbation scheme. At d > 2, the flow equation indicates two different regimes, namely a weak coupling regime where λ asymptotically vanishes leading to a flat EW phase with χ = 0, z = 2, and a strong coupling rough phase, the fixed point of which cannot be reached by perturbation analysis. Owing to this limitation of the RG analysis based on the 398 perturbation expansion, the scaling exponents in this strong coupling phase cannot be determined by this RG scheme. Different numerical methods yield z = 1.6 at d = 2. The phase transition governed by the unstable fixed point of λ is well under control with z = 2 for all d > 2. To explore the strong coupling phase, techniques like self-consistent mode coupling approach, functional RG, etc. have been employed, but even a basic question whether there is an upper critical dimension at which z will again become 2 remains controversial. Relation with other systems The relation of the KPZ equation with other quite unrelated topics in equilibrium and nonequilibrium statistical mechanics is impressive. Here, we provide a very brief account of these systems. Noisy Burgers equation: By defining a new variable v = ∇h, we obtain an equation ∂v = D∇2v+λv · ∇ν + f(x, t), ∂t (8) where the noise term f = ∇η. The above equation represents the noisy Burgers equation for vortex free (∇ × v = 0) fluid flow with a random force. This equation is very important in studies of turbulence. The tilt invariance of the KPZ equation turns out to be the conventional Galilean invariance for the Burgers equation (for λ= 1), and that is how the name stayed on. Directed polymer in a random medium: A directed polymer, very frequently encountered in different problems in statistical mechanics, is a string-like object which has a preferred longitudinal direction along which it is oriented, with fluctuations in the transverse direction. The flux lines in type II or high Tc superconductors are examples of such directed polymers in 3-dimensions, while the steps on a vicinal or miscut crystal surface or the domain walls in a uniaxial two-dimensional system are examples in twodimensions. The formal mathematical mapping to such objects follows from a simple (Cole– Hopf) transformation of the KPZ equation using W(x, t) = exp The Cole–Hopf transformation linearizes the nonlinear KPZ equation and the resulting linear diffusion equation (or imaginary time Schrödinger equation) is identical to that satisfied by the partition function of a directed polymer in a random potential. For such random problems, one is generally interested in the averages of thermodynamic quantities like the free energy and we see that the noise averaged height 〈h(x, t)〉 gives the average free energy of a directed polymer of length t with one end at the origin and the other end at x. This is a unique example of a system where the effect of such quenched averaging of free energy can be studied without invoking any tricks (like CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS the replica method). This has led to many important results and enriched our understanding of equilibrium statistical mechanics. Recently, this formulation has been extended to study details of the properties of the random system near the phase transition point and overlaps in lower dimensions6,7. It turns out that one needs an infinite number of exponents to describe the statistical behaviour of the configurations of the polymer in the random medium8. We do not go into this issue as this is beyond the scope of this article. An interesting connection between the 1 + 1dimensional KPZ equation and the equilibrium statistical mechanics of a two-dimensional smectic-A liquid crystal has been recently established by Golubovich and Wang9. This relationship further provides exact approach to study the anomalous elasticity of smectic-A liquid crystals. Apart from these, there are a number of other relations between KPZ equation and kinetics of annihilation processes with driven diffusion, the sine–Gordon chain, the driven diffusion equation and so on. Beyond KPZ Conservation condition: The situation encountered in molecular-beam epitaxy (MBE) for growth of thin films is quite different from the mechanism prescribed by the KPZ equation2. In MBE, surface diffusion takes place according to the chemical potential gradient on the surface, respecting the conservation of particles. If the particle concentration does not vary during growth, then a mass conservation leads to a volume conservation and the film thickness is governed by an underlying continuity equation ∂h +∇ · j = η, ∂t (9) where j is the surface diffusion current which states that the change of height at one point is due to flow into or out from that point. The current is then determined by the gradient of the chemical potential, and since the chemical potential has already been argued to be proportional to the curvature ∇2h, the growth equation thus becomes a simple linear equation involving ∇4h which, like the EW model, is exactly solvable. Taking into account the effect of nonlinearity the full equation can be written as ∂h λ = –∇2 ν∇ 2 h + (∇ h ) 2 +η(x, t), ∂t 2 (10) where the noise correlation is 〈η(x, t)η(x′, t′)〉 = 2D∇2 δ(x – x′)δ(t – t′), if the noise also maintains conservation (if it originates from the stochasticity of diffusion) or would be the same white noise as in the KPZ equation, if the noise is from random deposition. It goes without saying that the exponents are different from the EW model even for the linear theory. The invariance of λ in this case leads to a different relation between χ and z. At the dimension of CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 physical interest d = 2, this growth equation leads to an enhanced roughness than the KPZ case and may explain the results of experiments of high temperature MBE. Quenched noise: A different type of generalization of the KPZ equation was to explore the motion of domain walls or interfaces in a random medium. In this case, the noise is not explicitly dependent on time but on the spatial position and the height variable. Such a noise has been called quenched noise because the noise is predetermined and the interface or the surface moves in this random system. The simple features of the KPZ equation and the EW model are lost. Functional RG analysis and numerical studies are attempted to clarify the question of universality classes and details of dynamics in such cases. The important concept that emerged in this context is the depinning transition so that the surface remains pinned by the randomness until the drive exceeds a certain critical value. Interface depinning is an example of a nonequilibrium phase transition. The velocity of the surface near this depinning transition also has critical-like behaviour with long-range correlations. Below the threshold, the dynamics is sluggish, while just above the threshold, the velocity is in general not proportional to the drive but obeys a power law with a universal exponent. For a very strong drive (or large velocity of the interface) the moving surface encounters each site only once, and therefore the noise is effectively like a space–time dependent noise rather than the quenched one. The nature of the surface would then be like KPZ. Coloured noise: In the previous section we discussed the KPZ equation with white noise. If the noise is coloured in the sense that there is correlation in space or time or both, the universal behaviour, the phase transitions and the properties are different but still can be studied by the same RG technique. Several aspects of the problem, especially the role of noise correlation, have been explored10. All of the above seem to suggest that if there is no conservation law, then the KPZ equation is the equation to describe any nonlinear or nonequilibrium growth process and all phenomena can be put in one of the known universality classes. However, experimentally KPZ exponents seem to elude us so far1,2,11. Since results are known exactly in one-dimension, special one-dimensional experiments were conducted like paper burning, interface motion in paper, colloid suspension, etc., but KPZ exponents have not been seen. In the colloid experiment11, the surface formed by the depositing colloids on the contact line (d = 1) between the colloid latex film and a glass slide was measured from video images. This method yields χ = 0.71 but cannot determine the dynamic exponent. A recent analysis12 of tropical cumulus clouds in the upper atmosphere, from satellite and space shuttle data from 0.1 to 1000 km, seems to agree with the KPZ results in d = 2. Kinetic roughening with nonlocality 399 SPECIAL SECTION: In spite of a tremendous conceptual and quantitative success of the KPZ equation in describing the nonequilibrium growth mechanism, the agreement with experimentally observed exponents is rather unsatisfactory. One wonders whether there is any relevant perturbation that drives the systems away from the KPZ strong coupling perturbation. One goal of this section is to point out that indeed there can be long-range interactions that may give rise to non-KPZ fixed points. In many recently studied systems involving proteins, colloids, or latex particles the medium-induced interactions are found to play an important role13. This nonlocal interaction can be introduced by making a modification of the nonlinear term in the KPZ equation. Taking the gradient term as the measure of the local density of deposited particles, the long-range effect is incorporated by coupling these gradients at two different points. The resulting growth equation is a KPZ-like equation with the nonlinear term modified as14 1 2 ∫ dr′ V (r′)∇h(r + r′, t) · ∇h(r – r′, t). For generality, we take V (r′) to have both short- and long-range parts with a specific form in Fourier space as V (k) = λ0 + λρk – ρ such that in the limit λρ → 0, KPZ results are retrieved. The aim is to observe whether the macroscopic properties are governed by only λ0 and hence KPZ-like or the behaviour is completely different from KPZ due to the relevance of λρ around the KPZ fixed points. A scaling analysis as done in eq. (6) clearly indicates different scaling regimes and the relevance of λ0 and λρ for d > 2 at the EW fixed point. For any λρ(≠ 0) with ρ > 0, the local KPZ theory (i.e. λρ = 0 and χ + z = 2) is unstable under renormalization and a non-KPZ behaviour is expected. For 2 < d < 2 + 2ρ, only λρ is relevant at the EW fixed point. The exponents of the non-KPZ phases can be obtained by performing a dynamic RG calculation14. By identifying the phases with the stable fixed points, we then see the emergence of a new fixed point where the long-range features dominate (χ + z = 2 + ρ). Most importantly, at d = 2, the marginal relevance of λ is lost and there is a stable fixed point (LR) for ρ > 0.0194. On the experimental side, there are experiments on colloids with χ = 0.71 which is the value also obtained from paper burning exponents. For colloids, hydrodynamic interactions are important. Similar long-range interactions could also play a role in paper burning experiment due to the microstructure of paper. With this χ our exponents suggest ρ = – 0.12 at d = 1 at the long-range fixed point. Further experiments on deposition of latex particles or proteins yielding the roughness of growing surface have not been performed. Probably such experiments may reveal more insights on this growth mechanism. More recently, the effect of coloured noise in presence of nonlocality has been studied15 and the nature of the phases and the various phase transitions clarified. A conserved version of the nonlocal equation has also been considered and it shows rich behaviour16. 400 Roughening transition in nonequilibrium It is interesting to study the impact of equilibrium phase transitions on the nonequilibrium growth of a surface. This is the situation observed experimentally in growth of solid 4 He in contact with the superfluid phase17. There is an equilibrium roughening transition at TR = 1.28 K. For T > TR the growth velocity is linear in the driving force F (chemical potential difference), but for T < TR the velocity is exponentially small in the inverse of the driving force. For infinitesimal drive, the mobility which is the ratio of the growth velocity and F vanishes with a jump from a finite value at the transition. With a finite force the transition is blurred and the flat phase below TR in equilibrium becomes rougher over large length scale. The equilibrium roughening transition is an effect of discrete translational symmetry of the lattice. The equilibrium dynamics in this case is essentially governed by the Langevin equation ∂h 2π = K∇ 2 h (r , t) − V sin h (r, t ) + ζ (r, t ) , ∂t a (11) where the sine term favours a periodic structure of spacing a. Extensive investigations have been done on this equilibrium model. At low temperature, this periodic potential is relevant and it ensures that minimum energy configuration is achieved when φ is an integer multiple of lattice periodicity. In this phase, the surface is smooth and the roughness is independent of length. In the high temperature phase the equilibrium surface is thermally rough and the roughness is logarithmic C(L, τ) ~ ln[Lf(τ/Lz)]. (12) The critical point is rather complicated and goes by the name of Kosterlitz–Thouless transition, first discussed in the context of defect mediated transitions in twodimensional XY magnets18. For a nonequilibrium crystal growth problem, one needs to introduce the KPZ nonlinear term in eq. (11). There is no longer any roughening transition. The fact that away from equilibrium the roughening transition is blurred is manifested by the domination of the nonlinear term and the suppression of the pinning potential in the asymptotic regime19. A very nontrivial situation arises when the surface contains quenched disorder which shifts the position of the minima of the pinning potential in an arbitrary random fashion20,21. In this case, there is a new phase transition which is drastically different from the equilibrium roughening transition. This transition is called super roughening. Above the transition temperature, i.e. for T > Tsr, the surface is logarithmically rough as it is in the high temperature phase of the pure problem. However in the low temperature phase, i.e. for T < Tsr, the surface is no longer flat and is even rougher than the high temperature CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS phase. Recent numerical treatments suggest that the surface roughness behaves as (ln L)2. In the nonequilibrium situation, the linear response mobility vanishes continuously at the transition temperature unlike the jump discontinuity in the pure case. A general treatment with a correlated disorder elucidates the connection between the roughening and super roughening transition and one observes that the roughening turns into a super roughening transition if the disorder correlation decays sufficiently fast. Away from equilibrium, the super roughening transition is essentially dominated by the KPZ nonlinearity and instead of the logarithmic roughness, an asymptotic power law behaviour of the roughness is found over all temperature ranges. In a similar situation in the nonequilibrium case, one needs to study the role of the KPZ nonlinearity with longrange disorder correlation22. A functional renormalization scheme with an arbitrary form of the disorder correlation turns out to be useful, though a detailed solution is not available. It is found that the flow of the KPZ nonlinearity under renormalization, with power law form of the disorder correlation, is such that it decays with length. This implies that nonequilibrium feature does not set in over a certain length scale. Over this scale one would then expect usual roughening transition. However, there is generation of a driving force due to the nonlinearity, and the growth of this force with length scale would invalidate use of perturbative analysis. For large length scales, one expects a KPZ-type power law roughness of the surface. Nevertheless, the initial decay of the nonlinearity with the length scale due to the long-range correlation of the disorder is an interesting conclusion that seems to be experimentally detectable. Remarks In this brief overview, we attempted to focus on the difference between equilibrium and nonequilibrium growth problems with an emphasis on the scaling behaviour and RG approach. Many details with references to pre-1995 papers can be found in Halpin-Healy and Zhang1, and Barbási and Stanley2, which should be consulted for more detailed analysis. Though the success story of the KPZ equation is rather impressive, there are still many unresolved, controversial issues. In fact for higher dimensions, the behaviour is not known with as much confidence as for lower dimensions. Developments in this CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 direction are awaited. Note added in proof: 1. The growth mechanism of metal-organic films deposited by the Langmuir–Blodgett technique has been studied in ref. 23 by X-ray scattering and atomic force microscopy. The results have been interpreted by a combination of 1dimensional EW equation (eq. (4)) and 2-dimensional linear conserved equation (eq. (10)) with conserved noise. 2. For effects of nonlocality in equilibrium critical dynamics, see ref. 24. 1. Halpin-Healy, T. and Zhang, Y. C., Phys. Rep., 1995, 254, 215. 2. Barbási, A.-L. and Stanley, H. E., Fractal Concepts in Surface Growth, Cambridge Univ. Press, Cambridge, 1995. 3. Edwards, S. F. and Wilkinson, D. R., Proc. R. Soc. London A, 1982, 381, 17. 4. Kardar, M., Parisi, G. and Zhang, Y.-C., Phys. Rev. Lett., 1986, 57, 1810. 5. Medina, E. et al., Phys. Rev. A, 1989, 39, 3053. 6. Mezard, M., J. Phys. (Paris), 1990, 51, 1831. 7. Mukherji, S., Phys. Rev. E, 1994, 50, R2407. 8. Mukherji, S. and Bhattacharjee, S. M., Phys. Rev. B, 1996, 53, R6002. 9. Golubovic, L. and Wang, Z.-G., Phys. Rev. E, 1994, 49, 2567. 10. Chekhlov, A. and Yakhot, V., Phys. Rev. E, 1995, 51, R2739; ibid, 1995, 52, 5681; Hayat, F. and Jayaprakash, C., Phys. Rev. E, 1996, 54, 681; Chattopadhyay, A. K. and Bhattacharjee, J. K., Euro. Phys. Letts., 1998, 42, 119. 11. Lei, X. Y., Wan, P., Zhou, C. H. and Ming, L. B., Phys. Rev. E, 1996, 54, 5298. 12. Pelletier, J. D., Phys. Rev. Lett., 1997, 78, 2672. 13. Feder, J. and Giaever, I., J. Colloid Interface Sci., 1980, 78, 144; Ramsden, J. J., Phys. Rev. Lett., 1993, 71, 295; Pagonabarraga, I. and Rubi, J. M., Phys. Rev. Lett., 1994, 73, 114; Wojtaszczyk, P. and Avalos, J. B., Phys. Rev. Lett., 1998, 80, 754. 14. Mukherji, S. and Bhattacharjee, S. M., Phys. Rev. Lett., 1997, 79, 2502. 15. Chattopadhyay, A. K., Phys. Rev. E, cond-mat/9902194 (to appear). 16. Jung, Y., Kim, I. and Kim, J. M., Phys. Rev. E, 1998, 58, 5467. 17. Noziers, P. and Gallet, F., J. Phys. (Paris), 1987, 48, 353. 18. Chui, S. T. and Weeks, J. D., Phys. Rev. Lett., 1976, 38, 4978. 19. Rost, M. and Sphon, H., Phys. Rev. E, 1994, 49, 3709. 20. Tsai, Y.-C. and Shapir, Y., Phys. Rev. Lett., 1992, 69, 1773; Phys. Rev. E , 1994, 50, 3546; ibid, 1994, 50, 4445. 21. Scheidl, S., Phys. Rev. Lett., 1995, 75, 4760. 22. Mukherji, S., Phys. Rev. E, 1997, 55, 6459. 23. Basu, J. K., Hazra, S. and Sanyal, M. K., Phys. Rev. Lett., 1999, 82, 4675. 24. Sen, P., J. Phys. A., 1999, 32, 1623. 401 SPECIAL SECTION: Suspensions far from equilibrium Sriram Ramaswamy Centre for Condensed-Matter Theory, Department of Physics, Indian Institute of Science, Bangalore 560 012, India A review is presented of recent experimental and theoretical work on the dynamics of suspensions of particles in viscous fluids, with emphasis on phenomena that should be of interest to experimenters and theoreticians working on the statistical mechanics of condensed matter. The article includes a broad introduction to the field, a list of references to important papers, and a technical discussion of some recent theoretical progress in which the author was involved. Equilibrium and nonequilibrium suspensions SUSPENSIONS of particles in a fluid medium are all around us 1,2. Examples include river water, smog, blood, many liquid foods, many medicines, cosmetics, paints, and so on. The particles, which we shall call the solute, are generally submicron to several microns in size, and the suspending fluid, which we shall call the solvent, is frequently less dense than the solute. The viscosity of the solvent could range from that of water (or air) to several thousands of times higher. The field of suspension science has distinguished origins: Einstein’s3 interest in Brownian motion as evidence for the existence of molecules led him to calculate the viscosity and diffusivity of a dilute suspension (before diversions such as relativity and quantum mechanics took him over completely); Smoluchowskii’s4,5 studies of sedimentation and aggregation in colloids led to major advances in the theory of stochastic processes; somewhat more recently, the challenging many-body nature of the dynamics of suspensions was highlighted in the work of Batchelor6. Today, the study of the static and dynamic properties of suspensions from the point of view of statistical mechanics is a vital part of the growing field of soft condensed matter science. In applications and in industrial processing, suspensions are usually subjected to strongly nonequilibrium conditions. By nonequilibrium I mean that the system in question is driven by an external agency which does work on it – stirring, pumping, agitation – which the system dissipates internally. The bulk of interesting and, by and large, incompletely understood phenomena in suspension science, and in the area of complex fluids in general, are also those that occur far from equilibrium. Problems in which I have been or am currently interested are: the melting of e-mail: sriram@physics.iisc.ernet.in 402 colloidal crystals when they are sheared7–13; spontaneous segregation in sheared hard-sphere suspensions 14; the collapse of elastic colloidal aggregates under gravity15, and its possible relation to the instability of sedimenting crystalline suspensions12,16,17; the enhancement of redblood-cell sedimentation rates in the blood of a very sick person18; and the puzzle19–23 of the statistics of velocity fluctuations in ultraslow fluidized beds. (References 24–31 should give the reader an idea of the range of this field.) None of the observations in the papers I have mentioned can be understood purely with the methods used to study hydrodynamic instabilities: they are fluctuation phenomena, and therefore belong in this special issue on nonequilibrium statistical physics. A suspension can be out of equilibrium in a number of ways: in particular, it could be in a nonstationary state (in the process of settling or aggregating or crystallizing, for example), or it could be stuck in a metastable amorphous state 32 or it could be held, by the application of a driving force, in a time-independent but not time-reversal invariant state with characteristics different from the equilibrium state. In this article we shall mainly be concerned with these nonequilibrium steady states, characterized by a constant mean throughput of energy. These are to be contrasted with thermal equilibrium states which have a constant mean budget of energy, i.e. a temperature. A suspension of charged Brownian particles with precisely the same density as the solvent, such as are discussed in the review article by Sood33 is the standard example of an equilibrium suspension. The two most common ways of driving a suspension out of equilibrium are shear34, wherein the solute and solvent are jointly subjected to a velocity gradient, and sedimentation or fluidization35, where the velocity of solute relative to solvent is on average nonzero and spatially uniform. This latter class of problems is very close to the currently rather active area of driven diffusive systems 36, which has provided much insight into statistical physics far from equilibrium. Accordingly, this review will focus largely on sedimentation and fluidized beds, although a brief summary of shear-flow problems with relevant references will be provided. Even with this restriction, the field is much too vast to allow anything like representative coverage, so my choice of topics will be dictated by familiarity, in the hope that the problems I highlight will attract the reader to the area. It is in that sense not a true review article, but an advertisement for a field and therefore includes as an integral part a reasonably large list of references. The aim is CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS to give a general idea of the richness of phenomena in nonequilibrium suspensions, as well as a technical understanding of some of my theoretical work in this field. To theoreticians, especially in India, this article argues that the vast literature on suspension dynamics is a largely untapped lode of problems in the statistical physics of driven systems. Elegant models of the sort popular among practitioners of the more mathematical sort of statistical mechanics could acquire a greater meaning and relevance if born out of an attempt to understand phenomena in these systems (for an example of such an attempt, see the section on the stability of steadily drifting crystals). I hope in addition that this article persuades condensed-matter experimenters in India to look for problems in these and related soft-matter systems (including powders, on which I am not competent to write), which are as rich as traditional solid-state systems, without the complications of low temperatures, high vacuum, etc. I shall work exclusively in the limit of slow motions through highly viscous fluids, i.e. the limit of low Reynolds number Re ≡ Ua/ν, where U is a typical velocity, a the particle size, and the kinematic viscosity ν ≡ µ/ρ, µ and ρ being respectively the shear viscosity and mass density of the solvent. Re, which measures the relative importance of inertia and viscosity in a flow, can here be thought of simply as the fraction of a particle’s own size that it moves if given an initial speed U, before viscosity brings it to a halt. For bacteria (sizes of order 1 to 10 microns) swimming at, say, 1 to 10 microns a second in an aqueous medium, Re ~ 10–6 to 10–4, and for polystyrene spheres (specific gravity 1.05, radius 1 to 10 µm) sedimenting in water, Re ~ 10–7 to 10–4. So we are amply justified in setting Re to zero. Recall that in the low Re limit, things move at a speed proportional to how hard they are pushed, and stop moving as soon as you stop pushing. While this corresponds very poorly to our experience of swimming, it is an accurate picture of how water feels to a bacterium or to a colloidal particle. A good general introduction to the subject of zero Reynolds-number flow is given in Happel and Brenner37, although standard fluid dynamics texts38,39 also discuss it. A very detailed treatment of the dynamics of hydrodynamically interacting particles can be found in ref. 40. The dimensionless control parameter relevant to zero Reynolds number suspensions is the Peclet number Pe ≡ Ua/D (ref. 1), where D = T/6πµa is the Stokes–Einstein diffusivity of the particle at temperature T. In a shear flow with velocity gradient γ&, clearly U ~ γ& a, so that Pe ~ 2 which isγ& athe /Dratio , of a diffusion time to a shearing time. In sedimentation, Pe measures the relative importance of settling (gravitational forces) and diffusion (thermal fluctuations), and can be expressed as mRga/T, where mRg is the buoyancy-reduced weight of the particle, g being the acceleration due to gravity. Since Pe ∝ a 4, it is clear that small changes in the particle radius make a large difference. For polystyrene spheres in water, Pe ranges from 0.5 to 5000 CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 as the radius is varied from 1 to 10 µm. Suspensions with Pe >> 1 are termed non-Brownian, since their behaviour is dominated by the gravity-induced drift and the resulting solvent flow, not by thermal fluctuations. This Pe = ∞, Re = 0 limit turns out to be a very interesting one. The most trivial example of a nonequilibrium suspension is a single solute particle, heavier than its solvent, so that in the presence of gravity it settles to the bottom of the container. If we wish to study the steady-state properties of this settling process, we must make the particle settle forever. There are two ways of doing this: either use a very tall container and study the flow around the particle as it drifts past the middle, or arrange to be in the rest frame of the particle. The latter is realized in practice by imposing an upward flow so that the viscous drag on the particle balances its buoyancy-reduced weight, suspending the particle stably. The nature of the flow around such an isolated particle, without Brownian motion and in the limit of low velocity, was studied about a century and a half ago41. As soon as the number of particles is three or greater, the motion becomes random even in the absence of a thermal bath (this can be seen either in Stokesian dynamics simulations42 or simply by using particles large enough that Brownian motion due to thermal fluctuations is negligible) because the flow produced by each particle disturbs the others, leading to chaos43. In the limit of a large number of particles, the problem can thus be treated only by the methods of statistical mechanics (suitably generalized to the highly nonequilibrium situations we have in mind). A collection of particles stabilized against sedimentation by an imposed upflow is called a fluidized bed. It is useful here to distinguish two classes of nonequilibrium systems. In thermal driven systems the source of fluctuations is temperature, and the driving force (shear, for example) simply advects the fluctuations injected by the thermal bath. An example of this type would be a suspension of submicron particles, whose Brownian motion is substantial, subjected to a shear flow. Non-thermal driven systems are more profoundly nonequilibrium, in that the same agency is responsible for the driving force and the fluctuations. A sedimenting non-Brownian many-particle suspension is thus an excellent example of a non-thermal nonequilibrium system. The structure of this article is as follows. In the next section I summarize our present state of understanding of the shear-induced melting of colloidal crystals. Then, I discuss the physics of steadily sedimenting colloidal crystals, including the construction of an appropriate driven diffusive model for which exact results for many quantities of physical interest can be obtained. The next section introduces the reader to the seemingly innocent problem of the steady sedimentation of hard spheres interacting only via the hydrodynamics of the solvent. Puzzles are introduced and partly resolved. The last section is a summary. 403 SPECIAL SECTION: Shear-melting of colloidal crystals It has been possible for some years now to synthesize spheres of polystyrene sulphonate and other polymers, with precisely controlled diameter in the micron and submicron range. These ‘polyballs’ have become the material of choice for systematic studies in colloid science33. In aqueous suspension, the sulphonate or similar acid end group undergoes ionization. The positive ‘counterions’ go into solution, leaving the polyballs with a charge of several hundred electrons. The counterions together with any ionic impurities partly screen the Coulomb repulsion between the polyballs, yielding, to a good approximation in many situations, a collection of polymer spheres interacting through a Yukawa potential exp(– κ r)/r with a screening length κ–1 in the range of a micron, but controllable by the addition of ionic impurities (NaCl, HCl, etc.). Not surprisingly, when the concentration of particles is large enough that the mean interparticle spacing a s ~ κ–1, these systems order into crystalline arrays with lattice spacings ~ a s comparable to the wavelength of visible light. The transition between colloidal crystal and colloidal fluid is a perfect scale model of that seen in conventional simple atomic liquids33. It is first-order and the fluid phase at coexistence with the crystal has a structure factor whose height is about 2.8. The transition is best seen by varying not temperature but ionic strength. These colloidal crystals33 are very weak indeed, with shear moduli of the order of a few tens of dyn/cm2. The reason for this is clear: the interaction energy between a pair of nearest neighbour particles is of order room temperature, but their separation is about 5000 Å. Thus on dimensional grounds the elastic moduli, which have units of energy per unit volume, should be scaled down from those of a conventional crystal such as copper by a factor of 5000–3 ~ 10–11. It is thus easy to subject a colloidal crystal to stresses which are as large as or larger than its shear modulus, allowing one to study a solid in an extremely nonlinear regime of deformation. One can in fact make a colloidal crystal flow if the applied stress exceeds a modest minimum value (the yield stress) required to overcome the restoring forces of the crystalline state. When a colloidal crystal is driven into such a steadily flowing state, it displays at least two different kinds of behaviour, with a complex sequence of intermediate stages which appear to be crossovers rather than true nonequilibrium phase transitions, and whose nature depends strongly on whether the system is dilute and charge-stabilized or concentrated and hard-sphere-like7–9. I shall focus on the two main ‘phases’ seen in the experiments, not the intermediate ones. At low shear-rates, it flows while retaining its crystalline order: crystalline planes slide over one another, each well-ordered but out of registry with its neighbours. At large enough shear-rates, all order is lost, through what appears to be a nonequilibrium phase transition from a flowing colloidal crystal to a flowing 404 colloidal liquid. The shear-rate required to produce this transition depends on the ionic strength n i, and appears to go to zero as n i approaches the value corresponding to the melting transition of a colloidal crystal at equilibrium. This connection to the equilibrium liquid–solid transition prompted us to extend the classical theory44 of this transition to include the effects of shear flow. I will not discuss our work on that problem here: the interested reader may read about them in Ramaswamy and Renn10 and Lahiri and Ramaswamy11. The problem remains incompletely understood, and work on it especially in experiments and simulations continues13. I mention it here as an outstanding problem in nonequilibrium statistical physics on which I should be happy to see further progress. The stability of steadily drifting crystals The crystalline suspensions of the earlier section are generally made of particles heavier than water. Left to themselves, they will settle slowly, giving slightly inhomogeneous, bottom-heavy crystals with unit cells shorter at the bottom of the container than at the top. To get a truly homogeneous crystal, one must counteract gravity. This is done, as remarked earlier, in the fluidized bed geometry, where the viscous drag of an imposed upflow balances the buoyant weight of the particles. As a result, one is in the rest frame of a steadily and perpetually sedimenting, spatially uniform crystalline suspension, whose steady-state statistical properties we can study. Although most crystalline suspensions are made of heavierthan-water particles, and therefore do sediment, there have been only a few studies45 that focus on this aspect. Rather than summarizing the experiments, I shall let the reader read about them45. Our work was in fact inspired by attempts to understand drifting crystals in a different context, namely flux-lattice motion46, and the interest in crystalline fluidized beds arose when we chanced upon some papers by Crowley47, to whose work I shall return later in this review. As with crystals at equilibrium, the first thing to understand was the response to weak, long-wavelength perturbation. For a crystal at thermal equilibrium, elastic theory48 and broken-symmetry dynamics49,50 provide, in principle, a complete answer. Our crystalline fluidized bed, however, is far from equilibrium, in a steady state in which the driving force of gravity is balanced by viscous dissipation. We must therefore simply guess the correct form for the equations of motion, based on general symmetry arguments16. This general form should apply in principle to any lattice moving through a disspative medium without static inhomogeneities. Apart from the steadily sedimenting colloidal crystal, another example is a flux-point lattice moving through a thin slab of ultraclean type II superconductor under the action of the Lorentz force due to an applied current51. We will restrict our attention to the former case alone in this review. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS One technical note is in order before we construct the equations of motion. A complete analysis of the sedimentation dynamics of a three-dimensional crystalline suspension requires the inclusion of the hydrodynamic velocity field as a dynamical variable. This is because the momentum of a local disturbance in the crystalline fluidized bed cannot decay locally but is transferred to the nearby fluid and thence to more and more remote regions. We get around this difficulty by considering an experimental geometry in which a thin slab of crystalline suspension (particle size a << interparticle spacing l ) is confined in a container with dimensions Lx , Lz >> Ly ~ l (gravity is along − ẑ ). The local hydrodynamics that (see below) leads to the configuration-dependent mobilities16,47 is left unaffected by this, but the long-ranged hydrodynamic interaction is screened in the xz plane on scales >> Ly by the no-slip boundary condition at the walls, so that the velocity field of the fluid can be ignored. Instead of keeping track of individual particles, we work on scales much larger than the lattice spacing l, treating the crystal as a permeable elastic continuum whose distortions at point r and time t are described by the (Eulerian) displacement field u(r, t). Ignoring inertia as argued above, the equation of motion must take the general form velocity = mobility × force, i.e. ∂ u = M ( ∇u ) ( K ∇∇ u + F + f ) . ∂t (1) In eq. (1), the first term in parentheses on the right-hand side represents elastic forces, governed by the elastic tensor K, the second (F) is the applied force (gravity, for the colloidal crystal and the Lorentz force for the flux lattice), and f is a noise source of thermal and/or hydrodynamic origin. Note that in the absence of the driving force F the dynamics of the displacement field in this overdamped system is purely diffusive: ∂t u ~∇2u, with the scale of the diffusivities set by the product of a mobility and an elastic constant. All the important and novel physics in these equations, when the driving force is nonzero, lies in the local mobility tensor M, which we have allowed to depend on gradients of the local displacement field. The reason for this is as follows: The damping in the physical situations we have mentioned above arises from the hydrodynamic interaction of the moving particles with the medium, and will in general depend on the local configuration of the particles. If the structure in a given region is distorted relative to the perfect lattice, the local mobility will depart from its ideallattice value as well, through a dependence on the distortion tensor ∇u. Assuming, as is reasonable, that M can be expanded in a power series in ∇u, eq. (1) leads to u&x = λ1 ∂ z u x + λ2 ∂ x u z + O(∇∇u ) + O(∇u∇u) + f x , CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 (2) u&z = λ3∂x u x + λ4∂zu z + O(∇∇u) + O(∇u∇u) + f z , (3) where the nonlinear terms as well as those involving the coefficients λi are a consequence of the sensitivity of the mobility to local changes on the concentration and orientation, and are proportional to the driving force (gravity). They are thus absent in a crystal at equilibrium. The {λi} terms dominate the dynamics at sufficiently long wavelength for a driven crystal, since they are lower order in gradients than the O(∇∇u) elastic terms. It is immediately obvious that the sign of the product α≡ λ2λ3 decides the long-wavelength behaviour of the steadily moving crystal. If α> 0, small disturbances of the sedimenting crystal should travel as waves with speed ~ λi, while if α< 0, the system is linearly unstable: disturbances with wave vector k with k x ≠ 0 should grow at a rate Symmetry cannot tell ~ us | αwhich | k x . of these happens: the sign of α depends on the system in question, and is determined by a more microscopic calculation than those presented above. This is where the work of Crowley47 comes in. He studied the settling of carefully prepared ordered arrays of steel balls in turpentine oil, and found they were unstable. He also calculated the response of such arrays to small perturbations, taking into account their hydrodynamic interaction, and found that the theory said that they should indeed be unstable. Thus, one would expect crystalline fluidized beds to be linearly unstable (the analogous calculation for drifting flux lattices in type II superconductors finds linearly stable behaviour51) and is hence described by eqs (2) and (3) with α< 0. However, Crowley’s47 arguments and experiments were for an array of particles merely prepared in the form of an ordered lattice. Unlike in the case of a charge-stabilized suspension, there were no forces that favoured such order at equilibrium in the first place. Our model eqs (2) and (3), however, contain such forces as well as nonlinearities and noise. While the elastic terms are of course subdominant in a linearized treatment at long wavelength to the {λi} terms, which are O(∇u), we asked whether these terms, in combination with nonlinearities and noise could undo or limit the Crowley (α< 0) instability. We answer this question not by studying eq. (3) with α< 0, but instead by building a discrete Ising-like dynamical model embodying the essential physics of those equations. The crucial features of the dynamics implied by eq. (3) (see Happel and Brenner37 and Crowley47) are that a downtilt favours a drift of material to the right, an uptilt does the opposite, an excess concentration tends to sink, and a deficit in the concentration to float up. Let us implement this dynamics in a one-dimensional system with sites labelled by an integer i, and describe the state of the lattice of spheres in terms of an array of two types of two-state variables: ρi = ±, which tells us if the region around site i is compressed (+) or dilated (–) relative to the mean, and 405 b E θi = ± which tells us if the local tilt is up (+, which we will call ‘/’) or down (–, which we will denote ‘\’). Let us put the two types of variables on the odd and even sublattices. A valid configuration could then look like ρ1θ1ρ2θ2ρ3θ3ρ4θ4 = + \ + / – \ + \ – / – /. An undistorted lattice is then a statistically homogeneous admixture of + and – for both the variables (a ‘paramagnet’). The timeevolution of the model is contained in a set of transition rates for passing from one configuration to another, as follows16,17,52: W(+ \ – → – \ +) = D + a W(– \ + → + \ –) = D – a W(– \ + → + \ –) = D′ + a′ W(+ \ – → – \ +) = D′ – a′ (4) W(/ + \ → \ + / ) = E + b W( \ + / → / + \ ) = E – b W( \ – / → / – \ ) = E′ + b′ W( / – \ → \ – / ) = E′ – b′, where the first line, for example, represents the rate of + – going to – + in the presence of a downtilt \, and so on. D, E, D′, E′ (all positive) and a, b, a′, b′ are all in principle independent parameters, but it turns out to be sufficient on grounds of physical interest, relevance to the sedimentation problem, and simplicity to consider the case D = D′, E = E′, a = a′, b = b′, with γ ≡ ab > 0 corresponding to α= λ2λ3 < 0 in eqs (2) and (3). Associating ρi with ∂x u x and θi with ∂x u z we expect that the above stochastic dynamics yields, in the continuum limit, the same behaviour as a one-dimensional version of eqs (2) and (3) in which all z derivatives are dropped, and appropriate nonlinearities are included to ensure that the instability seen in the linear approximation is controlled. This mapping provides a convincing illustration of the close connection between quite down-to-earth problems in suspension science and the area of driven diffusive systems which is currently the subject of such intense study 36. Initial numerical studies16 of eq. (4) suggested a tendency towards segregation into macroscopic domains of + and –, as well of / and \ with interfaces between + and – are shifted with respect to those between / and \ by a quarter of the system size. This arrangement is just such as to make it practically impossible, given the dynamical rules eq. (4), for the domains to remix. The numerics seemed to suggest that enough interparticle repulsion or a high enough temperature could undo the phase separation, but this turned out to be a finite size effect. We have shown52 that the model always phase-separates for γ > 0. More precisely, we have shown exactly, for the symmetric case Σiρi = Σiθi = 0, if that the steady state of our model obeys detailed balance, (i.e. acts like a thermal equilibrium system) with respect to the energy function 406 = εΣ Nk=1[Σ kj=1θ j ] ρk . = a D , SPECIAL SECTION: H A little reflection will convince the reader that this is like the energy of particles (the {ρi}) on a hill-and-valley landscape with a height profile whose local slope is θi. Since the dynamics moves particles downhill, and causes occupied peaks of the landscape to turn into valleys, it is clear that the final state of the model will be one with a single valley, the bottom of which is full of pluses (and the upper half full of minuses). It is immediately clear that this phase separation is very robust, and will persist at any finite temperature (i.e. any finite value of the base rates D and E). Figure 1 demonstrates this graphically. Many properties of the model (eq. (4)) can be obtained exactly in the detailed-balance limit mentioned above. These include the prediction that the phase separation, while robust, is anomalously slow: domain sizes grow with time t as log t. It is important to note that the behaviour obtained exactly for the above special values of parameters can be shown to apply much more generally. This phase separation, in terms applicable to a real crystalline suspension, leads to macroscopic particle-rich and particlepoor regions. In the middle of each such region, one expects a fracture separating regions of opposite tilt. There are preliminary reports of such behaviour in experiments53, and it is tempting to think that some recent observations15 of the collapse of elastic aggregates in suspension are related to the above ideas, but this is mere speculation at this point. Detailed experiments on large, single-crystalline fluidized beds are needed to test the model. Velocity fluctuations in fluidized beds Hard-sphere suspensions, in which the only interactions are hydrodynamic, are a subject of continuing interest to fluid dynamicists, as should be clear from a glance at current issues of fluid mechanics journals (or physics journals, for that matter). In practice, these suspensions are chargestabilized, with ionic strength so large that electrostatics is screened within a tiny distance of the particle surface33, making the particles effectively hard spheres. Up to volume fractions of about 0.5, the particles in these suspensions Figure 1. A schematic picture of the final state of phase separation of the one-dimensional model: The tilt field has been summed to give the height of the profile at each point, the filled circles denote pluses and the open circles minuses. It is clear that for the phase separation to undo itself a plus, for example, must climb a distance of order 1/4 of the system size. The time for this to happen diverges exponentially with system size. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS have only short-ranged positional correlations, and move freely. They are thus fluid suspensions unlike the crystalline suspensions we discussed earlier. The suspensions of our interest are made of large particles (several microns in size), so that Brownian motion is unimportant, but (as discussed earlier) there is nonetheless a substantial random component to the motion if the system is sedimenting or sheared. Single-component suspensions are themselves the home of many mysteries, as the references in earlier sections will bear out, while two (or more) -component suspensions31,54 are understood even less. I will focus on just one puzzle in monodisperse suspensions, and on what I believe is its resolution using methods imported from time-dependent statistical mechanics. Until recently, theory and experiment disagreed rather seriously on the nature of velocity fluctuations in these suspensions in steady-state sedimentation. A simple theory19 predicted that σv(L), the standard deviation of the velocity of the particles sedimenting in a container of size L, L , should diverge as while experiments20,21 saw no such dependence (For a dissenting voice, see Tory et al.55). More precisely, Segrè et al.21 see size dependence for L smaller than a ‘screening length’ ξ~ 30 interparticle spacings, but none for L > ξ. Further confusion is provided by direct numerical simulations which do seem to see the sizedependence56, although these contain about 30,000 particles, which, while that sounds large, means they are only about 30 particles on a side, which probably just means that these huge simulations have not crossed the scale ξof Segrè et al.21! It is important to note that experiments in this area are frequently done by direct imaging of the particles at each time (Particle Imaging Velocimetry or PIV, see Adrian57). Since motions are slow (velocities of a few µm/s), this is relatively easy to do. Once the data on particle positions are stored, they can be analysed in detail on a computer and objects of interest such as correlation functions extracted. This is one of the nice things about the field of suspension science: problems of genuine interest to practitioners of statistical physics arise and can be studied in relatively inexpensive experiments, which measure quite directly the sorts of quantities a theoretician can calculate. Our contribution to this issue22,23 is to formulate the problem in the form of generalized Langevin equations, and then use methods well-known in areas such as dynamical critical phenomena to construct a phase diagram for sedimenting suspensions. Our approach is close in spirit to that of Koch and Shaqfeh58, but differs in detail and predicitive power. We find that there are two possible nonequilibrium ‘phases’, which we term ‘screened’ and ‘unscreened’, for a steadily sedimenting suspension. In the screened phase, σv (L) is independent of L, while in the unscreened phase, it diverges as in Caflisch and Luke19. The two phases are separated by a boundary which has the characteristics of a continuous phase transition, in that a CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 certain correlation length diverges there in a power-law manner. Although the relation between the parameters in terms of which our phase diagram is drawn and conventional suspension properties is still somewhat uncertain, we believe that the screened and unscreened phases should occur respectively at large and small Peclet numbers. Properties such as particle shape (aspect ratio) and Reynolds number also probably play a role in determining where in our phase diagram a given system lies. Let us begin by reconstructing the prediction of Caflisch and Luke19. Let δ v(r) and δ c(r) be respectively the local velocity and concentration fluctuations about the mean in a steadily sedimenting suspension, each of whose particles has a buoyancy-reduced weight mRg. Then, ignoring inertia, the balance between gravitational (acceleration g) and viscous (viscosity η) force densities is expressed in the relation η∇2δv ~ mRgδc(r, t). This implies that a concentration fluctuation at the origin leads to a velocity field ~ g/(ηr) a distance r away. Now, if you assume, with Caflisch and Luke19, that the δc’s are completely random in space or have at best a finite range of correlations, the variance 〈|δv|2〉 due to all the concentration fluctuations is obtained by simply squaring and adding incoherently giving, for a container of finite volume L3, (g/η)2 ∫d 3r (1/r2) ~ L. What this tells us, really, is that either 〈|δv|2〉 diverges or the concentration fluctuations are strongly anticorrelated at large length scales. What we should do, therefore, is not assume a spectrum of concentration fluctuations and calculate the velocity variance, but calculate both of them. To this end, let me first summarize the construction of the equations of motion for the suspension. Our description is phenomenological, to precisely the same extent as a continuum Ginzburg–Landau model or its time-dependent analogue for an equilibrium phase transition problem such as phase separation in a binary fluid. Our construction is constrained by the following general principles, each of which plays an indispensable role: (i) We need to keep track only of the slowest variables in the problem. (ii) Assuming our suspension has not undergone a phase transition into a state where some invariance (translation, rotation) is spontaneously broken, the only slow variables are the local densities of conserved quantities. For an incompressible suspension, these are just the particle concentration and the suspension momentum density (effectively, for a dilute suspension, the fluid velocity field). (iii) To get the long wavelength physics right, we can work at leading order in a gradient expansion. (iv) We must keep all terms not explicitly forbidden on grounds of symmetry, and impose no relations amongst the phenomenological parameters other than those forced on us by the symmetries of the problem. (v) Since the microscopic Stokesian dynamics shows chaotic behaviour and diffusion (see earlier sections), our coarse-grained model, since it is an effective description for the long-wavelength degrees of freedom, should contain stochastic terms (a direct effect of the 407 SPECIAL SECTION: eliminated fast degrees of freedom) as well as diffusive terms (an indirect effect) but with no special (fluctuation– dissipation) relation between them. Since only a limited range of modes (say, with wave numbers larger than a cutoff scale Λ, of order an inverse interparticle spacing) have been eliminated, the resulting noise can have correlations only on scales smaller than Λ–1. As far as a description on scales >> Λ–1 is concerned, the noise can be treated as spatially uncorrelated. This approach, we argue, should yield a complete, consistent description of the longtime, long-wavelength properties of the system in question. These premises accepted, one is led inevitably to a stochastic advection–diffusion equation ∂δc 2 + δv ·∇δc = [D⊥∇⊥ + Dz∇2z ]δc + ∇ · f(r, t), ∂t (5) for the concentration field δc and the Stokes equation η∇2δvi(r, t) = mR gPizδc(r, t). S (q ) = (6) for the velocity field δv. Equation (6) simply says that a local concentration fluctuation, since the particles are heavier than the solvent, produces a local excess force density which is balanced by viscous damping. In eq. (5), are respectively the projectors along and normal to the zδ ijz and δ ij⊥ axis, which is the direction of sedimentation. Incompressibility (∇ · δ v = 0) has been used to eliminate the pressure field in eq. (6) by means of the transverse projector Pij (in Fourier space Pij(q) = δij –q iq j/q 2). Equation (5) contains the advection of the concentration by the velocity, an anisotropic hydrodynamic diffusivity (D⊥, Dz), and a noise or random particle current f(r, t). The last two are of course a consequence of the eliminated small-scale chaotic modes. The noise is taken, reasonably, to have Gaussian statistics with mean zero and covariance 〈 fi (r , t) f j (r ′, t ′)〉 = c0 ( N ⊥δ ⊥j + N z δijz )δ( r − r ′)δ (t − t ′) , (7) where c0 is the mean concentration. In an ideal nonBrownian system, the noise variances (N⊥, Nz) and the diffusivities (D⊥, Dz) should, on dimensional grounds, scale (at fixed volume fraction) as the product of the Stokesian settling speed and the particle radius. However, no further relation between the noise and the diffusivities may be assumed, since this is a nonequilibrium system. In laboratory systems there will of course be in addition a thermal contribution to both noise and diffusivities. In either case, what matters, and indeed plays a crucial role in our nonequilibrium phase diagram, is that the parameter K ≡ N⊥Dz – D⊥Nz (8) is in general nonzero. Since at equilibrium the ratio of noise 408 strength to kinetic coefficient is a temperature, K measures the anisotropy of the effective ‘temperature’ for this driven system. As a first step towards extracting the behaviour of correlation functions and hence the velocity variance, note that eqs (5) and (6) can be solved exactly if the nonlinear term in eq. (5) is ignored. This amounts to allowing concentration fluctuations to produce velocity fluctuations while forgetting that the latter must then advect the former. If we do this, then it is straightforward to see by Fouriertransforming eq. (5) that the the static structure factor S(q) ≡ c0–1 ∫r e–iq·r 〈δc(0)δc(r)〉 (where the angle brackets denote an average over the noise) for concentration fluctuations with wave vector q = (q⊥, qz) in a suspension with mean concentration c0 is N ⊥ q 2⊥ + N z q 2z D ⊥ q 2⊥ + D z q 2z , (9) and is hence independent of the magnitude of q. In particular, it is therefore non-vanishing at small q. This can quickly be seen to imply, through eq. (6), that the velocity variance diverges exactly as in Caflisch and Luke19. In other words, Caflisch and Luke19 fail to take into account the hydrodynamic interaction between concentration fluctuations. If nonlinearities are to change this, they must leave the noise relatively unaffected while causing the relaxation rate (D⊥q ⊥2 + Dzq 2z in the linearized theory) to become nonzero at small q. This, if it happens, would be called ‘singular diffusion’ since diffusive relaxation rates normally vanish at small wave number. We shall see below that this does happen, in a substantial part of the parameter space of this problem. More precisely, we have been able to show22,23, in a fairly technical and approximate ‘self-consistent’ calculation which I shall not present here, that the behaviour once the advection term is included depends on the temperature anisotropy parameter K defined in eq. (8). If K = 0, i.e. if the noise and the diffusivities happen to obey a fluctuation– dissipation relation, then the static structure factor is totally unaltered by the advective nonlinearity, and therefore the velocity variance diverges as in Caflisch and Luke19. If K is larger than a critical value Kc , i.e. the fluctuations injected by the noise are substantially more abundant for wave vectors in the xy plane than for those along z, then there is a length scale ξ such that S(q) → 0 for qξ<< 1 with q ⊥ >> q z. Thus the velocity variance is finite, and independent of system size L for L > ξ. We call this ‘screening’, and the regions K > Kc and K < Kc as the screened and unscreened phases, respectively. A schematic phase diagram is given in Figure 2. However, ξ diverges as K → Kc . For K < Kc , according to preliminary calculations, the long-wavelength behaviour is the same as that at K = 0, although a detailed renormalization-group calculation to establish this is still in progress. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS Let me try to provide a qualitative understanding of these results. The basic question is: how does an imposed longwavelength inhomogeneity in the solute concentration decay in a steadily sedimenting suspension? It can, of course, always do so by hydrodynamic diffusion. In addition, it can scatter off the background of chaos-induced fluctuations, which I will call noise-injected fluctuations (NIF). This scattering is best thought of as the advection of the imposed inhomogeneity by the velocity field produced by the NIF. So consider two cases: (a) where the NIF has wave vector predominantly along z, and (b) where the wave vector is mainly in the xy plane. In (a), the induced flow has a z-velocity which alternates in sign as a function of z. The advection of the imposed inhomogeneity by this flow will concentrate it further, in general, thus enhancing the perturbation. In case (b), i.e. when the NIF has variation mainly along xy, the resulting z-velocity will alternate in sign along x and y, which will break up the inhomogeneity. Thus, a noise with Fourier components only with wave vector along z would give a negative contribution to the damping rate due to scattering, while one with Fourier components with wave vector only orthogonal to z would give a purely positive contribution. In general, it is thus clear that this mechanism gives a correction to the damping rate proportional to N⊥ – Nz (assuming, for simplicity, the same diffusivity in all directions). In addition, the long-ranged nature of the hydrodynamic interaction means that no matter how long-wavelength the NIF, it will produce macroscopic flows on scales comparable to its wavelength (and instantaneously, in the Stokesian approximation), hence the singular diffusion. In addition, we predict the form of static and dynamic correlation functions of the concentration or the velocity fields in detail, in the screened and unscreened phases as well as at the transition between them22,23. Very careful experiments, in particular some light scattering measurements at very small angles, are currently underway to test our predictions. We close this section by remarking that ours is not the only candidate theory of the statistics of fluctuations in zero Reynolds number fluidized beds. An earlier, nominally more microscopic approach58 had some similar conclusions; we, however, disagree with that work in several details. There are some who criticize the experiments of Segrè21 because they are done in narrow cells which could introduce finite size effects. There is also a very qualitative set of arguments59 based on an analogy with high Prandtl number turbulence; it is unclear at this stage whether that work is a recasting of our theory of the screened phase or distinct from it. Conclusion This review has tried to summarize experimental and theoretical work in the area of suspension hydrodynamics, CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 Figure 2. Schematic phase diagram for steadily sedimenting hard spheres (after Levine et al.22 ). On the dashed line and, we conjecture, near it, the structure factor is as in the linearized theory, and screening fails. The solid curve is the phase boundary between the screened and unscreened regions. from the point of view of a physicist interested in nonequilibrium statistical mechanics. The major aim has been to convince condensed matter physicists in India that this is a field which merits their attention. Apart from listing a large number of general references, I have tried to support my case by describing some problems on which I have worked, which have their origins squarely within suspension science, but whose solutions required all the machinery of statistical mechanics and used in a crucial way the fact that the systems concerned were not at thermal equilibrium. I hope this article will win some converts to this wonderful field. 1. Russel, W. B., Saville, D. A. and Schowalter, W. R., Colloidal Dispersions, Cambridge University Press, 1989. 2. Hulin, J. P., Hydrodynamics of Dispersed Media, Elsevier, North-Holland, 1990. 3. Einstein, A., Ann. Phys., 1906, 19, 289. 4. von Smoluchowskii, M., Phys. Zeit., 1916, 17, 55, and other papers cited in ref. 5. 5. Chandrasekhar, S., Rev. Mod. Phys., 1943, 15, 1. 6. Batchelor, G. K., J. Fluid Mech., 1970, 41, 545; ibid, 1972, 52, 245. 7. Ackerson, B. J. and Clark, N. A., Phys. Rev. A, 1984, 30, 906. 8. Lindsay, H. M. and Chaikin, P. M., J. Phys. Colloq., 1985, 46, C3–269. 9. Stevens, M. J., Robbins, M. O. and Belak, J. F., Phys. Rev. Lett., 1991, 66, 3004; Stevens, M. J. and Robbins, M. O., Phys. Rev. E, 1993, 48, 3778. 10. Ramaswamy, S. and Renn, S. R., Phys. Rev. Lett., 1986, 56, 945; Bagchi, B. and Thirumalai, D., Phys. Rev. A, 1988, 37, 2530. 11. Lahiri, R. and Ramaswamy, S., Phys. Rev. Lett., 1994, 73, 1043. 12. Lahiri, R., Ph D Thesis, Indian Institute of Science, 1997. 13. Palberg, T. and Würth, M., J. Phys. I, 1996, 6, 237. 14. Tirumkudulu, M., Tripathi, A. and Acrivos, A., Phys. Fluids, 1999, 11, 507. 409 SPECIAL SECTION: 15. Poon, W. C.-K., Pirie, A.. and Pusey, P. N., J. Chem. Soc. Faraday Discuss., 1995, 101, 65; Poon, W. C.-K. and Meeker, S. P., unpublished; Allain, C., Cloitre, M. and Wafra, M., Phys. Rev. Lett., 1995, 74, 1478. 16. Lahiri, R. and Ramaswamy, S., Phys. Rev. Lett., 1997, 79, 1150. 17. Ramaswamy, S,. in Dynamics of Complex Fluids (eds Adams, M. J., Mashelkar, R. A., Pearson, J. R. A. and Rennie, A. R.), Imperial College Press, The Royal Society, 1998. 18. Petrov, V. G. and Edissonov, I., Biorheology, 1996, 33, 353. 19. Caflisch, R. E. and Luke, J. H. C., Phys. Fluids, 1985, 28, 759. 20. Nicolai, H. and Guazzelli, E., Phys. Fluids, 1995, 7, 3. 21. Segrè, P. N., Herbolzheimer, E. and Chaikin, P. M., Phys. Rev. Lett., 1997, 79, 2574. 22. Levine, A., Ramaswamy, S., Frey, E. and Bruinsma, R., Phys. Rev. Lett., 1998, 81, 5944. 23. Levine, A., Ramaswamy, S., Frey, E. and Bruinsma, R., in Structure and Dynamics of Materials in the Mesoscopic Domain (eds Kulkarni, B. D. and Moti Lal), Imperial College Press, The Royal Society, (in press). 24. Davis, R. H., in Sedimentation of Small Particles in a Viscous Fluid (ed. Tory, E. M.), Computational Mechanics Publications, Southampton, 1996. 25. Davis, R. H. and Acrivos, A., Annu. Rev. Fluid Mech., 1985, 17, 91. 26. Farr, R. S., Melrose, J. R. and Ball, R. C., Phys. Rev. E, 1997, 55, 7203; Laun, H. M., J. Non-Newt. Fluid Mech., 1994, 54, 87. 27. Liu, S. J. and Masliyah, J. H., Adv. Chem., 1996, 251, 107. 28. Ham, J. M. and Homsy, G. M., Int. J. Multiphase Flow, 1988, 14, 533. 29. Nott, P. R. and Brady, J. F., J. Fluid Mech., 1994, 275, 157. 30. Van Saarloos, W. and Huse, D. A., Europhys. Lett., 1990, 11, 107. 31. Chu, X. L., Nikolov, A. D. and Wasan, D. T., Chem. Eng. Commun., 1996, 150, 123. 32. Kesavamoorthy, R., Sood, A. K., Tata, B. V. R. and Arora, A. K., J. Phys. C, 1988, 21, 4737. 33. Sood, A. K., in Solid State Physics (eds Ehrenreich, H. and Turnbull, D.), Academic Press, 1991, 45, 1. 34. Sheared suspensions are an old subject: see Reynolds, O., Philos. Mag., 1885, 20, 46. 35. Blanc, R. and Guyon, E., La Recherche, 1991, 22, 866. 36. Schmittmann, B. and Zia, R. K. P., in Phase Transitions and Critical Phenomena (eds Domb, C. and Lebowitz, J. L.), Academic Press, 1995, vol. 17. 37. Happel, J. and Brenner, H., Low Reynolds Number Hydrodynamics, Martinus Nijhoff, 1986. 410 38. Batchelor, G. K., An Introduction to Fluid Mechanics, Cambridge University Press, Cambridge, 1967. 39. Lamb, H., Hydrodynamics, Dover, New York, 1984. 40. Kim, S. and Karrila, S. J., Microhydrodynamics, Butterworths, 1992. 41. Stokes, G. G., Proc. Cambridge Philos. Soc., 1845, 8, 287; ibid, 1851, 9, 8. 42. Brady, J. F. and Bossis, G., Annu. Rev. Fluid Mech., 1988, 20, 111. 43. Jánosi, I. M., Tèl, T., Wolf, D. E. and Gallas, J. A. C., Phys. Rev. E, 1997, 56, 2858. 44. Ramakrishnan, T. V. and Yussouff, M., Phys. Rev. B, 1979, 19, 2775; Ramakrishnan, T. V., Pramana, 1984, 22, 365. 45. Rutgers, M. A., Ph D thesis, Princeton University, 1995; Rutgers, M. A., Xue, J.-Z., Herbolzheimer, E., Russel, W. B. and Chaikin, P. M., Phys. Rev. E, 1995, 51, 4674. 46. See, e.g. Balents, L., Marchetti, M. C. and Radzihovsky, L., Phys. Rev. B, 1998, 57, 7705. 47. Crowley, J. M., J. Fluid Mech., 1971, 45, 151; Phys. Fluids, 1976, 19, 1296. 48. Landau, L. D. and Lifshitz, E. M., Theory of Elasticity, Pergamon Press, Oxford, 1965. 49. Martin, P. C., Parodi, O. and Pershan, P. S., Phys. Rev. A, 1972, 6, 2401. 50. Forster, D., Hydrodynamic Fluctuations, Broken Symmetry and Correlation Functions, Benjamin, Reading, 1980. 51. Simha, R. A. and Ramaswamy, S., cond-mat 9904105, submitted to Phys. Rev. Lett., 1999. 52. Lahiri, R., Barma, M. and Ramaswamy, S., cond.-mat/9907342, submitted to Phys. Rev. E. 53. Chaikin, P. M., personal communication. 54. Batchelor, G. K. and Janse van Rensburg, W., J. Fluid Mech., 1986, 166, 379. 55. Tory, E. M., Kamel, M. T. and Chan Man Fong, C. F., Powder Technol., 1992, 73, 219. 56. Ladd, A. J. C., Phys. Rev. Lett., 1996, 76, 1392. 57. Adrian, R. J., Annu. Rev. Fluid Mech., 1991, 23, 261. 58. Koch, D. L. and Shaqfeh, E. S. G., J. Fluid Mech., 1991, 224, 275. 59. Tong, P. and Ackerson, B. J., Phys. Rev. E, 1998, 58, R6931. ACKNOWLEDGEMENT. with figures. I thank R. A. Simha and C. Das for help CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS Vehicular traffic: A system of interacting particles driven far from equilibrium§ Debashish Chowdhury*,†, Ludger Santen** and Andreas Schadschneider** *Department of Physics, Indian Institute of Technology, Kanpur 208 016, India and Institute for Theoretical Physics, University of Cologne, D-50923 Köln, Germany **Institute for Theoretical Physics, University of Cologne, D-50923 Köln, Germany In recent years statistical physicists have developed discrete ‘particle-hopping’ models of vehicular traffic, usually formulated in terms of cellular automata, which are similar to the microscopic models of interacting charged particles in the presence of an external electric field. Concepts and techniques of non-equilibrium statistical mechanics are being used to understand the nature of the steady states and fluctuations in these socalled microscopic models. In this brief review we explain, primarily to nonexperts, these models and the physical implications of the results. A RE you surprised to see an article on vehicular traffic in this special section of Current Science where physicists are supposed to report on some recent developments in the area of dynamics of nonequilibrium statistical systems? Aren’t civil engineers (or, more specifically, traffic engineers) expected to work on traffic? Solving traffic problems would become easier if one knows the fundamental laws governing traffic flow and traffic jam. For almost half a century physicists have been trying to develop a theoretical framework of traffic science, extending concepts and techniques of statistical physics1–6. The main aim of this brief review is to show how these attempts, particularly the recent ones, have led to deep insight in this frontier area of inter-disciplinary research. The dynamical phases of systems driven far from equilibrium are counterparts of the stable phases of systems in equilibrium. Let us first pose some of the questions that statistical physicists have been addressing in order to discover the fundamental laws governing vehicular traffic. For example, (i) What are the various dynamical phases of traffic? Does traffic exhibit phase-coexistence, phase transition, criticality or self-organized criticality and, if so, under which circumstances? (ii) What is the nature of fluctuations around the steadystates of traffic? † For correspondence (e-mail: debch@thp.Uni-koeln.DE) This is a modified and shortened version of a longer detailed review article to be published elsewhere. § CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 (iii) If the initial state is far from a stationary state of the driven system, how does it evolve with time to reach a true steady-state? (iv) What are the effects of quenched disorder (i.e. timeindependent disorder) on the answers to the questions posed in (i)–(iii) above? The microscopic models of vehicular traffic can find practical applications in on-line traffic control systems as well as in the planning and design of transportation network. There are two different conceptual frameworks for modelling vehicular traffic. In the ‘coarse-grained’ fluiddynamical description, the traffic is viewed as a compressible fluid formed by the vehicles but these individual vehicles do not appear explicitly in the theory. In contrast, in the ‘microscopic’ models traffic is treated as a system of interacting ‘particles’ driven far from equilibrium where attention is explicitly focused on individual vehicles, each of which is represented by a ‘particle’; the nature of the interactions among these particles is determined by the way the vehicles influence each others’ movement. Unlike the particles in a gas, a driver is an intelligent agent who can ‘think’, make individual decisions and ‘learn’ from experience. Nevertheless, many phenomena in traffic can be explained in general terms with these models provided the behavioural effects of the drivers are captured by only a few phenomenological parameters. The conceptual basis of the older theoretical approaches is explained briefly in the next section. Most of the ‘microscopic’ models developed in the recent years are ‘particle-hopping’ models which are usually formulated using the language of cellular automata (CA)7. The Nagel– Schreckenberg (NaSch)8 model and the Biham–Middleton– Levine (BML)9 model, which are the most popular CA models of traffic on idealized highways and cities, respectively, have been extended by several authors to develop more realistic models. Some of the most interesting aspects of these recent developments are discussed here. The similarities between various particle-hopping models of traffic and some other models of systems, which are also far from equilibrium, are pointed out followed by the concluding section. 411 SPECIAL SECTION: Older theories of vehicular traffic Fluid-dynamical theories of vehicular traffic In traffic engineering, the fundamental diagram depicts the relation between density c and the flux J, which is defined as the number of vehicles crossing a detector site per unit time10. Because of the conservation of vehicles, the local density c(x; t) and local flux J(x; t) satisfy the equation of continuity which is the analogue of the equation of continuity in the hydrodynamic theories of fluids. In the early works12 it was assumed that (i) the flux (or, equivalently, the velocity) is a function of the density; and (ii) following any change in the local density, the local speed instantaneously relaxes to a magnitude consistent with the new density at the same location. However, for a more realistic description of traffic, in the recent fluiddynamical treatments13–15 of traffic an additional equation (the analogue of the Navier–Stokes equation for fluids), which describes the time-dependence of the velocity V(x; t), has been considered. This approach, however, has its limitations; for example, viscosity of traffic is not a directly measurable quantity. Kinetic theory of vehicular traffic In the kinetic theory of traffic, one begins with the basic quantity g(x, v, w; t) dx dv dw which is the number of vehicles, at time t, located between x and x + dx, having actual velocity between v and v + dv and desired velocity between w and w + dw. In this approach, the fundamental dynamical equation is the analogue of the Boltzmann equation in the kinetic theory of gases3. Assuming reasonable forms of ‘relaxation’ and ‘interaction’, the problem of traffic is reduced to that of solving the Boltzmann-like equation, a formidable task, indeed16–18! Car-following theories of vehicular traffic In the car-following theories one writes, for each individual vehicle, an equation of motion which is the analogue of the Newton’s equation for each individual particle in a system of interacting classical particles. In Newtonian mechanics, the acceleration may be regarded as the response of the particle to the stimulus it receives in the form of force which includes both the external force as well as those arising from its interaction with all the other particles in the system. Therefore, the basic philosophy of the car-following theories1,2 can be summarized by the equation [Response]n ∝ [Stimulus]n, Cellular-automata models of highway-traffic In the car-following models, space is treated as a continuum and time is represented by a continuous variable t, while velocities and accelerations of the vehicles are also real variables. However, most often, for numerical manipulations of the differential equations of the car-following models, one needs to discretize the continuous variables with appropriately chosen grids. In contrast, in the CA models of traffic not only time but also the position, speed, and acceleration of the vehicles are treated as discrete variables. In this approach, a lane is represented by a one-dimensional lattice. Each of the lattice sites represents a ‘cell’ which can be either empty or occupied by at most one ‘vehicle’ at a given instant of time (see Figure 1). At each discrete time step t → t + 1, the state of the system is updated following a well-defined prescription. Nagel–Schreckenberg model of highway traffic In the NaSch model, the speed V of each vehicle can take one of the Vmax + 1 allowed integer values V = 0, 1, . . ., Vmax . Suppose, Xn and Vn denote the position and speed, respectively, of the nth vehicle. Then, d n = Xn + 1 – Xn, is the gap in between the nth vehicle and the vehicle in front of it at time t. At each time step t → t + 1, the arrangement of the N vehicles on a finite lattice of length L is updated in parallel according to the following ‘rules’: Step 1: Acceleration. If Vn < Vmax , the speed of the nth vehicle is increased by one, but Vn remains unaltered if Vn = Vmax , i.e. Vn → min(Vn + 1, Vmax ). Step 2: Deceleration (due to other vehicles). If d n ≤ Vn, the speed of the nth vehicle is reduced to d n – 1, i.e. (1) for the nth vehicle (n = 1, 2, . . .). The constant of proportionality in eq. (1) can be interpreted as a measure of the sensitivity coefficient of the driver; it indicates how 412 strongly the driver responds to unit stimulus. Each driver can respond to the surrounding traffic conditions only by accelerating or decelerating the vehicle. The stimulus and the sensitivity factor are assumed to be functions of the position and speed of the vehicle under consideration and those of its leading vehicle. Different forms of the equations of motion of the vehicles in the different versions of the carfollowing models arise from the differences in their postulates regarding the nature of the stimulus. In general, the dynamical equations for the vehicles in the carfollowing theories are coupled non-linear differential equations19–25 and thus, in this ‘microscopic’ approach, the problem of traffic flow reduces to problems of nonlinear dynamics. Figure 1. Typical configuration in a CA model. The number in the upper right corner is the speed of the vehicle. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS Vn → min(Vn, d n – 1). Step 3: Randomization. If Vn > 0, the speed of the nth vehicle is decreased randomly by unity with probability p but Vn does not change if Vn = 0, i.e. Vn → max(Vn – 1, 0) with probability p. Step 4: Vehicle movement. Each vehicle is moved forward so that Xn → Xn + Vn. The NaSch model is a minimal model in the sense that all the four steps are necessary to reproduce the basic features of real traffic; however, additional rules need to be formulated to capture more complex situations. Step 1 reflects the general tendency of the drivers to drive as fast as possible, if allowed to do so, without crossing the maximum speed limit. Step 2 is intended to avoid collision between the vehicles. The randomization in step 3 takes into account the different behavioural patterns of the individual drivers, especially, nondeterministic acceleration as well as overreaction while slowing down; this is crucially important for the spontaneous formation of traffic jams. So long as p ≠ 0, the NaSch model may be regarded as stochastic CA7. For a realistic description of highway traffic8, the typical length of each cell should be about 7.5 m and each time step should correspond to approximately 1 sec of real time when Vmax = 5. The update scheme of the NaSch model is illustrated with a simple example in Figure 2. Space-time diagrams showing the time evolutions of the NaSch model demonstrate that no traffic jam is present at sufficiently low densities, but spontaneous fluctuations give rise to traffic jams at higher densities (Figure 3 a). From Figure 3 b it should be obvious that the intrinsic stochasticity of the dynamics8, arising from non-zero p, is essential for triggering the jams8,26. The use of parallel dynamics is also important. In contrast to a random sequential update, it can lead to a chain of overreactions. Suppose, a vehicle slows down due the randomization step. If the density of vehicles is large enough this might force the following vehicle also to brake in the deceleration step. In addition, if p is not too small, it might brake even further in step 3. Eventually this can lead to the stopping of a vehicle, thus creating a traffic jam. This mechanism of spontaneous jam formation is rather realistic and cannot be modelled by the random sequential update. Relation between NaSch model and asymmetric simple exclusion process In the NaSch model with Vmax = 1, every vehicle moves forward with probability q = 1 – p in the time step t + 1 if the site immediately in front of it were empty at the time step t; this is similar to the fully asymmetric simple exclusion process (ASEP)27,29, where a randomly chosen particle can move forward with probablity q if the site immediately in front is empty. But, updating is done in parallel in the NaSch CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 model whereas that in the ASEP is done in a random sequential manner. Nevertheless, the special case of Vmax = 1 for the NaSch model derives special importance from the fact that so far it has been possible to derive exact analytical results for the NaSch model only in the special limits (a) Vmax = 1 and arbitrary p and (b) p = 0 and arbitrary Vmax . NaSch model in the deterministic limits If p = 0, the system can self-organize so that at low densities every vehicle can move with Vmax and the corresponding flux is cVmax ; this is, however, possible only if enough empty cells are available in front of every vehicle, i.e. for c ≤ cmdet = (Vmax + 1)–1 and the corresponding maximum flux is Jmdeatx= Vmax /(Vmax + 1). On the other hand, for c > the flow is limited by the density of holes. Hence, the fundamental diagram in the deterministic limit p = 0 of the NaSch model (for any arbitrary Vmax ) is (a) (b) (c) (d) Figure 2. Step-by-step example for the application of the update rules. We have assumed Vmax = 2 and p = 1/3. Therefore, on average one-third of the cars qualifying will slow down in the randomization step. 413 c det m , SPECIAL SECTION: given by the exact expression J = min (cVmax , (1 – c)). Aren’t the properties of the NaSch model with maximum allowed speed Vmax , in the deterministic limit p = 1, exactly identical to those of the same model with maximum allowed speed Vmax – 1? The answer to the question posed above is ‘No’; if p = 1, all random initial states lead to J = 0 in the stationary state of the NaSch model irrespective of Vmax and c! Analytical theory for the NaSch model In the ‘site-oriented’ theories one describes the state of the finite system of length L by completely specifying the state of each site. In contrast, in the ‘car-oriented’ theories the state of the traffic system is described by specifying the positions and speeds of all the N vehicles in the system. In the naive mean-field approximation, one treats the probabilities of occupation of the lattice sites as independent of each other. In this approximation, for example, the steady-state flux for the NaSch model with Vmax = 1 and periodic boundary conditions, one gets30 J = qc (1 – c). (2) It turns out30 that the naive mean-field theory underestimates the flux for all Vmax . Curiously, if instead of parallel updating one uses the random sequential updating, the NaSch model with Vmax = 1 reduces to the ASEP for which the eq. (2) is known to be the exact expression for the corresponding flux (see, e.g. Nagel and Schreckenberg8)! What are the reasons for these differences arising from parallel updating and random sequential updating? There are ‘Garden of Eden’ (GoE) states (dynamically forbidden states) 31 of the NaSch model which cannot be reached by the parallel updating, whereas no state is dynamically forbidden if the updating is done in a random sequential manner. For example, the configuration shown in Figure 4 is a GoE state (The configuration shown in Figure 1 is also a GoE state!) because it could occur at time t only if the two vehicles occupied the same cell simultaneously at time t – 1. The naive mean-field theory mentioned above does not exclude the GoE states. The exact expression, given in the next subsection, for the flux in the steady-state of the NaSch model with Vmax = 1 can be derived by merely excluding these states from consideration in the naive mean-field theory31, thereby indicating that the only source of correlation in this case is the parallel updating. But, for Vmax > 1, there are other sources of correlation because of which exclusion of the GoE states merely improves the naive mean-field estimate of the flux but does not yield exact results31. A systematic improvement of the naive mean-field theory of the NaSch model has been achieved by incorporating short-ranged correlations through cluster approximations. We define a n-cluster to be a collection of n successive sites. In the general n-cluster approximation, one divides the lattice into ‘clusters’ of length n such that two neighbouring clusters have n – 1 sites in common (see Figure 5). If n = 1, then the 1-cluster approximation can be regarded Figure 3. Typical space–time diagrams of the NaSch model with Vmax = 5. a, p = 0.25, c = 0.20; b, p = 0.0, c = 0.5. Each horizontal row of dots represents the instantaneous positions of the vehicles moving towards right Figure while 4. theA successive GoE state for rows theofNaSch dots represent model with theVmax positions ≥ 2. of the same vehicles at the successive time steps. 414 CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS as the naive mean-field approximation. You can easily verify, for example, in the special case of Vmax = 1, that the state of the 2-cluster at time t + 1 depends on the state of the 4-cluster at time t, which, in turn, depends on the state of a larger cluster at time t – 1 and, so on. Therefore, one needs to make an approximation to truncate this hierarchy in a sensible manner. For example, in the 2-cluster approximation for the NaSch model with Vmax = 1, the 4cluster probabilities are approximated in terms of an appropriate product of 2-cluster probabilities. Thus, in the n-cluster approximation30 a cluster of n neighbouring cells are treated exactly and the cluster is coupled to the rest of the system in a self-consistent way. Carrying out the 2-cluster calculation30 for Vmax = 1, one not only finds an effective particle-hole attraction (particle– particle repulsion), but also obtains the exact result J (c, p ) = 12 [1 − 1 − 4 qc(1 − c) ] , (3) for the corresponding flux. But one gets only approximate results from the 2-cluster calculations for all Vmax > 1 (see Schadschneider32 for higher order cluster calculations for Vmax = 2 and comparison with computer simulation data). Let us explain the physical origin of the generic shape of the fundamental diagrams shown in Figure 6. At sufficiently low density of vehicles, practically ‘free flow’ takes place whereas at higher densities traffic becomes ‘congested’ and traffic jams occur. So long as c is sufficiently small, the average speed 〈V〉 is practically independent of c as the vehicles are too far apart to interact mutually. However, a faster monotonic decrease of 〈V〉 with increasing c takes place when the forward movement of the vehicles is strongly hindered by others because of the reduction in the average separation between them. Because of this trend of variation of 〈V〉 with c, the flux J = 〈cV〉 exhibits a maximum10 at cm; for c < cm, increasing c leads to increasing J whereas for c > cm sharp decrease of 〈V〉 with increase of c leads to the overall decrease of J. An interesting feature of the eq. (3) is that the flux is invariant under charge conjugation, i.e. under the operation c → (1 – c) which interchanges particles and holes. Therefore, the fundamental diagram is symmetric about c = 1/2 when Vmax = 1 (see Figure 6 a). Although this symmetry breaks down for all Vmax > 1 (see Figure 6 b), the corresponding fundamental diagrams appear more realistic. Moreover, for given p, the magnitude of cm decreases with increasing Vmax as the higher is the Vmax the longer is the effective range of interaction of the vehicles (see Figure 6 b). Furthermore, for Vmax = 1, flux merely decreases with increasing p (see eq. (3)), but remains symmetric about c = 1/2 = cm. On the other hand, for all Vmax > 1, increasing p not only leads to smaller flux but also lowers cm. Spatio-temporal organization of vehicles CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 The distance from a selected point on the lead vehicle to the same point on the following vehicle is defined as the distance-headway (DH)10. In order to get information on the spatial organization of the vehicles, one can calculate the DH distribution P dh(∆X) by following either a site-oriented approach33 or a car-oriented approach34 if ∆Xj = Xj – Xj – 1, i.e. if the number of empty lattice sites in front of the jth vehicle is identified as the corresponding DH. At moderately high densities, P dh(∆X) exhibits two peaks; the peak at ∆X = 1 is caused by the jammed vehicles while that at a larger ∆X corresponds to the most probable DH in the free-flowing regions. The time-headway is defined as the time interval between the departures (or arrivals) of two successive vehicles recorded by a detector placed at a fixed position on the highway10. The time-headway distribution contains information on the temporal organization. Suppose, P m (t1) is the probability that the following vehicle takes time t1 to reach the detector, moving from its initial position where it was located when the leading vehicle just left the detector site. Suppose, after reaching the detector site, the following vehicle waits there for τ – t1 time steps, either because of the presence of another vehicle in front of it or because of its own random braking; the probability for this event is denoted by Q(τ – t1|t1). The distribution P th(τ), of the time-headway τ, can be obtained from35,36 P th(τ) = P m (t1) Q(τ– t1|t1). The most-probable timeheadway, when plotted against the density, exhibits a minimum36; this is consistent with the well-known exact relation J = 1/Tav between flux and the average timeheadway, Tav. a b c Figure 5. Decomposition of a lattice into: a, 1-clusters; b, 2clusters; and c, 3-clusters in the cluster-theoretic approach to the NaSch model. 415 Στt1−=11 SPECIAL SECTION: Is there a phase transition from ‘free-flowing’ to ‘congested’ dynamical phase of the NaSch model? No satisfacory order parameter has been found so far37,38, except in the deterministic limit39. The possibility of the existence of any critical density in the NaSch model is ruled out by the observations 32,37,38,40 that, for all non-zero p, (a) the equal-time correlation function decays exponentially with separation, and (b) the relaxation time and lifetimes of the jams remain finite. This minimal model of highway traffic also does not exhibit any first order phase transition and two-phase co-existence35. Extensions of the NaSch model and practical applications In recent years, other minimal models of traffic on highways have been developed by modifying the updating rules of the NaSch model41–43. In the cruise control limit of the NaSch model44, the randomization step is applied only to vehicles which have a velocity V < Vmax after step 2 of the update rule. Vehicles moving with their desired velocity Vmax are not subject to fluctuations. This is exactly the effect of a cruise-control which automatically keeps the velocity constant at a desired value. Interestingly, the cruise-control limit of the NaSch model exhibits self-organized criticality45,46. Besides, a continuum limit of the NaSch model has also been considered47. The vehicles which come to a stop because of hindrance from the leading vehicle may not be able to start as soon as the leading vehicle moves out of its way; it may start with a probability q s < 1. When such possibilities are incorporated in the NaSch model, the ‘slow-to-start’ rules48–52 can give rise to metastable states of very high flux and hysteresis effects as well as phase separation of the traffic into a ‘freeflowing’ phase and a ‘mega-jam’. The bottleneck created by quenched disorder of the a highway usually slows down traffic and can give rise to jams35,53 and phase segregation54,55. However, a different type of quenched disorder, introduced by assigning randomly different braking probabilities p to different drivers in the NaSch model, can have more dramatic effects56,57 which are reminiscent of ‘Bose–Einstein-like condensation’ in the fully ASEP where particle-hopping rates are quenched random variables58,59. In such Bose– Einstein-like condensed states, finite fraction of the empty sites are ‘condensed’ in front of the slowest vehicle (i.e. the driver with highest p). Several attempts have been made to generalize the NaSch model to describe traffic on multi-lane highways and to simulate traffic on real networks in and around several cities60. For planning and design of the transportation network61, for example, in a metropolitan area62–64, one needs much more than just micro-simulation of how vehicles move on a linear or square lattice under a specified set of vehicle–vehicle and road–vehicle interactions. For such a simulation, to begin with, one needs to specify the roads (including the number of lanes, ramps, bottlenecks, etc.) and their intersections. Then, times and places of the activities, e.g. working, shopping, etc. of individual drivers are planned. Micro-simulations are carried out for all possible different routes to execute these plans; the results give information on the efficiency of the different routes and these informations are utilized in the designing of the transportation network61,65,66. Some socio-economic questions as well as questions on the environmental impacts of the planned transportation infrastructure also need to be addressed during such planning and design. Cellular-automata models of city-traffic The Biham–Middleton–Levin model of city traffic b Figure 6. Fundamental diagram in the NaSch model: a, Vmax = 1, and b, Vmax > 1, both for p = 0.25. The data for all Vmax > 1 have been obtained through computer simulations. 416 CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS and its generalizations In the BML model9, each of the sites of a square lattice represents the crossing of a east–west street and a north– south street. All the streets parallel to the X̂ - direction of a Cartesian coordinate system are assumed to allow only single-lane east-bound traffic while all those parallel to the direction allow only single-lane northbound traffic. In the initial state of the system, vehicles are randomly distributed among the streets. The states of eastbound vehicles are updated in parallel at every odd discrete time step whereas those of the north-bound vehicles are updated in parallel at every even discrete time step following a rule which is a simple extension of the fully ASEP: a vehicle moves forward by one lattice spacing if and only if the site in front is empty, otherwise the vehicle does not move at that time step. Computer simulations demonstrate that a first-order phase transition takes place in the BML model at a finite non-vanishing density c*, where the average velocity of the vehicles vanishes discontinuously signalling complete jamming; this jamming arises from the mutual blocking of the flows of east-bound and north-bound traffic at various crossings 67,68. Note that the dynamics of the BML model is fully deterministic and the randomness arises only from the random initial conditions69. As usual, in the naive mean-field approximation one neglects the correlations between the occupations of different sites70. However, if you are not interested in detailed information on the ‘structure’ of the dynamical phases, you can get a mean-field estimate of c* by carrying out a back-of-the-envelope calculation71–73. In the symmetric case cx = cy , for which v x = v y = v, c = c* ~ 0.343. The BML model has been extended to take into account the effects of (i) asymmetric distribution of the vehicles71, i.e. cx ≠ cy , (ii) overpasses or two-level crossings72 that are represented by specifically identified sites, each of which can accommodate up to a maximum of two vehicles simultaneously, (iii) faulty traffic lights74, (iv) static hindrances or road blocks or vehicles crashed in traffic accident, i.e. stagnant points75,76, (v) stagnant street where the local density cs of the vehicles is initially higher than that in the other streets77, (vi) jam-avoiding drive78 of vehicles to a neighbouring street, parallel to the original direction, to avoid getting blocked by other vehicles in front, (vii) turning of the vehicles from east-bound (northbound) to north-bound (east-bound) streets79, (viii) a single north-bound street cutting across east-bound streets80, (ix) more realistic description of junctions of perpendicular streets 81,82, and (x) green-waves83. Marriage of NaSch and BML models At first sight, the BML model may appear very unrealistic CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 because the vehicles seem to hop from one crossing to the next. However, it may not appear so unrealistic if each unit of discrete time interval in the BML model is interpreted as the time for which the traffic lights remain green (or red) before switching red (or green) simultaneously in a synchronized manner, and over that time scale each vehicle, which faces a green signal, gets an opportunity to move from jth crossing to the j + 1-th (or, more generally84, to the j + rth where r > 1). However, if one wants to develop a more detailed ‘finegrained’ description then one must first decorate each bond 85 with D – 1 (D > 1) sites to represent D – 1 cells between each pair of successive crossings, thereby modelling each segment of the streets between successive crossings in the same manner in which the entire highway is modelled in the NaSch model. Then, one can follow the prescriptions of the NaSch model for describing the positions, speeds and accelerations of the vehicles82,86 as well as for taking into account the interactions among the vehicles moving along the same street. Moreover, one should flip the colour of the signal periodically at regular interval of T (T >> 1) time steps where, during each unit of the discrete time interval every vehicle facing green signal should get an opportunity to move forward from one cell to the next. Such a CA model of traffic in cities has, indeed, been proposed very recently87 where the rules of updating have been formulated in such a way that, (a) a vehicle approaching a crossing can keep moving, even when the signal is red, until it reaches a site immediately in front of which there is either a halting vehicle or a crossing; and (b) no grid-locking would occur in the absence of random Figure 7. Typical jammed configuration of the vehicles. The eastbound and north-bound vehicles are represented by the symbols → and ↑, respectively. (N = 5, D = 8. 417 SPECIAL SECTION: braking. A phase transition from the ‘free-flowing’ dynamical phase to the completely ‘jammed’ phase has been observed in this model at a vehicle density which depends on D and T. The intrinsic stochasticity of the dynamics, which triggers the onset of jamming, is similar to that in the NaSch model, while the phenomena of complete jamming through self-organization as well as the final jammed configurations (Figure 7) are similar to those in the BML model. This model also provides a reasonable time-dependence of the average speeds of the vehicles in the ‘free-flowing’ phase87. Relation with other systems and phenomena You must have noticed in the earlier sections that some of the models of traffic are non-trivial generalizations or extensions of the ASEP, the simplest of the driven– dissipative systems which are of current interest in nonequilibrium statistical mechanics28. Some similarities between these systems and a dynamical model of protein synthesis have been pointed out 88. Another drivendissipative system, which is also receiving wide attention from physicists in recent years, is granular material flowing through a pipe4,5. There are some superficial similarities between the clustering of vehicles on a highway and particle–particle (and particle–cluster) aggregation process 89. The NaSch model with Vmax = 1 can be mapped on to stochastic growth models of one-dimensional surfaces in a two-dimensional medium. Particle (hole) movement to the right (left) corresponds to local forward growth of the surface via particle deposition. In this scenario, a particle evaporation would correspond to a particle (hole) movement to the left (right) which is not allowed in the NaSch model. It is worth pointing out that any quenched disorder in the rate of hopping between two adjacent sites would correspond to columnar quenched disorder in the growth rate for the surface55. Inspired by the recent success in theoretical studies of traffic, some studies of information traffic on the computer network (internet) have also been carried out90,92. Summary and conclusion Nowadays the tools of statistical mechanics are increasingly being used to study self-organization and emergent collective behaviour of complex systems many of which, including vehicular traffic, fall outside the traditional domain of physical systems. However, as we have shown in this article, a strong theoretical foundation of traffic science, can be built on the basic principles of statistical mechanics. 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E, 1999, 59, R1311; Chowdhury, D., Klauck, K., Santen, L., Schadschneider, A. and Zittartz, J., (to be published). 88. Schütz, G. M., Int. J. Mod. Phys. B, 1997, 11, 197. 89. Ben-Naim, E. and Krapivsky, P. L., Phys. Rev. E, 1997, 56, 6680. 90. Csabai, I., J. Phys. A., 1994, 27, L417. 91. Ohira, T. and Sawatari, R., Phys. Rev. E, 1998, 58, 193. 92. Takayasu, M., Yu Tretyakov, A., Fukuda, K. and Takayasu, H., in ref. 5. ACKNOWLEDGEMENTS. It is our pleasure to thank R. Barlovic, J. G. Brankov, B. Eisenblätter, K. Ghosh, N. Ito, K. Klauck, W. Knospe, D. Ktitarev, A. Majumdar, K. Nagel, V. B. Priezzhev, M. Schreckenberg, A. Pasupathy, S. Sinha, R. B. Stinchcombe and D. E. Wolf for enjoyable collaborations, the results of some of which have been reviewed here. We also thank M. Barma, J. Kertesz, J. Krug, G. Schütz, D. Stauffer and J. Zittartz for useful discussions and encouragements. This work is supported by SFB341 Köln-AachenJülich. 419 SPECIAL SECTION: Dynamical transitions in network models of collective computation Sitabhra Sinha* and Bikas K. Chakrabarti†§ *Department of Physics, Indian Institute of Science, Bangalore 560 012, India and Condensed Matter Theory Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore 560 064, India † Saha Institute of Nuclear Physics, 1/AF Bidhan Nagar, Calcutta 700 064, India The field of neural network modelling has grown up on the premise that the massively parallel distributed processing and connectionist structure observed in the brain is the key behind its superior performance. The conventional network paradigm has mostly centered around a static approach – the dynamics involves gradient descent of the network state to stable fixed-points (or, static attractors) corresponding to some desired output. Neurobiological evidence however points to the dominance of nonequilibrium activity in the brain, which is a highly connected, nonlinear dynamical system. This has led to a growing interest in constructing nonequilibrium models of brain activity –several of which show extremely interesting dynamical transitions. In this paper, we focus on models comprising elements which have exclusively excitatory or inhibitory synapses. These networks are capable of a wide range of dynamical behaviour, including high period oscillations and chaos. Both the intrinsic dynamics of such models and their possible role in information processing are examined. SINCE the development of the electronic computer in the 1940s, the serial processing computational paradigm has successfully held sway. It has developed to the point where it is now ubiquitous. However, there are many tasks which are yet to be successfully tackled computationally. A case in point is the multifarious activities that the human brain performs regularly, including pattern recognition, associative recall, etc. which are extremely difficult, if not impossible to do using traditional computation. This problem has led to the development of non-standard techniques to tackle situations at which biological information processing systems excel. One of the more successful of such developments aims at ‘reverseengineering’ the biological apparatus itself to find out why and how it works. The field of neural network models has grown up on the premise that the massively parallel distributed processing and connectionist structure observed in the brain is the key behind its superior performance. By implementing these features in the design of a new class of architectures and algorithms, it is hoped that machines will approach human-like ability in handling real-world situations. § For correspondence. (e-mail: bikas@emp.saha.ernet.in) 420 The complexity of the brain lies partly in the multiplicity of structural levels of organization in the nervous system. The spatial scale of such structures span about ten orders of magnitude – starting from the level of molecules and synapses, going all the way up to the entire central nervous system (Figure 1). The unique capabilities of the brain to perform cognitive tasks are an outcome of the collective global behaviour of its constituent neurons. This is the motivation for investigating the network dynamics of model neurons. Depending upon one’s purpose, such ‘neurons’ may be either, extremely simple binary threshold-activated elements, or, described by a set of coupled partial differential equations incorporating detailed knowledge of cellular physiology and action potential propagation. However, both simplifying and realistic neural models are based on the theory of nonlinear dynamical systems in highdimensional spaces1. The development of nonlinear dynamical systems theory – in particular, the discovery of ‘deterministic chaos’ in extremely simple systems – has furnished the theoretical tools necessary for analysing nonequilibrium network dynamics. Neurobiological studies indicating the presence of chaotic dynamics in the brain and the investigation of its possible role in biological information processing has provided further motivation. Figure 1. Structural levels of organization of the nervous system (from Churchland and Sejnowski1 ). CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS Actual networks of neuronal cells in the brain are extremely complex (Figure 2). In fact, even single neurons (Figure 3) are much more complicated than the ‘formal neurons’ usually used in modelling studies, and are capable of performing a large amount of computation2,3. To gain insight into the network properties of the nervous system, researchers have focused on artificial neural networks. These usually comprise of binary neurons (i.e. neurons capable of being only in one of two states), S i (= ± 1; i = 1, 2, . . ., N), whose temporal evolution is determined by the equation: S i = F (Σj Wij S j – θi), (1) where θi is an internal threshold, Wij is the connection weight from element j to element i, and F is a nonlinear function, most commonly taken as a sign or tanh (for continuous value S i) function. Different neural network models are specified by • network topology, i.e. the pattern of connections between the elements comprising the network; • characteristics of the processing element, e.g. the explicit form of the nonlinear function F, and the value of the threshold θ; • learning rule, i.e. the rules for computing the connection weights Wij appropriate for a given task, and, • updating rule, e.g. the states of the processing elements may be updated in parallel (synchronous updating), sequentially or randomly. One of the limitations of most network models at present is that they are basically static, i.e. once an equilibrium state is reached, the network remains in that state, until the arrival of new external input4. In contrast, real neural networks show a preponderance of dynamical behaviour. Once we recall a memory, our minds are not permanently stuck to it, but can also roll over and recall other associated memories without being prompted by any additional external stimuli. This ability to ‘jump’ from one memory to another in the absence of appropriate stimuli is one of the hallmarks of the brain. It is an ability which one should try to recreate in a network model if it is ever to come close to human-like performance in intellectual tasks. One of the possible ways of simulating such behaviour is through models guided by non-equilibrium dynamics, in particular, chaos. This is because of the much richer dynamical possibilities of such networks, compared to those in systems governed by convergent dynamics5. The focus in this work will be on ‘simple’ network models: ‘simple’ not only in terms of the size of the networks considered when compared to the brain (consisting of ~ 1011 neurons and ~ 1015 synapses), but ‘simple’ also in terms of the properties of the constituent elements (i.e. the ‘neurons’) themselves, in that, most of the physiological details of real neurons are ignored. The objective is to see and retain what is essential for a particular function performed by the network, treating other details as being of secondary importance for the task at hand. To do that one has to discard as much of the complexity as possible to make the model tractable – while at the same time retaining those features of the system which make it interesting. So, while this kind of modelling is indeed inspired by neuroscience, it is not exclusively concerned with actually mimicking the activity of real neuronal systems. The Hopfield model The foundation for computational neural modelling can be traced to the work of McCulloch and Pitts in 1943 on the universal computing capabilities of logic circuits akin to neural nets. However, the interest of physicists was drawn much later, mostly due to the work of Hopfield6 who showed the equivalence between the problem of associative Figure 2. Neuronal network of purkinje cells in the cerebellum of a hedgehog (image obtained through golgi staining of neurons). (From http:// weber.u.washington.edu/ chudler/). CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 Figure 3. Schematic diagram of a neuron (from http://www. utexas.edu/research/asrec/neuron.html). 421 SPECIAL SECTION: memory – where, one of many stored patterns has to be retrieved which most closely matches a presented input pattern – and the problem of energy minimization in spin glass systems. In the proposed model, the 2-state neurons, S i (i = 1, . . ., N), resemble Ising spin variables and interact among each other with symmetric coupling strengths, Wij. If the total weighted input to a neuron is above a specified threshold, it is said to be ‘active’, otherwise it is ‘quiescent’. The static properties of the model have been well understood from statistical physics. In particular, the memory loading capacity (i.e. the ratio of the number of patterns, p, stored in the network, to the total number of neurons), α= p/N, is found to have a critical value at αc ~ 0.138, where the overlap between the asymptotic state of the network and the stored patterns show a discontinuous transition. In other words, the system goes from having good recall performance (α< αc ) to becoming totally useless (α> αc ). It was observed later that dynamically defined networks with asymmetric interactions, Wij, have much better recall performance. In this case, no effective energy function can be defined and the use of statistical physics of spin glasslike systems is not possible. Such networks have, therefore, mostly been studied through extensive numerical simulations. One such model is a Hopfield-like network with a single-step delay dynamics with some tunable weight λ: S i(n + 1) = sign [ΣjWij(S j(n) + λS j(n – 1))]. (2) Here, S i(n) refers to the state of the i-th spin at the n-th time interval. For λ> 0, the performance of the model improved enormously over the Hopfield network, both in terms of recall and overlap properties7. The time-delayed term seems to be aiding the system in coming out of spurious minimas of the energy landscape of the corresponding Hopfield model. It also seems to have a role in suppressing noise. For λ< 0, the system shows limit cycle behaviour. These limit– cycle attractors have been used to store and associatively recall patterns8. If the network is started off in a state close to one of the stored memories, it goes into a limit cycle in which the overlap of the instantaneous configuration of the network with the particular stored pattern shows large amplitude oscillations with time, while overlap with other memories remains small. The model appears to have a larger storage capacity than the Hopfield model and better recall performance. It also performs well as a pattern classifier if the memory loading level and the degree of corruption present in the input are high. The travelling salesman problem To see how collective computation can be more effective than conventional approaches, we can look at an example from the area of combinatorial optimization: the Travelling Salesman Problem (TSP). Stated simply, TSP involves 422 finding the shortest tour through N cities starting from an initial city, visiting each city once, and returning at the end to the initial city. The non-triviality of the problem lies in the fact that the number of possible solutions of the problem grows as (N – 1)!/2 with N, the number of cities. For N = 10, the number of possible paths is 181,440 – thus, making it impossible to find out the optimal path through exhaustive search (brute-force method) even for a modest value of N. A ‘cost function’ (or, analogously, an energy function) can be defined for each of the possible paths. This function is a measure of the optimality of a path, being lowest for the shortest path. Any attempt to search for the global solution through the method of ‘steepest descent’ (i.e. along a trajectory in the space of all possible paths that minimizes the cost function by the largest amount) is bound to get stuck at some local minima long before reaching the global minima. The TSP has also been formulated and studied on a randomly dilute lattice9. If all the lattice sites are occupied, the desired optimal path is easy to find; it is just a Hamilton walk through the vertices. If however, the concentration p of the occupied lattice sites (‘cities’) is less than unity, the search for a Hamilton walk through only the randomly occupied sites becomes quite nontrivial. In the limit p → 0, the lattice problem reduces to the original TSP (in continuum). A neural network approach to solving the TSP was first suggested by Hopfield and Tank10. A more effective solution is through the use of Boltzmann machines11, which are recurrent neural networks implementing the technique of ‘simulated annealing’12. Just as in actual annealing, a material is heated and then made to cool gradually, here, the system dynamics is initially made noisy. This means, that the system has initially some probability of taking up higher energy configurations. So, if the system state is a local optima, because of fluctuations, it can escape a sufficiently small energy barrier and resume its search for the global optima. As the noise is gradually decreased, this probability becomes less and less, finally becoming zero. If the noise is decreased at a sufficiently slow rate, convergence to the global optima is guaranteed. This method has been applied to solve various optimization problems with some measure of success. A typical application of the algorithm to obtain an optimal TSP route through 100 specific European cities is shown in Figure 4 (ref. 13). Nonequilibrium dynamics and excitatory– inhibitory networks The Hopfield network is extremely appealing owing to its simplicity, which makes it amenable to theoretical analysis. However, these very simplifications make it a neurobiologically implausible model. For these reasons, several networks have been designed incorporating known biological facts – such as, the Dale’s principle, which states that a neuron has either exclusively excitatory or exclusively inhibitory synapses. In other words, if the i-th neuron is CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS excitatory (inhibitory), then Wji > 0 (< 0) for all j. It is observed that, even connecting only an excitatory and an inhibitory neuron with each other leads to a rich variety of behaviour, including high period oscillations and chaos14–16. The continuous-time dynamics of pairwise connected excitatory–inhibitory neural populations have been studied before17. However, an autonomous two-dimensional system (i.e. one containing no explicitly time-dependent term), evolving continuously in time, cannot exhibit chaotic phenomena, by the Poincare–Bendixson theorem (see e.g. Strogatz18). Network models updated in discrete time, but having binary-state excitatory and inhibitory neurons, also cannot show chaoticity, although they have been used to model various neural phenomena, e.g. kindling, where epilepsy is generated by means of repeated electrical stimulation of the brain19. In the present case, the resultant system is updated in discrete-time intervals and the continuous-state (as distinct from a binary or discrete-state) neuron dynamics is governed by a nonlinear activation function, F. This makes chaotic behaviour possible in the model, which is discussed in detail below. If X and Y be the mean firing rates of the excitatory and inhibitory neurons, respectively, then their time evolution is given by the coupled difference equations: Xn + 1 = Fa(Wxx Xn – Wxy Yn), (3) Yn + 1 = Fb(Wyx Xn – Wyy Yn). The network connections are shown in Figure 5. The Wxy and Wyx terms represent the synaptic weights of coupling between the excitatory and inhibitory elements, while Wxx and Wyy represent self-feedback connection weights. Although a neuron coupling to itself is biologically implausible, such connections are commonly used in neural network models to compensate for the omission of explicit terms for synaptic and dendritic cable delays. Without loss of generality, the connection weightages Wxx and Wyx can be Figure 4. An optimal solution for a 100-city TSP (from Aarts et al.13 ). CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 absorbed into the gain parameters a and b and the correspondingly rescaled remaining connection weightages, Wxy and Wyy , are labelled k and k′, respectively. For convenience, a transformed set of variables, zn = Xn – kY n and zn′ = Xn –k′Yn, is used. Now, if we impose the restriction k = k′, then the two-dimensional dynamics is reduced effectively to that of an one-dimensional difference equation (i.e. a ‘map’), zn + 1= F (zn) = Fa(zn) – kF b(zn), (4) simplifying the analysis. The dynamics of such a map has been investigated for both piecewise linear and smooth, as well as asymmetric and anti-symmetric, activation functions. The transition from fixed point behaviour to a dynamic one (asymptotically having periodic or chaotic trajectory) has been found to be generic across the different forms of F. Features specific to each class of functions have also been observed. For example, in the case of piecewise linear functions, border-collision bifurcations and multifractal fragmentation of the phase space occur for a range of parameter values16. Anti-symmetric activation functions show a transition from symmetry-broken chaos (with multiple coexisting but disconnected attractors) to symmetric chaos (when only a single chaotic attractor exists). This feature has been used to show noise-free ‘stochastic resonance’ in such neural models20, as discussed in the following section. Stochastic resonance in neuronal assemblies Stochastic resonance (SR) is a recently observed cooperative phenomena in nonlinear systems, where the ambient noise helps in amplifying a sub threshold signal (which would have been otherwise undetected) when the signal frequency is close to a critical value21 (see Gammaitoni et al.22 for a recent review). A simple scenario for observing such a phenomenon is a heavily damped bistable dynamical system (e.g. a potential well with two minima) subjected to an external periodic signal. As a result, each of the minima is alternately raised and lowered in the course of one complete cycle. If the amplitude of the forcing is less than the barrier height between the wells, the system Figure 5. The pair of excitatory (x) and inhibitory (y) neurons. The arrows and circles represent excitatory and inhibitory synapses, respectively. 423 SPECIAL SECTION: cannot switch between the two states. However, the introduction of noise can give rise to such switching. This is because of a resonance-like phenomenon due to matching of the external forcing period and the noiseinduced (average) hopping time accross the finite barrier between the wells, and as such, it is not a very sharp resonance. As the noise level is gradually increased, the stochastic switchings will approach a degree of synchronization with the periodic signal until the noise is so high that the bistable structure is destroyed, thereby overwhelming the signal. So, SR can be said to occur because of noise-induced hopping between multiple stable states of a system, locking on to an externally imposed periodic signal. These results assume significance in light of the observation of SR in the biological world. It has been proposed that the sensory apparatus of several creatures use SR to enhance their sensitivity to weak external stimulus, e.g. the approach of a predator. Experimental studies involving crayfish mechanoreceptor cells23 and even, mammalian brain slice preparations24, have provided evidence of SR in the presence of external noise and periodic stimuli. Similar processes have been claimed to occur for the human brain also, based on the results of certain psychophysical studies25. However, in neuronal systems, a non-zero signal-to-noise ratio is found even when the external noise is set to zero26. This is believed to be due to the existence of ‘internal noise’. This phenomenon has been examined through neural network modelling, e.g. in Wang and Wang27, where the main source of such ‘noise’ is the effect of activities of adjacent neurons. The total synaptic input to a neuron, due to its excitatory and inhibitory interactions with other neurons, turns out to be aperiodic and noise-like. The evidence of chaotic activity in neural processes of the crayfish28 suggests that nonlinear resonance due to inherent chaos might be playing an active role in such systems. Such noise-free SR due to chaos has been studied before in a non-neural setting29. As chaotic behaviour is extremely common in a recurrent network of excitatory and inhibitory neurons, such a scenario is not entirely unlikely to have occurred in the biological world. There is also a possible connection of such ‘resonance’ to the occurrence of epilepsy, whose principal feature is the synchronization of activity among neurons. The simplest neural model20 which can use its inherent chaotic dynamics to show SR-like behaviour is a pair of excitatory–inhibitory neurons with anti-symmetric piecewise linear activation function, viz. Fa(z) = – 1, if z < – 1/a, Fa(z) = az, if – 1/a ≤ z ≤ 1/a, and Fa(z) = 1, if z > 1/a. From eq. (4), the discrete time evolution of the effective neural potential is given by the map, where I is an external input. The design of the network ensures that the phase space [– 1 +(kb/a),1 –(kb/a)] is divided into two well-defined and segregated sub-intervals L : [–1 +(kb/a), 0] and R : [0, 1 –(kb/a)]. For a < 4, there is no dynamical connection between the two sub-intervals and the trajectory, while chaotically wandering over one of the sub intervals, cannot enter the other sub interval. For a > 4, in a certain range of (b, k) values, the system shows both symmetry-broken and symmetric chaos, when the trajectory visits both sub intervals in turn. The chaotic switching between the two sub-intervals occurs at random. However, the average time spent in any of the sub-intervals before a switching event, can be exactly calculated for the present model as 〈 n〉 = 1 bk bk1 − −1 a . (5) As a complete cycle would involve the system switching from one sub-interval to the other and then switching back, the ‘characteristic frequency’ of the chaotic process is ωc = 1/(2〈n〉). For example, for the system to have a characteristic frequency of ω= 1/400 (say), the above relation provides the value of k ~ 1.3811 for a = 6, b = 3.42. If the input to the system is a sinusoidal signal of amplitude δ and frequency ~ ωc , we can expect the response to the signal to be enhanced, as is borne out by numerical simulations. The effect of a periodic input, In = δsin (2πωn), is to translate the map describing the dynamics of the neural pair, to the left and right, periodically. The presence of resonance is verified by looking at the peaks of the residence time distribution30, where the strength of the j-th peak is given by Pj = ∫ n j +α n 0 n j −α n 0 N (n ) dn ( 0 < α < 0 .25 ). (6) For maximum sensitivity, α is set as 0.25. As seen in Figure 6, the dependence of Pj( j = 1, 2, 3) on external signal frequency, ω, exhibits a characteristic non-monotonic profile, indicating the occurrence of resonance at ω~ 1/(2〈n〉). For the system parameters used in the simulation, 〈n〉 = 200. The results clearly establish that the switching between states is dominated by the subthreshold periodic signal close to the resonant frequency. This signal enhancement through intrinsic dynamics is an example of how neural systems might use noise-free SR for information processing. Formation of neural assemblies via activity synchronization zn+1 = F (zn + In) = Fa(zn + In) – kF b(zn + In), 424 CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS Dynamical transitions leading to coherence in brain activity, in the presence of an external stimulus, have received considerable attention recently. Most investigations of these phenomena have focussed on the phase synchronization of oscillatory activity in neural assemblies. An example is the detection of synchronization of ‘40 Hz’ oscillations within and between visual areas and between cerebral hemispheres of cats31 and other animals. Assemblies of neurons have been observed to form and separate depending on the stimulus. This has led to the speculation that, phase synchronization of oscillatory neural activity is the mechanism for ‘visual binding’. This is the process by which local stimulus features of an object (e.g. colour, motion, and shape), after being processed in parallel by different (spatially separate) regions of the cortex, are correctly integrated in higher brain areas, forming a coherent representation (‘gestalt’). Recent neurobiological studies32 have shown that many cortical neurons respond to behavioural events with rapid modulations of discharge correlation. Epochs with a particular correlation may last from ~ 10–2 to 10 secs. The observed modulation of correlations may be associated with changes in the individual neuron’s firing rates. This supports the notion that a single neuron can intermittently participate in different computations by rapidly changing its coupling to other neurons, without associated changes in firing rate. The mechanisms of such dynamic correlations are unknown. The correlation could probably arise from changes in the pattern of activity of a large number of neurons, interacting with the sampled neurons in a correlated manner. This modification of correlations between two neurons in relation to stimulation and behaviour most probably reflects changes in the organi- zation of spike activity in larger groups of neurons. This immediately suggests the utilization of synchronization by neural assemblies for rapidly forming a correlated spatial cluster. There are indeed indications that such binding between neurons occurs and the resultant assemblies are labelled by synchronized firing of the individual elements with millisecond precision, often associated with oscillations in the so-called gamma-frequency range, centered around 40 Hz. Mostly due to its neurobiological relevance as described above, the synchronization of activity has also been investigated in network models. In the case of the excitatory–inhibitory neural pair described before, even N = 2 or 3 such pairs coupled together give rise to novel kinds of collective behaviour15. For N = 2, synchronization occurs for both unidirectional and bidirectional coupling, when the magnitude of the coupling parameter is above a certain critical threshold. An interesting feature observed is the intermittent occurrence of desynchronization (in ‘bursts’) from a synchronized situation, for a range of coupling values. This intermittent synchronization is a plausible mechanism for the fast creation and destruction of neural assemblies through temporal synchronization of activity. For N = 3, two coupling arrangements are possible for both unidirectional and bidirectional coupling: local coupling, where nearest neighbours are coupled to each other, and global coupling, where the elements are coupled in an all-to-all fashion. In the case of bidirectional, local coupling, we observe a new phenomenon, referred to as mediated synchronization. The equations governing the dynamics of the coupled system are given by: z1n +1 = (z1n + λ z 2n ), z 2n +1 = (z n2 + λ [z1n + z 3n ]), z 3n +1 = F (z 3n + λ z 2n ). Figure 6. Peak strengths of the normalized residence time distribution, P1 (circles), P2 (squares) and P3 (diamonds), for periodic stimulation of the excitatory–inhibitory neural pair (a = 6, b = 3.42 and k = 1.3811). Peak amplitude of the periodic signal is δ = 0.0005. P1 shows a maximum at a signal frequency ωc ~ 1/400. Averaging is done over 18 different initial conditions, the error bars indicating the standard deviation. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 For the set ofF activation parameters a = 100, b = 25 (where F is of anti-symmetric, sigmoidal nature), we observe the following feature F over a range of values of the coupling parameter, λ: the neural pairs, z1 and z3 which have no direct connection between themselves synchronize, although z2 synchronizes with neither. So, the system z2 appears to be ‘mediating’ the synchronization interaction, although not taking part in it by itself. This is an indication of how longrange synchronization might occur in the nervous system without long-range connections. For a global, bidirectional coupling arrangement, the phenomenon of ‘frustrated synchronization’ is observed. The phase space of the entire coupled system is shown in Figure 7. None of the component systems is seen to be synchronized. This is because the three systems, each trying to synchronize the other, frustrate all attempts at collective synchronization. Thus, the introduction of structural disorder in chaotic systems can lead to a kind of 425 SPECIAL SECTION: ‘frustration’33, similar to that seen in the case of spin glasses. These features were of course sudied for very small systems (N = 2 or 3), where all the possible coupling arrangements could be checked. For larger N values, the set of such combinations quickly becomes a large one, and was not checked systematically. We believe, however, that the qualitative behaviour remains unchanged. Image segmentation in an excitatory–inhibitory network Sensory segmentation, the ability to pick out certain objects by segregating them from their surroundings, is a prime example of ‘binding’. The problem of segmentation of sensory input is of primary importance in several fields. In the case of visual perception, ‘object-background’ discrimination is the most obvious form of such sensory segmentation: the object to be attended to, is segregated from the surrounding objects in the visual field. This process is demonstrated by dynamical transitions in a model comprising excitatory and inhibitory neurons, coupled to each other over a local neighbourhood. The basic module of the proposed network is a pair of excitatory and inhibitory neurons coupled to each other. As before, imposing restrictions on the connection weights, the dynamics can be simplified to that of the following onedimensional map: zn + 1 = Fa(zn + In) – kF b(zn + I′n ), (7) where the activation function F is of asymmetric, sigmoidal nature: Fa(z) = 1– e–az, if z > 0, = 0, otherwise. Without loss of generality, we can take k = 1. In the Figure 7. Frustrated synchronization: Phase space for three bidirectional, globally coupled neural pairs (z1 , z2 , z3 ) with coupling magnitude λ = 0.5 (a = 100, b= 5 for all the pairs). 426 following, only time-invariant external stimuli will be considered, so that: In = In′ = I. The autonomous behaviour (i.e. I, I′ = 0) of the isolated pair of excitatory–inhibitory neurons show a transition from fixed point to periodic behaviour and chaos with the variation of the parameters a, b, following the ‘perioddoubling’ route, universal to all smooth, one-dimensional maps. The introduction of an external stimulus of magnitude I has the effect of horizontally displacing the map to the left by I, giving rise to a reverse period-doubling transition from chaos to periodic cycles to finally, fixed-point behaviour. The critical magnitude of the external stimulus which leads to a transition from a period-2 cycle to fixed point behaviour is given as34. 1− Ic = ( µa ) 1/ µ 2 µ − ( a /µ) + 1 [ln( µa ) − 1]. µa (8) To make the network segment regions of different intensities (I1 < I2, say), one can fix µ and choose a suitable a, such that I1 < Ic < I2. So elements, which receive input of intensity I1, will undergo oscillatory behaviour, while elements receiving input of intensity I2, will go to a fixedpoint solution. The response behaviour of the excitatory–inhibitory neural pair, with local couplings, has been utilized in segmenting images and the results are shown in Figure 8. The initial state of the network is taken to be totally random. The image to be segmented is presented as external input to the network, which undergoes 200–300 iterations. Keeping a fixed, a suitable value of µ is chosen from a consideration of the histogram of the intensity distribution of the image. This allows the choice of a value for the critical intensity (Ic ), such that, the neurons corresponding to the ‘object’ converge to fixed-point behaviour, while those belonging to the ‘background’ undergo period-2 cycles. In practice, after the termination of the specified number of iterations, the neurons which remain unchanged over successive iterations (within a tolerance value) are labelled as the ‘object’, the remaining being labelled the ‘background’. The image chosen is that of a square of intensity I2 (the object) against a background of intensity I1 (I1 < I2). Uniform noise of intensity ε is added to this image. The signal-tonoise ratio is defined as the ratio of the range of grey levels in the original image to the range of noise added (given by ε). Figure 8 shows the results of segmentation for unit signal-to-noise ratio. Figure 8 a shows the original image while segmentation performance of the uncoupled network is presented in Figure 8 b. As is clear from the figure, the isolated neurons perform poorly in identifying the CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999 NONEQUILIBRIUM STATISTICAL SYSTEMS ‘background’ in the presence of noise. The segmentation performance improves remarkably when spatial interactions are included in the model. We have considered discrete approximations of circular neighbourhoods of excitatory and inhibitory neurons with radii rex and rin(r = 1, 2), respectively, in our simulations. Results for rex = 1, rin = 2 and rex = rin = 2 are shown in Figure 8 c, d respectively. The two architectures show very similar segmentation results, at least up to the iterations considered here, although the latter is unstable. Excepting for the boundary of the ‘object’, which is somewhat broken, the rest of the image has been assigned to the two different classes quite accurately. More naturalistic images have also been considered, such as a 5-bit ‘Lincoln’ image, and satisfactory results have been obtained34. Note that, a single value of a (and hence Ic ) has been used for the entire image. This is akin to ‘global thresholding’. By implementing local thresholding and choosing a on the basis of local neighbourhood information, the performance of the network can be improved. Outlook We have pointed out some of the possible uses of dynamical transitions in a class of network models of computation, namely excitatory–inhibitory neural networks updated at discrete time-intervals. Dynamics however plays an important role in a much broader class of systems implementing collective computation – cellular automata35, lattices of coupled chaotic maps36, ant-colony models37, etc. Other examples may be obtained from the ‘Artificial Life’38 genre of models. However, even in the restricted region that we have focused on, several important issues are yet to be addressed. One important point not addressed here is the issue of a b c d learning. The connection weights {Wij} have been assumed constant, as they change at a much slower time scale compared to that of the neural activation states. However, modification of the weights due to learning will also cause changes in the dynamics. Such bifurcation behaviour, induced by weight changes, will have to be taken into account when devising learning rules for specific purposes. The interaction of chaotic activation dynamics at a fast time scale and learning dynamics on a slower time scale might yield richer behaviour than that seen in the present models. The first step towards such a programme would be to incorporate time-varying connection weights in the model. Such time-dependence of a system parameter has been shown to give rise to interesting dynamical behaviours, e.g. transition between periodic oscillations and chaos. This suggests that varying the environment can facilitate memory retrieval if dynamic states are used for storing information in a neural network. The introduction of temporal variation in the connection weights, independent of the neural state dynamics, should allow us to develop an understanding of how the dynamics at two time-scales interact with each other. Parallel to this, one has also to look at the learning dynamics itself. Freeman39, among others, has suggested an important role of chaos in the Hebbian model of learning40. This is one of the most popular learning models in the neural network community and is based on the following principle postulated by Hebb40 in 1949: When an axon of cell A is near enough to excite cell B and repeatedly or consistently takes part in firing it, some growth process or metabolic change takes place in one or both cells such that A’s efficiency, as one of the cells firing B, is increased. According to the principle known as synaptic plasticity, the synapse between neurons A and B increase its ‘weight’, if the neurons are simultaneously active. By invoking an ‘adiabatic approximation’, we can separate the time scale of updating the connection weights from that of neural state updating. This will allow us to study the dynamics of the connection weights in isolation. The final step will be to remove the ‘adiabatic approximation’, so that the neural states will evolve, guided by the connection weights, while the connection weights themselves will also evolve, depending on the activation states of the neurons, as: Wij(n + 1) = F ε (Wij(n), Xi(n), Xj (n)), Figure 8. Results of implementing the proposed segmentation method on noisy synthetic image: a, original image; b, output of the uncoupled network; c, output of the coupled network (rex = 1, rin = 2); and d, output of the coupled network (rex = rin = 2), after 200 iterations (a = 20, b/a = 0.25 and tolerance = 0.02). 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O., The Organization of Behavior, Wiley, New York, 1949. 41. Although the brain certainly shows non-converging dynamics, there is as yet no consensus as to whether this is stochastic in origin, or due to deterministic chaos. Although the successful use of chaos control in brain-slice preparations, reported in Schiff, S. J., Jerger, K., Duong, D. H., Chang, T., Spano, M. L. and Ditto, W. L., Nature, 1994, 370, 615, might seem to indicate the latter possibility, it has been shown that such control algorithms are equally effective in controlling purely stochastic neural networks. See Christini, D. J. and Collins, J. J., Phys. Rev. Lett., 1995, 75, 2782; Biswal, B., Dasgupta, C. and Ullal, G. R., in Nonlinear Dynamics and Brain Functioning (ed. Pradhan, N., Rapp, P. E. and Sreenivasan, R.), Nova Science Publications, (in press). Hence, ability to control the dynamics is not a conclusive proof that the underlying behaviour is deterministic. ACKNOWLEDGEMENTS. We thank R. Siddharthan (IISc) for assistance during preparation of the electronic version of the manuscript. CURRENT SCIENCE, VOL. 77, NO. 3, 10 AUGUST 1999