Supercond. Sci. Technol. 1 (1989) 242-248. Printed in the UK P H Kes, J Aarts, J van den Berg,C J van der Beek andJ A Mydosh Kamerlingh Onnes Laboratorium, Leiden University, PO Box 9506. 2300 R A Leiden, The Netherlands Received 26 September 1988 Abstract. The theory for thermally assisted flux flow (TAFF) in the limit of small driving forces is used to derive exact expressions for the time-dependent behaviour of the magnetisation and permeability. The problem is especially relevant for the high-temperature superconductors where large variationsof the transition temperature in small DC fields are observed as a function of the frequency of the probing AC field. The parameters of the theory are extensively discussed in relation to the present understanding of flux pinning. 1. Introduction It has been observed recently that the phase transition temperature of the superconducting oxide YBa,Cu,O, in an applied DC field depends strongly on the frequency v of a small superimposed AC field [l, 21. Malozemoff and co-workers have argued that the real critical temperature in a field T,,(B) is not observed, but rather that experiments determine a lower temperature denoted as an irreversibility temperature Trr [l]. At Trr the permeability shows a maximum in the out-of-phase signal p" and a steepest decay in the in-phase component p'. The maximum will occur in thetransition regime between almost reversible fluxflow above Trr and strong irreversible screening due to flux pinning below T,, . In the range Trr< T < flux lines are depinned by thermalactivation,a process we call thermally assisted fluxflow (TAFF) to discriminate it from flux creep. Although both processes have thesame origin and are in principle described by thesamecontinuity equation,thisequationcan be linearised and solved analytically only in these two limiting cases. Flux creep is the phenomenon that occurs when the driving force is almostequal to the pinning force, i.e. just below the onset of the usual flux flow regime. TAFF only occurs in superconductors with an intrinsically low pinningbarrierand at temperatures high enough to overcome this barrier, and is therefore observed already in the limit of small driving forces. The importance of TAFF for the high-temperature superconductors was first pointed out by Dew-Hughes [3]. Herethe ratio of pinning potential height' U to thermal activation energy kT is much smaller than in conventional superconductors, U/kT < 10 rather than 100. In the accompanying .experimental paper [4] it is shown that such effects are clearly manifested in the Bi compound with a T, of 87 K. The shift of the transition temperature with fre- T,, 0953-2048/89/050242 + 07 $02.50 @ 1989 IOP Publishing Ltd quency is much larger thanYBa,Cu,O,, 6 K per decade instead of 0.7 K per decade [17]. This large difference may be related to the effect of twin planes [S]. Related to this frequency dependence is the unusual low value of the field B,(T), at which the irreversibility in themagnetisationdisappears, especially when measured with the field along the c axis of the crystal [6]. The relation B,(T) defines the 'irreversibility line', which has been formerly described as Trr(B)[l]. In previous work [l, 2, 71 attempts have been made to model Trr(B) and Trr(v) by intuitively constructed expressions. In this paper an exact derivation is presented from which these effects can be obtained in principle. It is argued that the results depend sensitively on the pin mechanism and the choice of parameters. Therefore fitting results should be considered with some care, as long as detailedinformation about the pinning-force density is lacking, partially because TAFF does not allow a straightforward determination of critical current and flux pinning effects [6]. On the other hand, references [l, 2, 71 serve to point out the importance of TAFF and the consequences it may have on the interpretation of importantparameters for thesuperconducting oxides, like the upper critical field B,,. The outline of our paper is as follows. After developing the theory in $2, several possible choices for the parameters will be discussed in $ 3 based upon our present knowledge of flux pinning. 2. Theory For small values of the parameter U/kT the flux creep theory [S, 91 in the presence of a driving force must be extended to consider the possibility of reverse hopping [lo]. Because of flux conservation the flux density B is Thermally assisted flux flow described by the continuity equation at = V [ ( z ) B w v , exp( )2-; sinh( g)], (1) Here the notation of [S] has been adopted in which v, is the attempt frequency, W the distance by which a certain volume V , of the flux line lattice (FLL) moves in a thermally activatedjump, U the energy required to depin the volume V,, and A W the work done to move this same volume against the driving force. In $ 3 relevant choices for V , and W willbe discussed. It willbe shown there that U can be related to the critical current density J, , and A W to the actual currentdensity J by U = JcBV,rp J J c/ \rp/ Both U and AW are functions of B and T, and rp is the range of the pinning potential. For defects acting as pinning centres, with the relevant dimensions smaller than the Ginzburg-Landau coherence length, ((T), rp x for isolated vortex cores, i.e., b = B/BC2c 0.2. Alternatively, rp z a,/2 for overlapping vortex cores, i.e. b > 0.2 [1l]. Otherwise the defect size would be a more appropriate measureof rp. Beasley et a1 [S] treatedthe flux creep sitation in which U is very much larger than kT, so that the effects are only observable for (J, - J)/J, < 1. In this case it follows that 2sinh(AW/kT) = exp(AW/kT). We, however, will solve equation (1) in thesmall-J limit (TAFF), where 2 sinh(AW/kT) = 2AW/kT. This factor in equation (1) generates the driving force which is simply J B and J = p G I V x B, because for the hightemperature superconductors ic (the Ginzburg-Landau parameter) is large and H,,small [l2], so that p * , the slope of the reversible induction curve, may be set equal to unity. Two geometries areconsidered:aslab defined by -1 < x < l and a solid cylinder r < a, both with their surfaces parallel to the field direction which is along the z axis. After substitution equation (1) becomes H(t) = H, (ii) H(t) = H , 2 - f i t 1 a (7) (8) which describe, respectively, the AC experiments and the DC magnetisation measurements (irreversibility line). Thesolution is outlined for theslabgeometry; full details are given in appendix 1. In case (i) the solution is SB(x, t ) = A(x)sin(2nvt &)). Theamplitude A(x) decays approximately exponentially with a decay length + k” (9) = (Do/.~)1’2. 1 sinh 2u PI = 2u cosh 2u cylinder + sin 2u + cos 2u (10) 1 sinh 2u - sin 2u =- < aB + h sin 2nvt (i) The average induction follows from integration of x over the slab and yields the expressions for both permeability components: w A W = U( T\)T ( ) . \ tions of equations (4) and ( 5 ) for many geometries and boundary conditions can be foundin [ 131. Two applied field modes have been considered here: 2u cosh 2u + cos 2u * The results depend on temperature via the variable = ( ~ v I ~ / D , ) ”The ~ . functions $(U) and pff(u),as obtained in appendix 1, areshown in figure 1. The maximum in p f f for the slab geometry is attainedat M, = 1.1275. By substitutingtheaboveintoequation (6) an expression is derived that relates the temperature and field at the maximum of p’’ to the frequency v of the AC field : U = kl U = kT In 2Miv, BUw2 nvp, J, kTl2rP Analogously, for the solid cylinder we obtain MEv, BUw2 nvp, J, kTa2rp U = kT In It is expected that M, will also be of order unity. In addition, the definition of the decay length in the case of (5) with D =~ (”) (t) W V k , T ( ~ ) Po J, ex,( - 3). (6) D is related to the flux-flow density D defined in [S] and is analogous to the diffusion constant in a diffusion problem. It is obvious that D depends on B and T and is further influenced by the pin characteristics. However, since J is taken to be small over the entire superconductor, B is almost uniform, i.e. B = B, + SB with SB 6 B , . It is shown in appendix 3 that, for SBO.lB,, D may be replaced by its constant value D , D(B,). Solu- 1 0 I I I 1 I 1 2 3 4 5 U Figure 1. Graph of the permeability components against the parameter U . 243 P H Kes et a/ a cylindrical geometry differs by afactor ,b, which explains the missing factor of two in the argument of the logarithm. These results differ from the intuitive equation suggested in [7]. For instance, because of the exponential decay, our present results do not depend on the amplitude of the AC field. This is in agreement with our experiments on the ‘B? single crystals [4]. In fact, the difference in the arguments of the logarithms is a factor B,w/GBa. Fortuitously,thisfactor is of order unity, although both 6B/Bo and w/a may be of order The physics of the problem is clearly demonstrated by the plots of A(x) and C#J(X)for various kl given in [13]. If kl = 0.5 corresponding to a relatively large D,, the behaviour is almost reversible. If kl = 10, the screening already amounts to 90%. It also follows that M , and M , must be of order unity. The solution for case (ii) is relatively easy (see [13]) and gives the magnetisation M = @po - H as for the slab. Here 7, = z0/(2n + l), T, = 412/712D0. (15) (1 6) Assuming that the measurement is carried out slowly enough to neglect the transient part in equation (14) (see appendix 2 in which the response to a step-like change in field is treated), a condition is derived for the field-temperature relation at which, in decreasing fields, amagnetisation signal can be observed for the first time. For high-rc materials the reversible magnetisation below H , , is negligibly small, M x ( H , , - H)/2rc2. Therefore, the condition can be expressed in the form of a ‘minimal-observable’ current density Jmin= 2 I M [/l, which dependsontheexperimentalresolution.The ‘irreversibility line’ should thus follow from U = kT In for theslab. which yields 3Vo B U W ~ J , , , ~ , p, HkTlr, J , For the solid cylinder Jmin= 3 I M [/a, U = kT In 16v0 BUw2Jmi, 3p0 HkTar, J , If the measurements are carried out in pulsed magnetic fields [S], it should be carefully checked whether the above analysis is still applicable. For high field rates it is more likely that a current density closer to J , is probed. In that case analytic solutions of equation (1) may not be available, so that numerical methods should be used. Equations (12), (1 3), (17) and (1 8 ) serve as a starting point for the interpretation of the TAFF effects. It is clear, however, that even a qualitative description depends on the waywe choose the parameters and this requires a detailed understanding of the flux-pinning mechanism as will be discussed in the following section. 244 Finally, it should be noted that the above theory describes TAFF when the driving force is caused by a flux density gradient. The situation of TAFF due to a transport current shows a striking formal analogy with the preceding result, since from the formalism of [3] it follows that the flux flow resistivity pf can be expressed as Pr = PODO with thesame D, as in equation (6). Bothkinds of experiment, therefore, provide comparable information. 3. Discussion For comparison a with experiment, the physical meaning of theparametersin the theoryshould be understood. In general, the parameters V,, r , , W , v, and F , = J , B can be well defined. In practice, however, it is the defect morphology of the superconductor that determines thecharacter of thepinningcentres and the actual assignment of theparameters.Thelatter is a complicated problem and leaves many possibilities for the ultimatetemperatureand field dependence, especially when it is not obvious what the predominant pins of thematerialare.Inthe following discussion we restrict ourselves to pins that have at least one dimension, namely that in the direction of the driving force, L of the pins smaller than r p . Themutualdistances should form a random distribution.Theirinteraction, the so-called coreinteraction, is through local perturbations of the mean free path or the coupling constant, which couple to the modulation of the superconducting order parameter. 3.1. The volume V, The theory of flux creep actually deals with the problem of hopping over a potential barrier by independent particles driven by an external force and thermally activated by theinteraction with aheatbath,as in the treatment of Brownian motion by Kramers [14]. As has been already recognised by Anderson [S], the analogue of an independent particle in a FLL is a ‘flux bundle’ with volume V , that is elastically independent of the other ‘particles’ of the FLL. This volume is the same as the correlated region in the theory of collective pinning [15]. It is the volume in which the FLL maintains its positional short-range order, which is either determined by the correlation lengths R , and L,, or by the density of dislocations in the FLL, or more generally, the amount of disorder of the FLL [16]. In this sense it might be that the interaction with the thermal bath contributes to the disorder and the size of V , [17]. The choice of V , for an actualpinningproblem is not unique. In the case of a thin superconducting film with many small pins it can be predicted [18-201. For a system of grain boundaries which exert a very strong elementary interaction on the FLL one can make a reasonable estimate [21, 221. The final result for V, Thermally assisted flux flow depends on the strength of the elementary interactionf, or the elementary pin potential R,, and the distance L between the pins. Since many details are not yet known for the high-T, superconductors, it is impossible to make a unique choice, so that several possibilities can be considered. One should realise,however, that the study of collective pinning on thin amorphous films has revealed that the FLL usually is highly disordered even for very weak pins [20]. It is therefore assumed that the ‘amorphous’ limit is appropriate for most strong pinning systems. In this limit V , x a; L , , where a, = 1 . 0 7 5 m B is the FLL parameter and L, is the correlation length along the flux line. As argued in C231 and [24] it is not clear how L, can be predicted for point pins from theory. Several approaches can be used. In [l51 a formula was derived which in the clean limit (to> I t r , with to the BCS coherence length and I,, the transport mean free path) and for b > 0.2 can be cast into the form where 1 is the penetration depth and W below). For instance (with b > 0.2), = n( f 2, (see for dislocation loops, and W, = C,BC2e b 3 ( l - b)2 (21) forvoids, and probably also for precipitates [18, 241. Using a somewhat different elastic constant for tilt, which turned out to be veryuseful in predicting the transition from two- to three-dimensional disorder [24], one arrives at L, x. (Q: b2(1 - b)’)”) 4112p; A4 W 3.2. Relation between F,, rpand U Once V , has been established one can obtain the pinning force density F , by summing the individual contributions of all the pins in V,. For a dense system of randomly distributed pins this leads to a net force on V , which is equal to the fluctuation in the total effect of the pins in the correlated region ( t ~ V , ( f ~ ) )where ’ / ~ , n is the concentration of pins and the average should be taken over the entire correlated volume. F , then follows by dividing through V , . If V , contains only one very strong pin a direct summation is more appropriate.One can imagine,for instance, that the strong interaction of the FLL with the boundary of a grain will probably confine V , to the volume of the grain itself, providing it is not too large or contains other strong pins. The pin potential in which this ‘particle’ istrapped is now @veri by U = FpV,I , where, as in equation (2), I , is the range of the potential. In $2 we stated that rP is either 5: or a,/2, but such is only true when pure collective pinning is encountered [18].If many flux-line dislocations determine the disorder, r, is a smaller fraction of 5 (or a,) corresponding to the distance overwhich the volume V , can be reversibly moved in its potential [25, 261. 3.3. Attempt frequency and hopping range Due to thermal motion of the pins the values of F,, and probably also V,, fluctuate in time, causing the ‘particle’ to hop over the barrier. It seems reasonable to relate the attempt frequency to the relevant dimensions of V,. Using a sound velocity of 3 x lo3 m s - l , the typical valuefor one fluxline to hop would range between v , = 10” and3 x 10” Hz for corresponding fields between 20 mT and 2 T. As has been discussed by Kramers [l41 the viscosity of the system damps the motion of the particle. This can beexpressed as a reduction in the attempt frequency. For the flux-creep situation the viscous damping becomesincreasingly important because the effective barrier heightdecreaseswith larger driving forces. In the flux-flow state ( J > J,) the viscosity determines, and is inversely proportional to, the flux flow resistivity. The hopping range W for a dense system of pins can be taken equal to I , . This is because moving the lattice over a distance of the order r, destroys the original short-range order in the correlated region, which has to be redefined. The same holds forall kinds of pin distributions when b > 0.2, because the potential then has the sinusoidal variation of the superconducting order parameter. Only for b < 0.2may considerable deviations between W and r, occur. At large a, the order parameter changes only at the location of thevortex core in a range 5: < a,. If in this situation L > a, and the interaction is strong, so that there is only one large pin per V,, then the hopping distance willbeof order a,, while r, x 5:. And W x L if 5 < L c a, under the same conditions. The discrimination between W , I , in terms of a,, t and L isof importance if one wants to compare experimental results with the TAFF expressions. Experimentally, the temperature and field dependence is investigated intheregionclose to T,, so that every factor t contributes a factor ( 1 - t)”” to the expression, whereas a, contributes a factor 3.4. Application to YBa,Cu,O, and Bi,Sr,CaCu,O, Wenow apply the above ideas toa single crystal of YBa2Cu30, with the field parallel to the c axis. In this situation we presume that the twin planes dominate the pinning but there is a significant background pinning as well. This follows from the large critical currents measured in the other orientation, i.e. with the field in the ab plane. The background will determine the length and width of the correlated region, but the distance between the twin planes forms the other dimension. Namely, if a flux line, which is pinned at the twin plane, jumps loose the whole row behind it moves to fill the vacancy. So 245 P H Kes et a / V , = a, L, L and, because the experiments under discussion arecarriedoutat lowfields (but still with L ( % 1 0 0 nm) > a,) I , = ( and W = a,. Therefore F, = f p J L a , [S] with f,, x 0.5p0H:(0/ptr; thereby we obtain U = fpl L, ( a (1 using equation (19) for L, and [(l - t)5/B2]116when equation (22) is substituted. The argument of the logarithm in equations (12), (13), (17) and (18) is proportional to (1 - t)li2/kTB in the former case above and to B’I6/kT(1 - t),I3 in the latter.The experiments show the (1 - t)3i2/B scaling c11. As a second example we apply our model to Bi,Sr,CaCu,O, single crystals. Now there are no twin planes that can contribute to the pinning force. In [4] it is shown that pinning is much weaker andthe TAFF effects are considerably stronger. Consider pinning due to point defects in the isolated vortex limit. W, (equation (21)) should then read [1 l] W, = C:’B:B (- Combining these expressions with the collective pinning a (1 - t). So U only theory gives U = W,’12V:i2rp depends on temperature and not on field, which seems natural for isolated vortices. This temperature dependence is indeed observed [4], but the exact scaling with field is not yet known. Such behaviour has to be studied in future work. Our purpose in this last section was to put forward the relevant considerations and procedures necessary toarriveatthe expression for U andthe argument of the logarithmic term. 4. Summary The flux-creep theory has been investigated in the limit of low driving force. Expressions were derived for the permeability in a magnetic field near T, and the magnetisation close to B,, at lower temperatures when these quantitiesarepredominantly determined by thermally assisted fluxflow (TAFF). The response of the magnetisation to a field step has been treated separately (appendix 2). This theory provides the exact formulae with which to analyse the experiments. The physical interpretation of the parameters occurring in the theory has been discussed and special attention paid tothe relation between the thermally assisted effects and the known principles of flux pinning theory. Acknowledgments P H Kes wishes to thank A P Malozemoff for many helpful discussions and H CFreyhardtand his colleagues at the Institut fur Metallphysik in Gottingen for their hospitality duringthe time this paper was pre246 Appendix 1. Derivation of the formulae for U The derivation of equations (12), (13), (17) and (18) is given explicitly for the slab geometry - 1 < x G 1. The solution for the infinitely long solid cylinder involves much morealgebra and is therefore postponed for a future publication. (i) With H(t) = H, h sin 2nvt the solution for the induction increment according to [13, p 1051 is + &?(x, t ) = A(x) sin(2nvt (23) and L, (equation (19)) becomes L, x pared. This visit was made possible by a research grant from DFG Sonderforschungsbereich 126, project E10. We also acknowledge financial support from the Dutch Foundation for Fundamental Research on Matter (FOM). + &)) (A. 1) in which /l= 6B/po h , and A(x) and 4(x) are the amplitude and phase of the function Z(x) = cosh kx(1 + i ) cosh kl(1 + i ) (A4 Theinduction increment averaged over x determines the permeability components via p’ = f [Re(Z) dx (A.3) p” = f [Im(Z) dx (A.4) from which equations (10) and (1 1) follow in a straightforward way. (ii) For H(t) = H,, - kt the solution of B(x, t ) for bothslaband cylinder can be found in c133 PP 104, 2013 : B(x, t ) = B, - - p, k(12 - x,) 200 16p0 HI2 n3D, .f n=O cos (2n + 1)nx ((-(2n exp(t/r,) + 21 1)” (A.5) for the slab - 1 < x < l with B, = p, H(t) and 7, defined in equations (15) and (16). Computing the average and subtracting H yields equation (14) for M(t). Thesituation in increasing field is less well defined because we are returning from the critical state. But at the criterion for the irreversibility line theinductiongradient is so small that we may safely assume that I M ( t ) I is the same as in decreasing field. Theanalogousderivation for the solid cylinder r < a yields the expression B(r, t ) = B , - p. h ( a z - rZ) 40, Thermally assisted flux flow and dicts a slope independent of temperature, which would be observed aroundacharacteristic time 2,/2, and this time would vary strongly with temperature via D,(T). The results of [2] are probably better described by the flux-creep approximation of sinh(AW/kT) exp(AW/kT); although closer to T,, the behaviour given by TAFF should be observed. Recently, evidence has been obtained [29] that the magnetisation in single crystals decays according to a stretched exponential:6M/6H0 = exp[-(t/~)~]. It can be shownthatequation (A.8)isnicely described in terms of a stretched exponential with B x 0.6 and T x zo . In carrying out such experiments one should beware of the fact that the initial flux distribution can influence the precise time dependence observed afterwards. - J o and J , are Bessel functions and the a,, are the positive roots of J,(aa) = 0. Appendix 2. Response to a field step Solutions similar to the transient term in equations (14) and (A.7) occur in the response of M after a step-like increase of the field by an increment 6H.We assume a uniform induction at t = 0 and obtain for a slab (see c139 P 1@u Appendix 3. Restrictions for D, and J + with the same definitions for z, = z0/(2n l)' and zo = 4 l 2 / n ~ ,as given previously. In figure 2 6M in units 6 H o is plotted as a function of t expressed in units of 7,. The inset shows a part of the same graphonan expanded scale. The decay already sets in roughly three decades below z, due to the higher z,, terms. As is seen from the above formula, however, thecontribution of these terms decreases n. At about 22, the relaxation rapidly with increasing has reduced Mto10% of the initial value. The inset clearly shows that there is no time interval in which 6M changes linearly with ln(t). Such a time dependence is observed in [2] for YBa2Cu,0, single crystals, but otherbehaviourhas been reported as well for this material [27,281. Yeshurun and Malozemoff [2] also reported a reduction of dM/d ln(t) for T approaching T,. Such a behaviour cannot be described by equation (A.2), as follows from the scaling. This expression pre- 1.0 - 0.8 - 0.6 - The condition for approximating D by D, is worked out for theslab geometry, but is not sensitive to the geometry. D is defined in equation (6). The B-dependent part can be written as w2V, B2 exp( - U / k T ) . As has been discussed in $3, it is not possible to give a general relation for the B dependence. Yet, the most likely possibilities for thehigh-temperaturesuperconductors at relatively small fields (b < 0.5) are W a, or (, V , U: or ai and U U. + cBp with U , the pin potential at B = 0, some coefficient c and small power p 3 or 1. The factor w2V,B2is thusproportionalto Bs with - -3 - - c S c 1. Substitution ofBs exp[ - U(B)/kT] into equation (4: leads to the conclusion that (x) dB ' ~ B ~ ( s - PU+- U ) -l (A.9 E P 2 0.4- 0.2- 0I 10- I lo-& I I I 100 102 I I IO4 1o6 f IT0 Figure 2. Time-dependent decay of the magnetisation after a field step in the limit of small driving current plotted on a normal scale (full curve) and a largely expanded scale (broken curve). The inset shows the log T derivative. 247 P H Ker, el el must be obeyed. A reasonable condition to allow for the J x 0 limit is (U - U,)/kT 10, so equation (A.9) becomes (A. 10) The solutions for B(x) studied in case (i) are of the kind B = B, + dB,(cosh(kx)/cosh(kl)), hence we arrive at dBo 4 O.lB,. F o r case (ii) thecondition is similar: dB, 4 0.05Bo. In addition, the maximum of J, J(x = I), should be small enough for AW/kT -4 1. This requirement is fulfdled if J -4 (kT/U)J, x O.lJ,, which can be recast in the form kl = U 4 kTJ,l/Uh = kTAB/UGBo, where AB is the maximum flux density difference that the critical state would create. This should be checked retrospectively. From the analysis for the Bi compound, con[4], the above tained in the accompanying paper requirement is easily fulfilled. References [l] Malozemoff A P, Worthington T K, Yeshurun Y, Holtzberg F and Kes P H 1988 Phys. Reo. B to be published [2] Yeshurun Y and Malozemoff A P 1988 Phys. Rev. Lett. 60 2202 [3] Dew-Hughes D 1988 Cryogenics to be published [4] van den Berg J, van der Beek C J, Kes P H, Mydosh J A, Menken M J V and Menovsky A A 1989 Supercond. Sci. 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