letters to nature ................................................................. Vortex dynamics in superconducting MgB2 and prospects for applications Y. Bugoslavsky, G. K. Perkins, X. Qi, L. F. Cohen & A. D. Caplin Centre for High Temperature Superconductivity, Blackett Laboratory, Imperial College, London SW7 2BZ, UK .............................................................................................................................................. The recently discovered1 superconductor magnesium diboride, MgB2, has a transition temperature, Tc, approaching 40 K, placing it intermediate between the families of low- and high-temperature superconductors. In practical applications, superconductors are permeated by quantized vortices of magnetic ¯ux. When a supercurrent ¯ows, there is dissipation of energy unless these vortices are `pinned' in some way, and so inhibited from moving under the in¯uence of the Lorentz force. Such vortex motion ultimately determines the critical current density, Jc, which the superconductor can support. Vortex behaviour has proved to be more complicated in high-temperature superconductors than in low-temperature superconductors and, although this has stimulated extensive theoretical and experimental research2, it has also impeded applications. Here we describe the vortex behaviour in MgB2, as re¯ected in Jc and in the vortex creep rate, S, the latter being a measure of how fast the `persistent' supercurrents decay. Our results show that naturally occurring grain boundaries are highly transparent to supercurrents, a desirable property which contrasts with the behaviour of the high-temperature superconductors. On the other hand, we observe a steep, practically deleterious decline in Jc with increasing magnetic ®eld, which is likely to re¯ect the high degree of crystalline perfection in our samples, and hence a low vortex pinning energy. –0.2 b 1.5 TC= 37.5 K –0.4 –0.6 1.0 106 0.5 –0.8 ∆ = 8 meV –1.0 10 20 30 40 0.0 50 –20 10 20 Jc (A cm–2) m (10–6 A m–2) 0 V (meV) T (K) c 105 –10 0.1 0 104 10 K 4 103 µ Hirr (T) ° 0.0 σ/σn m (a.u.) a Measurements of Jc on polycrystalline MgB2 Ðthe only form available so farÐhave to be analysed carefully, because experience of the high-temperature superconductor (HTS) phases has shown that their grain boundaries impede the ¯ow of supercurrent. This problem is particularly severe in the YBa2Cu3O7 phase, which intrinsically has the highest Jc of the HTS oxides, but behaves poorly in bulk polycrystalline form, with Jc depressed by several orders of magnitude at even modest-angled grain boundaries3. We extracted from MgB2 powder (Alfa Aesar Co., 98% purity) several fragments of above 100 mm size; they were somewhat irregular in shape, and X-ray diffraction indicated no obvious crystalline texture. The superconducting transition (Fig. 1a) of a single particle is sharp with a Tc of 37.5 K, and particles have wellde®ned tunnelling characteristics (Fig. 1b) with a gap 2¢ of ,5 kBTc (for a weakly coupled BCS superconductor this factor is 3.5, for the HTS phases Bi2Sr2CaCu2O8 and YBa2Cu3O7, it is 10 and 5.5, respectively4,5). The key data are derived from magnetization loops that have excellent signal-to-noise ratios (Fig. 1c). Before proceeding further, we applied a number of cross-checks that have been developed in the context of HTS studies6. These measurements yield for this fragment a superconducting screened volume of 7:4 6 0:4 3 10 2 12 m3 , independent of ®eld and temperature. In a scanning electron microscope, the fragment appeared roughly ellipsoidal in shape, with cross-section axes of 450 and 250 mm, and between 100 and 150 mm in the third direction; its physical volume ­ is therefore 5±7 3 10 2 12 m3 . The screened volume might be up to a factor of 1.5 greater than this because of the demagnetizing effects, so within the uncertainties involved, there is excellent agreement with that obtained magnetically. Thus, the straightforward conclusion is that screening currents ¯ow in a wellconnected fashion around this small polycrystalline fragment, and that over the ®eld and temperature range studied, the grain boundaries are transparent to supercurrent, just as in low-temperature superconductor (LTS) materials. In contrast, a polycrystalline 2 20 K Tc 0 35 K 102 –0.1 20 –1 0 1 2 3 4 µ H (T) ° 0.01 Figure 1 Characterization of superconductivity. a, Magnetic moment of a single small MgB2 fragment as a function of temperature in a ®eld of 10 mT (the sample was previously cooled in zero ®eld), showing a sharp superconducting transition at 37.5 K. b, Typical tunnelling characteristic (differential conductance, j V dI=dV , normalized to its normal-state value jn jn 0 of a similar fragment; the parabola is an estimate of the background conductivity. c, Magnetization loop (obtained using a vibrating sample magnetometer; Model TVSM5, Oxford Instruments) at 20 K of the fragment shown in a; data were taken at a ramp rate of 13.3 mT s-1. The initial and `reverse leg' slopes (dashed lines) of the loop are a measure of the volume from which superconducting screening currents exclude changes in magnetic ¯ux. If the sample is a single well-connected entity, these slopes should be equal to the actual sample volume (apart from an enhancement associated with classical demagnetizing effects). NATURE | VOL 410 | 29 MARCH 2001 | www.nature.com 30 T (K) 30 K 25 K 40 0.1 1 10 µ H (T) ° Figure 2 Critical current density Jc of a MgB2 single fragment as a function of magnetic ®eld. In order to convert the irreversible magnetic moment to Jc, we model the fragment as a disk of radius a 300 mm and thickness t 100 mmÐthat is, a volume ­ of 7 3 10 2 12 m3 , at the upper bound of our geometrical estimateÐso as to yield conservative values for Jc. The standard Bean model13 gives J c 3Dm=2­a (in SI units, but in keeping with standard practice in the ®eld, we report Jc in units of A cm-2 rather than A m-2), where Dm is the full-width of the m(H ) loop. Inset, the irreversibility ®eld Hirr, above which irreversible (that is, screening) currents cannot be sustained, as a function of temperature; here we de®ne Hirr as the ®eld where Jc drops below the noise level, ,103 A cm-2. © 2001 Macmillan Magazines Ltd 563 letters to nature 100 0 35K YB a 30K 2 Cu 10–1 O 7 χIn S 3 –5 25K 35K 30K 25K self-field 10–2 0 1 2 3 0.1 0.2 0.3 0.4 S Figure 3 Vortex creep rate, S, as a function of ®eld. We use the `dynamic relaxation' Ç to a method10 in which the full-width of the m(H ) loops depends on the ®eld ramp rate H; Ç These data are derived from the differences of good approximation, S ] ln m=] ln H. irreversible magnetic moment between loops taken at ramp rates of 13 and 3 mT s-1. Because the differences are small, the signal has been increased by using a sample of ten MgB2 fragments. The oscillations in the curves, which become more severe as the temperature is reduced, are artefacts arising from small ¯uctuations in sample temperature, whose effects are ampli®ed by the differencing of the data used to extract S. In the region below the dotted line, the self-®eld (the ®eld generated by the screening currents themselves) is comparable to or larger than the applied ®eld, and so complicates the interpretation. sample of YBa2Cu3O7 (unless very well textured crystallographically) would behave as an assembly of disconnected grains at all but the lowest applied ®elds. The values of Jc (Fig. 2) are high; as a benchmark, at 20 K and 1 T, Jc is 1:0 3 105 A cm 2 2 . However, Jc decreases quite rapidly with applied ®eld, and an `irreversibility ®eld' Hirr (Fig. 2, inset) can be de®ned above which supercurrents cannot be sustained; that is, Jc becomes unmeasurably small. Because we have established that the sample is well connected, the Jc values shown in Fig. 2 are a reliable measure of the intragranular critical current density in MgB2. There have already been several magnetic studies of pressed and sintered pellets of MgB2 (refs 7±9). All the irreversibility ®elds are similar to the values shown in Fig. 2, but in two cases7,8 the Jc values are more than an order of magnitude less than reported here. Takano et al.9, who sintered their material at high temperatures and pressures, report a rather larger Jc, ,4 3 104 A cm 2 2 at 20 K and 1 T, but still a factor of 2 or 3 less than we measure. Overall, these results can be understood straightforwardly: in sintered pellets of MgB2 the intergrain contact is less perfect than in our polycrystalline as-grown fragments, to a degree dependent upon processing. The reduced cross-sectional contact area limits the magnitude of the macroscopic critical current, but its ®eld and temperature dependences appear to be essentially independent of the source or preparation of the materialÐin sharp contrast to the sensitivity of the HTS phases to processing. The other key aspect of the vortex physics is that because of thermal activation, the vortices are never totally immobile, and the screening current and associated magnetic moment decay with time in a quasi-logarithmic fashion. The relevant parameter is the vortex creep rate, S, de®ned as the logarithmic derivative -] ln m/] ln t. S is small at low ®elds (Fig. 3), but increases quasi-exponentially as the ®eld approaches Hirr. The creep rate is related directly to the current±voltage (or equivalently, current density J±electric ®eld E) characteristic of the material10, with E ~ J 1=S ; thus in MgB2 the E±J characteristics at low ®elds are very steep, which is desirable for 564 –10 0.0 µ H (T) ° Figure 4 Comparison of the vortex behaviour in MgB2 and YBa2Cu3O7. Within the context of standard vortex pinning theory, a plot (at ®xed temperature) of xln Ðthe dimensionless slope of the ln Jc ±ln H curves of Fig. 2Ðagainst the creep rate S, with H as implicit parameter, should have some simple form11. The oscillations in the data are instrumental artefacts, as described in Fig. 3 legend. The dotted line represents the behaviour of the HTS superconductor YBa2Cu3O7 at temperatures not too close to Tc (ref. 11). applications. At ®elds above Hirr, the vortex response becomes linear, E ~ J; consequently, it is to be expected that at ®elds close to Hirr, S should approach unity. The two quantities Jc and S, measured over a range of ®eld and temperature, together provide the essential information for an understanding of the vortex behaviour. Rather than use Jc itself, it is better to consider the dimensionless derivative ] ln Jc/] ln H; that is, the slope of the curves of Fig. 2. This quantity is identical to ] ln m/] ln H, and so is a logarithmic susceptibility, which we denote xln. A plot of xln (at a ®xed temperature) against S with H as the implicit parameter has a direct physical interpretation11: in YBa2Cu3O7, these plots are linear, with slopes almost independent of T (except close to Tc). This linearity indicates simple power-law dependences on H of two fundamental quantities: the current density J0 that would be attained if there were no thermal activation of the vortices, and the energy U0, which measures the vortex pinning as modi®ed by vortex±vortex interactions. In MgB2, these plots (Fig. 4) are again close to linear, and at 35 K (that is, close to Tc) have almost the same slope as that seen in YBa2Cu3O7. However, as the temperature drops, they become considerably steeper, which indicates that in MgB2 at temperatures not too close to Tc, U0 decreases very rapidly with increasing ®eld. Detailed measurements of xln in conventional LTS superconductors are technically dif®cult, so that no comparison of this kind can be made at present. MgB2 is certainly a promising material in some respectsÐJc is high and the grain boundaries appear benign in the context of supercurrent ¯owÐbut the irreversibility ®eld is rather low, only about half of the upper critical ®eld Hc2 (refs 7, 8). The sharp rise in the vortex creep rate S as the ®eld approaches Hirr, and the steep xln ±S plots, suggest that the vortex pinning interactions weaken catastrophically with increasing ®eld. Perhaps there is a paucity of pinning defects in the `as-grown' material, which would be consistent with the high degree of crystalline perfection of this compoundÐindicated by the very low residual resistivity12, and by the reproducibility of Tc and Hirr between samples from different sources. For MgB2 to become more useful for applications, it will be essential to ®nd ways to enhance the vortex pinning energy. M © 2001 Macmillan Magazines Ltd NATURE | VOL 410 | 29 MARCH 2001 | www.nature.com letters to nature Received 20 February; accepted 6 March 2001. 1. Nagamatsu, J., Nakagawa, N., Muranaka, T., Zenitani, Y. & Akimitsu, J. Superconductivity at 39 K in magnesium diboride. Nature 410, 63±64 (2001). 2. Cohen, L. F. & Jensen, H. J. Open questions in the magnetic behaviour of high temperature superconductors. Rep. Prog. Phys. 60, 1581±1672 (1997). 3. Mannhart, J., Chaudhari, P., Dimos, D., Tsuei, C. C. & McGuire, T. R. Critical currents in [001] grains and across their tilt boundaries in YBa2Cu3O7 ®lms. Phys. Rev. Lett. 61, 2476±2479 (1988). 4. Miyakawa, N. et al. Predominantly superconducting origin of large energy gaps in underdoped Bi2Sr2CaCu2O8+ from tunneling spectroscopy. Phys. Rev. Lett. 83, 1018±1021 (1999). 5. Cucolo, A. M. et al. Quasiparticle tunneling properties of planar YBa2Cu3O7-d/PrBa2Cu3O7-d/ HoBa2Cu3O7-d heterostructures. Phys. Rev. Lett. 76, 1920±1923 (1996). 6. Caplin, A. D., Cohen, L. F., Perkins, G. K. & Zhukov, A. A. The electric-®eld within high-temperature superconductorsÐmapping the E-J-B surface. Supercond. Sci. Technol. 7, 412±422 (1994). 7. Larbalestier, D. C. et al. Strongly linked current ¯ow in polycrystalline forms of the superconductor MgB2. Nature 410, 186±189 (2001). 8. Finnemore, D. K., Ostenson, J. E., Bud'ko, S. L., Lapertot, G. & Can®eld, P. C. Thermodynamic and transport properties of superconducting MgB2. Preprint cond-mat/0102114 at hhttp://xxx.lanl.govi (2001). 9. Takano, Y. et al. Superconducting properties of MgB2 bulk materials prepared by high pressure sintering. Preprint cond-mat/0102167 at hhttp://xxx.lanl.govi (2001). 10. Pust, L., Jirsa, M. & Durcok, S. Correlation between magnetic hysteresis and magnetic-relaxation in YBaCuO single-crystals. J. Low Temp. Phys. 78, 179±186 (1990). 11. Perkins, G. K. & Caplin, A. D. Collective pinning theory and the observed vortex dynamics in (RE)Ba2Cu3O7-d crystals. Phys. Rev. B 54, 12551±12556 (1996). 12. Can®eld, P. C. et al. Superconductivity in dense MgB2 wires. Preprint cond-mat/0102289 at hhttp://xxx.lanl.govi (2001). 13. Bean, C. P. Magnetization of high-®eld superconductors. Rev. Mod. Phys. 36, 31±36 (1964). Acknowledgements Y.B. is on leave of absence from the General Physics Institute, Moscow, Russia. We thank D. Cardwell and N. H. Babu for the supply of MgB2 powder, and A. J. P. White for crystallographic advice. This work was supported by the UK Engineering and Physical Sciences Research Council. Correspondence and requests for materials should be addressed to Y.B. (e-mail: y.bugoslav@ic.ac.uk). ................................................................. Extreme damping in composite materials with negativestiffness inclusions R. S. Lakes*²³§k, T. Lee³, A. Bersie*² & Y. C. Wang*² * Department of Engineering Physics; ² Engineering Mechanics Program; ³ Biomedical Engineering Department; § Materials Science Program; and k Rheology Research Center, University of Wisconsin-Madison, 147 Engineering Research Building, 1500 Engineering Drive, Madison, Wisconsin 53706-1687, USA .............................................................................................................................................. When a force deforms an elastic object, practical experience suggests that the resulting displacement will be in the same direction as the force. This property is known as positive stiffness1. Less familiar is the concept of negative stiffness, where the deforming force and the resulting displacement are in opposite directions. (Negative stiffness is distinct from negative Poisson's ratio2±6, which refers to the occurrence of lateral expansion upon stretching an object.) Negative stiffness can occur, for example, when the deforming object has stored7 (or is supplied8 with) energy. This property is usually unstable, but it has been shown theoretically9 that inclusions of negative stiffness can be stabilized within a positive-stiffness matrix. Here we describe the experimental realization of this composite approach by embedding negative-stiffness inclusions of ferroelastic vanadium dioxide in a pure tin matrix. The resulting composites exhibit extreme mechanical damping and large anomalies in stiffness, as a consequence of the high local strains that result from the inclusions deforming more than the composite as a whole. Moreover, for NATURE | VOL 410 | 29 MARCH 2001 | www.nature.com certain temperature ranges, the negative-stiffness inclusions are more effective than diamond inclusions for increasing the overall composite stiffness. We expect that such composites could be useful as high damping materials, as stiff structural elements or for actuator-type applications. Composite materials were prepared with inclusions of vanadium dioxide (VO2) in a pure (99.99%) tin matrix. Particulate inclusions 150 mm in size or smaller were incorporated into a tin matrix by rolling sheets of tin with particles, followed by casting into a cylindrical mould 3 mm in diameter. Vanadium dioxide is a ferroelastic material10±12 that undergoes a transformation from monoclinic to tetragonal at transformation temperature T c 67 8C; the transition exhibits hysteresis. It is similar in structure10 to the stiff mineral rutile (TiO2) with elastic moduli13 C11 271 GPa and C33 483 GPa. By contrast, steel has a Young's modulus of E 200 GPa (C 11 C 33 269 GPa); for tin E 50 GPa. The material properties were measured using a broadband viscoelastic spectroscopy apparatus14,15, capable of a range of eleven decades of time and frequency in torsion. Specimens were mounted using cyanoacrylate cement: at the top to its support rod, and at the bottom, to a high magnetic intensity neodymium iron boron magnet. The dynamic experiments were conducted by applying a sinusoidal voltage at 100 Hz, from a digital function generator to a Helmholtz coil. The lowest specimen resonance was at several kilohertz. The coil imposed a magnetic ®eld on the permanent magnet and transmitted an axial torque to the specimen. The angular displacement of the specimen was measured using laser light re¯ected from a mirror mounted on the magnet to a splitdiode light detector. The detector signal was ampli®ed with a wideband differential ampli®er. Torque was inferred from the Helmholtz coil current, supported by calibrations using the well characterized 6061 Al alloy29. Input and output voltages and the phase between them were recorded using a lock-in ampli®er (SRS 850, Stanford Research Systems). Data were reduced using the analytical relationship for the torsional rigidity of a viscoelastic cylinder. Constituent stiffness was tuned by varying the temperature. An insulated inner chamber was heated to above 85 8C and the temperature was maintained for at least 30 minutes. The heater was shut off and the chamber allowed to cool. Cooling rate over the temperature range of interest was less than 1 8C per minute. Material properties, stiffness and damping (tand, where d is the phase between stress and strain) as a function of temperature of a particulate VO2 ±tin composite with 1% by volume of inclusions are shown in Fig. 1. Although the concentration of inclusions is dilute, large anomalies are observed in the mechanical damping, tand, as well as in the stiffness. For comparison, tand of pure Sn is 0.019 and varies little with temperature, as shown. The sharp dependence on temperature we attribute to the fact that the inclusions are much stiffer than the matrix (away from the transition temperature) and can only balance the matrix stiffness near the transition. The peaks observed in the present 1% VO2 composite are larger than in 100% VO2, which had a peak12 of 0.04 to 0.05 in tand and a dip of 8% in stiffness at the transition. In the composite, there is interplay between constituents of positive and negative stiffness; by contrast, 100% VO2 has positive stiffness at all temperatures due to the formation of domains. A negative-stiffness lumped element (a structure) can be stabilized by a hard constraint. For an unconstrained block (or, surface traction boundary condition, in the language of elasticity1) of isotropic material to be stable, the shear modulus G and the bulk modulus B, as stiffness quantities, must be positive. This corresponds to a range of Poisson's ratio n (de®ned as the negative transverse strain of a stretched or compressed body divided by its longitudinal of strain) 2 1 , n , 0:5. Materials of negative Poisson's ratio, while exhibiting the unusual property of transverse expansion when stretched, can have all positive-stiffness values, and hence stability. For most solids1, n is between 0.25 and 0.33. © 2001 Macmillan Magazines Ltd 565