INSTITUTE OF PHYSICS PUBLISHING SUPERCONDUCTOR SCIENCE AND TECHNOLOGY Supercond. Sci. Technol. 15 (2002) 315–319 PII: S0953-2048(02)28059-8 Magnetic relaxation and critical current density of the new superconductor MgB2 H H Wen, S L Li, Z W Zhao, H Jin, Y M Ni, Z A Ren, G C Che and Z X Zhao National Laboratory for Superconductivity, Institute of Physics and Center for Condensed Matter Physics, Chinese Academy of Sciences, PO Box 603, Beijing 100080, People’s Republic of China E-mail: hhwen@aphy.iphy.ac.cn Received 20 August 2001 Published 25 January 2002 Online at stacks.iop.org/SUST/15/315 Abstract Magnetic relaxation rate, critical current density and transport properties have been investigated on MgB2 bulks from 1.6 K to Tc at magnetic fields up to 8 T. A vortex phase diagram is depicted based on these measurements. A large separation between the bulk irreversibility field Hirr(T ) and the upper critical field Hc2(T ) has been found. It is thus proposed that there is a quantum vortex liquid due to strong quantum fluctuation of vortices at 0 K. It is also found that the magnetic relaxation rate is weakly dependent on temperature but strongly dependent on field indicating a trivial influence of thermal fluctuation on the vortex depinning process. Therefore, the phase line Hirr(T ) is attributed to quantum vortex melting in the rather clean system at a finite temperature. 1. Introduction The recently discovered new superconductor MgB2 generates enormous interest in the field of superconductivity [1]. Many important thermodynamic parameters have already been derived, such as the upper critical field Hc2(0) = 13–20.4 T [2], the Ginzburg–Landau parameter κ ≈ 26 [5] and the bulk critical superconducting current density jc ≈ 8 × 104 A cm−2 at 4.2 K and 12 T [6] in thin films. However, one big issue is concerned with how fast the critical current will decay under a magnetic field and in which region on the field–temperature (H–T ) phase diagram the superconductor can carry a large critical current density ( jc). This jc is determined by the mobility of the magnetic vortices, and vanishes at the melting point between the vortex solid and liquid. A finite linear resistivity ρlin = (E/j )j →0 will appear and the relaxation rate will reach 100% at this melting point showing the starting of the reversible flux motion. In this paper we present an investigation on the flux dynamics by magnetic relaxation and transport measurement. A vortex phase diagram will be depicted based on the magnetic relaxation data. 2. Experimental details Samples investigated here were fabricated by both highpressure (HP) (P = 6 GPa at 950 ◦ C for 0.5 h) and 0953-2048/02/030315+05$30.00 © 2002 IOP Publishing Ltd ambient-pressure (AP) syntheses [7]. High-pressure synthesis is a good technique for producing the MgB2 superconductor since it can make the sample more dense and uniform (in submicron scale) and also prevent the oxidization of Mg element during the solid reaction. Our HP samples are very dense and look like metals with shiny surfaces after polishing. Scanning electron microscopy (SEM) shows that the HP sample is uniform in the submicron scale, but some disordered fine structures are found in the 10 nm scale, which are similar to the internal structure of large grains seen in the AP sample. X-ray diffraction (XRD) analysis on both type of samples show that they are nearly in a single phase with the second phase (probably MgO or MgB4) less than 1 wt%. For simplicity we present mainly the results from the HP sample in this paper. The resistive measurements were carried out using the standard four-probe technique with a Keithley 220 dc current source and a Keithley 182 nanovoltmeter, and the magnetic field was applied with a vibrating sample magnetometer (VSM, Oxford 3001), with the field range varying from 0 to 8 T. For transport measurements the sample was given a rectangular shape with dimensions of 4 mm × 3 mm × 0.5 mm. Four silver pads were deposited onto the sample’s surface for electric contacts with low contacting resistance. The magnetic measurements were carried out by a superconducting quantum interference device (SQUID, Printed in the UK 315 2.0 High Pressure Sample 1.5 FC 1.0 1.0 M ( emu ) 2 0 -2 -4 -6 -8 -10 -12 -14 -16 0 0.8 R ( mΩ ) -3 M ( 10 emu ) H H Wen et al 0.6 0.4 0.2 ZFC 0.0 20 30 40 50 0.5 0.0 -0.5 dH / dt = 100 Oe / s T = 2, 4, 6, 8, 10, 14, 18, 22, 26, 30, 32, 35, 37, 38 K -1.0 -1.5 60 T(K) -2.0 -2 10 20 30 40 50 60 70 80 90 0 2 10 6 10 5 10 4 10 3 316 22 K 18 K 14 K 35 K 32 K 10 K 8K 0.001 0.000 -0.001 10 2 10 1 -0.002 -0.003 0 0.01 T = 30 K M ( emu ) Figure 1 shows the diamagnetic transition of one of the HP samples measured in the field-cooled (FC) and zero-fieldcooled (ZFC) processes. All of the other samples show almost similar quality. In the FC process, the temperature was lowered from above Tc to a desired temperature below Tc under a magnetic field, and the data were collected in the warming up process with a field. Its signal generally describes the surface shielding current and the internal frozen magnetic flux profile. In the ZFC process, the temperature was lowered from above Tc to a desired temperature below Tc at a zero field and the data were collected in the warming up process with a field. Its signal generally describes the internal magnetic flux profile which is ultimately related to the flux motion. The inset shows the resistive measurement on the sample. In zero field, the superconducting transition temperature Tc0 and Tc (onset) are 38.9 and 39.9 K, respectively. Both resistive and diamagnetic measurements show that the transition is very sharp with a perfect diamagnetic signal. In figure 2 we show the magnetization hysteresis loops (MHLs) measured at temperatures ranging from 2 to 38 K. The symmetric MHLs observed at temperatures up to 38 K indicate the dominance of the bulk current instead of the surface shielding current. The MHLs measured at low temperatures, such as 2 and 4 K, show quite a strong flux jump which will be discussed elsewhere [8]. It is easy to see that the MHLs measured at low temperatures (e.g., 2–10 K) are too close to be distinguishable. This indicates that both the critical current density jc and the irreversibility field Hirr are weak 30 K 26 K 37 K 2 3. Results 8 Figure 2. Magnetization hysteresis loops measured at 2, 4, 6, 8, 10, 14, 18, 22, 26, 30, 32, 35, 37 and 38 K (from outer to inner). All curves show a symmetric behaviour indicating the importance of bulk current instead of surface shielding current. The MHLs measured at low temperatures (e.g., 2–10 K) are too close to be distinguishable. Strong flux jump has been observed at 2 and 4 K near the central peak. Jc( A/cm ) Quantum Design MPMS 5.5 T) and a vibrating sample magnetometer (VSM 8T, Oxford 3001). To precisely calculate the critical current density jc, the sample was cut with a diamond saw into a rectangular shape with dimensions of 3.2 mm (length) × 2.7 mm (width) × 0.4 mm (thickness). 6 µ0H ( T ) T(K) Figure 1. Temperature dependence of the superconducting diamagnetic moment measured in the ZFC and FC processes at a field of 10 Oe. A perfect diamagnetic signal can be observed here. The inset shows the resistive transition with Tc0 and Tc (onset) are 38.9 and 39.9 K, respectively. 4 6K 4K 2K 1 2 3 µ0H ( T ) 0.1 1 µ0H( T ) 10 Figure 3. Critical current density jc calculated based on the Bean critical state model. At each temperature the data has been measured with three field sweeping rates: 200, 100 and 50 Oe s−1. The faster sweeping rate corresponds to a higher dissipation and thus higher current density. From these data one can calculate the dynamical magnetic relaxation rate Q. The jc(H) curves measured at low temperatures are very close to each other showing a rather stable value of Hirr(T ) when T approaches 0 K. The dashed horizontal line marks the criterion of jc = 30 A cm−2 for determining the Hirr(T ). temperature-dependent functions in low-temperature region. From these MHLs one can calculate jc as jc = 20M/Va (1 − a/3b) based on the Bean critical state model, where M is the width of the MHL, V , a and b are the volume, width and length of the sample, respectively. The results of calculated jc(H) are shown in figure 3. It is clear that the bulk critical current density jc of our sample is rather high. To investigate the flux dynamics, the jc(H) curves have been measured with three different field sweeping rates 200, 100 and 50 Oe s−1. The so-called irreversibility line Hirr(T ) has been determined by taking a criterion of jc = 30 A cm−2. Hc2(T ) is determined 20 18 Hc2 16 14 V ort 12 ex Li q 10 u id 8 6 4 Vortex Solid 2 0 0 5 10 15 1.0 2K Hc2-Bulk-SQUID Hc2-Takano Hc2-Bulk-Trans Hirr-Bulk-VSM Hirr-Bulk-SQUID Hirr-Bulk-Trans 0.8 Relaxation Rate 0 Magnetic relaxation and critical current density of the new superconductor MgB2 0.6 0.4 0.2 0.0 20 25 30 35 40 T(K) Figure 4. H–T phase diagram for the new superconductor MgB2. The filled circles represent the bulk irreversibility lines Hirr(T ) measured by the VSM; half-filled circles represent Hirr(T ) for another sample measured by SQUID; open diamond represent Hirr of the HP sample measured by resistive transport. The filled squares represent the Hc2(T ) data of Takano et al [4] from resistive measurement; open squares represent this work from the M(T ) measurement by SQUID; filled diamond represent this work by transport measurement. All the lines are guide to the eye. from the M(T ) curve at the point where the magnetization starts to deviate from the normal state linear background. Another method to determine Hirr(T ) and Hc2(T ) is to measure the resistive transitions at different magnetic fields. Hirr(T ) was determined by taking a minimum value of resistivity as the criterion, while for the upper critical field Hc2(T ), we (and Takano et al [4]) determined the upper critical point Tc2 from the point at which the resistance starts to deviate from the normal state resistance. All the phase lines determined by using these methods are presented and discussed below. 4. Discussion 4.1. Vortex phase diagram of MgB2 The phase lines of Hirr(T ) and Hc2(T ) determined by the methods mentioned above are shown in figure 4. It is clear that the irreversibility line Hirr(T ) determined from the MHL is very close to that determined by resistive measurement. This strongly indicates that Hirr(T ) is a vortex melting line which signals the appearance of a finite linear resistivity. Plotted together in figure 4 are the upper critical field Hc2(T ) determined from (1) the temperature-dependent magnetization by defining Hc2(T ) as the point at which the magnetization starts to deviate from the normal state linear background [9], and (2) the resistive measurement by Takano et al [4] and by us on HP samples. Although the samples are from different groups and different techniques have been used to obtain the data, the vortex phase diagram derived here has a good consistency. A striking result from this vortex phase diagram is that Hirr(T ) extrapolates to a rather low field at 0 K, here, for example, Hirr(0) ≈ 8 T, while Hc2(T ) extrapolates to a much higher value Hc2(0) Hirr(0) T = 2, 4, 6, 8, 10, 14, 18, 22, 26, 30, 32,35,37 K 0 2 4 6 8 10 12 14 16 18 20 µ0H ( T ) Figure 5. Field dependence of the relaxation rate at temperatures 2, 4, 6, 8, 10, 14, 18, 22, 26, 30, 32, 35 and 37 K. The dashed line is a guide to the eye for 2 K. It is clear that Q will rise to 100% at 8 T and 2 K. Since Hirr(T ) is rather stable at low temperatures, it is anticipated that Hirr(0) ≈ 8 T, which is much smaller than Hc2(0) ≈ 15 T. (Hc2(0) ≈ 15 T) [2] at 0 K. There is a large separation between the two fields Hirr(0) and Hc2(0). If following the hypothesis of the vortex liquid above Hirr(T ), we would conclude that there is a large region of magnetic field for the existence of a vortex liquid at 0 K. This can be attributed to a quantum fluctuation effect of vortices in bulk MgB2. Although the lowest temperature in our present experiment is 1.6 K, from the experimental data one cannot find any tendency for Hirr(T ) to turn upward rapidly to meet Hc2(0). One may argue that the Hirr(T ) probably can be increased to higher values by introducing more pinning centres into this sample. This is basically correct since recently a higher irreversibility line Hirr(T ) has been found in some MgB2 thin films [6] and bulk samples irradiated by protons [10]. Actually in our recent experiment on MgB2 thin films, the irreversibility line Hirr(T ) is also close to that of bulks. This indicates that the large separation between Hirr(0) and Hc2(0) may be an intrinsic property of MgB2 in the clean limit. 4.2. Large separation between Hirr(0) and Hc2(0) and possible evidence for strong quantum fluctuation of vortices In order to investigate the flux dynamics in the vortex solid state below Hirr(T ) and to see more clearly the evidence for the quantum vortex melting in a relatively pure system, we have carried out the dynamical relaxation measurement. According to Schnack et al [11] and Jirsa et al [12], in a field sweeping process, if the field sweeping rate is high enough, the quantity Q = d ln M/d ln(dH/dt) is close to the relaxation rate S = −d lnM/d ln t measured in the conventional relaxation method, where Q is called the dynamical relaxation rate, M is the width of the MHL and dH/dt is the field sweeping rate. The raw data with three different sweeping rates (200, 100 and 50 Oe s−1) are shown in figure 3. The Q values versus field for different temperatures are determined and shown in figure 5. It is clear that the relaxation rate increases monotonically with 317 H H Wen et al is probably induced by a strong pinning barrier relative to the thermal energy, i.e. kBT Uc, where Uc is the intrinsic pinning energy. Recently, it was concluded [15, 16] that Uc is in the scale of 1000 K, which is much higher than the thermal energy kBT. Therefore, for the new superconductor MgB2 the pinning well is too deep leading to a trivial influence of the thermal activation and fluctuation. It thus naturally suggests that the quantum fluctuation and tunnelling of vortices are quite strong in MgB2. We strongly suggest that the melting between a vortex solid and a liquid is due to the quantum fluctuation instead of the thermal fluctuation. Relaxation Rate 1.0 6T 5T 10 15 4T 3T 2T 1T 30 35 0.8 0.6 0.4 0.2 0.0 0 5 20 25 40 T(K) Figure 6. Temperature dependence of the relaxation rate at fields 1, 2, 3, 4, 5 and 6 T. The dashed lines are guide to the eye. The arrows point at the bulk irreversibility temperatures Tirr determined from the jc(H) curve. the external magnetic field and extrapolates to 100% at the bulk melting point Hirr(T ). At 2 K it is found from the Q(H ) data that the vortex melting field (where Q = 100%) is about 8 T, which is very close to Hirr(T = 2 K) determined from the jc(H) curve. It is known that Hirr(T ) is rather stable in a low-temperature region; therefore we can anticipate a rather low value of Hirr(0) which is below 9 T being much lower than Hc2(0). Again one can see a large separation between Hirr(0) and Hc2(0). This effect has recently been found also in rather pure MgB2 films [13] with Tc(0) = 38 K and jc(0 T, 14 K) = 1.8 × 107 A cm−2. All these may strongly suggest the existence of the quantum vortex liquid due to strong quantum fluctuation of vortices in the pure system of MgB2. The reason for the strong quantum fluctuation is still unknown. It may share the same reason as the relatively low upper critical field. 4.3. Residual relaxation rate at 0 K and weak temperature dependence of the relaxation rate Figure 6 shows the temperature dependence of the dynamical relaxation rate Q. The arrows point at the irreversibility temperatures at the corresponding fields Hirr(T ). It is clear that the relaxation rate extrapolates to a finite value at 0 K for all fields. This effect was also observed in high-Tc cuprate superconductors and attributed to the quantum tunnelling of vortices. The difference between the MgB2 and the HTS is that the residual relaxation rate Q at 0 K in the former case has a strong field dependence, but in the latter it is weakly dependent on the field, especially for the 3D YBa2Cu3O7 system. Another striking point for MgB2 is that in a wide temperature region the relaxation rate is rather stable against the thermal activation and fluctuation. However, when the bulk melting point Hirr(T ) is approached the relaxation rate will quickly jump to 100%. The small relaxation rate at a relatively low field has also been measured by Thompson et al [14] who regarded it as a highly stable superconducting current density in MgB2. Actually the relaxation rate can be rather high when the magnetic field is increased to a higher value. The extremely small relaxation rate and weak temperature dependence at a finite temperature 318 5. Conclusion In conclusion, in rather pure samples of MgB2, the irreversibility field is rather low compared to the upper critical field in the low-temperature region showing the possible existence of the quantum vortex liquid due to strong quantum fluctuation of vortices. The temperature and field dependence of the relaxation rate may further suggest that the vortex melting at a finite temperature is also induced by strong quantum fluctuation in pure systems, such as single crystals and bulks. Magnetic relaxation measurement shows that the pinning barrier is much higher than the thermal energy; this may also interpret the trivial importance of the thermal activation and thermal fluctuation. In comparison the quantum tunnelling and the fluctuation show a much stronger influence. 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