PHYSICAL REVIEW B VOLUME 60, NUMBER 21 1 DECEMBER 1999-I Frequency and ac field scaling of the nonlinear ac susceptibility of a HgBa2CaCu2O6ⴙ ␦ thin film B. J. Jönsson-Åkerman* and K. V. Rao Department of Condensed Matter Physics, Royal Institute of Technology, S-100 44 Stockholm, Sweden E. H. Brandt Max-Planck-Institut für Metallforschung, Institut für Physik, D-70506 Stuttgart, Germany 共Received 16 February 1999兲 We confirm a recently proposed scaling relation for the nonlinear ac susceptibility response of type-II superconductors by high-precision measurements on a c-axis oriented HgBa2CaCu2O6⫹ ␦ thin film. From measurements in different ac field and frequency combinations, given by the scaling relation, the flux creep exponent n(T,H) of the superconducting film can be determined. At T⫽100 K and in the field range studied, n(T,H) is found to vary with the dc bias field as H ⫺0.18 . 关S0163-1829共99兲00245-3兴 dc I. INTRODUCTION Scaling procedures have played a significant role in gaining insight into the basic understanding of the length scale of various fundamental properties of high-T c superconductors. One of the most widely reported scaling procedures1 uses nonlinear dc conductivity data (J) to extract the glass temperature T g and the static and dynamic critical exponents v and z. Similar information can also be extracted from a scaling analysis of the linear ac susceptibility response of thin superconducting disks.2 Recently another scaling relation has been predicted for the nonlinear ac susceptibility response of type-II superconductors.3 For any nonlinear conductor with power-law E-J characteristics E(J)⫽E c (J/J c ) n the ac susceptibility response should be invariant to a simultaneous change in ac field amplitude and frequency following n⫺1 H ac ⫽const. 共1兲 This scaling relation does not originate from a phase transition, as is the case for glass scaling around T g , but is rather a consequence of Maxwell’s equations and the material law relating the current density and the electric field. In this work we experimentally confirm that the ac susceptibility response of a c-axis oriented HgBa2CaCu2O6⫹ ␦ 共Hg-1212兲 thin film is invariant under the transformation Eq. 共1兲 and show how this invariance can be used to determine the flux creep exponent n(T,H). By varying the applied dc bias field we also determine the dc field dependence of the flux creep exponent at 100 K. The explicit form of the kernel Q(r,r⬘ ) for a cylinder has been given in Ref. 4. The momentary screening current can be found from numerical time integration of Eq. 共2兲 and the corresponding magnetic moment of the disk is at each time given by m 共 t 兲 ⫽2 R d dr 0 0 冋 dy ⬘ Q 共 r,r⬘ 兲 ⫺1 E 共 J 兲 ⫺ 0163-1829/99/60共21兲/14913共4兲/$15.00 drr 2 0 冕 d 0 ⫽ 1 h 0V 冕 2 0 册 r⬘ Ḣ 共 t 兲 . 2 0 a 共2兲 PRB 60 dyJ 共 r,y,t 兲 . m 共 t 兲 e ⫺i t d 共 t 兲 , 共3兲 共4兲 where V is the sample volume. Once the material law E(J) is known, the ac susceptibility response of a thin circular disk can be readily calculated using Eqs. 共2兲–共4兲. Both the collective creep6 and the vortex glass7 theories predict a current-density-dependent activation energy for vortex depinning, U 共 J 兲 ⫽U 0 共 J c /J 兲 ␣ ⫺1 ␣ , 共5兲 where ␣ is a small positive exponent. When inserted into the Arrhenius law, 冉 E 共 J 兲 ⫽E c exp ⫺ The problem of how an external axial magnetic field 0 H a (t) penetrates into a superconducting cylinder of radius R and thickness 2d can be formulated as an equation of motion for the screening current J(r,t)⫽J(r,y,t), 冕 ⬘冕 R In a typical ac susceptibility measurement the external magnetic field varies sinusoidally in time as H a (t)⫽h 0 cos t. The fundamental ac susceptibility ⫽ ⬘ ⫺i ⬙ can then be defined5 as II. SCALING RELATION J̇ 共 r,t 兲 ⫽ ⫺1 0 冕 冊 U共 J 兲 , kT 共6兲 Eq. 共5兲 yields a highly nonlinear E-J relation. In the limit ␣ →0, one has the so-called logarithmic approximation8 U(J)⫽U 0 ln(Jc /J) that is generally considered to describe single-vortex creep.9 Within this approximation Eq. 共6兲 becomes E 共 J 兲 ⫽E c 共 J/J c 兲 n with n⫽U 0 /kT, 14 913 共7兲 ©1999 The American Physical Society B. J. JÖNSSON-ÅKERMAN, K. V. RAO, AND E. H. BRANDT 14 914 PRB 60 which is often experimentally observed.10,11 Even in an experimental situation when the full expression for the activation energy 关Eq. 共5兲兴 should be used, an effective flux creep exponent can be defined as4 n̄⬅ 冉冊 ln E U 0 J c ⫽ ln J kT J ␣ ⭓ U0 . kT 共8兲 Such an effective flux creep exponent will depend on the ratio J c /J, i.e., on how much the current density has relaxed from its initial value J c , and hence on the driving frequency . For small enough ␣ this frequency dependence may, however, be neglected. It has recently been shown3 that when E(J) is given by a power-law relation as in Eq. 共7兲, the equation of motion for the screening current density 关Eq. 共2兲兴 is invariant to a simultaneous change in the time unit, by a factor of c, and in the current and field units, by a factor of c 1/(n⫺1) . This means that if Eq. 共2兲 is expressed in a new time unit t̃ ⫽t/c, then the new functions J̃(r, t̃ )⫽J(r,t) * c 1/(n⫺1) and H̃ a ( t̃ ) ⫽H a (t) * c 1/(n⫺1) will satisfy the same equation. The resulting magnetic moment will consequently scale by the same factor, m̃( t̃ )⫽m(t) * c 1/(n⫺1) . In the case of a periodic applied field H a (t)⫽h 0 cos t, the ac susceptibility (h 0 , ) will hence remain unchanged if the frequency is increased by, say, a factor of 10 and the amplitude by a factor of 101/(n⫺1) , which is the condition given by Eq. 共1兲. The same scaling relation will hold approximately for the effective flux creep exponent n̄, provided n̄ does not change considerably in the frequency range studied. III. EXPERIMENT Hg-1212 films with nominal thickness of 400 nm were prepared by a conventional two-step method involving deposition of Hg-free precursor films on SrTiO3 substrates followed by annealing at 820 °C for 30 min in a controlled Hg-vapor atmosphere. The x-ray-diffraction pattern collected within 5°⬍2 ⬍70° shows predominantly lines corresponding to the c-axis oriented Hg-1212 phase with minor traces of c-axis oriented Hg-1223. A rectangular sample with lateral dimensions 2.8⫻3.6 mm2 was chosen for this study. A home-built high-sensitivity susceptometer,12,13 based on a three-coil mutual inductance bridge and a two-position background subtraction scheme, was used for all measurements. ac fields of H ac⫽1 – 2 Oe 共root-mean-square, H ac ⫽2 ⫺1/2h 0 ) and dc fields in the range H dc⫽20– 100 Oe were applied by the same primary coil. Driving frequencies ranged from f ⫽89.1– 891 Hz. The software allows for consecutive measurements at different field and frequency settings specified by a list that is run through repeatedly. To minimize flux trapping, a decrease in ac field is always done gradually with the minimum step given by the resolution of the digital lock-in output 共⬃0.3%兲. The temperature may be ramped slowly or held constant during the measurement. The ac susceptometer is calibrated in emu/Oe and hence measures ⬘ V and ⬙ V. For thin films measured in the perpendicular geometry, it is not practical to divide by the film volume. In the following we will therefore always express the susceptibility in emu/Oe, which for brevity will be denoted by ⬘ and ⬙ . FIG. 1. ⬘ and ⬙ vs T for H ac⫽1 mOe, f ⫽181 Hz. In the inset is shown ⬘ vs T for H ac⫽15 Oe, f ⫽8.91, 27.3, 89.1, 273, and 891 Hz. IV. RESULTS AND DISCUSSION From a typical low-field 共1 mOe兲 ac susceptibility temperature scan, shown in Fig. 1, we find T c ⫽120 K with ⌬T c ⫽4.5 K given by the temperatures where 10% and 90% of complete screening is reached, respectively. The fullscreening susceptibility of a thin circular disk with radius a is 0 ⫽2a 3 /3 in cgs units. Numerical simulations of thin rectangular samples with sides 2a and 2b show that the thincircular-disk expression can be used provided it is multiplied with a prefactor that depends on the aspect ratio b/a. 14 The experimentally determined susceptibility at 77 K in Fig. 1, 0,exp⫽⫺9.4⫻10⫺4 emu/Oe, is only about 3% smaller than 0,th⫽⫺1.67⫻2a 3 /3 ⫽⫺9.7 the theoretical value ⫺4 ⫻10 emu/Oe. In the inset is shown a temperature scan in an ac field of H ac⫽15 Oe and f ⫽8.91– 891 Hz. Due to the higher ac field the transition broadens considerably and also there is a clear increase in the transition width as the frequency is decreased. The observation of these two different causes for a broadened transition gives additional insight into the physical meaning of Eq. 共1兲: broadening due to an increase in H ac can be annulled by a corresponding increase in excitation frequency; the ratio between the factors describing the respective increases is given by the flux creep exponent through Eq. 共1兲. It is experimentally known that n(T,H) in Hg-1212 thin films depends strongly on both field and temperature.10 Since the scaling relation assumes that the flux creep exponent does not vary during the ac field period, we perform all measurements in a dc bias field to ensure that n(T,H) is kept constant. It has recently been shown that for H dcⱿ2H ac , n(T,H) in Hg-1212 thin films does not show any detectable ac field dependence.15 In this study we use H ac⬇2 Oe in dc bias fields of H dc⫽20– 100 Oe. In Table I we give the applied ac fields and frequencies used in the experiments, which satisfy Eq. 共1兲 for trial flux creep exponents n ⬘ ⫽10– 17. If n ⬘ equals the actual flux creep exponent n(T,H) we expect a collapse of all the data; if n ⬘ is too large, the increased broadening due to a lower frequency will not be fully compensated for by the corre- FREQUENCY AND ac FIELD SCALING OF THE . . . PRB 60 14 915 TABLE I. Listing of ac field 共in Oe rms兲 and frequency combinations used in experiments to test the trial exponents n ⬘ ⫽10– 17. f 关Hz兴 891 413 273 181 127 89.1 n ⬘ ⫽10 n ⬘ ⫽11 n ⬘ ⫽12 n ⬘ ⫽13 n ⬘ ⫽14 n ⬘ ⫽15 n ⬘ ⫽16 n ⬘ ⫽17 2.000 1.836 1.754 1.675 1.611 1.549 2.000 1.852 1.777 1.795 1.646 1.589 2.000 1.865 1.796 1.730 1.675 1.622 2.000 1.876 1.812 1.751 1.700 1.651 2.000 1.885 1.826 1.769 1.722 1.675 2.000 1.893 1.838 1.785 1.740 1.697 2.000 1.900 1.848 1.798 1.756 1.715 2.000 1.906 1.857 1.810 1.770 1.732 sponding weaker ac field and consequently 兩 ⬘ ( f ) 兩 will be smaller than 兩 ⬘ (891 Hz) 兩 for all frequencies f ⬍891 Hz; if n ⬘ is too small, on the other hand, 兩 ⬘ ( f ) 兩 will be larger than 兩 ⬘ (891 Hz) 兩 . A typical measurement run at T⫽100 K and H dc⫽20 Oe with ac fields corresponding to n ⬘ ⫽10 is shown in Fig. 2. Data are taken over a period of approximately 2 h and averaged to improve the accuracy. For this particular choice of n ⬘ ⫽10 the data clearly do not collapse. On the contrary, the magnitude of the in-phase component increases with decreasing frequency, which indicates that the applied ac field is decreased too rapidly with frequency for a collapse to occur, i.e., n ⬘ ⫽10 is smaller than the actual n(T,H). In Fig. 3 we show the same data together with data for all trial flux creep exponents n ⬘ ⫽10– 17 in dc fields ranging from 20 to 100 Oe. For all dc fields we see that there is a monotonic change in how well the data collapse for different values of the trial value n ⬘ . While for n ⬘ ⫽10 in a field of H dc⫽20 Oe no overlap was observed in Fig. 2, the overlap is almost perfect for n ⬘ ⫽16. For too small n ⬘ values all data lie below ⬘ (891 Hz) and for larger n ⬘ values data points consequently lie above ⬘ (891 Hz). When data points taken at the same frequency are connected with straight lines, as shown for H dc⫽45 Oe, the lines intersect almost perfectly in a single point. For each dc field we thus determine the actual flux creep exponent n(T⫽100 K, H dc) from the intersection point of these lines. We also take the extension of the inter- FIG. 2. ⬘ ( f )/ 兩 ⬘ (891 Hz) 兩 for n ⬘ ⫽10, H dc⫽20 Oe at T ⫽100 K measured during 2 h. ac fields and frequencies taken from the first column of Table I. To the right is plotted the time average of the same data. section region along the trial exponent axis as a measure of how well the data overlap. The flux creep exponent is plotted vs dc field in Fig. 4. n clearly decreases with increasing field and a log-log plot of the same data, shown in the inset, suggests a field depen⫺0.18 dence as H dc in the field range studied. The error bars indicate the size of the intersection regions extracted from Fig. 3 and confirm a close overlap of the experimental data. In a dc bias field of 100 Oe there is, however, an increased uncertainty in n that might indicate the scaling as given by Eq. 共1兲 is not adequate at this field. FIG. 3. Time-averaged data ⬘ ( f )/ 兩 ⬘ (891 Hz) 兩 for all combinations n ⬘ ⫽10– 17 and H dc⫽20– 100 Oe. The lines for H dc⫽45 Oe show how the value for the actual flux creep exponent n(T,H) is determined from their intersection. The dashed line is a guide to the eye to indicate how this intersection point moves with H dc . 14 916 B. J. JÖNSSON-ÅKERMAN, K. V. RAO, AND E. H. BRANDT PRB 60 n̄ is a useful concept that well describes the vortex dynamics in this field and temperature range. It is, however, quite likely that the increased uncertainty observed for H dc⫽100 Oe is due to a breakdown of this approximation. Since both ␣ and the ratio J c /J in Eq. 共8兲 are expected to increase with field, H dc⫽100 Oe might be a threshold field where n̄ depends too strongly on frequency for the scaling relation to be meaningful. V. CONCLUSION FIG. 4. n(T,H) vs H dc at T⫽100 K. The error bars correspond to the width of the intersection region in Fig. 3. In the inset is shown a log-log plot of the same data together with a power-law fit n(T,H)⬀H ⫺0.18 . dc In recent studies on the vortex dynamics of Hg-1212 thin films it has been shown that the logarithmic approximation 关Eq. 共7兲兴 can accurately describe the frequency dependence of the nonlinear ac susceptibility response.11 Below a certain line T cm(H) in the H-T plane, n(T,H) shows a monotonic decrease with temperature and is inversely proportional to the square root of the applied field, n(T,H)⬀H ⫺0.5. 12 Above this line, n(T,H) increases with increasing temperature and shows a weaker field dependence. Since T cm(H) is ascribed to a crossover from single-vortex creep to collective creep of flux bundles, a finite and increasing value for ␣ in Eq. 共5兲 is expected. At T⫽100 K we are above T cm for the fields used in this work, which is confirmed by the rather weak field dependence of the experimentally determined flux creep exponent. From the close overlap of the data in Fig. 共3兲 we conclude that, although the logarithmic approximation may no longer be strictly valid, the effective flux creep exponent *Current address: Physics Department, University of California– San Diego, 9500 Gilman Drive, La Jolla CA 92093-0319. Electronic address: jjonsson@ucsd.edu 1 R. H. Koch, V. Foglietti, W. J. Gallagher, G. Koren, A. Gupta, and M. P. A. Fisher, Phys. Rev. Lett. 63, 1511 共1989兲. 2 J. Kötzler, G. Nakielski, M. Baumann, R. Behr, F. Goerke, and E. H. Brandt, Phys. Rev. B 50, 3384 共1994兲. 3 E. H. Brandt, Phys. Rev. B 55, 14 513 共1997兲. 4 E. H. Brandt, Phys. Rev. B 58, 6506 共1998兲; ibid. 58, 6523 共1998兲. 5 T. Ishida, R. B. Goldfarb, S. Okayasu, Y. Kazumata, J. Franz, T. Arndt, and W. Schauer, Mater. Sci. Forum 137-139, 103 共1993兲. 6 M. V. Feigel’man, V. B. Geshkenbein, A. I. Larkin, and V. M. Vinokur, Phys. Rev. Lett. 63, 2303 共1989兲. 7 D. S. Fisher, M. P. A. Fisher, and D. A. Huse, Phys. Rev. B 43, 130 共1991兲. In conclusion, we have shown that high-precision ac susceptibility measurements on a c-axis oriented Hg-1212 thin film experimentally confirm a recently suggested scaling relation for the nonlinear ac susceptibility response of type-II superconductors with flux creep. By varying the applied dc bias field we demonstrate how the field dependence of the flux creep exponent n(T,H) can be determined. At T ⫽100 K and in a dc field range of H dc⫽20– 100 Oe we find that the field dependence of the flux creep exponent is well ⫺0.18 . From the close overlap of the described by n(T,H)⬀H dc data and the rather weak field dependence we conclude that our measurements are made in a regime where an effective flux creep exponent n̄ describes the vortex dynamics rather well, although, in a strict sense, the logarithmic approximation might not be valid anymore. At H dc⫽100 Oe the scaling is not adequate, which we interpret as an increase in the frequency dependence of n̄. ACKNOWLEDGMENTS We are grateful to S. H. Yun and U. O. Karlsson for providing us with their Hg-1212 thin-film sample. We thank A. M. Grishin for many discussions and comments during this work. B.J.J-Å. is most obliged to the Ericsson Research Foundation for a partial travel grant. This research was supported by the Swedish Natural Science Research Council 共NFR兲. 8 E. Zeldov, N. M. Amer, G. Koren, A. Gupta, M. W. McElfresh, and R. J. Gambino, Appl. Phys. Lett. 56, 680 共1990兲. 9 V. M. Vinokur, M. V. Feigel’man, and V. B. Geshkenbein, Phys. Rev. Lett. 67, 915 共1991兲. 10 L. Fàbrega, J. Fontcuberta, S. Piñol, C. J. van der Beek, and P. H. Kes, Phys. Rev. B 47, 15 250 共1993兲; L. Fàbrega, J. Fontcuberta, L. Civale, and S. Piñol, ibid. 50, 1199 共1994兲. 11 B. J. Jönsson, K. V. Rao, S. H. Yun, and U. O. Karlsson, Phys. Rev. B 58, 5862 共1998兲. 12 B. J. Jönsson, Ph.D. thesis, Royal Institute of Technology, Sweden, 1998. 13 V. Ström, Ph.D. thesis, Royal Institute of Technology, Sweden, 1999. 14 E. 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