PHYSICAL REVIEW B VOLUME 62, NUMBER 22 1 DECEMBER 2000-II Spectral distribution of activation energies in YBa2Cu3O7À ␦ thin films R. Warthmann, J. Albrecht, and H. Kronmüller Max-Planck-Institut für Metallforschung, Heisenbergstrasse 1, D-70569 Stuttgart, Germany Ch. Jooss Institut für Materialphysik, Georg-August-Universität, Windausweg 2, D-37073 Göttingen, Germany 共Received 2 August 2000兲 Local magnetic relaxation experiments are carried out on YBa2Cu3O7⫺ ␦ thin films by magneto-optics. The current density is calculated quantitatively by an inversion scheme of Biot Savart’s law which gives direct information about the time evolution of the current density with a high spatial resolution of about 5 m. We determine the local activation energies U 0 (x,y) by fitting different relaxation laws at different positions 共x, y兲 in the film plane. This analysis yields a spectral distribution of the activation energies that is independent of the applied model. Possible mechanisms which could lead to such a distribution are discussed. In contrast to conventional low-T c superconductors thermal depinning of flux lines leads to a pronounced time decay of the supercurrents in high-temperature superconductors at finite temperatures. This process is described essentially by two parameters: the critical current density j c up to which the pinning force equals the Lorentz force and the activation energy U depending on the pinning potential U 0 and on the macroscopic current density that acts as a driving Lorentz force on the flux lines. Global measurements, mostly done by superconducting quantum interference device 共SQUID兲 magnetometers, often yield some deviations from a pure logarithmic time decay as proposed by Anderson and Kim.1 It is still an open question, whether this is due to a more complex U( j) law2,3 or to a spectral distribution of activation energies as suggested by Hagen and Griessen4 and Theuss and Kronmüller.5 In this paper we report on local magnetic relaxation experiments in YBa2Cu3O7⫺ ␦ 共YBCO兲 thin films by magnetooptics. In particular, quantitative results on the time evolution of the local current density with a high spatial resolution of about 5 m are given. This analysis has become possible by a recently developed inversion scheme of Biot Savart’s law which uses Fourier transformation and convolution theorem and is described in detail in Ref. 6. It allows us to calculate the local current density from the measured field distribution with a high accuracy of better than 5% and without assuming any specific model for the critical state, e.g., Bean’s model.7 Compared to global SQUID measurements8 or to measurements by Hall sensor arrays9 with a spatial resolution of about 50 m in one dimension, much more information about the flux-creep process can be gathered using quantitative magneto-optics. In this paper we give results on the spatially resolved time evolution of the current density and then extend our analysis to calculate the local pinning potentials U 0 (x,y) from the observed time decay of the current-density distribution. Though our data can be fitted by different U( j) laws, we shall prove that a distribution of activation energies exists. The measurements presented in this paper were carried out on a square-shaped YBCO thin film with thickness d⫽300 nm and a side length of 3 mm. The film was evapo0163-1829/2000/62共22兲/15226共4兲/$15.00 PRB 62 rated by a sputtering technique on a 10⫻10 mm2 SrTiO3 substrate and patterned afterwards by chemical etching. As a sensitive layer for the visualization of the flux density distribution by magneto-optics10,11 an iron garnet film12 was used. In Fig. 1 the perpendicular component of the magnetic flux density is plotted as a grayscale image. The external field B ex⫽80 mT is applied after the sample was cooled to T⫽5 K in zero field; this leads to flux penetration into about half of the sample. The flux penetrates in a cushionlike FIG. 1. Grayscale plot of the flux-density distribution in a square-shaped YBCO thin film. The applied external field is B ex ⫽80 mT and T⫽5 K. The grayscale from black to white corresponds to the value of the perpendicular magnetic flux ranging from zero to the maximum. The full lines represent the current stream lines. Also shown is a profile of the current density along the dashed line. The sample is located between the two peaks, the finite values of the current density outside are artifacts of the measurement technique. 15 226 ©2000 The American Physical Society PRB 62 SPECTRAL DISTRIBUTION OF ACTIVATION . . . 15 227 magnetometers, the flux front cannot penetrate further into the sample and thus the current density is reduced in the whole sample during the flux-creep process. Determining the time evolution j(x,y,t) of the current density with a high spatial resolution 共about 10 m after noise filtering兲 we are able to obtain the activation energies U 0 (x,y) with the same spatial resolution. This is achieved by fitting our data to the predicted decrease of the current density for different U( j) models. All models of flux creep assume the motion of flux lines to be thermally activated with an Arrhenius-like relaxation rate 冉 冊 1 1 U共 j 兲 ⫽ exp ⫺ . 0 k BT FIG. 2. Grayscale plot of the changes in the absolute value of the current-density distribution. This image was obtained by subtracting the initial current density distribution at t⫽2 s from the one at t⫽300 s. Dark and bright parts therefore refer to areas where the current density decreased or increased during flux creep, respectively. form, which is typical for square-shaped samples. The discontinuity lines along the diagonals,13 where the current stream lines bend sharply, are clearly visible. The roughly constant critical current density can be clearly distinguished from the shielding currents in the flux-free part of the sample. In the upper right part of the sample the flux and current distributions are altered due to a macroscopic defect. This defect leads to two additional, nearly parabolic discontinuity lines, between which the current stream lines are slightly curved inwards. For a detailed description of the changes in the flux and current-density distribution caused by macroscopic defects, see, e.g., Refs. 6, 13, and 14. To measure the relaxation of the flux and current distribution by magneto-optics, a sequence of images was taken for a constant time step up to a total time t⫽300 s. The first image is acquired about 2 s after the field of B ex⫽80 mT was applied to the zero-field-cooled sample. The temporal changes in the flux density distribution can be obtained by subtracting images measured for different times, as was done before by Forkl.15 Furthermore, our quantitative determination of the supercurrents allows to visualize the changes in the current-density distribution. Figure 2 shows this differential picture as a grayscale image. The area which was filled up with magnetic flux directly after applying the external field is depicted dark gray, corresponding to a reduction of the local current density. However, the areas near the flux front and along the discontinuity lines show an increase of the current density 共the bright parts in Fig. 2兲. This increase is due to the further penetration of the flux lines during the flux-creep process and illustrates a special feature of the partly penetrated state, namely, that the shielding currents turn into critical currents. In the fully penetrated state, which is mostly studied in relaxation measurements using SQUID 共1兲 Here, the characteristic relaxation rate 0 has to be considered as a ‘‘macroscopic’’ time scale rather than the microscopic attempt frequency.16 The models differ in the prediction of the U( j) law and therefore show a different form of the decrease of the current density. The earliest and most simple relaxation model was given by Anderson and Kim,1 who proposed the activation energy U to be a linear function of the current density 冉 冊 U 共 j 兲 ⫽U 0 1⫺ j , jc 共2兲 i.e., U⫽0 at j⫽ j c and U⫽U 0 at j⫽0. Equations 共1兲 and 共2兲 yields a logarithmic time decay of the current density, 冋 j 共 t 兲 ⫽ j c 1⫺ 冉 冊册 k BT t ln U0 t0 . 共3兲 The model of Kim and Anderson assumes the volume of the moving flux line bundle to be constant in time. An improved model should take into account that the bundle size increases with decreasing current density. This was pointed out by Beasley and co-workers.17 Zeldov et al.2 assumed a logarithmic U( j) law U 共 j 兲 ⫽U 0 ln 冉冊 jc , j 共4兲 and obtained 冋 j 共 t 兲 ⫽ j c exp ⫺ 冉 冊册 t k BT ln U0 t0 共5兲 for the time decay of the current density. Feigel’man et al. treated the flux creep in the framework of collective-pinning theory3 and obtained an inverse power law U 共 j 兲 ⫽U 0 冋冉 冊 册 jc j ⫺1 共6兲 in the case of single vortex pinning. The exponent depends on the current density and according to Ref. 3 changes from ⫽1/7 to ⫽3/2 and ⫽7/9 during flux creep. However, there is evidence that pinning in YBCO thin films may be dominated by correlated pinning at planar defects18 and it is therefore questionable whether the collective-pinning theory is applicable in this case. The results given in this paper are for ⫽7/9 which fits our data best. From Eqs. 共1兲 and 共6兲 the time evolution of the current density is described by WARTHMANN, ALBRECHT, KRONMÜLLER, AND JOOSS 15 228 PRB 62 FIG. 3. Fit of the time decay of the current density for different U( j) laws at a randomly chosen point of the sample. The values for the fit parameters given in the plot are for the linear U( j) law. All curves coincide within the linewidth. 冋 j 共 t 兲 ⫽ j c 1⫹ 冉 冊册 t k BT ln U0 t0 ⫺1/ . 共7兲 The local activation energies are obtained by fitting either Eqs. 共3兲, 共5兲, or 共7兲 for each data point 共x,y兲 to the measured time evolution j(x,y,t) of the current density distribution. Besides the activation energy U 0 (x,y), the critical current density j 0 (x,y) and the characteristic time scale t 0 (x,y) were used as fit parameters. The critical current density, i.e., j 0 (x,y,t⫽0), has to be treated as a fit parameter, because of the time delay of t⫽2 s between applying the external field and the acquisition of the first magneto-optical image. Fits of our data by all three models are shown in Fig. 3, where we plot the measured time decay of the current density 共points兲 and the fitted curves for the different U( j) laws at a randomly chosen position 共x,y兲 on the sample. All three models show the same good agreement with the measured data. The fit parameters which are given in Fig. 3 correspond to the linear U( j) law. The logarithmic U( j) 共U 0 ⫽19.86 meV, t 0 ⫽6.30 s, j 0 ⫽2.72⫻1011 A/m2兲 and the inverse power law 共U 0 ⫽23.07 meV, t 0 ⫽4.36 s, j 0 ⫽2.74 ⫻1011 A/m2兲 yield similar values for the fit parameters. The spatial distribution of the activation energy as obtained for the linear model of Kim and Anderson is depicted in Fig. 4 as a grayscale image. Obviously, Eq. 共3兲 is only valid in those parts of the sample where the superconductor is in the critical state when relaxation starts. Therefore, the values of U 0 obtained in the center of the sample 共bright area兲 do not have any physical meaning and will be neglected in the further discussion. The different gray values in the penetrated area show clearly the existence of a distribution of activation energies throughout the sample. The line profile below the grayscale plot shows values in the range of 20–40 meV. An increase of the energy values towards the flux front is visible. The spectral distribution of the activation energies is plotted for the linear 共solid line兲, the logarithmic 共dashed line兲 and the inverse power 共dash-dotted line兲 U( j) law in Fig. 5. The histograms were obtained by dividing the range of the activation energies in N⫽100 equidistant intervals and FIG. 4. Grayscale plot of the local activation energy U 0 (x,y). Dark areas refer to low values and bright areas to high values of the activation energy. counting the number of data points in each channel. All distributions show some broadened peak with a maximum at about 25 meV and a full width at half maximum of roughly 10 meV. Note, that the fit at each point in the sample was done with a single value for the activation energy and the spectral distribution arises from summing up over the whole sample. Therefore, Fig. 5 clearly proves the existence of a spectral distribution of activation energies. We now discuss which mechanisms could lead to a distribution of the activation energies. First, one may consider a field dependence of the activation energy. To investigate FIG. 5. Distribution of activation energies for the linear 共solid line兲, logarithmic 共dashed line兲 and inverse power law 共dash-dotted line兲 U( j) law. The inset shows the magnetic-field dependence of the activation energy obtained for the model of Anderson and Kim. PRB 62 SPECTRAL DISTRIBUTION OF ACTIVATION . . . FIG. 6. Spectral distribution of activation energies at fixed local flux density B z (x,y)⫽60 mT for the different U( j) laws. The solid line represents the linear, the dashed line the logarithmic and the dot-dashed line the inverse power law. this, the activation energy is plotted versus the local magnetic field B z in the inset of Fig. 5. The curve is depicted for the linear model of Kim and Anderson but similiar results are obtained for the other models. A decrease of the activation energy with increasing local flux density is clearly visible. U 0 drops from U 0 ⫽40 meV at B z ⫽15 mT to U 0 ⫽20 meV at B z ⫽80 mT. This suggests that the activation energy depends on the number of vortices, i.e., on the fluxbundle size moving collectively during flux creep. P. W. Anderson and Y. B. Kim, Rev. Mod. Phys. 36, 39 共1964兲. E. Zeldov et al., Phys. Rev. Lett. 62, 3093 共1989兲. 3 M. Feigel’man et al., Phys. Rev. Lett. 63, 2303 共1989兲. 4 C. W. Hagen and R. Griessen, Phys. Rev. Lett. 62, 2857 共1989兲. 5 H. Theuss and H. Kronmüller, Physica C 229, 17 共1994兲. 6 Ch. Jooss et al., Physica C 299, 215 共1998兲. 7 C. P. Bean, Rev. Mod. Phys. 36, 36 共1964兲. 8 Y. Yeshurun, A. P. Malozemoff, and A. Shaulov, Rev. Mod. Phys. 68, 911 共1996兲. 9 Y. Abulafia et al., Phys. Rev. Lett. 75, 2404 共1995兲. 10 A. Forkl, Phys. Scr. 49, 148 共1993兲. 15 229 Finally, we consider the question, whether the distribution of activation energies is additionally caused by variations of the microstructure. For this analysis, one has to subtract the field dependence 共inset of Fig. 5兲 from the distribution of activation energies given in Fig. 5. This is done by determining the spectral distribution with the same method used in Fig. 5 but for a fixed value of the local flux density. Figure 6 gives the distribution of the activation energies for all positions 共x, y兲 where B z (x,y)⫽60 mT. Note, that in the inset of Fig. 5 the values of the activation energy are given by the average values of distributions such as in Fig. 6. The existence of the similar distribution for all different U( j) laws proves, that the distribution of activation energies is due to both a field dependence and variations of the microstructure of the sample. In conclusion, we a presented quantitative method to determine the time evolution of the current density and the activation energies in superconducting samples with high spatial resolution. Our data can be described by different models for flux creep. Independent of the U( j) law we obtained a similar spectral distribution of the activation energies. We discussed two mechanisms which can explain the obtained distributions: 共i兲 variations in the microstructure and 共ii兲 a dependence of U(x,y) on the local field B(x,y). We showed that both mechanisms contribute to the distribution of the activation energies. The authors are grateful to U. Sticher and H.-U. Habermeier for the preparation of the excellent YBCO thin films and to E. H. Brandt for stimulating discussions. T. Schuster et al., Phys. Rev. B 52, 10 375 共1995兲. L. A. Dorosinskii et al., Physica C 203, 149 共1992兲. 13 T. Schuster et al., Phys. Rev. B 49, 3443 共1994兲. 14 A. M. Campell and J. E. Evetts, Critical Currents in Superconductors 共Taylor & Francis, London, 1972兲. 15 A. Forkl et al., Physica C 211, 121 共1993兲. 16 V. B. Geshkenbein et al., Physica C 162–164, 239 共1989兲. 17 M. R. Beasley, R. Labush, and W. W. Webb, Phys. Rev. 181, 682 共1969兲. 18 Ch. Jooss et al., Phys. Rev. Lett. 82, 632 共1999兲. 1 11 2 12