# Reduction of the Superfluid Density in the Vortex-Liquid Phase of 𝐁𝐢_𝟐⁢𝐒𝐫_𝟐⁢𝐂𝐚𝐂𝐮_𝟐⁢𝐎_𝐲

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## Abstract

In-plane complex surface impedance of a $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ single crystal was measured in the mixed state at 40.8 GHz. The surface reactance, which is proportional to the real part of the effective penetration depth, increased rapidly just above the first-order vortex-lattice melting transition field and the second magnetization peak field. This increase is ascribed to the decrease in the superfluid density rather than the loss of pinning. This result indicates that the vortex melting transition changes the electronic structure as well as the vortex structure.

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The electronic structure of high-$`T_c`$ superconductors (HTSC’s) in the mixed state attracts much attention. In conventional superconductors (CSC’s) with $`s`$-wave gap, quasiparticle (QP) states in the mixed state are localized in the vortex cores where the superconducting gap is suppressed. The QP excitation spectrum inside the vortex core consists of quantized energy levels separated by $`\mathrm{\Delta }E\mathrm{\Delta }_0/k_F\xi `$, where $`\mathrm{\Delta }_0`$ is the bulk gap, $`k_F`$ is the Fermi momentum and $`\xi `$ is the coherence length . Since $`\mathrm{\Delta }E`$ in CSC’s is much smaller than the scattering energies, the vortex core can be regarded as a normal metal. In HTSC’s, above picture can not be applied because of the following reasons. First, the symmetry of the superconducting gap in HTSC’s is not an $`s`$-wave but is most likely a $`d`$-wave . Since the amplitude of the $`d`$-wave gap is zero at the node, QP’s are not localized in the vortex core but extend along the node direction . Calculations based on the Bogoliubov-de Gennes equations suggest that there are no truly localized states in the vortex core of pure $`d`$-wave superconductors . Secondly, even if there are localized QP states inside the vortex core owing to the mixing of the different gap symmetry , $`\mathrm{\Delta }E`$ may exceed any other energy scales, since $`k_F\xi `$ of HTSC’s is very small. Therefore the vortex core in HTSC’s should be different from that of CSC’s in either cases. Finally, in HTSC’s, the greater part of the mixed state is a vortex liquid phase which is practically lost in CSC’s. It may be possible that the difference in the vortex structure brings the difference in the electronic state.

Experimentally, scanning tunneling spectroscopies  and thermal conductivity measurements  have been used to study the QP state of HTSC’s in the mixed states. High frequency surface impedance $`Z_s=R_s+iX_s`$ also provides useful information on the electronic state. Using high enough frequencies, one can be free from the vortex pinning and the information not only on QP’s but also on superfluids can be deduced from $`R_s`$ and $`X_s`$, respectively. So far, a vortex flow resistivity and a QP lifetime inside the vortex core were discussed from the $`R_s`$ measurements in $`\mathrm{YBa}_2\mathrm{Cu}_3\mathrm{O}_\mathrm{y}`$ . Recently, Mallozzi et al. measured the complex resistivity in the mixed state of $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ and argued a possible $`d`$-wave effect . However, measurements of $`Z_s`$ near the vortex-melting transition are still lacking. In this paper, we report both $`R_s`$ and $`X_s`$ measurements on a $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ single crystal and show that the high-frequency response can not be explained in terms of simple vortex flow. Moreover, we succeeded in measuring $`Z_s`$ across the first-order vortex melting transition line and found that the reactive part, $`X_s`$, increases rapidly above the transition while there was little change in $`R_s`$. This result indicates that the superfluid density or the amplitude of the order parameter decreases in the vortex liquid phase.

A $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ single crystal was grown by the floating zone method. The as grown crystal was annealed in air at 800 $`{}_{}{}^{}\mathrm{C}`$ for 3 days and was quenched to room temperature to achieve an optimum oxygen content. A superconducting transition temperature $`T_c`$ defined at zero resistivity was 91 K. Prior to the surface impedance measurements, we measured the magnetic-field dependence of the local magnetization of the same crystal using the micro Hall probe magnetometry and determined the first-order vortex melting transition field from the position of the magnetization jump. Surface impedance was measured by the cavity perturbation technique with a cylindrical Cu cavity operated at 40.8 GHz in the TE<sub>011</sub> mode. The sample was located at the center of the cavity which is the anti-node of the microwave magnetic field $`H_{rf}`$ being parallel to the $`c`$-axis of the sample. The dimensions of the sample were 0.5$`\times `$0.5$`\times `$0.02 mm<sup>3</sup>, which is appreciably larger than the normal-state skin depth ($``$$`\mu `$m at 40.8 GHz). The surface resistance $`R_s`$ and the surface reactance $`X_s`$ can be obtained from the changes in the quality factor of the cavity and the resonance frequency, respectively. We determined absolute values of $`R_s`$ and $`X_s`$ from comparison with the dc resistivity and assuming that $`R_s=X_s`$ (Hagen-Rubens limit) in the normal state. Using this procedure, we obtained the reasonable zero-temperature penetration depth of $``$2$`\times `$10<sup>2</sup> nm. Surface impedance measurements were performed with swept temperature $`T`$ under field cooled conditions to avoid any extrinsic effects associated with pinning e.g. giant magnetostriction . In all the measurements, the static magnetic fields $`H_{dc}`$ were applied along the $`c`$-axis.

First, we briefly introduce the general behavior of the surface impedance of type-II superconductors . The surface impedance $`Z_s`$ is related to the complex effective penetration depth $`\stackrel{~}{\lambda }`$ as $`Z_s=i\mu _0\omega \stackrel{~}{\lambda }`$, where $`\mu _0`$ is the vacuum permeability and $`\omega `$ is the angular frequency. The complex resistivity $`\stackrel{~}{\rho }`$ is also expressed by $`\stackrel{~}{\lambda }`$ as $`\stackrel{~}{\rho }=i\mu _0\omega \stackrel{~}{\lambda }^2`$. In the Meissner state, the response is reactive and $`\stackrel{~}{\lambda }`$ is purely real. Therefore, $`R_s0`$ and $`X_s=\mu _0\omega \lambda _L`$ where $`\lambda _L`$ is the London depth. In the normal state, the response is dissipative and $`\stackrel{~}{\lambda }^2`$ is purely imaginary. Therefore, $`R_s=X_s=\mu _0\omega \delta /2`$ where $`\delta =(2\rho _n/\mu _0\omega )^{1/2}`$ is the skin depth and $`\rho _n`$ is the normal resistivity. In the mixed state, vortex dynamics affects $`\stackrel{~}{\lambda }`$. If the frequency is low, vortices are effectively pinned and a response is similar to that of the Meissner state except that $`\stackrel{~}{\lambda }^2\lambda _L^2+B\mathrm{\Phi }_0/\mu _0\kappa _p`$, where $`B`$ is the magnetic induction, $`\varphi _0`$ is the flux quantum and $`\kappa _p`$ is the Labusch parameter which denotes the pinning strength. On the other hand, if the frequency is high enough, the viscous loss becomes dominant and a response is similar to that of the normal state except that $`\delta `$ is replaced by the vortex flow skin depth $`\delta _f(2B\mathrm{\Phi }_0/\mu _0\omega \eta )^{1/2}`$, where $`\eta `$ is the viscosity of the vortex motion being related to the QP excitation inside the vortex core. Within the vortex flow theory of Bardeen and Stephen , $`\eta `$ is independent of $`B`$ and $`R_sX_sB^{1/2}`$ at high enough fields where $`\delta _f\lambda _L`$ and $`R_sB`$, $`X_s\mu _0\omega \lambda _L`$ at low fields. A crossover from the pinned regime to the dissipative regime occurs at the pinning frequency $`\omega _p=\kappa _p/\eta `$.

The field dependence of $`Z_s`$ of the $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ single crystal is shown in Fig. 1. At high fields above 0.2 T, $`R_s`$ is almost proportional to $`B^{1/2}`$. However, $`X_s`$ is larger than $`R_s`$ up to the highest field we used. This result means that the contribution from the reactive parts, superfluid and/or pinned vortices, can not be neglected. Therefore, the observed $`B^{1/2}`$ dependence of $`Z_s`$ can not be attributed to the high-field region of the Bardeen-Stephen type vortex flow.

At low fields, a prominent anomaly can be seen. Above a certain field, $`X_s`$ increases rapidly and saturates at a higher field while there is little change in $`R_s`$ in the same field region. To examine this anomaly in more detail, we plot the field induced changes in the real part of the effective penetration depth Re$`\mathrm{\Delta }\stackrel{~}{\lambda }(H_{dc})(X_s(H_{dc})X_s(0))/\mu _0\omega `$ in Fig. 2. At low fields and low temperatures, Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ is independent of $`T`$ and linear in $`H_{dc}`$. At high temperatures, Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ begins to deviate from the linear $`H_{dc}`$ dependence and rapidly increases above a certain field $`H_{kink}`$. In Fig. 3, $`H_{kink}`$ is plotted on the magnetic phase diagram together with the vortex melting transition field $`H_m`$ and the second magnetization peak field $`B_{sp}`$. Here, $`H_{kink}`$ is defined at the onset of the rapid increase in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }(T)`$ as shown in the inset of Fig. 3. The agreement between $`H_m`$ and $`H_{kink}`$ is excellent, indicating that the vortex melting affects Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$. In the present crystal, the “critical point” is located at 45 K and 33 mT. Above this field, the sharp feature in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }(T)`$ disappears as shown in the inset of Fig. 3. However, as shown in Fig. 2, the small deviation from the linear $`H_{dc}`$ dependence is still observed in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }(H_{dc})`$ around 40 mT, somewhat higher than $`B_{sp}`$. Considering the difference between the applied field and the magnetic induction inside the sample and the different processes of the field applications in the local magnetization and the microwave measurements, it is reasonable to regard that the increase in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }(H_{dc})`$ below 45 K and the second magnetization peak have the same origin, most likely the field induced vortex decoupling . To sum up, Re$`\mathrm{\Delta }\stackrel{~}{\lambda }(H_{dc})`$ increases when the 3-dimensional vortex lattice model is no longer valid. Note that this anomaly only appears in the reactive response (Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ or $`X_s`$) and almost no anomaly appears in the dissipative response ($`R_s`$).

Now we discuss the origin of the change in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$. Since $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ does not contain magnetic ions, we can recognize that Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ consists of two components: the London penetration depth $`\lambda _L`$ and the vortex motion. First we interpret our results in terms of the change in the vortex motion, which has been widely assumed so far , and will show that this scenario is inappropriate at least near the vortex melting transition of $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$. From the vortex-motion point of view, the increase in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ should be attributed to the loss of pinning at the vortex melting transition. Since contributions from $`\lambda _L`$ and the vortex motion can be separated if the response is written by the complex resistivity . When the effect of vortex creep, which is important only near $`T_c`$, is neglected, the real ($`\rho _1`$) and the imaginary ($`\rho _2`$) parts of the complex resistivity are given by:

$$\frac{\rho _1}{\mu _0\omega \lambda _L^2}=\frac{s}{1+s^2}+\frac{r^2+sr}{(1+s^2)(1+r^2)}b,$$
(2)   
$$\frac{\rho _2}{\mu _0\omega \lambda _L^2}=\frac{1}{1+s^2}+\frac{rsr^2}{(1+s^2)(1+r^2)}b.$$
(3)   
Here, $`s=(2\lambda _L^2/\delta _{nf}^2)`$, $`\delta _{nf}`$ is the normal-fluid skin depth, $`r=\omega /\omega _p`$ and $`b=B\varphi _0/\mu _0\omega \eta \lambda _L^2`$. The parameters $`s`$ and $`r`$ denote the normal-fluid fraction relative to the superfluid density and the weakness of the pinning, respectively. Note that all the parameters related to the vortex motion ($`r`$ and $`b`$) are included only in the second terms of the right hand sides of Eq. Reduction of the Superfluid Density in the Vortex-Liquid Phase of $`\mathrm{𝐁𝐢}_\mathrm{𝟐}\mathrm{𝐒𝐫}_\mathrm{𝟐}\mathrm{𝐂𝐚𝐂𝐮}_\mathrm{𝟐}𝐎_𝐲`$. Therefore, if only the vortex motion is considered, magnetic field dependent parts of the complex resistivity $`\mathrm{\Delta }\rho _1`$, $`\mathrm{\Delta }\rho _2`$ are nothing but these terms. Here, we introduce the ratio of these two terms: $`\mathrm{\Delta }\rho _2/\mathrm{\Delta }\rho _1=(rsr^2)/(r^2+sr)`$. Let us consider the behavior of this ratio at the vortex melting transition. If the vortices melt, the effective pinning strength must be weakened. Accordingly, $`r1/\kappa _p`$ should increase above the transition. Since $`\mathrm{\Delta }\rho _2/\mathrm{\Delta }\rho _1`$ monotonically decreases with increasing $`r`$, $`\mathrm{\Delta }\rho _2`$ should decrease relative to $`\mathrm{\Delta }\rho _1`$ at the transition. This behavior is expected to be irrespective of the nature of pinning, surface or bulk, because any depinning processes cause energy losses which mainly affect $`\rho _1`$. To compare the above arguments with the experimental results, we calculated $`\stackrel{~}{\rho }`$ from $`Z_s`$. As shown in Fig. 4, the experimentally obtained $`\mathrm{\Delta }\rho _2`$ increases relative to $`\mathrm{\Delta }\rho _1`$ at the vortex melting transition and the second magnetization peak field. Therefore, the increase in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ can not be attributed to the loss of pinning. Instead, it should be originated from the increase in $`\lambda _L`$ itself. Since $`1/\lambda _L^2`$ is proportional to the superfluid density, this result strongly suggest that the superfluid density decreases in the vortex liquid phase of $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ due to the additional pair breaking. If all the QP’s are localized in the vortex core as in $`s`$-wave superconductors, the electronic state might be insensitive to the change in the vortex structure. Therefore, we speculate that the reduction of the superfluid density at the vortex melting transition is related to the $`d`$-wave superconductivity.

Next we discuss the behavior of Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ in the vortex solid phase. Since $`R_s0`$ in this regime, we can recognize that vortices are effectively pinned so that $`r1`$, and $`\stackrel{~}{\lambda }(\lambda _L^2+B\mathrm{\Phi }_0/\mu _0\kappa _p)^{1/2}\lambda _L+B\mathrm{\Phi }_0/2\lambda _L\mu _0\kappa _p`$. If $`\lambda _L`$ is independent of $`H_{dc}`$, $`\kappa _p`$ should also be independent of $`H_{dc}`$ and $`T`$, since Re$`\mathrm{\Delta }\stackrel{~}{\lambda }B`$ and independent of $`T`$ as shown in Fig. 2. Field independent $`\kappa _p`$ is only expected when the vortices are individually pinned by strong pinning centers. This is unreasonable because we observed the sharp first-order magnetization jump in our sample. Therefore, $`\lambda _L`$ as well as $`\kappa _p`$ should be $`H_{dc}`$ dependent even in the vortex solid phase. Let us assume that the field dependence of $`\lambda _L`$ is dominant, as has been argued by Mallozzi et al. in the vortex liquid phase . The field dependent $`\lambda _L`$ in the mixed state of $`d`$-wave superconductors is discussed in terms of the magnetic-field effect on the extended QP state by introducing the Doppler energy shift due to the circulating current around the vortices . According to these theories, normal-fluid density, which is proportional to the change in $`\lambda _L`$, varies as $`H_{dc}^{1/2}`$ when $`E_H>\mathrm{\Gamma }`$ and varies as linear in $`H_{dc}`$ when $`E_H<\mathrm{\Gamma }`$, where $`E_H`$ is the averaged QP energy shift given by $`E_H\mathrm{\Delta }_0(H_{dc}/H_{c2})^{1/2}`$ and $`\mathrm{\Gamma }`$ is the QP scattering rate by impurities or the thermal agitation. In terms of this scenario, since the observed Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ in the vortex solid phase is linear in $`H_{dc}`$ and independent of $`T`$, $`E_H<\mathrm{\Gamma }`$ and $`\mathrm{\Gamma }`$ should be dominated by the impurity scattering. However, the zero-field penetration depth of the same sample is found to be linear in $`T`$ at low temperatures. This suggests that the dominant pair breaking mechanism should not be the impurity scattering but the thermal smearing. To resolve the discrepancy between Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ in the vortex solid phase and the zero-field $`\lambda _L`$, knowledge of the field dependence of $`\kappa _p`$ and/or more detailed theoretical treatment must be needed.

Finally, we should briefly consider Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ above $`H_m`$. As shown in Fig. 2, change in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ just above the transition is rather gradual one. Considering that the melting transition is of the first order, there should be a small discontinuity in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ at $`H_m`$, which, we believe, is not observed because of sparse data points. The succeeding gradual change at higher fields may come from the increasing pair breaking and/or the vortex motion. If all the changes in Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$ in the vortex liquid phase arise from the pair breaking , the quantity $`\lambda _L(T=0)^2/(\mathrm{Re}\stackrel{~}{\lambda })^2`$ at low temperatures represents the superfluid fraction $`f_s`$. We calculated this quantity at 10 K and found that $`\lambda _L(T=0)^2/(\mathrm{Re}\stackrel{~}{\lambda })^20.3`$ at $`H_{dc}`$=1 T. Even if $`d`$-wave effect is taken into account, this value is too small since $`f_s`$ is given by $`f_s(H_{dc})1(H_{dc}/H_{c2})^{1/2}`$ and $`H_{c2}`$ is considered to be around 100 T. Therefore, both the increase in $`\lambda _L`$ and the contribution from the vortex motion should be considered in the vortex liquid phase. We stress here again that the behavior of $`\mathrm{\Delta }\rho _2/\mathrm{\Delta }\rho _1`$ at the transition can not be explained in terms of the vortex motion alone, even though the two effects contribute to Re$`\mathrm{\Delta }\stackrel{~}{\lambda }`$. To separate both contributions, detailed frequency dependence measurements are indispensable. This experiment is now underway.

In conclusion, we have measured the complex surface impedance $`Z_s=R_s+iX_s`$ of a $`\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{CaCu}_2\mathrm{O}_\mathrm{y}`$ single crystal in the mixed state. We succeeded in detecting the change in $`Z_s`$ at the first-order vortex melting transition and the second magnetization peak field for the first time. Above the transition, $`X_s`$ which is proportional to the real part of the effective penetration depth increases while there was little change in $`R_s`$. From the analysis of the complex resistivity deduced from $`Z_s`$, we showed that the increase in $`X_s`$ can not be ascribed to the loss of pinning but arises from the reduction of the superfluid density. Namely, the additional pair breaking mechanism may exist in the vortex liquid phase. Our results indicate that not only the phase but also the amplitude of the order parameter take different values in different vortex phases. We speculate that this effect is related to the $`d`$-wave superconductivity.

The authors thank to Y. Matsuda and H. Kitano for helpful discussions. This work was partly supported by the Grant-in-Aid for Scientific Research from the Ministry of Education, Science, Sports and Culture of Japan.