# Effects of carrier concentration on the superfluid density of high-Tc cuprates

## Abstract

The absolute values and temperature, T, dependence of the in-plane magnetic penetration depth, $`\lambda _{ab}`$, of La<sub>2-x</sub>Sr<sub>x</sub>CuO<sub>4</sub> and HgBa<sub>2</sub>CuO<sub>4+δ</sub> have been measured as a function of carrier concentration. We find that the superfluid density, $`\rho _s`$, changes substantially and systematically with doping. The values of $`\rho _s(0)`$ are closely linked to the available low energy spectral weight as determined by the electronic entropy just above T<sub>c</sub> and the initial slope of $`\rho _s(T)/\rho _s(0)`$ increases rapidly with carrier concentration. The results are discussed in the context of a possible relationship between $`\rho _s`$ and the normal-state (or pseudo) energy gap.

Superconductivity arises from the binding of electrons into Cooper pairs thereby forming a superfluid with a superconducting energy gap, $`\mathrm{\Delta }`$, in the single-particle excitation spectrum. In high-temperature superconductors (HTS) $`\mathrm{\Delta }`$ has essentially $`d_{x^2y^2}`$ symmetry in k-space with $`\mathrm{\Delta }_k=\mathrm{\Delta }_0cos(2\varphi )`$ , where $`\varphi =arctan(k_y/k_x)`$ and $`\mathrm{\Delta }_0`$ is the superconducting gap amplitude which will in general be $`\varphi `$ dependent. Changes in carrier concentration affect the superconducting \[2-8\] and normal state (NS) \[4-7\] properties of HTS and there is evidence \[3-7\] that in addition to $`\mathrm{\Delta }_k`$ there is a normal state (or pseudo) gap, $`\mathrm{\Delta }_N`$, in the NS energy excitation spectrum in under- and optimally doped samples which increases with decreasing doping. The maximum gap amplitude shows little variation with underdoping even though T<sub>c</sub> is reduced \[3-8\], in disagreement with the standard mean-field Bardeen-Cooper-Schrieffer (BCS) theory. This unusual behaviour is probably linked to the presence of $`\mathrm{\Delta }_N`$ . However, fundamental problems such as the origin of $`\mathrm{\Delta }_N`$ and its possible effect on the superfluid density, $`\rho _s`$, have not been clearly resolved experimentally or theoretically.

The physical quantity most directly associated with $`\rho _s`$ is the magnetic penetration depth $`\lambda `$. Appropriate systems to investigate $`\rho _s`$ as a function of doping are La<sub>2-x</sub>Sr<sub>x</sub>CuO<sub>4</sub> and HgBa<sub>2</sub>CuO<sub>4+δ</sub>. Both have a simple crystal structure with one CuO<sub>2</sub> plane per unit cell, can have their carrier concentration controlled, and there is experimental evidence suggesting the presence of $`\mathrm{\Delta }_N`$ which closes with doping \[3-5,9\]. Here we report in-plane penetration depth, $`\lambda _{ab}`$, measurements for high-quality La<sub>2-x</sub>Sr<sub>x</sub>CuO<sub>4</sub> (LSCO) with x = 0.10, 0.15, 0.20, 0.22, 0.24 measured by the ac-susceptibility ($`acs`$) and muon spin relaxation ($`\mu `$SR) techniques and for HgBa<sub>2</sub>CuO<sub>4+δ</sub> (Hg-1201) with $`\delta `$ = 0.10, 0.37 measured only by $`\mu `$SR. We find systematic changes in $`\rho _s`$ with carrier concentration and a correlation with $`\mathrm{\Delta }_N`$.

Single-phase polycrystalline samples of LSCO were prepared in Cambridge using solid-state reaction procedures. No other phases were detected by powder x-ray diffraction and the phase purity is thought to be better than 1%. Lattice parameters were in good agreement with published work . High field magnetic susceptibility measurements showed no signatures of excess paramagnetic centres. The measured T<sub>c</sub>’s are 30, 37.7, 36, 27.5 and 20.3 K for x = 0.10, 0.15, 0.20, 0.22 and 0.24, respectively. These values are also in very good agreement with previous measurements . $`\mu `$SR experiments as a function of T were performed on the same powders for x = 0.10 and 0.15. Although unoriented powders can be used to determine $`\lambda _{ab}`$ by $`\mu `$SR , the $`acs`$ technique requires the powders to be magnetically aligned . To eliminate grain agglomerates, powders were ball-milled in ethanol and dried after adding a defloculant. Scanning electron microscopy confirmed the absence of grain boundaries and showed that the average grain diameter was $`5\mu m`$. The powders were mixed with a 5 min curing epoxy and aligned in a static field of 12T at room temperature. Debye-Scherrer x-ray scans showed that $`90\%`$ of the grains were aligned within $`2.0^o`$. Low-field susceptibility measurements were performed at an $`ac`$-field H<sub>ac</sub> = 1 G rms (parallel to the c-axis) and a frequency f = 333 Hz down to 1.2K. Details of the application of London’s model for deriving $`\lambda `$ from the measured susceptibility can be found in an earlier publication . Transverse-field-cooled $`\mu `$SR experiments were performed at 400 Gauss in the ISIS, Rutherford-Appleton Laboratory. The field produced a flux-line lattice whose field distribution was probed by muons. The depolarisation rate, $`\sigma (T)`$, of the initial muon spin is proportional to $`\lambda _{ab}^{}{}_{}{}^{2}(T)`$ . Checks were made to ensure that the values of $`\lambda _{ab}`$ obtained were independent of the applied field. The Hg-1201 \[$`\delta `$ = 0.10 (T<sub>c</sub> = 60K) and 0.37 (T<sub>c</sub> = 35K)\] samples were prepared in Houston by the controlled solid-vapour reaction technique .

The values of $`\lambda _{ab}(0)`$ derived from the $`acs`$ data for LSCO are 0.28, 0.26, 0.197, 0.193, 0.194 $`\mu `$m for x = p = 0.10, 0.15, 0.20, 0.22 and 0.24, respectively. Here p is the hole content per planar copper atom. The estimated error for $`\lambda _{ab}(0)`$ obtained by the $`acs`$ technique is $`\pm 15\%`$ and within this uncertainty the $`\lambda _{ab}(0)`$ values agree with the $`\mu `$SR measurements. We thus find that $`\lambda _{ab}^2(0)`$ is strongly suppressed on the underdoped side, including optimal doping, but there is no suppression with increasing overdoping (up to p = 0.24) in contrast to reports for Tl<sub>2</sub>Ba<sub>2</sub>CuO<sub>6+δ</sub> . Values of $`\lambda _{ab}(0)`$ as obtained by $`\mu `$SR for Hg-1201 are 0.194 and 0.148 $`\mu `$m for $`\delta `$ = 0.10 and 0.37, respectively. We note that $`\delta `$ = 0.10 and 0.37 in Hg-1201 correspond to p = 0.075 and 0.22, respectively .

The T-dependence of $`\lambda _{ab}`$ for LSCO is shown in Fig. 1(a) as a plot of $`[1/\lambda _{ab}(T)]^2\rho _s(T)`$. Data for x = 0.10 and 0.15 obtained by $`\mu `$SR are also included for comparison. Overall there is good agreement between the results from the two techniques. From the $`acs`$ data we find that the initial linear term in $`\lambda _{ab}(T)`$, characteristic of a clean d-wave superconductor, persists up to the highest doping measured (x = 0.24) in agreement with electronic specific heat studies on polycrystalline LSCO samples from the same batch as those studied here . Figure 1(b) depicts data for Hg-1201 powders measured only by $`\mu `$SR, including data from Ref.  for a Hg-1201 sample (also from Houston) with $`\delta `$ = 0.154 (p = 0.17). As in LSCO, we observe a change in the shape of $`\sigma (T)`$ $`[1/\lambda _{ab}(T)]^2`$ of Hg-1201 with doping. Namely, in the underdoped region $`[1/\lambda _{ab}(T)]^2`$ shows a more pronounced curvature. Taking the slope of the low-T linear term to be proportional to $`\rho _s(0)/\mathrm{\Delta }_0`$ the observed trend of $`[1/\lambda _{ab}(T)]^2`$ with p would imply that $`\mathrm{\Delta }_0`$ remains approximately constant in the underdoped region and decreases rapidly with overdoping.

Figure 2 shows a comparison of the present results for LSCO with specific heat data taken on the same samples  where $`\mathrm{\Delta }_N`$ was observed for x = p $`<`$ 0.19. In the inset we observe a good correlation between $`[1/\lambda _{ab}(0)]^2`$ and \[S/T(T<sub>c</sub>) - S/T(2K)\] both plotted versus Sr content x, where S(T) is the electronic entropy obtained by integrating the electronic specific heat coefficient $`\gamma `$(T) from 0 to T. The quantity \[S/T(T<sub>c</sub>) - S/T(2K)\] is a measure of the energy-dependent NS electronic density of states (DOS), $`g_n`$(E), averaged over $`\pm 2k_BT_c`$ around the Fermi energy E<sub>F</sub>. The effect of an energy -dependent DOS on the London penetration depth $`\lambda _L`$ or $`\rho _s(0)`$ is not usually considered in standard theory which implicitly assumes a constant DOS and a parabolic E($`\stackrel{}{k}`$) dispersion relation. It has been argued elsewhere  that $`\rho _s(0)=4\pi ^2v_{x}^{}{}_{}{}^{2}g_n(E)/e^2`$ where the average is over an (anisotropic) energy shell $`E_F\pm \mathrm{\Delta }_0`$. Note that this result agrees with the standard expression for the NS conductivity and the usual relation between $`\lambda _L(0)`$ and the real part of the frequency-dependent electronic conductivity in the normal and superconducting states $`\sigma _{1}^{}{}_{}{}^{n}(\omega )`$ and $`\sigma _1^s(\omega )`$, respectively. Namely, $`\lambda _L(0)`$ is determined by the area under the \[$`\sigma _{1}^{}{}_{}{}^{n}(\omega )\sigma _{1}^{}{}_{}{}^{s}(\omega )`$\] curve in the frequency range $`0<h\omega /2\pi <2\mathrm{\Delta }_0`$. Thus the inset to Fig. 2 suggests that the strong decrease of $`\rho _s(0)`$ with x from x = 0.20 to 0.10 is related to the suppression of spectral weight with energy range $`E_F\pm \mathrm{\Delta }_0`$ due to the presence of $`\mathrm{\Delta }_N`$.

The main panel in Fig. 2 shows a correlation between the doping dependence of the initial linear terms of $`\lambda _{ab}(T)`$ and the low-T specific heat coefficient $`\gamma `$, both quantities being related to the number of excited quasi-particles n<sub>e</sub>(T). For low values of x, n<sub>e</sub>(T=10) is much smaller than expected from the T<sub>c</sub> value and this probably implies that the average value of $`\mathrm{\Delta }_0(\varphi )`$ is significantly larger than T<sub>c</sub>. The rapid rise above x = 0.20 may arise from the combined effects of the closure of $`\mathrm{\Delta }_N`$ at x = 0.19 , the decreasing T<sub>c</sub> plus the fact that for LSCO there is significant pile up of states near E<sub>F</sub> in the overdoped region $`0.20<x<0.35`$ .

In Fig. 3(a) we present the LSCO $`acs`$ data as $`[\lambda _{ab}(0)/\lambda _{ab}(T)]^2`$ versus T/T<sub>c</sub> and compare the data with the mean-field calculation for a d-wave weak-coupled BCS superconductor with a cylindrical Fermi surface (FS) which gives $`\mathrm{\Delta }_0/T_c2.14`$ . There appears to be a systematic deviation of the data from the weak-coupling T-dependence with a greater (weaker) curvature on the underdoped (overdoped) side. We note however, that particularly in the overdoped samples there is positive curvature near T<sub>c</sub> which may arise from a small amount of doping inhomogeneity giving a distribution of T<sub>c</sub> values in this region where $`dT_c/dp`$ is maximal . The effect of this is to rescale the curves with a slightly lower value of T<sub>c</sub>. We have modelled $`\rho _s(T)`$ using the d-wave T-dependence and a normal distribution of T<sub>c</sub> values with standard deviation of 3%, 5% and 9% for x = 0.20, 0.22 and 0.24, respectively. These corrections, plotted in Fig. 3(b), bring the curves for x = 0.20 and 0.22 into good agreement with weak-coupling BCS with $`\mathrm{\Delta }_0/T_c2.14`$. Similar deductions, as to the magnitude and p-dependence of $`\mathrm{\Delta }_0/T_c`$, were made in the specific heat studies on these overdoped samples . However, the x = 0.24 sample still shows significant deviations that possibly reflect changes in the electronic structure. This would not be surprising given the changes in the FS with the rapid crossover from hole-like to electron-like states near x = 0.27 . We note that the data for x = 0.24 is in excellent agreement with a weak-coupling d-wave calculation for a rectangular FS .

In contrast to the overdoped samples the optimal and underdoped samples \[Fig. 3(a)\], both possessing very small rounding near T<sub>c</sub>, diverge significantly from the weak-coupling curve and in the opposite direction. We note that accounting for inhomogeneities in these samples will, if anything, move the curves even further from the weak-coupling BCS fit.

A central conclusion of the present work is that there is a crossover in both $`\rho _s(0)`$ and $`\rho _s(T)`$ near p = 0.20. Such behaviour is characteristic of many other NS and superconducting properties which have been interpreted in terms of the presence of $`\mathrm{\Delta }_N`$ in the underdoped region. The rate of depression of T<sub>c</sub> due to impurity scattering ($`1/\gamma `$ at T<sub>c</sub>) remains constant across the overdoped region then rises sharply with the opening of $`\mathrm{\Delta }_N`$, beginning in the lightly overdoped region at p $``$ 0.19 . Boebinger and coworkers  using intense pulsed magnetic fields observe a crossover from insulating to metallic behaviour at T = 0 occurring near p = 0.18 and angle-resolved photoemission studies show the development, in the overdoped region, of a full NS Fermi surface . In this region the resistivity coefficient, $`[\rho (T)\rho (0)]/T`$, exhibits a low-T suppression due to the opening of $`\mathrm{\Delta }_N`$ . These considerations provide a compelling motivation for interpreting our penetration depth data within a similar scenario.

The proper means of incorporating the pseudogap effects within a realistic model, and indeed the very nature of the pseudogap is a matter of current debate. However, a key characteristic of $`\mathrm{\Delta }_N`$ is the loss of NS spectral weight near E<sub>F</sub>. The loss of spectral weight can cause, as discussed above, both a strong reduction in $`\rho _s(0)`$ and, in a simple model, enhanced curvature in $`\rho _s(T)/\rho _s(0)`$ above the BCS weak-coupling d-wave T-dependence , the very features we observe for the optimal and underdoped samples.

We note that our data are in reasonable agreement with earlier reports for slightly underdoped grain-aligned HgBa<sub>2</sub>Ca<sub>2</sub>Cu<sub>3</sub>O<sub>8+δ</sub>  and single crystal LSCO with x = 0.15 . In contrast to the strong p dependence we have found in $`[\lambda _{ab}(0)/\lambda _{ab}(T)]^2`$ for LSCO and Hg-1201, studies in YBCO  reported that $`[\lambda _{ab}(0)/\lambda _{ab}(T)]^2`$ scaled approximately with $`1/T_c`$ for various dopings, at all temperatures. However, systematic changes in $`[\lambda _{ab}(0)/\lambda _{ab}(T)]^2`$ with p were noted at the time  although these were too small to allow further analysis. This may simply be due to the fact that the YBCO samples were not as heavily underdoped as the x = 0.10 LSCO sample. We also note that YBCO is complicated by a mixed s+d order parameter  and the effect of the Cu-O chains on the total $`\rho _s`$ .

In summary, using the $`acs`$ and $`\mu `$SR techniques we have obtained consistent and systematic results on the effects of carrier concentration on $`\rho _s`$ of monolayer cuprates. In the overdoped region we find a more or less constant value of $`\rho _s(0)`$ (up to p = 0.24), and $`\rho _s(T)/\rho _s(0)`$ is in reasonably good agreement with the weak-coupling d-wave T-dependence. In the optimal and underdoped regions $`\rho _s(0)`$ is rapidly suppressed and above 0.1T<sub>c</sub> there is a marked departure of $`\rho _s(T)/\rho _s(0)`$ from the weak-coupling curve. In a comparative study with available specific heat data we found evidence supporting a link in the behaviour of $`\rho _s`$ and the normal state gap $`\mathrm{\Delta }_N`$.

We thank P.A. Lee, P.B. Littlewood, T. Xiang and J.F. Annett for stimulating discussions; J. Chrosch for assistance with part of the x-ray analysis of the grain-aligned samples, and P. King and C. Scott (ISIS) for technical support during the $`\mu `$SR measurements. C.P. thanks Trinity College, Cambridge for financial support and J.B. the European Union for a Marie Curie grant.