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# Structural and Magnetic Instabilities of La2-xSrxCaCu2O6

## Abstract

A neutron scattering study of nonsuperconducting La2-xSrxCaCu2O6 (x=0 and 0.2), a bilayer copper oxide without CuO chains, has revealed an unexpected tetragonal-to-orthorhombic transition with a doping dependent transition temperature. The predominant structural modification below the transition is an in-plane shift of the apical oxygen. In the doped sample, the orthorhombic superstructure is strongly disordered, and a glassy state involving both magnetic and structural degrees of freedom develops at low temperature. The spin correlations are commensurate.

The interplay between ordering phenomena of charge, spin and lattice degrees of freedom has been a focus of recent research on high temperature superconductors. Most of the work has thus far concentrated on two systems: La2-xSrxCuO4 (LSCO) and YBa2Cu3O6+x (YBCO). In both systems, spin freezing phenomena  as well as magnetic and structural superlattice formation  have been observed. The relationship between these effects, some of which were attributed to charge ordering, and anomalies detected by spectroscopic probes (such as the pseudogap and phonon anomalies) is currently an area of very active investigation. As only two compounds have been studied in detail, it has proven difficult to disentangle aspects that are generic to the cuprates from those that are consequences of some non-generic element of the lattice structure of a specific compound. Such elements include the CuO chains in YBCO, and soft optical phonons associated with tilting of the CuO6 octahedra in LSCO. For instance, charge carriers in the YBCO chains are prone to localization and charge order and may induce related instabilities in the CuO2 planes. Tilt instabilities of the CuO6 octahedra, on the other hand, are known to be an important stabilizing factor for static “stripe” order in LSCO and its derivatives .

In order to further explore the universality of the structural and electronic instabilities in the cuprates, we have carried out a neutron scattering study of La2-xSrxCaCu2O6 (LSCCO), a compound that crystallizes in a bilayer structure akin to YBCO, but without any electronically active element other than the CuO2 layers (inset in Fig. 2) . Further, tilt instabilities of the kind observed in LSCO are not expected in LSCCO because of the fivefold, pyramidal coordination of copper. LSCCO has thus been termed the simplest bilayer cuprate . We report the discovery of an unexpected low temperature tetragonal-to-orthorhombic transition in undoped and doped LSCCO. In the doped sample, the orthorhombic superstructure does not develop long range order, and the magnetic and structural correlations evolve with temperature in a strikingly parallel manner. Despite the large nominal hole concentration (0.1 holes per Cu), the spin correlations are commensurate.

Single crystals of La2-xSrxCaCu2O6 were grown by the travelling-solvent floating zone method under 1 atm oxygen flow. Most of the measurements were taken on an x=0.2 single crystal of volume $`3\times 3\times 3`$ mm3, which is insulating at low temperature, although a metallic behavior of the resistivity is observed at high temperature. (For reasons that are poorly understood at present, superconductivity occurs only in samples treated under high oxygen pressure.) The neutron experiments were carried out on the four-circle diffractometer E5 at the BER II reactor of the Hahn-Meitner-Institut in Berlin, Germany, and on the triple axis spectrometer IN22 at the Institut Laue-Langevin in Grenoble, France. The former instrument was used to acquire a catalogue of Bragg intensities for an accurate refinement of the crystal structure, while the latter instrument allowed us to measure the temperature dependences of selected structural and magnetic reflections with good statistics. On E5, neutron wavelengths of 0.889 Å or 2.36 Å were selected by a copper or a pyrolytic graphite (PG) monochromator, respectively, and the data were collected with a two-dimensional position sensitive 3He-detector. On IN22 the (002) reflection of PG, set for a neutron wavelength of 2.36 Å, was used as both monochromator and analyser, and in order to avoid second order contamination a PG filter was inserted into the incident beam. In order to optimize the intensity, the instrument was used in a focusing mode without collimations.

Two data sets with a total of 623 (259 unique) and 791 (256 unique) reflections were collected on E5 at room temperature and 10 K, respectively. Excellent structure refinements of the room temperature data could be obtained using the tetragonal space group $`I4/mmm`$. The resulting lattice parameters, atomic coordinates and isotropic temperature factors are listed in Table I and are in good agreement with those of previous reports ; further details will be reported elsewhere. At 10 K, however, weak additional (and hitherto unobserved) reflections were found, as shown in Fig. 1. Since their intensity increases with increasing momentum transfer $`Q`$, these reflections must be attributed to a structural modulation. Their temperature dependence (Fig. 2b) shows that the superstructure develops around 100 K, with diffuse scattering persisting to somewhat higher temperatures.

The superstructure reflections can be indexed as $`(h/2,k/2,l)`$ with $`h`$, $`k`$ odd and $`l`$ even but $`0`$, indicating a doubling of the unit cell. From these conditions, the orthorhombic space group $`Bmab`$ (No. 64, standard setting $`Cmca`$) with lattice dimensions $`a\sqrt{2}\times b\sqrt{2}\times c`$ can be deduced. The momentum resolution of our experiment was not sufficient to resolve the small difference between $`a`$ and $`b`$, and for simplicity we continue to use the $`I4/mmm`$ indexing for the remainder of this article. The atomic coordinates resulting from a refinement of the low temperature data are also given in Table I. The primary difference between the $`I4/mmm`$ and $`Bmab`$ structures is a shift of the apical oxygen along the tetragonal (110) direction by $``$ 0.05 Å.

The single-layer sister compound LSCO also undergoes a transition from a high temperature tetragonal ($`I4/mmm`$) to a low temperature orthorhombic ($`Bmab`$) structure , but this transition occurs at a much higher temperature and is commonly believed to be due to steric effects: a mismatch between the natural lattice spacings of the (La/Sr)O and CuO2 layers is thought to be relieved through a staggered tilt of the CuO6 octahedra (which involves motions of both in-plane and apical oxygen atoms). In LSCCO, on the other hand, the coordination of copper is fivefold (inset in Fig. 2) and the displacement pattern (Table I) involves almost exclusively the apical oxygen. The origin of the tetragonal-to-orthorhombic transition in LSCCO thus merits some consideration, and as a resistivity minimum occurs for LSCCO samples in this doping range around the same temperature at which the superstructure reflections first appear , one may wonder whether the transition could be a consequence of charge localization.

In order to explore this possibility, we have carried out a neutron diffraction study of a Sr-free La2CaCu2O6 (LCCO) powder. Although as-prepared LCCO contains a small density of excess oxygen, its resistivity is much larger (and the charge carrier concentration therefore lower) than in LSCCO with x=0.2 . The experiment was carried out on the 3T2 powder diffractometer at the Laboratoire Léon Brillouin in Saclay, France, with a neutron wavelength of 1.2252 Å. While the room temperature data were consistent with previous work , additional weak structural reflections obeying the same extinction rules as for the x=0.2 compound were again observed at lower temperature (Fig. 2a). The displacement of the apical oxygen is significantly larger than for x=0.2, and the structural transition temperature ($`170\pm 20`$ K) is higher.

These data demonstrate the presence of an intrinsic structural instability even without charge carriers, and the enhanced transition temperature in LCCO suggests that the doped carriers suppress the structural phase transition. This is confirmed by considering the widths of the corresponding reflections which are strongly broadened in the x=0.2 sample (Fig. 2c). At low temperature we infer correlation lengths of about ten lattice parameters both in plane and out of plane. Further, the correlation length decreases rapidly as the temperature is increased, which indicates pronounced low energy fluctuations of the corresponding order parameter (that is, the apical oxygen displacement). This result contrasts sharply with the situation in LSCO: While doping-induced local structural defects have been reported , the orthorhombic superstructure remains long range ordered even in highly doped LSCO. The structural data of Fig. 2c are in fact reminiscent of the rapid evolution of the magnetic correlation length with doping and temperature in underdoped LSCO .

With this correspondence in mind, we now turn to the magnetic properties of LSCCO. In addition to the orthorhombic superstructure reflections discussed above, Fig. 1 shows that some intensity develops at low temperature around the antiferromagnetic positions $`𝐐=(1/2,1/2,l)`$ with $`l`$ odd. In contrast to the structural reflections, this intensity is only observed at low $`Q`$ and can hence be identified as magnetic. It also exhibits a sinusoidal intensity modulation as a function of $`l`$ that extinguishes the $`l=0`$ reflection. A similar modulation is observed in antiferromagnetic YBCO and is known to arise from antiferromagnetic interlayer exchange within a bilayer unit . The integrated intensity of a structurally forbidden but magnetically allowed reflection, (1/2, 1/2, 3), is shown in Fig. 3b as a function of temperature. Its onset temperature ($`90`$ K) is identical to the structural transition temperature (Fig. 2b) to within the experimental error . The magnetic correlation length is somewhat shorter than that of the orthorhombic superstructure at low temperatures but shows a similar evolution with temperature.

As noted above, this behavior of the magnetic correlation length is characteristic of underdoped LSCO, where the electronic spins are known to freeze out gradually and a spin glass state develops at low temperatures . Upon lowering the temperature, manifestations of magnetic ordering thus appear progressively in neutron scattering and muon spin rotation ($`\mu `$SR) measurements (which are sensitive to fluctuations on meV and $`\mu `$eV energy scales, respectively). In order to complete the description of the microscopic magnetic properties of LSCCO, we have carried out zero-field $`\mu `$SR measurements on the same LSCCO sample studied by neutrons. The experiment was performed at the GPS spectrometer at the Paul-Scherrer-Institute, Switzerland; typical data are shown in the inset to Fig. 3. A gradual onset of muon spin relaxation by slow electronic spin fluctuations is observed upon cooling below 100 K, consistent with the onset of antiferromagnetic diffuse scattering in the neutron experiment (Fig. 3b). However, a precession signal heralding magnetic order that is static on the energy scale set by the muon Larmor frequency only appears at the much lower temperature of 10 K (Fig. 3a). A magnetic anomaly previously found around 10 K in this doping regime  can hence be identified as a spin glass transition. Although the temperature scale is somewhat larger as compared to LSCO, our neutron scattering and $`\mu `$SR data on LSCCO underscore the universality of the spin freezing phenomena for the cuprates.

In summary, we have reported a detailed neutron scattering study of the LSCCO system. The magnetically disordered state we have uncovered is common to the underdoped cuprates. However, the spin correlations found in LSCCO are commensurate, whereas incommensurate spin correlations are observed in LSCO at comparable Sr concentrations . This may either indicate an effective doping level much lower than suggested by the Sr concentration, or it may be a consequence of bilayer interactions; indeed, commensurate quasielastic spin correlations have also been reported in underdoped YBCO . Another novel feature of the data presented here is the strongly disordered orthorhombic superstructure in the doped sample. While the substitutional disorder on the La/Ca sites (Table I) may play some role, the broadening originating from such factors is expected to be temperature independent. The parallel temperature evolution of the magnetic and structural order parameters and correlation lengths suggests that structural relaxation of doped holes is the predominant factor inhibiting long range order of both magnetic and lattice degrees of freedom. The comparison with LSCO is also interesting in this context: LSCCO undergoes its structural transition at a temperature that roughly coincides with the localization of the doped holes, so that structural disorder created by localized holes can effectively frustrate the development of long range order. Charge localization in LSCO, on the other hand, takes place at a temperature at which the orthorhombic superstructure is already well developed, which may explain why the structural manifestations of charge localization are more subtle in that system .

As these considerations show, the full implications of our data are yet to be clarified. It is already clear, however, that the characterization of magnetic and lattice superstructures for a lattice type different from those of LSCO and YBCO constitutes an important step in an ongoing effort to develop a comprehensive description of the interplay between spin, charge and lattice degrees of freedom in the cuprates.


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# Evidence for hadronic deconfinement in 𝑝̄-𝑝 collisions at 1.8 TeV

## Abstract

We have measured deconfined hadronic volumes, $`4.4<V<13.0`$ fm3, produced by a one dimensional (1D) expansion. These volumes are directly proportional to the charged particle pseudorapidity densities $`6.75<dN_c/d\eta <20.2`$. The hadronization temperature is $`T=179.5\pm 5`$ (syst) MeV. Using Bjorken’s 1D model, the hadronization energy density is $`ϵ_F=1.10\pm 0.26`$ (stat) GeV/fm3 corresponding to an excitation of $`24.8\pm 6.2`$ (stat) quark-gluon degrees of freedom.

Corresponding Author:  Prof. Rolf P. Scharenberg Department of Physics 1396 Purdue University West Lafayette, IN 47907-1396 phone: (765) 494-5393 fax: (765) 494-0706 email: schrnbrg@physics.purdue.edu

The observation of high total multiplicity, high transverse energy, non jet, isotropic events led Van Hove and Bjorken to conclude that high energy density events are produced in high energy $`\overline{p}`$-$`p`$ collisions. These events have a far greater cross section than jet production. In these events the transverse energy is proportional to the number of low transverse momentum particles. This basic correspondence can be explored over a wide range of the charged particle pseudorapidity density $`dN_c/d\eta `$ in $`\overline{p}`$-$`p`$ collisions at center of mass energy $`\sqrt{s}=1.8`$ TeV. The various measurements from the Fermilab quark-gluon plasma search experiment E-735 have already been published. In this letter, we present for the first time a coherent picture based on the relationship between the volume $`V`$, temperature $`T`$, energy density $`ϵ_F`$, and pions per fm3 $`n_\pi `$ emitted from $`V`$. Spectra of identified particles, $`\pi `$, $`K`$, $`\phi `$, $`p`$, $`\overline{p}`$, $`\mathrm{\Lambda }^o`$ $`\overline{\mathrm{\Lambda }^o}`$, $`\mathrm{\Xi }^{}`$, $`\overline{\mathrm{\Xi }^{}}`$ are used to extract the $`V`$, $`ϵ_F`$, and $`n_F`$ values and to determine the strange quark content and relative yields of the hadrons.

Previously the various individual measurements did not provide an overall understanding of these $`\overline{p}`$-$`p`$ collisions. Prompted by the new analysis of the initial collision, we have developed a self-consistent picture of hadronic deconfinement. This letter discusses: (1) The role of parton-parton (gluon) scattering; (2) The volume at decoupling, resulting from the one dimensional longitudinal expansion; (3) The number of pions per fm3 emitted by the source; (4) The hadronization temperature of the source; (5) The hadronization energy density of the source; (6) The number of quark-gluon degrees of freedom in the source; (7) The deconfined volumes and plasma lifetimes, estimates of initial energy densities and temperatures.

Experiment E-735  was located at the C$`\mathrm{}`$ interaction region of the Fermi National Accelerator Laboratory (FNAL). The $`\overline{p}`$-$`p`$ interaction region was surrounded by a cylindrical drift chamber which in turn was covered by a single layer hodoscope including endcaps. This system measured the total charged particle multiplicity $`10<N_c<200`$ in the pseudorapidity range $`|\eta |<3.25`$. A magnetic spectrometer with tracking chambers and time of flight counters, provided particle identified momenta spectra in the range $`0.1<p_t<1.5`$ GeV/c. The spectrometer covered $`0.37<\eta <+1.00`$ with $`\mathrm{\Delta }\phi 20^{}`$ ( $`\phi `$ is the azimuthal angle around the beam direction ).

(1) Recently the E-735 collaboration has analyzed the charged particle multiplicity distributions arising from $`p`$-$`p`$ and $`\overline{p}`$-$`p`$ collisions over a range of center of mass energies 0.06 $`\sqrt{s}1.8`$ TeV. Results at 1.8 TeV support the presence of double $`(\sigma _2)`$ and triple $`(\sigma _3)`$ parton interactions. These processes increase the non-single diffraction cross section (NSD) from $``$ 32 mb at $`\sqrt{s}=0.06`$ TeV to $``$ 48 mb at $`\sqrt{s}=1.8`$ TeV. The variation of the double encounter and triple encounter cross sections $`\sigma _2`$ and $`\sigma _3`$ with center of mass energy $`\sqrt{s}`$ is shown in Fig. 1.

The multiplicity distribution is made up of three contributions corresponding to single, double and triple parton-parton collisions. Our work on multiparton interactions shows that the increase in the $`p`$-$`p`$ inelastic cross section with energy is nearly completely accounted for by the increase in multiparton interactions. Previously this increase in the $`p`$-$`p`$ inelastic cross section was ascribed to copious minijet production . As the energy is increased, a decreasing fraction of the center of mass energy appears in the NSD part of the inelastic cross section. This may be due to the decrease of the Feynman $`x`$ of the partons involved in these collisions. It is thus likely that gluons become more involved with increasing energy leading to rapid thermalization .

(2) To measure the hadronization volume $`V`$, pion HBT (Hanbury Brown, Twiss) correlation measurements were made as a function of both $`\stackrel{}{P}_{\pi \pi }=\stackrel{}{p}_1+\stackrel{}{p}_2`$ the total momentum of the pion pair and of $`dN_c/d\eta `$. The $`\stackrel{}{P}_{\pi \pi }`$ momentum dependent results are shown in Table I . $`R_G`$ is the Gaussian radius parallel to the beam, $`\tau `$ the Gaussian lifetime, and $`\lambda `$ the chaoticity parameter. The lifetime $`\tau `$ can be viewed as a measure of the radius perpendicular to the beam . The increase of $`R_G`$ and $`\tau `$ with decreasing $`P_{\pi \pi }`$ is the characteristic signature for the expansion of the pion source . The dependence of $`R_G`$ and $`\tau `$ on $`dN_c/d\eta `$ is shown in Table II . A clear increase of $`R_G`$ with $`dN_c/d\eta `$ is evident. The dependence of $`R_G`$ and $`\tau `$ on $`P_{\pi \pi }`$ and $`dN_c/d\eta `$ is consistent with a one dimensional (1D) longitudinal expansion of the pion source. The effect of a 1D expansion on the Bose Einstein correlation has been calculated for a massless relativistic ideal gas. This calculation provides correction factors $`\mathrm{}_R`$ and $`\mathrm{}_\tau `$ to our values of $`R_G`$ and $`\tau `$ obtained from the HBT analysis. Both $`\mathrm{}_R`$ and $`\mathrm{}_\tau `$ are a function of $`P_{\pi \pi }`$ and $`\mathrm{\Delta }\eta `$, where $`\mathrm{\Delta }\eta `$ is the spectrometer aperture. The cylindrical volume $`V`$ of the pion source is $`V=\pi (\mathrm{}_\tau \tau )^2\mathrm{\hspace{0.33em}2}\mathrm{}_RR_G`$ where $`R_G`$ varies with $`dN_c/d\eta `$ and $`\mathrm{}_\tau \tau `$ reaches an asymptotic value for the larger $`dN_c/d\eta `$ values. From our data $`R_G=e+h`$ $`dN_c/d\eta `$ where $`e=(0.0788\pm 0.013)`$ fm and $`h=(0.0730\pm 0.011)`$ fm and $`\chi ^2/NDF`$ = 3.09/4.00 as shown in Fig. 2. We neglect $`e`$ since $`hdN_c/d\eta `$ is 6 to 20 times larger than $`e`$. The cylindrical volume becomes,

$`V=\pi \mathrm{}_\tau ^2\tau ^2\mathrm{\hspace{0.33em}2}\mathrm{}_RhdN_c/d\eta `$ (1)
The largest measured value of $`\tau =0.95`$ fm is used to evaluate $`V`$. We estimate the $`\mathrm{}`$ factors using the extrapolation procedure ($`P_{\pi \pi }`$$``$0) outlined in Ref. . ( See in particular Fig.4 and Eq.(7) in Ref ). For our $`P_{\pi \pi }`$ values and a 1D expansion, $`\mathrm{}_\tau =1`$ independent of $`P_{\pi \pi }`$. For the data in Table II $`\mathrm{}_R=1.56`$. Thus V = (0.645 $`\pm `$ 0.130)$`dN_c/d\eta `$ fm3 and the range of V is 4.4$`\pm 0.9<`$ V$`<`$ 13.0$`\pm 2.6`$ fm3 for 6.75 $`<`$ $`dN_c/d\eta <`$ 20.2.

(3) We assume that for $`dN_c/d\eta >6.75`$ the system is above the deconfinement transition. The hot thermalized system expands, cools and then hadronizes. We attribute all of the measured volume to the expansion before hadronization. We neglect the subsequent expansion of the hadronic phase. Following Bjorken’s derivation, we further assume that hydrodynamics of a massless relativistic ideal gas can describe the 1D expansion and that the observed number of pions/fm3 are proportional to the entropy density $`s`$ at hadronization. To estimate the pions/fm3 emitted by the source, the Bjorken 1D boost invariant equation becomes

$`sn_\pi ={\displaystyle \frac{3/2dN_c/d\eta }{A\mathrm{\hspace{0.33em}\hspace{0.33em}2}𝒯}}`$ (2)
where $`A`$ is the transverse area and $`𝒯`$ is the proper time . The collisions occur at longitudinal coordinate $`z=0`$ and time $`t=0`$. Eq. (2) describes an isentropic expansion $`s(𝒯)/s(𝒯_0)=𝒯_0/𝒯`$ and

$`𝒯=(t^2z^2)^{1/2}`$ (3)
where $`𝒯_0`$ is the initial proper time when thermalization has occurred. For a relativistic massless ideal gas above the phase transition the maximum expansion velocity, responsible for most of the longitudinal expansion, is likely to be the sound velocity, $`v_s^2=1/3`$. The expansion time $`t=z/v_s=\mathrm{}_RR_G/v_s`$ and $`𝒯=(3z^2z^2)^{1/2}=\sqrt{2}z`$. We note that $`𝒯_f`$ is the proper time at hadronization.

$`𝒯_f=\sqrt{2}\mathrm{}_RR_G=\sqrt{2}\mathrm{}_RhdN_c/d\eta `$ (4)
and Eqn. (2) becomes

$`n_\pi ={\displaystyle \frac{3/2dN_c/d\eta \mathrm{\hspace{0.33em}\hspace{0.33em}1}/\sqrt{2}}{\pi \tau ^2\mathrm{\hspace{0.33em}\hspace{0.33em}2}\mathrm{}_RhdN_c/d\eta }}={\displaystyle \frac{3/\mathrm{2\hspace{0.33em}\hspace{0.33em}\hspace{0.33em}1}/\sqrt{2}}{\pi \tau ^2\mathrm{\hspace{0.33em}\hspace{0.33em}2}\mathrm{}_Rh}}`$ (5)
where $`1/\sqrt{2}`$ is the effective $`\mathrm{\Delta }\eta `$ slice. Thus $`n_\pi `$ is independent of $`dN_c/d\eta `$ and one obtains

$`n_\pi =1.64\pm 0.33\text{(stat) pions fm}^3`$ (6)
This $`n_\pi `$ value indicates that the deconfinement transition occurs at a definite entropy density. Since $`sn_\pi `$ is constant we can directly evaluate $`n_\pi `$ using the total number of pions emitted divided by the total volume for the data set in Table I. We choose the lowest $`P_{\pi \pi }`$ value where $`\tau =0.95`$ fm, $`R_G`$ = 1.2 fm, and $`\mathrm{}_R=`$ 1.43. Here the average pseudo-rapidity density is $`<dN_c/d\eta >=14.4`$ and Eqns. (2) and (4) become

$`n_\pi ={\displaystyle \frac{3/2dN_c/d\eta \mathrm{\hspace{0.33em}\hspace{0.33em}1}/\sqrt{2}}{\pi \tau ^2\mathrm{\hspace{0.33em}2}\mathrm{}_RR_G}}`$ $`=`$ $`1.57\pm 0.25\text{(stat) pions fm}^3`$ (7)
which has a smaller statistical error than (6).

(4) The negative particle $`p_t`$ spectrum is used to measure the temperature. A slope parameter $`b^1`$ is obtained from a fit of the invariant cross section $`d^2N_c/dyd^2p_t`$ to the function $`A\mathrm{exp}(bp_t)`$ for $`0.15p_t0.45`$ GeV/c . The $`b^1`$ value is constant to $`\pm `$ 1% for $`6.75<dN_c/d\eta <20.2`$. Transverse flow has not been seen in $`p`$-$`p`$ reactions at lower energies . In heavy ion reactions the transverse flow is attributed to final state interactions of the hadrons which presumably are not important in $`\overline{p}`$-$`p`$ collisions. The fact that $`R_G`$ increases by a factor of three and $`b^1`$ remains constant to $`\pm `$ 1%, suggests that the transverse flow is negligible. The components $`\sigma _2,\sigma _3`$ in the NSD cross section indicate that the parton-parton mean free paths are shorter in high energy collisions. Since gluon-gluon interactions dominate in the initial encounters, early thermalization $``$ 0.5 fm/c when $`T`$ 200 MeV is likely. We interpret $`b^1=T=179.5\pm 5`$ MeV (syst) as the hadronization temperature. We neglect the expansion of the hadronic phase following hadronization i.e. decoupling is associated with hadronization. The systematic error estimate is based on possible kaon ($`K_s^0`$) misidentification in the negative particle spectrum at low $`p_t`$. We have not made a correction for the effect of resonance decays on the negative particle $`p_t`$ spectrum. We note that the negative particle temperature is significantly higher than the temperature based on the spectra of idenitified pions which include resonance particle decay pions (T$``$168 MeV). A hadronization inverse slope parameter $`T_m`$ can be estimated from our measurement of the relative yields of mesons and hyperons as shown in Fig. 3, using all the events with $`dN_c/d\eta >6.75`$. The hadron yield versus rest mass inverse slope parameters indicates $`162<T_m<173`$ MeV. Similar $`T_m168`$ MeV values, based on thermal model analyses of hadron yield ratios, have been seen in high energy $`\overline{p}`$ p, p p, $`e^+e^{}`$ and heavy ion reactions . This has been interpreted as evidence for a universal limiting temperature $`T_m`$ for hadrons, the Hagedorn temperature.

(5) We can also use the average measured energies to estimate the hadronization energy density $`ϵ_F`$ . Since $`ϵ_F=3/4Ts_F`$, $`ϵ_F`$ is also constant versus $`dN_c/d\eta `$ ,

$`ϵ_F={\displaystyle \frac{_hF_h\times (m_h)_{}\times 1/\sqrt{2}}{\pi \tau ^2\times 2\times \mathrm{}_R\times h}}`$ (8)
where $`(m_h)_{}=(m_h^2+p_t^2)^{1/2}`$ is the average transverse mass of hadron $`h`$, $`F_h`$ is a hadron abundance factor which also accounts for the neutral hadrons of each species. We have determined $`F_h`$ for $`\pi ,K,\phi ,p,n,\mathrm{\Lambda }^0,\mathrm{\Xi }`$, etc. For $`\tau =0.95`$ fm, $`\mathrm{}_R`$ = 1.56, h=0.073, $`ϵ_F`$ becomes

$`ϵ_F=1.10\pm 0.26\text{(stat) GeV/fm}^3`$ (9)
(6) We can estimate the average number $`n_c`$ of constituents in volume $`V`$ at temperature $`T`$, for a system without boundaries

$`n_c=V{\displaystyle \frac{G(T)\mathrm{\hspace{0.33em}1.202}(kT)^3}{\pi ^2\mathrm{}^3c^3}}`$ (10)
where $`G(T)`$ are the number of degrees of freedom (DOF). For a pion gas $`G(T)=3`$, $`V=`$ 1 fm3, and $`T=179.5`$ MeV. The average number of pions (pion gas) in the source is $`n_\pi =0.28`$ pions/fm3. We observe 1.57 pions/fm3, emitted from the source at temperature $`T=179.5`$ MeV, which requires many more DOF.

For a quark-gluon plasma $`G(T)=G_g(T)+G_q(T)+G_{\overline{q}}(T)=16+21/2(f)`$ where $`f`$ are the number of quark flavors . $`G_g(T)`$ are the gluon DOF; $`G_q(T)`$, $`G_{\overline{q}}(T)`$ are the quark, antiquark DOF. We $`\mathrm{𝑎𝑠𝑠𝑢𝑚𝑒}`$ that pion emission from the source can be determined by the number of constituents in the source at hadronization, that one pion is a quark antiquark $`(q,\overline{q})`$ pair and that two gluons $`(2g)`$ are required to produce two pions (see insert Fig. 2).

$$n_\pi =n_g+(n_q+n_{\overline{q}})/2$$
(11)
Our data indicates that $``$ 6% strange quarks are present at hadronization . Thus we use $`f=2`$ to evaluate Eqn. (10) where $`V=1`$ fm3 and,

$$n_\pi =(1+2\times 21/64)G_g\times 16.1T^3\text{(GeV)}$$
(12)
where $`G_g`$ are the effective number of gluon DOF. For $`n_\pi =1.57`$/fm3 and $`T=0.1795`$ GeV, we obtain $`G_g=10.18`$. The total number of DOF are,

$$G(T)=n_g+n_q+n_{\overline{q}}=(1+21/16)G_g=23.5\pm 6\text{DOF}$$
(13)
nearly eight times the DOF for a pion gas. A second method for estimating the DOF is to use the energy density and temperature at hadronization. For the isentropic expansion, the energy $`E`$ in the volume $`V`$ at temperature $`T`$ is

$$E=V\frac{G(T)\pi ^2k^4}{30\mathrm{}^3c^3}T^4.$$
(14)
For $`ϵ_F=1.10\pm 0.22`$ (stat) GeV/fm3 and $`T=179.5\pm 5`$ MeV, we find $`G(T)=24.8\pm 6.2`$ (stat) quark gluon DOF, in good agreement with the DOF using the number of constituents (Eq. 13).

(7) Two Lorentz contracted nucleons collide at $`t=0`$, $`z=0`$ and the thermalized constituents are assumed to emerge at $`𝒯_0`$. Suppose we choose $`𝒯_0=1.0`$ fm/c. For a given expansion velocity, the data determines the hadronization proper time $`𝒯_f`$ and $`1.09<𝒯_f<3.25`$ fm/c. For $`6.75<dN_c/d\eta <20.2`$, the deconfined volumes $`V`$, determined by the data, range between $`4.4<V<13.0`$ fm3. For $`dN_c/d\eta >6.75`$ and using $`G(T)`$ from Eq. (14)

$$ϵ/T^4=\pi ^2/30G(T)=8.15\pm 2.0(stat)$$
(15)
in general agreement with lattice gauge calculations . The ratio of the initial temperature $`T_i`$ to the final $`T_f`$ is $`T_i/T_f=(𝒯_f/𝒯_0)^{1/3}`$ and $`185<T_i<266`$ MeV. The ratio of the initial energy density $`ϵ_i`$ to the final energy density $`ϵ_f`$ is $`ϵ_i/ϵ_f=(𝒯_f/𝒯_0)^{4/3}`$ and $`ϵ_i`$ is $`1.23<ϵ_i<5.30`$ GeV/fm3 for $`6.75<dN_c/d\eta <20.2`$. Note a different choice of $`𝒯_0`$ would change the $`T_i`$ and $`ϵ_i`$ estimates.

In summary, the HBT analysis and the constant temperature versus $`dN_c/d\eta `$ are consistant with a model in which a pion source undergoes a 1D expansion with total longitudinal dimension 2 $`l_RR_G`$ directly proportional to $`dN_c/d\eta `$. We have used the Bjorken 1D model to analyze our data. We find that there is a unique hadronization entropy density and temperature at which the pions are produced independent of $`dN_c/d\eta `$. We have used phase space estimates of the average number of thermalized constituents in volume $`V`$ at temperature $`T`$ and the measured energy density $`ϵ_F`$ to compute the number of DOF in the source. However, we note that reducing the average expansion velocity from $`v^2=1/3`$ to $`v^2=1/5`$ reduces the DOF estimate by 30%. Then the lower limit for the DOF is 16.6$`\pm `$4.2, still substantially larger than the pion gas DOF of 3. This lower limit allows a more conservative argument that quark-gluon constituents are present in the large deconfined volumes. Our estimate of the number of DOF in the source (23.5$`\pm `$6, 24.8$`\pm `$6.2) is in general agreement with those expected for a quark-gluon plasma. The $`n_\pi `$, $`ϵ_F`$, and $`T`$ values characterize the quark-gluon to hadron thermal phase transition. We expect that these hadronization conditions will be observed in $`p`$-$`p`$ collisions at the CERN Large Hadron Collider where higher pseudorapidity density $`dN_c/d\eta `$ values will produce even larger deconfined volumes and longer plasma lifetimes.

We would like to acknowledge the important support for Fermi National Laboratory experiment E-735 by J. D. Bjorken and L. M. Lederman. This work was supported in part by the United States Department of Energy and the National Science Foundation.


text:
# Materials with Colossal Dielectric Constant: Do They Exist?

## Abstract

Experimental evidence is provided that colossal dielectric constants $`\epsilon ^{}1000`$, sometimes reported to exist in a broad temperature range, can often be explained by Maxwell-Wagner type contributions of depletion layers at the interface between sample and contacts, or at grain boundaries. We demonstrate this on a variety of different materials. We speculate that the largest intrinsic dielectric constant observed so far in non-ferroelectric materials is of order $`10^2`$.

PACS numbers: 77.22.Ch, 77.22.Gm

Materials exhibiting a colossal dielectric constant (CDC), $`\epsilon ^{}>10^3`$, have recently gained considerable attention. CDC behavior is of technical importance for applications using high-$`\epsilon `$ electronic materials, such as random access memories based on capacitive elements. Fundamental interest was initiated by the observation of CDC behavior in some high-$`T_c`$ parent compounds . Indeed, CDC behavior may indicate a colossal polarizability, which was invoked in early polaronic and bipolaronic models as a possible mechanism for high-$`T_c`$ superconductivity . During the last decade, similar observations of CDC behavior have been reported in an increasing number of materials, such as transition metal oxides .

Large dielectric constants are expected for ferroelectrics in a narrow temperature range close to $`T_c`$, or for systems with hopping charge carriers yielding a dielectric constant that diverges towards low frequencies. However, in various recent reports  giant values of the dielectric constant were claimed to persist over broad temperature ranges and, when plotted as a function of frequency, revealing an almost constant low-frequency value and a step-like decrease of the dielectric constant towards higher frequencies. This step-like decrease, which is accompanied by a loss peak in the imaginary part of the permittivity, $`\epsilon ^{\prime \prime }`$, shifts exponentially to higher frequencies with increasing temperature, characteristic of Debye-like dipolar relaxation with a thermally activated relaxation rate. Several intrinsic physical interpretations have been given. Examples include almost incipient ferroelectricity in high-$`T_c`$ materials , highly polarizable relaxation modes , or a relaxor-like slowing down of dipolar fluctuations in nano-size domains .

In the present letter we provide evidence that many of these observations are not intrinsic in origin and we speculate that most, if not all, of the CDCs reported so far are based on Maxwell-Wagner type extrinsic effects . We will promote the notion that the most natural explanation of apparent CDCs are contact effects, and that in ceramic samples grain boundary effects may play a similar role and further ”enhance” the dielectric constant. At these interfaces (metal to insulator contacts, inter-grain boundaries) depletion layers are formed yielding Maxwell-Wagner type relaxations when measured by standard dielectric techniques that use metallic electrodes and two point contact configurations. Thus, while some of the reports may indeed be based on intrinsic effects, extrinsic effects have to be excluded by carefully studying the materials using different sample geometries, different contact configurations, and analyzing the results in terms of electronic networks as considered in detail decades ago . In the present letter, we propose a simple network that is derived from the models outlined by the classical works of Jonscher , Macdonald , and others, and also from our years of experience in dielectric spectroscopy on doped semiconductors. We show examples on a series of different materials, where we observed CDCs, all of which being due to contact effects. Most of the investigated samples are single crystals, but we also provide results on a ceramic sample to evidence effects of grain boundaries on the dielectric response. Finally, in addition to the analysis in terms of electronic networks, we will make some suggestions on experiments that exclude extrinsic effects.

The inset to Fig. 1a shows the equivalent circuit that describes the main features of the dielectric response of almost all doped or dirty semiconductors. The circuit consists of a leaky capacitor connected in series with the bulk sample. As indicated in the equivalent circuit, the intrinsic bulk response is given by the sum of dc conductivity $`(\sigma _{dc})`$, frequency-dependent ac conductivity - for which we use the universal dielectric response (UDR) ansatz $`\sigma _{ac}^{}=\sigma _0\omega ^s`$, $`s<1`$  \- and the high-frequency dielectric constant $`\epsilon _{\mathrm{}}`$ . The UDR is the most common approach to take into account hopping conductivity of localized charge carriers . Under these assumptions, the intrinsic complex conductivity $`\sigma _{\mathrm{intrinsic}}^{}=\sigma _i^{}+i\sigma _i^{\prime \prime }`$ is given by

$$\sigma _i^{^{}}=\sigma _{dc}+\sigma _0\omega ^s,$$
(1)
$$\sigma _i^{^{\prime \prime }}=\mathrm{tan}(\frac{s\pi }{2})\sigma _0\omega ^s+\omega \epsilon _0\epsilon _{\mathrm{}},$$
(2)
where $`\epsilon _0`$ is the permittivity of free space. From the conductivity, the complex dielectric permittivity can be calculated by $`\epsilon ^{}(\omega )=\epsilon ^{}(\omega )i\epsilon ^{\prime \prime }(\omega )=i\sigma ^{}(\omega )/\omega \epsilon _0`$. This formalism does not assume any dipolar relaxation phenomenon in the compound under investigation. The leaky capacitor in the equivalent circuit of Fig. 1a represents the most common way to model contributions from the electrode-sample interface . For semiconducting samples, these arise mainly due to the formation of Schottky barriers in the region close to the metallic electrodes. If the electron work function in a metal is higher than in an electron semiconductor, then in the contact region of the semiconductor the electron concentration is suppressed, and a depletion layer appears. This relatively thin layer of small conductivity, acts as a high capacitance in parallel with a large resistor, connected in series to the bulk sample. But also an accumulation of defects or deviations from stoichiometry (e.g. oxygen deficiency) near the sample surface may lead to such a capacitive surface layer.

The prototypical dielectric response that results from the equivalent circuit of Fig. 1a is shown in Fig. 1. The solid lines represent the full dielectric response, the response of the intrinsic part alone is indicated by the dashed lines. At low frequencies, $`\sigma ^{}(\omega )`$ (Fig. 1c) exhibits a step-like increase, which can be ascribed to a successive bridging of the contact resistance (dominating the low-frequency response) by the contact capacitance acting like a short at high frequencies. The intrinsic contribution, following Eq. (1), is revealed only at high frequencies. Via the relation $`\epsilon ^{\prime \prime }\sigma ^{}/\omega `$, the step in $`\sigma ^{}(\omega )`$ transfers into a peak in $`\epsilon ^{\prime \prime }(\omega )`$ (Fig. 1b), thereby resembling the response of a Debye-like dipolar relaxation process. It is accompanied by a large step-like increase of $`\epsilon ^{}(\omega )`$ towards low frequencies (Fig. 1a). At low frequencies $`\epsilon ^{}(\omega )`$ is dominated by the very high contact capacitance, $`C_c`$, which when divided by the empty capacitance of the sample $`C_0`$, leads to the apparently colossal values of $`\epsilon ^{}=C_c/C_0>10^3`$. Also for $`\epsilon ^{}(\omega )`$, the intrinsic response is detected only at sufficiently high frequencies. The time constant of the circuit is approximately $`\tau RC_c`$, with $`R`$ being the intrinsic sample resistance. Assuming that the contact capacitance is nearly constant, the temperature dependence of the time constant is driven by the exponential increase of the charge carrier density of the semiconducting sample, leading to $`\tau R_0C_c\mathrm{exp}(E/T)`$, with $`E`$ being a characteristic activation energy for charge carriers. Of course the contact step depends on the thickness and the capacitance of the depletion layer, and is strongly sample dependent in addition to its temperature dependence. We will show that in some cases at room temperature the contact step can be shifted well into the GHz frequency region. Before demonstrating this type of response in a series of samples, we would like to state that in some cases the electronic equivalent circuit, shown in the inset to Fig. 1a, is still too simple . We have found that in more metallic samples the influence of inductance has to be taken into account at high frequencies, and sometimes the contacts are better represented using a distribution of time constants (several $`RC`$ values). Furthermore, in ceramic samples other depletion layers can be formed at the interfaces of grain boundaries, yielding an additional step in $`\epsilon ^{}(\omega )`$ and further increase of the low-frequency dielectric constant. This will be demonstrated in one specific sample. However, we provide clear evidence that in most cases the simple equivalent circuit of Fig. 1a works rather well and accounts for the CDCs as well as for the relaxational behavior observed in many semiconducting dielectrics.

Our first example deals with measurements on single crystals of $`\mathrm{CdF}_2`$ doped with indium with contacts made from sputtered gold (for details, see ). The experimental results and fits performed simultaneously for real and imaginary part with the simple equivalent circuit of Fig. 1a are shown in Fig. 2. Here $`\epsilon ^{}(\omega )`$ (Fig. 2a) and $`\epsilon ^{\prime \prime }(\omega )`$ (Fig. 2b) are shown in double-logarithmic representation. $`\epsilon ^{}(\omega )`$ exhibits the characteristic relaxation steps reaching low-frequency values of about 2000, which are accompanied by well pronounced loss peaks in $`\epsilon ^{\prime \prime }(\omega )`$. For the higher temperatures, at frequencies below the loss peaks, $`\epsilon ^{\prime \prime }(\omega )`$ shows a minimum marking the transition to the contact-dominated region. Compared to Fig. 1b, this minimum is rather shallow, but using a distribution of contact barriers a very good agreement of fits and experimental data could be achieved. For the frequency and temperature range of Fig. 2, the UDR contribution can be neglected. In this specific semiconductor we carefully checked the influence of the contacts by measuring samples of different thickness and employing different contact electrodes. As an example, in Fig. 2 a second result obtained on the same sample ($`T=126`$ K), but with the electrodes separated from the bulk by a thin insulating layer of mica , is given. Here no Schottky barriers are formed and the electrode capacitance is simply given by the mica layer. As shown by the dashed lines, the results can be fitted by the same equivalent circuit, leading to nearly identical bulk-, but markedly different contact-parameters. In both cases the intrinsic dielectric constant $`\epsilon _{\mathrm{}}10`$ is far from being colossal or even unusually large. In order to exclude a Debye dipolar relaxation process, we also illuminated the sample by laser light . It is obvious, that the Debye relaxation time $`\tau _D`$ should not depend on the light intensity. In our experiment the ”relaxation frequency” $`\omega _p=1/\tau =1/(RC_c)`$ was proportional to the light intensity due to an increase of the charge carrier density of the semiconducting sample.

Figure 3 shows $`\epsilon ^{}(\omega )`$ for three transition metal oxides, all exhibiting apparently colossal dielectric constants at low frequencies. In Fig. 3a, the dielectric response of $`\mathrm{LaMnO}_3`$ , the parent compound of all colossal magnetoresistance materials is given. Pure $`\mathrm{LaMnO}_3`$ is an antiferromagnetic insulator. The finite carrier density probably results from a slight oxygen excess. The curves in Fig. 3a were taken at temperatures below the antiferromagnetic phase transition. Again we find the step-like decrease of $`\epsilon ^{}`$ on increasing frequencies. The solid lines represent fits using our simple equivalent circuit. Here, the UDR had to be included in the fits, leading to a $`\omega ^{s1}`$ contribution, which smears out the contact-dominated step in $`\epsilon ^{}(\omega )`$ at high frequencies. For the intrinsic dielectric constant we obtain, $`\epsilon _{\mathrm{}}15`$. For doped manganates similar results were obtained, yielding somewhat higher, but certainly not colossal intrinsic dielectric constants . We also want to refer the reader to our earlier work on single-cystalline $`\mathrm{La}_2\mathrm{CuO}_{\text{4+}\delta }`$, a parent compound of high-$`T_c`$ materials, which also reveals high non-intrinsic values of $`\epsilon ^{}`$ .

Figure 3b shows the results for single-crystalline $`\mathrm{SrNbO}_{3.41}`$, which is derived from the high-$`T_c`$ ferroelectric compound $`\mathrm{SrNbO}_{3.5}`$, and has been characterized as one-dimensional metal . In this case the intrinsic dielectric constant is rather high, reaching values of approximately 100. The low-frequency response approaches 20000, simulating strong CDC behavior, which, however, arises only from the contacts.

Finally, in Fig. 3c we provide experimental evidence that in ceramic samples the response may be even more complicated. Fig. 3c shows $`\epsilon ^{}(\omega )`$ for a perovskite-derived cobaltite  revealing clear evidence for two successive steps. The high-frequency step, yielding values of $`\epsilon ^{}`$ close to 6000, is followed by a further increase towards low frequencies, which elevates $`\epsilon ^{}`$ to 8000 at MHz frequencies and $`T=225`$ K. While the low-frequency step is due to contact contributions, the second step can be attributed to grain boundary contributions, which yield a significantly different effective relaxation rate .

In conclusion, using a variety of different compounds we demonstrated the occurrence of apparent ”colossal dielectric constants” at audio and radio frequencies over a broad temperature range. By an in-depth analysis of the frequency- and temperature-dependent dielectric response, all these CDCs were revealed to result from contact or grain boundary effects. In the case of $`\mathrm{CdF}_2:\mathrm{In}`$ we demonstrated how an extrinsic CDC can be excluded by investigating different contact configurations and different sample geometries. We strongly urge that in all further reports of CDC behavior, its intrinsic nature must be verified by a variation of contact type and/or sample geometry. Especially if the CDC exhibits a Debye-like relaxation process, an intrinsic source within the bulk sample is unlikely. In these cases it is advisable to analyze the data in terms of the equivalent circuits introduced decades ago , to obtain information on the true dielectric response of the sample material. This is also important for measurements on the divergence of the zero-temperature dielectric susceptibility in the insulating regime, which is one of the most important probes of a metal-to-insulator transition. To check this behavior experimentally  it seems important to correct the effective dielectric constants for contact contributions even at high temperatures.

Here it is also interesting to discuss the early results on charge-density wave (CDW) systems, which show CDCs at audio- and radiowave frequencies (see, e.g., ). One is tempted to assume that this behavior also results from the existence of depletion layers as outlined in this report. However, a detailed analysis of the dielectric response of $`\mathrm{K}_{0.3}\mathrm{MoO}_3`$, measured with different types of contacts, was performed by Cava et al. , excluding significant contact contributions. Furthermore, the unusually large low-frequency response of CDW systems has been explained theoretically by Littlewood to stem from pinned phason excitations .

In the materials investigated in the present work, the highest intrinsic dielectric constant observed is $`\epsilon ^{}100`$. What are the highest values of dielectric constants one can expect in bulk condensed matter systems? If the origin of the CDCs lies in colossal ionic or relaxational polarizabilities, they only can be reached in narrow temperature ranges close to ferroelectric (or relaxor ferroelectric) transitions, or over broader temperature ranges in incipient ferroelectrics, like in $`\mathrm{SrTiO}_3`$ at low temperatures (see, e.g., ). If the CDCs result from electronic degrees of freedom in semiconductors, within a nearly free-electron model with an average energy gap $`E_g`$, high values of $`\epsilon ^{}`$ imply very low values of $`E_g`$ . In this case the dc conductivity certainly would dominate the dielectric response even at moderately elevated temperatures. Thus, with the exception of CDW systems, we believe that the uppermost limit of an intrinsic dielectric constant that can occur over broad temperature and frequency ranges will be of the order of $`\epsilon ^{}10^2`$.

This work was supported by the BMBF via VDI/EKM 13N6917-A and partly by the Deutsche Forschungsgemeinschaft via the SFB 484 (Augsburg).


text:
# The Average Kinetic Energy of the Superconducting State

## I Introduction

The average kinetic energy in Classical Physics is a useful quantity that helps to obtain important information about several many-body systems, such as the Sun, whose internal temperature can be estimated in this way. In cases when the interaction among particles is only partly known, and the Virial Theorem applies, the total energy can be directly related to the average kinetic energy, and the average kinetic energy to the equipartion theorem, leading to the prediction of thermal properties of the classical system. In this paper we demonstrate, both theoretically and experimentally, that the average kinetic energy of the superconducting state can be directly read from isothermal magnetization curves, for superconductors such that the Ginzburg-Landau parameter $`\kappa `$ is larger than a few units. Thus this average only involves the paired electrons that form the condensate.

It is often the case in Physics that just expressing data in a different way is sufficient to bring a new insight into the problem under investigation. This is exactly the present situation and we claim here that an interesting and new insight is obtained if isothermal magnetization ($`4\pi M`$) data is plotted differently, namely, as the product $`4\pi MB`$, where the magnetic induction is $`B=H+4\pi M`$ and $`H`$ is the equilibrium applied field. In this paper we show that this new curve $`4\pi MB`$ directly determines the average kinetic energy for superconductors with $`\kappa >\kappa _c`$, with an accuracy of less than one percent for $`\kappa _c3`$.

A remarkable property of the product $`4\pi MB`$ is that it may have several local minima along the mixed state. This property follows from the fact that $`4\pi MB`$ vanishes at both critical fields, $`H_{c1}`$ and $`H_{c2}`$. At $`H_{c1}`$, $`M`$ reaches a minimum and $`B`$ vanishes, whereas at $`H_{c2}`$, $`B`$ is maximum and $`M`$ vanishes. Since $`4\pi MB`$ vanishes at two fields, the two extremes of the mixed state, it must necessarily have an absolute minimum in between, and possibly several local minima. The connection between the average kinetic energy and the isothermal magnetization follows from the Virial Theorem for superconductivity which states that,

$`{\displaystyle \frac{𝐇𝐁}{4\pi }}=F_{kin}+2F_{field},`$ (1)
where $`F_{kin}`$ and $`F_{field}=𝐡^2/8\pi `$, are the average kinetic energy and the average magnetic energy, respectively. The local magnetic field inside the superconductor is $`𝐡`$ and $`\mathrm{}`$ represents an average value taken over the volume of the superconductor. This theorem has been discovered rather late for the Ginzburg-Landau (GL) theory and it has been proven very useful since then, because it avoids taking the derivative of the free energy for the determination of $`H`$. The theorem has been extended to the microscopic theory in the context of the quasi-classical Eilenberger theory. There it was found that the above theorem holds for temperatures well below $`T_c`$ and also in presence of non-magnetic impurities. Thus one expects that even in presence of some types of pinning the above relationship still holds.

In this paper we obtain $`4\pi MB`$ curves both theoretically and experimentally for isotropic superconductors. We only discuss here examples such that the symmetry along the direction defined by the applied field turns the theoretical problem into a two-dimensional one. In this case the vector notation is no longer necessary and so, is dropped hereafter. The $`4\pi MB`$ theoretical curve is derived in three situations of the macroscopic GL theory. We obtain analytical expressions for it in the Abrikosov and the London limits. we also calculate this curve numerically, using the iterative scheme proposed by E.H. Brandt, a very accurate method that gives the periodic solution of the GL theory for any field in the mixed state. Using the iterative method we show that for $`\kappa `$ larger than a few units the curve $`4\pi MB`$ indeed gives the average kinetic energy. The absolute minimum of the new curve,

$`{\displaystyle \frac{d(4\pi MB)}{dH}}|_H^{}=0.`$ (2)
determines a critical field called $`H^{}`$. A consequence of the connection established here is that this field determines the maximum average kinetic energy, and from this one obtains the maximum root mean square current density, $`J_{max}\sqrt{J^2}`$. Thus using the present approach one obtains information about the maximum current density without the use of Bean’s model. For this one needs the London expression $`F_{kin}2\pi \lambda ^2J^2/c^2`$, where $`\lambda `$ is the penetration depth. Actually at $`H^{}`$ the order parameter is not constant but we consider as such, to obtain the order of magnititude of this maximum current density circulating in the superconducting state.

In this paper we also show that the ratio $`H^{}/H_{c2}`$ becomes $`\kappa `$ independent for $`\kappa `$ larger than a few units. This property can be useful because it suggests that $`H_{c2}`$ can be determined at a lower field, namely, $`H^{}`$. Frequently the upper critical field of many compounds cannot be reached experimentally just because it falls beyond the capabilities of a given experimental set up.

The $`4\pi MB`$ experimental curves were obtained here using a Niobium sample with an approximately spherical shape, mass $`m=0.6487g`$, and critical temperature $`T_c=8.5`$K with a transition width of $`\mathrm{\Delta }T0.3`$K. The sample was obtained in an arc melt furnace from 99.9 % pureness Nb wire. X-ray diffraction done in this sample shows the expected metallic Nb phase. Isothermal magnetization data was always obtained starting from a zero-field cooled procedure and using a commercial Quantum Design PPMS extraction magnetometer facility.

New features and properties, not visible in the traditional way of plotting magnetization curves, are unveiled here by this $`4\pi MB`$ plot. Some of them are explained in this paper, but there are others, such as the multi-minima structure in the irreversible region, that require further discussion and is not done here. In the reversible region, only one minimum remains and we find good agreement between theory and experiment. Close to $`T_c`$ the experimental and theoretical $`4\pi MB`$ curves show good agreement and the experimental ratio $`H^{}/H_{c2}`$ is well predicted by the present theoretical models. Notice that the Virial Theorem, Eq.(1), holds for the microscopic theory , and for this reason the connection between the curve $`4\pi MB`$ and $`F_{kin}`$, remains valid beyond the GL theoretical framework of this paper.

This paper is organized as follows. In Section II we show that the curve $`4\pi MB`$ gives the average kinetic energy of the superconducting state and derive this curve both analytically and numerically in different theoretical situations. The field $`H^{}`$ is calculated and, its properties, discussed here. In Section III the experimental $`4\pi MB`$ curves for the Nb sample are obtained, and the field $`H^{}`$ determined. The phase diagram of this Nb sample is obtained with the curve $`H^{}(T)`$ included. Finally we draw conclusions in Section IV.

## II Theory

Let us first obtain analytical expressions for the energy function $`4\pi MB`$ in two simple situations and determine there the critical field $`H^{}`$. The lower and upper critical fields are given by $`H_{c1}=(\mathrm{\Phi }_0/4\pi \lambda ^2)\mathrm{ln}\lambda /\xi `$ and $`H_{c2}=\mathrm{\Phi }_0/2\pi \xi ^2`$, respectively, $`\xi `$ is the coherence length and $`\kappa =\lambda /\xi `$ the Ginzburg-Landau parameter. The first case investigated here is Abrikosov’s theory which calculates the vortex lattice near $`H_{c2}`$ in the framework of the GL free energy. There the magnetic induction is given by

$`B=H{\displaystyle \frac{H_{c2}H}{(2\kappa ^21)\beta _A}},`$ (3)
where $`\beta _A=|\mathrm{\Delta }|^4/|\mathrm{\Delta }|^2^2`$ is a parameter determined from the vortex lattice symmetry, $`\mathrm{\Delta }`$ being the wavefunction that describes the superconducting state. One obtains that

$`4\pi MB={\displaystyle \frac{H_{c2}H}{(2\kappa ^21)\beta _A}}\left(H{\displaystyle \frac{H_{c2}H}{(2\kappa ^21)\beta _A}}\right),`$ (4)
is a parabola that vanishes at $`H_{c2}/(1+(2\kappa ^21)\beta _A)`$ and at $`H_{c2}`$. Although Abrikosov’s theory is valid only near $`H_{c2}`$, still, for $`\kappa \sqrt{2}/2`$, the first vanishing field approaches $`2/(1+2\beta _A)\mathrm{\Phi }_0/4\pi \lambda ^2`$, which is of the same order of magnitude as the true $`H_{c1}`$ field. The absolute minimum of $`4\pi MB`$ is achieved at the field

$`H^{}={\displaystyle \frac{H_{c2}}{2}}\left({\displaystyle \frac{2\beta _A\kappa ^2\beta _A+2}{2\beta _A\kappa ^2\beta _A+1}}\right).`$ (5)
A simpler expression is obtained noting that $`\beta _A`$ is very close to one, which is true for the triangular lattice ($`\beta _A=1.1595953\mathrm{}`$): $`H^{}(H_{c2}/2)(1+1/\kappa ^2)`$. Thus for any superconductor with $`\kappa `$ larger than a few units, this critical field is given by $`H0.5H_{c2}`$.

The second model is London theory, known to provide a good description of the superconducting state in the intermediate field region far away from the critical fields. This is a fairly good approximation as long as variations of the order parameter near the vortex cores can be ignored, and so, the order parameter can be considered constant all over the superconductor. In this region the magnetic induction is very well approximated by

$`B=HH_{c1}{\displaystyle \frac{\mathrm{ln}(H_{c2}/B)}{\mathrm{ln}\kappa }}.`$ (6)
Then the energy function becomes

$`4\pi MB=BH_{c1}{\displaystyle \frac{\mathrm{ln}(H_{c2}/B)}{\mathrm{ln}\kappa }}.`$ (7)
whose minimum absolute is at the field value

$`H^{}={\displaystyle \frac{H_{c2}}{e}}{\displaystyle \frac{H_{c1}}{\mathrm{ln}\kappa }}.`$ (8)
Since $`H_{c1}/H_{c2}=\mathrm{ln}\kappa /2\kappa ^2`$, notice, once more, that in case $`\kappa `$ is larger than a few units the last term can be neglected, rendering $`H^{}0.37H_{c2}`$.

The product $`4\pi MB`$ is related to the average kinetic energy of the condensate, without any approximation, through the Virial Theorem (Eq.(1)).

$`4\pi MB=F_{kin}/2\left(hh\right)^2`$ (9)
is expressed here in reduced units, such that the thermodynamical fields and energies are scaled in the following way: $`hh/\sqrt{2}H_c`$, $`HH/\sqrt{2}H_c`$, and $`F_{kin}F_{kin}/(H_c^2/4\pi )`$, $`H_c`$ being the thermodynamic field. The same scaling holds for the magnetic induction which is just the average local field, $`Bh`$. These reduced units are convenient because to retrieve the above quantities at any given temperature $`T`$ from a single temperature independent plot, it is enough to scale energies by $`H_c(T)^2/4\pi `$, and fields by $`\sqrt{2}H_c(T)`$.

To show that the function $`4\pi MB`$ yields the average kinetic energy, $`F_{kin}`$, is just a matter of determining how the mean square deviation of the local field, $`(hh)^2`$, behaves as a function of $`\kappa `$. Thus is done here for the GL theory using the iterative method of E. H. Brandt. This iterative procedure assumes an initial solution, from which one obtains very accurately, after a few iterative steps, the local magnetic field and the order parameter for any applied field in the mixed state. The $`4\pi MB`$ (continuous line) and $`F_{kin}`$ (points) curves, obtained using this method, are shown in Fig. 1 for several $`\kappa `$, ranging from $`0.75`$ to $`50`$. The conclusion is that these two curves, $`4\pi MB`$ and $`F_{kin}/2`$ become very similar for large $`\kappa `$. The field $`H^{}`$ is obtained by determining the absolute minimum of the $`4\pi MB`$ curves in Fig. 1, and Fig. 2 summarizes these results as a $`H^{}/H_{c2}`$ vs $`\kappa `$ plot.

The difference between $`4\pi MB`$ and $`F_{kin}/2`$ is best quantified , as function of $`\kappa `$, by two variance ratios introduced here and both computed at the field $`H^{}`$. We compute $`(hh)^2/|4\pi MB|_H^{}`$ for a few points ($`\kappa `$,$`(hh)^2/|4\pi MB|_H^{}`$): ($`0.75,\mathrm{\hspace{0.33em}0.11}`$), ($`0.85,\mathrm{\hspace{0.33em}0.094}`$), ($`1.0,\mathrm{\hspace{0.33em}0.072}`$), ($`1.5,\mathrm{\hspace{0.33em}0.034}`$), ($`2.0,\mathrm{\hspace{0.33em}0.020}`$), ($`3.0,\mathrm{\hspace{0.33em}0.0088}`$), ($`5.0,\mathrm{\hspace{0.33em}0.0032}`$), ($`10.0,\mathrm{\hspace{0.33em}7.83\hspace{0.33em}10}^4`$), ($`20.0,\mathrm{\hspace{0.33em}1.99\hspace{0.33em}10}^4`$), ($`30.0,\mathrm{\hspace{0.33em}8.8\hspace{0.33em}10}^5`$), and ($`50.0,\mathrm{\hspace{0.33em}3.2\hspace{0.33em}10}^5`$). Notice that for $`\kappa >3`$ the two curves can be regarded as the same with an error of less than one per cent in the neighborhood of $`H^{}`$. This error is not uniform for all fields, being smaller near $`H_{c2}`$ and larger near $`H_{c1}`$. In Fig. 2 one has that $`H^{}/H_{c2}=0.51`$ for $`\kappa =3.0`$, and essentially, for $`\kappa >3`$, $`H^{}`$ is fairly well approximated by its limiting value of $`0.5H_{c2}`$. The inset of Fig. 2 shows the relative root mean square deviation of the local magnetic field, $`\left((hh)^2\right)^{1/2}/h|_H^{}`$, as a function of $`\kappa `$. Again we see a sharp drop of this quantity as $`\kappa `$ increases. For instance for $`\kappa =3.0`$, $`\left((hh)^2\right)^{1/2}/h|_H^{}=0.0213`$.

Analytical expressions for these two variances are obtained in the Abrikosov approximation which starts from the well-known Abrikosov relation between the local field and the order parameter, $`h=H2\pi |\mathrm{\Delta }|^2/\kappa `$, in reduced units. From it one obtains an interesting expression that relates thr variance to the magnetization: $`(hh)^2=(4\pi M)^2(\beta _A1)`$. From it one finds that at the field $`H^{}`$, given by Eq.(5), the following expressions:

$`{\displaystyle \frac{\left((hh)^2\right)^{1/2}}{h}}|_H^{}=\left({\displaystyle \frac{\beta _A1}{\beta _A}}{\displaystyle \frac{1}{4\beta _A\kappa ^44(\beta _A1)\kappa ^2+(\beta _A1)}}\right)^{1/2},`$ (10)
and,

$`{\displaystyle \frac{(hh)^2}{|4\pi MB|}}|_H^{}={\displaystyle \frac{\beta _A1}{2\beta _A\kappa ^2+1\beta _A}}.`$ (11)
Both expressions display a $`1/\kappa ^2`$ behavior for large $`\kappa `$. For the triangular lattice, one obtains that $`\left((hh)^2\right)^{1/2}/h|_H^{}0.172256/\kappa ^2`$, and $`(hh)^2/|4\pi MB|_H^{}0.068815/\kappa ^2`$, which agree quite well with the numerical method results. We conclude that the curve $`4\pi MB`$ can be obtained from the average kinetic energy for $`\kappa >\kappa _c`$, with a precision better than one percent for $`\kappa _c3`$. Next we study a Niobium sample and obtain the curve $`4\pi MB`$ experimentally, starting from the isothermal magnetization curves.

## III Experiment

To exemplify the present ideas we have studied superconductor Niobium, which along the years has been an important reference for the understanding of type II superconducting properties. The observation of the irreversibility line in pure Nb  as observed in high-$`T_c`$ superconductors, has renewed the interest on this superconductor. Also, effects which are easier to study and understand in Nb, such as surface pinning, vortex avalanches , and peak effect, has shed some light on the understanding of similar effects in high-Tc superconductors.

The sample has critical temperature below of pure Nb ($`T_c=9.2`$K), indicating that it contains non-magnetic impurities. This causes no problem here, on the contrary, the impurities turn the compound into a more type II superconductor, with a larger value of $`\kappa `$. Very pure Nb has $`\kappa 1.0`$, whereas we find here $`\kappa 4`$ for this sample, when comparing the present theory to the experiment.

Next we discuss our data as shown in the figures.

The transition properties of this sample are seen in Fig. 3, which shows a rather small reversible temperature region. For fields below $`4.0`$kOe, the magnetization becomes essentially irreversible. Values of $`H_{c2}(T)`$ are extracted from this diagram following the standard linear extrapolation of the magnetization curve.

Fig. 4 shows a total of nine isothermal magnetization cycles, $`0.5`$K apart from each other, for temperatures ranging from $`3.5`$K to $`8`$K. Notice that in the neighborhood of zero applied field all the magnetization curves overlap forming one single temperature independent line. The slope of this line defines the demagnetization factor. For finite size samples the demagnetization factor must be included; for a sphere this factor is $`1/3`$ such that $`B=H_{in}+4\pi M/3`$, where $`H_{in}=H+4\pi M/3`$ is the internal field. Our sample is an ellipsoid with axis $`2r_1=4.7`$mm and $`2r_2=5.3`$mm, whose sphere with equivalent volume has radius $`5.1`$mm. We have experimentally determined the demagnetization of our sample using the following procedure. We assume that $`B=H+2dM`$ where $`d`$ is a factor to be determined from our data such that, in the Meissner phase, the magnetic induction must vanish. We find that, in this region, a linear extrapolation of the magnetization data for all $`4\pi M`$ vs $`H`$ curves produces the same value of $`2d=4.16`$, independent of temperature.

Another important issue here is the removal of the background magnetization as a function of $`H`$ for all temperatures. The construction of the curve $`4\pi MB`$ is only useful, e.g. to determine the critical field $`H^{}`$, if all magnetic contributions that are not of superconducting origin are totally removed from the original isothermal $`M`$ vs $`H`$ data. For the Nb sample the following procedure was applied. The raw magnetization data displays a linear non-zero positive slope as a function of $`H`$ that goes beyond the $`H_{c2}`$ field. This curve is universal and temperature independent. We subtract from the raw magnetization data at all temperatures this single linear curve $`M`$ vs $`H`$. This is possible because the background magnetization is temperature independent, and just a single measurement of the paramagnetic background signal close or above $`T_c`$ is enough to subtract the unwanted background for any temperature. It is well-known that this source of magnetic signal is the Pauli paramagnetism of the normal electrons.

Selected isothermal curves $`2dMB`$ vs $`H`$ are shown for three different temperatures, corresponding to $`T=4.5,\mathrm{\hspace{0.33em}6},\text{and}\mathrm{\hspace{0.33em}8}`$K (Figs. 5, 6, and 7, respectively). The basic features of the $`M`$ vs $`H`$ curves, such as the critical fields and the peak effect, are also present in the $`2dMB`$ vs $`H`$ curves, although in a somewhat different way. However the $`2dMB`$ shows a new feature, not noticed in the traditional $`M`$ vs $`H`$ plot, namely the new minimum at $`H^{}`$. For $`T=4.5`$K the absolute minimum of the curve $`2dMB`$ occurs at $`H=6.0`$kOe, a field associated with the peak effect. Still the $`H^{}`$ is observable there. However for increasing temperature, $`T=6`$K, $`H^{}`$ becomes the absolute minimum and the peak effect turns into a local minimum, in this case around $`4`$kOe. Finally at $`T=8`$K only one minimum remains, $`H^{}`$, and the peak effect is essentially absent. Notice that two $`H^{}`$ fields are defined, measured in ascending (zero field cooled - zfc) and descending (field cooled - fc) fields. The zfc and fc $`H^{}`$ fields are separated by approximately $`500`$Oe for the $`T=4.5`$K curve whereas for $`8`$K they become the same.

In Fig. 8 we compare the $`\kappa =3,\mathrm{\hspace{0.33em}4},\text{and}\mathrm{\hspace{0.33em}5}`$ theoretical and the $`T=8.0`$K experimental curves obtained in this paper. All $`2dMB`$ data sets are normalized along the $`2dMB`$ axis to their maximum absolute values, achieved at $`H^{}`$. Along the $`H`$ axis, the theoretical curves are scaled by the inverse of their upper critical fields, such as in Fig. 1. However for the experimental curve we adopted another normalization procedure, namely we scaled fields by $`796.98H`$ due to the following reason. Our goal is to shift the $`2dMB`$ experimental curve along the $`H`$ axis in search of the best theoretical fit, which we find to occur when experimental and theoretical $`H^{}`$ fields coincide. The experimental absolute maximum of $`|2dMB|`$ is reached at $`H^{}=329.81`$Oe. Next we apply the scale transformation $`\alpha H/329.81`$ and search for $`\alpha `$ that gives the best agreement with the theoretical curves. This happens at $`\alpha =0.46`$, very close to the theoretical expected ratio of $`\alpha =H^{}/H_{c2}0.5`$ of the theoretical curve, described in Fig. 2. Notice that the three theoretical curves coincide near $`H_{c2}`$, as they should, because of the normalization, but not near $`H_{c1}`$. From this figure we conclude that the theoretical $`\kappa =4`$ curve provides the best fitting to the experimental data. It is worth mentioning that this value of $`\kappa `$ agrees with its experimental estimate derived from the ratio of the critical fields. $`H_{c2}/H_{c1}`$.

Fig. 9 presents the phase diagram, obtained from the values of $`H_{c2}`$ that follows from the curves of Fig. 3. Also plotted in this figure are the values of $`H^{}`$ found in the increasing and decreasing field branches of plots, such as shown in Figs. 5, 6, and 7.

We find a quite perfect match between the experimental values of $`H^{}`$ and $`H_{c2}(T)`$ with the expression obtained from the theories previously discussed. Thus for this Nb sample we find that the curve $`H_{c2}/2`$ fits fairly well the experimental $`H^{}`$ curve.

We estimate the maximum root mean square average current, $`J_m`$, for $`T=8`$K. Firstly one must obtain the London penetration depth from the lower critical field for this temperature: $`H_{c1}18`$Oe. We obtain that $`\lambda 0.36\mu `$m and taking that the maximum of $`|2dMB|`$ is reached at $`\mathrm{3.88\hspace{0.33em}10}^3\text{G}^2`$, it follows that $`J_m\mathrm{4.2\hspace{0.33em}10}^5\text{A.cm}^2`$. Notice that this maximum mean square average current density is being obtained in the reversible regime.

In summary we find here that this $`4\pi MB`$ curve naturally enhances many aspects of traditional $`4\pi M`$ vs $`H`$ plots, such as the peak effect, the first entry field ($`H_{c1}`$), which is also much more clearly resolved in this kind of plot. Obviously the theories considered in the previous section do not describe the many features of the experimental curves $`2dMB`$ vs $`H`$, especially when irreversible processes are present. This is expected because those theories do not take into account pinning effects. When pinning effects become small and there is reversibility in the magnetization, we found agreement between theory and experiment. It is always possible to cast isothermal magnetic data as a $`4\pi MB`$ curve, but the question is whether the present connection between the $`4\pi MB`$ curve and $`F_{kin}`$ still holds when irreversible effects are present, such as the peak effect. We believe that this connection indeed remains valid in the irreversible region in some large $`\kappa `$ limit. Obviously this connection should always be regarded approximately and corrections are expected due to pinning. We believe that these corrections should be small, based on the fact that the Virial Theorem gets little, or no modification at all when some types of defects are present. For temperatures close to $`T_c`$, where irreversible effects become small, we found that the present ideas hold and the average kinetic energy interpretation of the curve $`4\pi MB`$ is applicable.

## IV Conclusions

In conclusion the present proposal of casting isothermal magnetization data as the product of the magnetization times the magnetic induction is useful because it directly gives the average kinetic energy of the superconducting state for any applied field. We have studied here this curve both theoretically and experimentally. The field of maximum average kinetic energy in the condensate is just the minimum point of the new curve. From this field we estimate the maximum mean square average current density. We show using the Ginzburg Landau theory that this field value is half the upper critical field value for large $`\kappa `$ superconductors. Thus its experimental determination can help to understand properties of the upper critical field which often falls beyond the experimental capabilities of a given equipment. We found analytical expressions for this curve in two special limits of the Ginzburg-Landau theory, namely the Abrikosov and the London limits. In the general situation we have obtained this curve numerically for several values of the Ginzburg-Landau constant, using an efficient iterative method to solve the Ginzburg-Landau theory. We find that for a Ginzburg-Landau constant larger than a few units the mean square deviation of the local magnetic field becomes extremely small. Only for such parameter values the product magnetization times the magnetic induction gives the average kinetic energy.

In summary we find the present proposal of plotting the isothermal magnetization useful because it provides a new insight into the properties of the mixed state.

###### Acknowledgements.

This work was supported by a collaboration agreement DAAD-CNPq and in part by FAPERJ and CAPES.