text:
# Effective interactions between parallel-spin electrons in two-dimensional jellium approaching the magnetic phase transition

Abstract

We evaluate the effective interactions in a fluid of electrons moving in a plane, on the approach to the quantum phase transition from the paramagnetic to the fully spin-polarized phase that has been reported from Quantum Monte Carlo runs. We use the approach of Kukkonen and Overhauser to treat exchange and correlations under close constraints imposed by sum rules. We show that, as the paramagnetic fluid approaches the phase transition, the effective interactions at low momenta develop an attractive region between parallel-spin electrons and a corresponding repulsive region for antiparallel-spin electron pairs. A connection with the Hubbard model is made and used to estimate the magnetic energy gap and hence the temperature at which the phase transition may become observable with varying electron density in a semiconductor quantum well.

Keywords: A. Quantum wells; D. Electron-electron interactions; D. Phase transitions.

PACS numbers: 05.30.Fk, 71.10.Ca

Electronic fluids with an essentially two-dimensional (2D) dynamics, as are realized in semiconductor heterostructures, present a very rich phenomenology especially at low density, where the interactions between carriers come to play a crucial role . This fact continues to motivate theoretical studies of the simplified system consisting of a gas of electrons described by the basic Coulomb Hamiltonian with a uniform neutralizing background (EG). More generally, this has been for many decades a basic reference model for calculations of electronic structure in molecular and condensed-matter systems .

Quantum Monte Carlo (QMC) simulation studies have been highlighting the formation of spontaneous spin polarization in the EG at strong coupling. A continuous transition from the paramagnetic to spin-polarized states has been reported to take place in the 3D EG with increasing coupling strength , before a first-order transition into a ferromagnetic Wigner electron crystal occurs. Spontaneous partial spin polarization (”weak ferromagnetism”) has been observed in doped hexaborides . In the 2D EG, on the other hand, the quantum simulation studies indicate a first-order transition to a fully spin-polarized (”ferromagnetic”) fluid before crystallization, no evidence being found for partially spin-polarized states \[6 - 8\].

Theoretical studies of the equation of state described by the ground-state energy $`E(n,\zeta )`$ of the EG with spin densities $`n_{}`$ and $`n_{}`$ as a function of the electron density $`n=n_{}+n_{}`$ and of the spin polarization $`\zeta =(n_{}n_{})/n`$ are clearly called for in both dimensionalities. The ground-state energy is in turn determined by the pair distribution functions, stressing the importance of two-body electron-electron scattering via effective interactions in the many-body system .

Exchange between parallel-spin electrons and correlations from the Coulomb repulsions are crucial in determining the pair distribution functions. These effects are embodied in the so-called local-field factors (LFF) entering the expressions of the charge and spin susceptibilities of the EG . The LFF play the same role as vertex corrections in accounting for the difference between the effective potentials experienced by an electron and their mean-field value. From their knowledge one can also calculate the quasi-particle self-energies and the effective electron- electron interactions, as is well known from work on the unpolarized EG .

In this letter we are concerned with the effective electron-electron interactions in the paramagnetic phase of the 2D EG as functions of the coupling strength on the approach to the magnetic quantum phase transition. We adopt the linear-response approach of Kukkonen and Overhauser  to construct these interactions from recent determinations of the LFF , embodying their asymptotic behaviours from exact sum rules and information from QMC studies. The difference between the $``$ and $``$ effective interactions is related to the magnetic susceptibility and in the low scattering-momentum region most strikingly reflects the approaching phase transition in its behaviour with increasing coupling strength. After pointing out how these results could be used to reveal the magnetic phase transition in a theoretical calculation based on the solution of Schrödinger equations for two-electron problems, we establish an approximate connection with a simple mean-field solution of the Hubbard model for itinerant electrons and use it to estimate the temperature of the magnetic transition in the 2D EG at the density predicted by the QMC studies.

Following, therefore, Kukkonen and Overhauser , the effective interaction potential between two electrons with spin indices $`\sigma _1`$ and $`\sigma _2`$ is written in momentum space as

$$V_{\sigma _1\sigma _2}(q)=V_0(q)J(q)\sigma _1\sigma _2$$
(1)
where by convention the product $`\sigma _1\sigma _2`$ equals +1 for parallel spins and -1 for antiparallel spins. The functions $`V_0(q)`$ and $`J(q)`$ are expressed in terms of the bare Coulomb potential $`v(q)=2\pi e^2/q`$ and of the ideal-gas Lindhard susceptibility $`\chi _0(q)`$ as

$$V_0(q)=v(q)\frac{1+[1G_+(q)]G_+(q)v(q)\chi _0(q)}{1+[1G_+(q)]v(q)\chi _0(q)}$$
(2)
and

$$J(q)=v(q)\frac{G_{}^2(q)v(q)\chi _0(q)}{1G_{}(q)v(q)\chi _0(q)}$$
(3)
Here, $`G_+(q)`$ and $`G_{}(q)`$ are the charge-charge and spin-spin LFF in the paramagnetic 2D EG. It is important to remark for later use that the denominator in Eq. (3) also enters the microscopic magnetic susceptibility $`\chi (q)`$ of the EG, which is given by

$$\chi (q)=\frac{\chi _0(q)}{1G_{}(q)v(q)\chi _0(q)}$$
(4)
in units such that the Bohr magneton equals unity.

The limiting behaviours of the LFF at low and high momenta are determined by a set of exact sum rules . Considering first $`G_+(q)`$, these are the compressibility sum rule yielding

$$\underset{q0}{lim}G_+(q)=\left\{\frac{1}{\pi }\frac{r_s^3}{8\sqrt{2}}\left[\frac{d^2\epsilon _c(r_s)}{dr_s^2}\frac{1}{r_s}\frac{d\epsilon _c(r_s)}{dr_s}\right]\right\}\frac{q}{k_F}$$
(5)
with the Fermi momentum given by $`k_F=\sqrt{2\pi n}`$ in terms of the areal density $`n`$ , and the Kimball-Niklasson-Holas relation yielding

$$\underset{q\mathrm{}}{lim}G_+(q)=[1g(0)]\frac{r_s}{2\sqrt{2}}\frac{d[r_s\epsilon _c(r_s)]}{dr_s}\frac{q}{k_F}.$$
(6)
In these equations $`\epsilon _c(r_s)`$ is the correlation energy per particle as a function of the density parameter $`r_s=(\pi na_B^2)^{1/2}`$ with $`a_B`$ the effective Bohr radius, and $`g(0)`$ is the pair distribution function at contact. The corresponding limiting values of $`G_{}(q)`$ are determined by the magnetic susceptibility sum rule,

$$\underset{q0}{lim}G_{}(q)=\left[\frac{1}{\pi }\frac{r_s}{2\sqrt{2}}\frac{^2\epsilon _c(r_s)}{\zeta ^2}|_{\zeta =0}\right]\frac{q}{k_F}$$
(7)
and by the Santoro-Giuliani-Holas relation,

$$\underset{q\mathrm{}}{lim}G_{}(q)=g(0)\frac{r_s}{2\sqrt{2}}\frac{d[r_s\epsilon _c(r_s)]}{dr_s}\frac{q}{k_F}.$$
(8)
Ample data from QMC studies are available for the correlation energy of the 2D EG as a function of density  and for its long-wavelength magnetic susceptibility determining the coefficient in Eq. (7) \[8, 18 - 20\]. The value of $`g(0)`$ is also known over a wide range of density , from the solution of the two-body scattering problem and from many-body calculations in the ladder approximation.

Complete analytical expressions for both LFF have been obtained in the density range $`r_s10`$, using all the above information and further QMC data from \[18 - 20\] to describe their behaviour in the region of intermediate wave number. We have now extended this work to determine the LFF at $`r_s=20`$, with the results that are shown in Figure 1. Especially relevant for this purpose have been the newly available QMC data on the magnetic susceptibility , which reaches the value $`\chi (0)/\chi _0(0)25`$ at $`r_s=20`$. The corresponding values of the effective interactions between parallel-spin and antiparallel-spin electrons at several values of $`r_s`$ are shown in Figures 2 and 3, respectively. Some smoothing of apparently noisy features has been made in obtaining these results.

As was shown in Ref.  and as again assumed in constructing $`G_{}(q)`$ in Figure 1, the long-wavelength behaviour reported for this LFF in Eq. (7) holds over a rather wide range of scattering momentum $`q`$, extending almost up to $`q=2k_F`$. The plateau shown by the effective interactions in this range of momentum is, therefore, essentially determined by the value of the magnetic susceptibility $`\chi (0)`$. As already noted, this thermodynamic parameter is approaching very large values as the paramagnetic phase of the 2D EG approaches the quantum phase transition to a fully spin-polarized state, that the latest QMC evidence places at $`r_s25`$. The effective interaction between parallel-spin electrons in Figure 2 becomes correspondingly strongly attractive in the momentum range $`q2k_F`$, while a repulsive structure grows at momenta above $`2k_F`$. In parallel to this behaviour, and as is evident from Eq. (1), the effective interaction between antiparallel-spin electrons in Figure 3 becomes strongly repulsive in the momentum range $`q2k_F`$. Although the quantitative details of these results are rather sensitive to the precise value of $`\chi (0)`$, their significance is evidently correct: the approach to the transition into an ordered phase having a space-independent order parameter is driven by the emergence of effective interactions favouring spin alignments over a scale of distances which is becoming long compared with $`(2k_F)^1`$.

In Figure 2 we have also reported the values of $`V_{}(q)`$ as calculated in the fully spin- polarized state at $`r_s=40`$, to show that the effective interactions regain a ”standard shape” after the magnetic phase transition has taken place. That is, the electron-electron interactions in momentum space are repulsive and show a rapid variation as $`q`$ goes through $`2k_F`$, corresponding to Friedel oscillations in coordinate space.

As was shown in the work of Takada  (see also Richardson and Ashcroft ), the effective electron-electron interactions may be used to assess the possibility of superconductive s-wave or p-wave pairing in the EG through the solution of an Eliashberg equation in the absence of phonons. It is natural to ask whether they may play a similarly useful role in regard to a magnetic phase transition. In fact, Ortiz et al. have stressed in their work  that a precise signal of the transition of an electron fluid to a magnetically ordered state is carried by the spin- spin radial distribution function, which is proportional to the difference $`g_{}(r)g_{}(r)`$ between the radial distribution functions for the two spin populations. Near a magnetic transition the function $`g_{}(r)g_{}(r)`$ can be expected to change sign at short range, going from negative in the deep paramagnetic phase (where it reflects a preference for spin alternation) to positive as magnetically ordered domains emerge. Methods to evaluate pair distribution functions in a many-body system through the solution of a Schrödinger equation for a two-body scattering problems have drawn some attention in the recent literature  and could easily be adapted to the study of magnetic phase transitions with the help of the effective potentials that we have determined in this work.

Here we adopt a much simpler and cruder route in order to estimate the magnetic energy gap $`\mathrm{\Delta }`$ which would be required for spin flips at zero momentum transfer in the magnetically ordered phase. This estimate is based on the remark that Eq. (4) for the magnetic susceptibility takes at low momenta the form that is obtained in the Hubbard model for a system of itinerant electrons . The value of the Hubbard parameter $`U`$ appropriate for the 2D EG near the magnetic transition can therefore be estimated as

$$U\underset{k0}{lim}\left[G_{}(k)v(k)\right]=\chi _0^1(0)\chi ^1(0)$$
(9)
Setting $`\mathrm{\Delta }nU`$ for a fully spin-polarized state we estimate

$$\mathrm{\Delta }k_BT_c\frac{2}{r_s^2}\left(1\frac{\chi _0(0)}{\chi (0)}\right)\mathrm{Ryd},$$
(10)
that is, taking $`r_s25`$ and $`\chi (0)/\chi _0(0)25`$ as from Ref. , $`\mathrm{\Delta }3.10^3\mathrm{Ryd}`$ and $`T_c400\mathrm{K}`$ for the EG model. This value is reduced by about three orders of magnitude when one takes account of an effective mass correction and of screening by a background dielectric constant in a semiconducting material. For instance, for the high-mobility GaAs/GaAlAs heterostructures studied by Yoon et al. we estimate $`T_c1\mathrm{K}`$.

In summary, we have evaluated the effective interactions in momentum space between electrons in the paramagnetic phase of the 2D EG at various densities and shown how their shape reflects the emergence of magnetically ordered domains on the approach to the quantum phase transition into a fully spin-polarized phase. We have also given an estimate for the transition temperature at the density predicted by the QMC runs.

This work was partially funded by MIUR under the PRIN2001 Initiative.

References

 See, e.g. E. Abrahams, S. V. Kravchenko, M. P. Sarachik, Rev. Mod. Phys.

73 (2001) 251.

 See, e.g. D. Ceperley, Nature, 397 (1999) 386.

 D. M. Ceperley, B. J. Alder, Phys. Rev. Lett. 45 (1980) 566.

 G. Ortiz, M. Harris, P. Ballone, Phys. Rev. Lett. 82 (1999) 5317.

 D. P. Young, D. Hall, M. E. Torelli, Z. Fisk, J. L. Sarrao, J. D. Thompson, H.-R.

Ott, S. B. Oseroff, R. G. Goodrich, R. Zysler, Nature 397 (1999) 412.

 B. Tanatar, D. M. Ceperley, Phys. Rev. B 39 (1989) 5005.

 D. Varsano, S. Moroni, G. Senatore, Europhys. Lett. 53 (2001) 348.

 C. Attaccalite, S. Moroni, P. Gori-Giorgi, G. B. Bachelet, cond-mat/0109492.

 C. A. Kukkonen, A. W. Overhauser, Phys. Rev. B 20 (1979) 550.

 A. W. Overhauser, Can. J. Phys. 73 (1995) 683.

 See, e.g. K. S. Singwi, M. P. Tosi, Solid State Phys. 36 (1981) 177.

 S. Yarlagadda, G. F. Giuliani, Phys. Rev. B 61 (2000) 12556, and references given

there.

 B. Davoudi, M. Polini, G. F. Giuliani, M. P. Tosi, Phys. Rev. B 64 (2001) 153101.

 B. Davoudi, M. Polini, G. F. Giuliani, M. P. Tosi, Phys. Rev. B 64 (2001) 233110.

 G. E. Santoro, G. F. Giuliani, Phys. Rev. B 37 (1988) 4813.

 M. Polini, M. P. Tosi, Phys. Rev. B 63 (2001) 045118.

 F. Rapisarda, G. Senatore, Austr. J. Phys. 49 (1996) 161.

 S. Moroni, D. M. Ceperley, G. Senatore, Phys. Rev. Lett. 69 (1992) 1837.

 G. Senatore, S. Moroni, D. M. Ceperley, in Quantum Monte Carlo Methods

in Physics and Chemistry, ed. M. P.Nightingale and C. J. Umrigar (Kluwer,

Dordrecht 1999).

 G. Senatore, S. Moroni, D. Varsano, Solid State Commun. 119 (2001) 335.

 M. Polini, G. Sica, B. Davoudi, M. P. Tosi, J. Phys.: Condens. Matter 13, 3591

(2001).

 G. Sica, M. Polini, M. P. Tosi, Mod. Phys. Lett. B 15 (2001) 1053.

 Y. Takada, Phys. Rev. B 47 (1993) 5202.

 C. F. Richardson and N. W. Ashcroft, Phys. Rev. B 54 (1996) R764.

 P. Gori-Giorgi, J. P. Perdew, Phys. Rev. B 64 (2001) 155102.

 T. Izuyama, D. J. Kim, R. Kubo, J. Phys. Soc. Japan 18 (1963) 1025.

 J. Yoon, C. C. Li, D. Shahar, D. C. Tsui, M. Shayegan, Phys. Rev. Lett. 82 (1999)

1744.

Figure caption


format: text

text:
# Strongly disordered spin ladders

## I Introduction

Low dimensional quantum spin systems, chains and ladders are fascinating objects, which are the subject of intensive experimental and theoretical research. The main source of this activity is due to the observation that quantum fluctuations could result in qualitatively different low-energy behavior in these interacting many-body systems. It was first Haldane who conjectured that antiferromagnetic (AF) spin chains with integer spin have a gap in the energy spectrum (Haldane phase), whereas the spectrum of chains with half-integer spins is gapless. By now a large amount of experimental and theoretical evidence have been collected in favor of the Haldane conjecture. It has been realized by Affleck, Kennedy, Lieb and Tasaki (AKLT) that the ground state structure of the Haldane phase for $`S=1`$ is closely related to that of the valence-bond solid model, where the ground state is built up from nearest-neighbor valence bonds. The hidden, topological order in the chain is measured by the non-local string order parameter:

$$O^\alpha =\underset{|ij|\mathrm{}}{lim}S_i^\alpha \mathrm{exp}\left(i\pi \underset{l=i+1}{\overset{j1}{}}S_l^\alpha \right)S_j^\alpha ,$$
(1)
where $`S_i^\alpha `$ is a spin-1 operator at site $`i`$, $`\alpha =x,y,z`$ and $`\mathrm{}`$ denotes the ground state expectation value.

Another source of activity in the field of low-dimensional quantum spin systems is due to the discovery of spin ladder materials. It has been realized that spin ladders with even number of legs have a gapped spectrum, whereas the spectrum of odd-leg ladders is gapless. For two-leg ladders, which are analogous objects to $`S=1`$ spin chains, the ground state structure can be related to nearest-neighbor valence bonds and a topological hidden order parameter, similar to that in Eq.(1) can be defined.

More recently, ladder models with competing interactions, such as with staggered dimerization and with rung and diagonal couplings, have been introduced and studied. In these models, depending on the relative strength of the couplings, there are several gapped phases with different topological order, which are separated by first- or second-order phase transition lines.

Disorder turns out to play a crucial role in some experiments on low dimensional magnets. For instance, the NMP-TCNQ compound can be well described by $`S=1/2`$ spin chains with random AF couplings. More recently, non magnetic substitutions in low dimensional oxydes such as CuGeO3 (being a spin-Peierls compound), PbNi2V2O8 (being a Haldane gap compound) or Y2BaNiO5 (being a Haldane gap compound) have been the subject of intense investigations. The essential feature of these compounds is the appearance of antiferromagnetism at low temperature which can be well described by the effective low energy models introduced in Refs.. Sr(Cu1-xZnx)2 O3 is a realization of the two-leg ladder, and can be doped by Zn, a non magnetic ion. The specific heat and spin susceptibility experiments indicate that the doped system is gapless even with low doping concentrations. We note that the experimentally found phase diagram of this compound, as well as other quantities, such as staggered susceptibility have been obtained by quantum Monte Carlo simulations.

Theoretically, spin chains in the presence of strong disorder can be conveniently studied by a real-space renormalization group (RG) method introduced by Ma, Dasgupta and Hu (MDH). In this method strong bonds in the system are successively eliminated and other bonds are replaced by weaker ones through a second order perturbation calculation. As realized later by Fisher for the random spin-1/2 chain and for the related model of random transverse-field Ising spin chain the probability distribution of the couplings under renormalization becomes broader and broader without limit and therefore the system scales into an infinite randomness fixed point (IRFP), where the MDH renormalization becomes asymptotically exact. Fisher has also succeeded to solve the fixed-point RG equations in analytical form and to show, that for any type of (non-extremely singular) initial disorder the system scales into the same IRFP. Later numerical and analytical work has confirmed Fisher’s results.

Generalization of the MDH approach for AF chains with larger values of the spin is not straightforward, since for not too strong initial disorder the generated new couplings could exceed the value of the already decimated ones. To handle this problem for the $`S=1`$ chain Hyman and Yang and independently Monthus, Golinelli and Jolicaeur have introduced an effective model with spin-1 and spin-1/2 degrees of freedom and with random AF and ferromagnetic (F) couplings. From an analysis of the RG equations they arrived to the conclusion that the IRFP of the model will be attractive if the original distribution parametrized by the power-law form

$$P_{pow}(J)=\frac{1}{D}J^{1+1/D}.$$
(2)
is strongly random, i.e. if $`0<D^1<D_1^1`$. For weaker initial disorder the system is still gapless, which is called the gapless Haldane phase.

Theoretical work about disordered spin ladders is mainly concentrated on the weak disorder limit. Results in this direction are obtained in the weak interchain coupling limit via the bosonization approach and by the random mass Dirac fermion method. In particular a remarkable stability of the phases of the pure system against disorder with $`XY`$ symmetry has been observed.

In the experimental situation, however, as described before the effect of disorder is usually strong and we are going to consider this limiting case in this paper. Our aim is to provide a general theoretical background for strongly disordered spin ladders by studying in detail several models (conventional ladder, dimerized ladder, zig-zag ladder, and the full ladder with rung and diagonal couplings), which could have experimental relevance. Since often a small change in the couplings or in the strength of disorder could cause large differences in the low-energy singular properties of the models, therefore we have studied the phase diagrams in the space of several parameters. As a method of calculation we used a numerical implementation of the MDH approach, which could treat the combined effect of disorder, frustration, correlations and quantum fluctuations, while some problems are also studied by density matrix renormalization (DMRG). In particular we have investigated the stability of the different topologically ordered phases and studied the region of attraction of the IRFP.

The structure of the paper is the following. In Sec. 2 we define different spin ladder models and present their phase diagram for non-random couplings. A short overview about the MDH RG method and its application to random spin chains are given in Sec. 3. Our results about random spin ladders are presented in Sec. 4 and discussed in Sec. 5.

## II The models and their phase diagram for non-random couplings

We start with two spin-1/2 Heisenberg chains, labeled by $`\tau =1,2`$ and described by the Hamiltonians

$$H_\tau =\underset{l=1}{\overset{L}{}}J_{l,\tau }𝐒_{l,\tau }𝐒_{l+1,\tau },$$
(3)
where $`𝐒_{l,\tau }`$ is a spin-1/2 operator at site $`l`$ and on chain $`\tau `$ and $`J_{l,\tau }>0`$. For non-random spin chains dimerization can be introduced as

$$J_{l,\tau }=J\left[1+\gamma (1)^{l+n(\tau )}\right],0\gamma <1,$$
(4)
with $`n(\tau )=0,1`$, whereas for random dimerized couplings the even and odd bonds are taken from different distribution. The pure chain without dimerization ($`\gamma =0`$) has a gapless spectrum, and spin-spin correlations decay as a power for large distance, which is called as quasi-long-range-order (QLRO). Introducing dimerization for $`\gamma >0`$ a gap opens in the spectrum, which is accompanied by non-vanishing dimer order, $`O_{dim}^\alpha 0`$. This is measured as the difference between the string order parameters in Eq(1) calculated with spin-1/2 moments at even (e) and odd (o) sites:

$$O_{dim}^\alpha =O_e^\alpha O_o^\alpha .$$
(5)
In the following we generally consider non-dimerized chains, otherwise it is explicitly mentioned.

Now we introduce the interchain interaction

$$H_R=\underset{l=1}{\overset{L}{}}J_l^R𝐒_{l,1}𝐒_{l,2},$$
(6)
which describes the usual rung coupling between the ladders (see Fig. 1.a). The conventional ladder model is described by the Hamiltonian: $`H=H_1+H_2+H_R`$. In the pure model by switching on the AF rung couplings, $`J_l^R=J^R>0`$, a Haldane-type gap opens above the ground state and the system has a non-vanishing even string topological order, which is measured by:

$$O_{even}^\alpha =\underset{|ij|\mathrm{}}{lim}(S_{i+1,1}^\alpha +S_{i,2}^\alpha )\mathrm{exp}\left(i\pi \underset{l=i+1}{\overset{j1}{}}(S_{l+1,1}^\alpha +S_{l,2}^\alpha )\right)(S_{j+1,1}^\alpha +S_{j,2}^\alpha ).$$
(7)
For strong AF rung couplings every spin-pair on the same rung form a singlet, therefore this phase is called the rung singlet (RUS) phase.

Dimerization of the chain couplings could occur in two different ways. For parallel dimerization, when equal bonds in the two chains are on the same position, i.e. in Eq.(4) $`n(1)=n(2)`$, the combined effect of rung coupling and dimerization will always result in a gapped phase. In the other possible case of staggered dimerization, i.e. with $`n(1)=n(2)`$ (see Fig. 1.b), the two chains have an opposite dimer order, which competes with the rung coupling. As a result the phase diagram of the system (see Fig. 2) consists of two gapped phases, which are separated by a gapless transition line, starting in the pure, decoupled chains limit.

Next, we extend our model by diagonal interchain couplings, given by the Hamiltonian term:

$$H_Z=\underset{l=1}{\overset{L}{}}J_l^Z𝐒_{l,2}𝐒_{l+1,1}.$$
(8)
The complete Hamiltonian, $`H=H_1+H_2+H_R+H_Z`$, describes a zig-zag ladder (see Fig. 1.c) or can be considered as a spin chain with nearest neighbor ($`J_l^R,J_l^Z`$) and next-nearest neighbor ($`J_l`$) couplings (Fig. 1.d). The pure model with $`J_l^R=J_l^Z=J_1`$ and $`J_l=J_2`$ has two phases: a gapless phase for $`J_2/J_1<.24`$ is separated from a gapped phase by a quantum phase transition point.

Finally, we extend our model by two types of diagonal couplings, which are represented by the Hamiltonian:

$$H_D=\underset{l=1}{\overset{L}{}}J_l^D(𝐒_{l,1}𝐒_{l+1,2}+𝐒_{l,2}𝐒_{l+1,1}).$$
(9)
It is known that the pure AF diagonal ladder described by the Hamiltonian, $`H=H_1+H_2+H_D`$ with $`J_l^D=J^D>0`$ has a gapped spectrum. Its ground state is of the AKLT-type and has a non-vanishing odd string order, defined in analogy to Eq.(7)

$$O_{odd}^\alpha =\underset{|ij|\mathrm{}}{lim}(S_{i,1}^\alpha +S_{i,2}^\alpha )\mathrm{exp}\left(i\pi \underset{l=i+1}{\overset{j1}{}}(S_{l,1}^\alpha +S_{l,2}^\alpha )\right)(S_{j,1}^\alpha +S_{j,2}^\alpha ).$$
(10)
In the full ladder there are both rung and diagonal couplings (see Fig. 1.e) and it is described by the Hamiltonian $`H=H_1+H_2+H_R+H_D`$. For non-random AF couplings there is a competition between rung and diagonal couplings, so that the ground state phase diagram of the system consists of two topologically distinct gapped phases (see Fig. 3). The phase transition between the two phases is of first order.

The main subject of our paper is to investigate how the phase diagrams of the pure ladder models, in particular in Figs. 2 and 3 are modified due to the presence of quenched disorder.

## III The MDH renormalization: results for spin chains

In the MDH renormalization group method for random spin-1/2 chains the random AF bonds are arranged in descending order according to their strength, and the strongest bond, say $`J_{23}`$, connecting sites $`2`$ and $`3`$ sets the energy scale in the problem, $`\mathrm{\Omega }=J_{23}`$. We denote by $`1`$ the nearest neighbor site to $`2`$ with a connecting bond $`J_{12}`$ and similarly denote by $`4`$ the nearest neighbor site to $`3`$ with a connecting bond $`J_{43}`$. If $`J_{23}`$ is much larger then the connecting bonds the spin pair $`(2,3)`$ acts as an effective singlet. It follows that the strongly correlated singlet pair can be frozen out. Due to the virtual triplet exciations, an effective coupling $`\stackrel{~}{J}_{14}`$ is generated between the sites $`1`$ and $`4`$. These two sites become nearest neighbors once the singlet has been eliminated. In a second-order perturbation calculation one obtains

$$\stackrel{~}{J}_{14}=\kappa \frac{J_{12}J_{43}}{\mathrm{\Omega }},\kappa (S=1/2)=1/2.$$
(11)
The new coupling is thus smaller than any of the original ones. The energy scale $`\mathrm{\Omega }`$ is continuously reduced upon iterating the procedure and at the same time the probability distribution of the couplings $`P(J,\mathrm{\Omega })`$ approaches a limiting function. In a gapless random system $`\mathrm{\Omega }`$ tends to zero at the fixed point of the transformation and the low energy tail of the distribution is typically given by:

$$P(J,\mathrm{\Omega })\mathrm{d}J\frac{1}{z}\left(\frac{J}{\mathrm{\Omega }}\right)^{1+1/z}\frac{\mathrm{d}J}{\mathrm{\Omega }}.$$
(12)
The dynamical exponent $`z`$ determines how the length scale $`L`$ scales with the time scale $`\tau `$:

$$\tau \mathrm{\Omega }^1L^z.$$
(13)
In general $`z`$ is not a universal quantity: its value depends on the form of the original disorder. However $`z`$ stays invariant under renormalization. Therefore one can deduce its value from the renormalized distribution in Eq.(12). Varying the parameters of the initial distribution one can reach a situation where the width of the distribution in Eq.(12) grows without limits, i.e. $`z`$ formally tends to infinity. In this case, according to exact results on the random AF spin-1/2 chain, one should formally replace $`z`$ in Eq.(12) by $`\mathrm{ln}\mathrm{\Omega }`$, so that the scaling relation in Eq.(13) takes the form:

$$\mathrm{ln}t_rL^\psi ,\psi =1/2.$$
(14)
This type of fixed point, where the ratio of any two neighboring bonds typically tends to zero or infinity, is called an infinite randomness fixed point (IRFP). It has been conjectured that the MDH renormalization group transformation (11) leads to exact results regarding the singular properties of the transformation, namely the value of $`\psi `$ in Eq. (14) is exact .

For the random AF spin-1/2 chain, according to exact results any amount of disorder is sufficient to drive the system into the IRFP. Similarly, the gapped dimer phase will turn into a gapless random dimer phase for any amount of disorder, where the dimerization parameter is defined as

$$\delta _{dim}=\left[\mathrm{ln}J_{odd}\right]_{\mathrm{av}}\left[\mathrm{ln}J_{even}\right]_{\mathrm{av}}$$
(15)
in terms of the couplings $`J_{odd}`$ and $`J_{even}`$ at odd and even sites, respectively. The random dimer phase is a quantum version of the Griffiths-phase, which has been originally introduced for classical disordered systems. The schematic RG-flow diagram of the random dimerized chain is drawn in Fig. 4.

The MDH method has also been used to study the singular properties of the random AF spin-1 chain. Here we first note that the spectrum of the pure system has a Haldane gap, which is stable against weak randomness. Consequently the MDH renormalization, which is by definition a strong disorder approach, becomes valid if the initial disorder is increased over a limit, say $`D_0`$. Our second remark concerns the “projecting onto the lowest level” procedure when after decimating out a strongly coupled singlet the generated new coupling is in the form of Eq.(11), however with a constant of $`\kappa (S=1)=4/3`$. Consequently at the initial RG steps the energy scale could behave non-monotonically, so that an IRFP behavior is expected only for strong enough initial disorder. To cure this problem a modified RG scheme was proposed, which is based on the principle of “projecting out the highest level”. By this method an effective Hamiltonian with spin-1 and spin-1/2 degrees of freedom has been introduced, where between the spins both AF and F couplings could be present but their distribution should respect some constraints. The RG analysis of this effective model leads to two different types of strongly disordered phases, provided the disorder of the original distribution exceeds the limiting value of $`D_0`$. For an intermediate range of disorder, so that $`D_0<D<D_1`$ the system scales into a quantum Griffiths-phase, the so-called gapless Haldane phase, where $`z=z(D)`$ is a monotonously increasing function of disorder and $`1/z(D)>0`$. When the strength of disorder exceeds a second limit, say $`D>D_1>D_0`$, the dynamical exponent becomes infinite and the singular behavior of the system is controlled by the IRFP (see Fig 5).

Till now there are no numerical estimates about the limiting disorder strengths, $`D_0`$ and $`D_1`$. For the uniform distribution, which corresponds to $`D=1`$ in Eq.(2), the system is in the gapless Haldane phase with $`z1.5`$.

Finally, we mention the work by Westerberg et al. about renormalization of spin-1/2 Heisenberg chains with mixed F and AF couplings. In this problem, due to the presence of strong F bonds under renormalization spin clusters with arbitrary large effective moment $`S^{eff}`$ are generated, such that $`S^{eff}\mathrm{\Delta }^\omega `$, where $`\mathrm{\Delta }`$ is the largest local gap in the system and $`\mathrm{\Delta }0`$ at the fixed point. Singularities of different physical quantities are related to the scaling exponent $`\omega `$.

## IV Renormalization of AF spin ladders

With a ladder geometry, spins are more interconnected than in a chain, which leads to a modification of the decimation procedure described in the previous section. As shown in Fig. 6 both spins of a strongly coupled pair, say $`(2,3)`$, are generally connected to the nearest neighbor spins, denoted by $`1`$ and $`4`$. After decimating out the singlet pair the new, effective coupling between $`1`$ and $`4`$ is of the form:

$$\stackrel{~}{J}_{14}^{eff}=\kappa \frac{(J_{12}J_{13})(J_{43}J_{42})}{\mathrm{\Omega }},\kappa (S=1/2)=1/2,$$
(16)
which should replace Eq.(11) obtained in the chain topology, i.e. with $`J_{13}=J_{42}=0`$. With the rule in Eq.(16) F couplings are also generated. As a consequence, the renormalized Hamiltonian contains both AF and F bonds. When at some step of the renormalization an F bond becomes the strongest one, it will lead to the formation of an effective spin-1 cluster. In further RG steps the system renormalizes into a set of effective spin clusters having different moments and connected by both AF and F bonds. The detailed renormalization rules have already been given in Ref..

Due to the ladder topology and the complicated renormalization rules the RG equations can not be treated analytically and one resorts to numerical implementations of the renormalization procedure. We note that a variant of the MDH renormalization has been successfully applied numerically for the two-dimensional random transverse-field Ising model (RTIM) (also for double chains of the RTIM). An IRFP has been obtained both for the 2D RFIM and the double chain RFIM.

In practice we use a finite size version of the MDH renormalization, as for the RTIM in Ref. In this method we start with a finite ladder of $`L`$ sites and with periodic boundary conditions and perform the decimation procedure until one spin pair with a first gap $`\mathrm{\Delta }`$ remains in the system. Since $`\mathrm{\Delta }`$ plays the role of the energy scale at length scale $`L`$, $`\mathrm{\Delta }`$ and $`L`$ should be related by the relation (13) involving the dynamical exponent $`z`$. Performing the above decimation for different samples the probability distribution of $`\mathrm{\Delta }`$ in the small $`\mathrm{\Delta }`$ limit is described by the form in Eq.(12), where the energy scale $`\mathrm{\Omega }`$ is replaced by $`L^z`$.

The IRFP is signalled by a diverging $`z`$, or more precisely the $`P_L(\mathrm{\Delta })\mathrm{d}\mathrm{\Delta }`$ distributions have strong $`L`$ dependence, so that the appropriate scaling combination is

$$\mathrm{ln}\left(L^\psi P_L(\mathrm{\Delta })\right)f\left(L^\psi \mathrm{ln}\mathrm{\Delta }\right),$$
(17)
which can be obtained from Eq.(12) by formally setting $`z\mathrm{ln}\mathrm{\Delta }L^\psi `$.

In the actual calculations we have considered several 100.000 realizations of random ladders of length up to $`L=512`$. Then, from the distribution of the gap at the last step of the RG iteration we have calculated the dynamical exponent, $`z`$. The random couplings were taken from the power-law distribution in Eq.(2), where the strength of disorder is measured by the parameter $`D`$. In the following we present our results for the specific ladder models discussed in Sec. 2.

### A Random conventional ladders

We start with the conventional ladders in Fig. 1.a where the couplings along the chains ($`J_l^\tau ,\tau =1,2`$) and the couplings along the rungs ($`J_l^R`$) are taken from the same random distributions. In Fig. 7 we show the probability distribution of the gaps at the last step of the RG iteration calculated with the disorder parameter $`D=1`$ (see Eq.(2)). As seen in the figure the small energy tail of the distribution follows the functional form given by Eq. (12) and the dynamical exponent $`z`$ given by the asymptotic slope of the distributions is finite and has only a very weak size dependence.

Repeating the calculation for other values of $`D`$ we obtain a set of $`D`$-dependent dynamical exponents which are represented on Fig. 8. For strong disorder we obtain $`z(D)<D`$, which means that disorder is reduced in the course of the renormalization. In the terminology of Motrunich et al., this system is a finite randomness system, as opposed to the infinite randomness systems that will be considered in the next subsections. For weak disorder the dynamical exponent predicted by the approximative MDH renormalization is lowered below one for $`D<D_01`$. Here we argue that in this region the effect of disorder is irrelevant, so that the system is in the gapped RUS phase. Indeed, in a pure quantum system, where scaling in time and space is isotropic, the dynamical exponent is $`z_{pure}=1`$. Similarly, for disorder induced gapless systems, where disorder in the time direction is strictly correlated, the dynamical exponent can not be smaller, than in the pure system, so that $`z_{dis}z_{pure}=1`$. Consequently, if the disorder induced dynamical exponent is $`z_{dis}<1`$, then disorder could only influence the correction to scaling behavior, but the system stays gapped. In view of this remark $`D_0`$ can be considered as the lower limiting value of the disorder, where the conventional finite randomness behavior ends. So that the phase diagram of random conventional two-leg spin ladders consists of two phases: a gapped RUS (Haldane) phase and a random gapless Haldane phase. The latter is characterized by a finite dynamical exponent $`z(D)`$ for any strong but finite initial disorder. Consequently there is an important difference with the random AF spin-$`1`$ chain which flows into the IRFP above a finite critical value of randomness (see Fig. 5).

### B Random ladders with staggered dimerization

In this subsection we consider conventional ladders with staggered dimerization having a dimerization parameter, $`0\gamma 1`$, in Eq.(4). The different type of couplings in the ladder are taken from the power-law distribution in Eq.(2), each having the same disorder parameter, $`D`$, however the range of the distribution for the different type of couplings are, $`0<J_l^R<J_{max}^R`$ for the rung couplings, $`0<J_l^{weak}<(1\gamma )J_{max}`$ and $`0<J_l^{strong}<(1+\gamma )J_{max}`$ for the weaker and stronger chain couplings, respectively. For a fixed value of $`\gamma `$ and $`D`$ we have calculated the finite-size dependent effective dynamical exponent, $`z`$, as a function of the coupling ratio, $`J_{max}^R/J_{max}`$.

As shown in Fig. 9 the effective exponents have the same type of qualitative behavior for different values of the dimerization parameter, $`\gamma `$. In each case the curves have a maximum at some value of the couplings, where the finite-size dependence is the strongest, whereas more far from the maximum the convergence of the data is faster. To decide about the possible limiting value of $`z`$, in particular at the maximum of the curves, we analyze the behavior for $`\gamma =1`$ in Fig. 9c, which is just a dimerized random chain, the properties of which are exactly known by some extent.

The random critical point of this system is situated at $`J_{max}^R/J_{max}=2`$, where the critical behavior is governed by an IRFP, so that the dynamical exponent, $`z`$, is formally infinity. For any other values of the couplings, $`J_{max}^R/J_{max}`$, the system is in the random dimer phase, where the dynamical exponent is finite and coupling dependent. To see the general tendency of finite-size convergence of the $`z`$ exponent around the critical point we have repeated the calculation at the $`D=1,\gamma =1`$ case for the random $`XX`$-chain and the numerical finite-size results are compared in Fig. 9d with the exact value of the dynamical exponent, as given by the solution of the equation:

$$\frac{J_{max}^R}{J_{max}}=2\left(\frac{D^2}{D^2z^2}\right)^z,$$
(18)
known from Ref.. As seen in Fig. 9 the dynamical exponents of random $`XX`$\- and Heisenberg-ladders have very similar coupling dependence and one expects the same type of divergence at the critical point for all values of $`\gamma `$. In Fig. 10 we illustrate the scaling behavior of the gap at the transition point, i.e. at the maximum of the curves in Fig. 9a.

The distributions in Fig. 10a become broder and broder with the size and the effective dynamical exponent is increasing with the size without limits. An appropriate scaling collaps of the gap-distributions has been obtained in Fig. 10b, where the scaling variable in Eq.(17), with $`\psi =1/2`$ is used. Similar type of infinite randomness behavior is observed at other points of the critical lines, with the same exponent $`\psi =1/2`$, which turned out to be universal. Thus we conclude that the random conventional ladder with staggered dimerization has two Griffiths-type gapless phases, the random dimer phase and the random rung singlet phase, which are separated by a random critical line, along which there is infinite randomness behavior. For different disorder parameter, $`D`$, the position of the random critical line is modified, generally stronger disorder is in favor of the random rung singlet phase, see Fig. 11.

We note that the previously studied random conventional ladder is contained as a special point in this phase diagram at $`J_{max}^R/J_{max}=1`$ and $`\gamma =0`$. This point is in the random rung singlet phase for any value of $`D`$, thus the dynamical exponent is finite in accordance with the previous results.

### C Random zig-zag ladders

For the zig-zag ladders the nearest neighbor couplings $`(J_l^R=J_l^ZJ_l^1)`$ are taken from the power-law distribution in Eq.(2) with the coupling $`J_l^1`$ within the range $`0<J_l^1<J_{max}^1`$. Similarly, the next-nearest neighbor couplings ($`J_lJ_l^2`$) are taken from the same type of power-law distribution and the range of couplings is now $`0<J_l^2<J_{max}^2`$.

The calculated dynamical exponent, $`z`$, as shown in Figs. 12 has its maximum at $`J_{max}^2/J_{max}^1=0`$ and around this point one can observe strong finite-size dependence, the range of which is wide, in particular for weak disorder (see Fig. 12). At $`J_{max}^2/J_{max}^1=0`$, where the zig-zag ladder reduces to a random AF chain, the system is in the IRFP, thus the extrapolated value of the dynamical exponent is formally infinity. Given the strong finite-size corrections in the numerical RG data of the dynamical exponent in Fig. 12, it is difficult to decide whether the IRFP behavior of the zig-zag ladders is extended to a finite region of the couplings $`J_{max}^2/J_{max}^1>0`$ or whether this region shrinks to a single point only. The first scenario may be related to the existence of a gapless phase of the pure model for $`J^2/J^1<0.24`$.

To discuss this issue we have calculated the dynamical exponent by an independent method based on density matrix renormalization. In principle, the dynamical exponent is related to the distribution of the first gap, $`\mathrm{\Delta }`$, in the small $`\mathrm{\Delta }`$ limit, see in Eq.(12) with $`\mathrm{\Delta }J`$. However, a precise numerical calculation of a small $`\mathrm{\Delta }`$ by the DMRG method is very difficult, therefore we used another strategy, as described in details in Refs.. By this method one considers the equivalent AF chain with random first- and second-neighbor couplings (see Fig. 1d) and with fixed-free boundary conditions and calculate the surface magnetization, $`m_s`$, at the free end, which can be done very accurately by the DMRG method. As argued in Refs. for a random chain $`m_s`$ and $`\mathrm{\Delta }`$ can be considered as dual quantities, so that the distribution of the surface magnetization is asymptotically given by

$$P(\mathrm{ln}m_s)m_s^{1/z},m_s0.$$
(19)
Thus the dynamical exponent $`z`$ can be obtained from an analysis of the small $`m_s`$ tail of the distribution, as illustrated in Fig. 13 where the distribution function of $`\mathrm{ln}m_s`$ is given in a log-log plot for different lengths of the ladder. As seen in this Figure the slope of the distribution is well defined for larger systems, from which one can obtain an accurate estimate for the dynamical exponent, which is finite. Repeating the calculation for other values of the coupling ratio, $`J_{max}^2/J_{max}^1`$, we have obtained a set of the dynamical exponents, which are plotted in Fig. 12. These accurate DMRG data show that the extrapolated values of the effective exponents calculated by the numerical RG-method are finite for any $`J_{max}^2/J_{max}^1>0`$. Consequently the random zig-zag ladder has just one IRFP at $`J_{max}^2/J_{max}^1=0`$, whereas the system in the region of $`J_{max}^2/J_{max}^1>0`$ is in a gapless random dimer phase. In view of the numerical results in Fig. 12, where $`z_{\mathrm{}}`$ seems to stay over $`z_{pure}=1`$, it is quite probable that the randum dimer phase exists for any small value of the disorder.

### D Random $`J_1`$$`J_2`$ ladders

The full ladder, as represented in Fig. 1.e has three different type of couplings: $`J_l,J_l^R`$ and $`J_l^D`$. Here we consider a special case of this model, when the chain $`(J_l)`$ and rung $`(J_l^R)`$ couplings are taken from the same power-law distribution with a disorder parameter $`D`$ and having a range of $`0<J_l,J_l^R<J_{max}^1`$. On the other hand the diagonal couplings are taken from the same type of power-law distribution and are within the interval $`0<J_l^D<J_{max}^2`$. This model, having first- and second-neighbor interactions, is called a $`J_1`$$`J_2`$ ladder. We have calculated the finite-size dynamical exponents as a function of the coupling ratio $`J_{max}^2/J_{max}^1`$ for different strengths of disorder (see Fig. 14). These curves show similar qualitative behavior as those calculated for the random conventional ladders with staggered dimerization in Figs. 9, so that we can draw similar conclusions.

The extrapolated position of the maximum of the $`z`$ curves is identified as a quantum critical point with infinite randomness behavior. Indeed, repeating the calculation as indicated for the dimerized ladder model in Fig. 10 we obtained a scaling behavior as in Eq.(14). with an exponent which is compatible with $`\psi =1/2`$. The random quantum critical point separates two gapless Haldane phases, having odd and even topological order, respectively.

Repeating the calculation for different disorder parameters we obtain a phase diagram shown in Fig. 15. In the range of disorder we used in the calculation the random critical point is always attracted by the IRFP, this property probably remains true for any small value of disorder.

## V Discussion

In this paper different type of random AF spin ladder models have been studied by a numerical strong disorder RG method. In particular we asked the questions i) how the phase diagrams of the pure models are modified due to quenched disorder and ii) how the concepts observed in random AF chains, such as infinite randomness and Griffiths-type singularities are valid for these more complicated, quasi-one-dimensional models.

In our numerical calculations we observed as a general rule that for strong enough disorder the ladder models, like the random chains, become gapless. The dynamical exponent of the models is generally non-universal: $`z`$ depends on both the strength of disorder and on the value of the couplings. In models where there is a competition between different types of phases, either due to staggered dimerization or due to frustration, such as in the $`J_1`$$`J_2`$ model, at the phase boundary the critical behavior of the random model is generally controlled by an infinite randomness fixed point, at least for strong enough disorder. The low-energy properties of the systems in this IRFP are asymptotically exactly known from analytical calculations in random AF spin chains. Thus the general phase diagram consists of Griffiths-type phases with different topological order separated by a random critical point of the IRFP type. The zig-zag ladder is an exception, where there is just one Griffiths phase and the random critical point is located at its boundary.

Next we turn to discuss about possible cross-over effects when the strength of disorder is varied. These problems can not be directly studied by the simple strong disorder RG method, however, from arguments considering the sign of $`z_{dis}z_{pure}`$ and from analogous investigations on quantum spin chains we can suggest the following picture. Originally gapped phases could stay gapped for weak disorder and become gapless only if the strength of disorder exceed some finite limiting value, as seen for the random conventional ladder. However, for frustrated ladders, such as the zig-zag and the $`J_1J_2`$ ladders, any small amount of disorder seems to bring the system into a random gapless phase. At a phase boundary, such as in the staggered dimerized ladder and the $`J_1`$$`J_2`$ model, the random critical behavior is of the IRFP type, probably for any small amount of disorder.

At this point we comment on the similarity of the low-energy behavior of spin chains with $`2S=odd`$ ($`2S=even`$) spins and that of spin-1/2 ladders with $`n=odd`$ ($`n=even`$) legs. If the pure systems are gapless, i.e. $`2S=n=odd`$, strong enough disorder is expected to bring both systems into the IRFP. For $`2S=n=odd3`$, there is a limiting disorder strength, $`D_c(n)`$, below which the system is described by a conventional random fixed point with $`z<\mathrm{}`$. On the other hand for $`2S=n=even`$ we have only a partial analogy: for weak disorder both systems are gapped, which turn into a gapless Griffiths-type phase for stroger disorder. While the random ladder stays in this conventional random phase for any strength of the disorder the random spin chain will turn into a IRFP behavior at some finite limiting randomness. This type of infinite randomnass behavior can, however, be seen for frustrated even-leg $`J_1J_2`$ ladders at the transition point. We can thus conclude that random ladders with even and odd number of legs belong to different universality classes.

Finally, we comment on random square lattice antiferromagnets, which can be obtained in the limit when the number of legs, $`n`$, goes to infinity. By increasing $`n`$ the value of the limiting strength, $`D_c(n)`$, is expected to increase, too, both for $`n=even`$ (for frustrated ladders) and $`n=odd`$. In the limit, $`n\mathrm{}`$, $`D_c(n)`$ very probably tends to infinity, so that the critical behavior of that system is described by a conventional random fixed point. Work is in progress to verify this scenario and to obtain a general physical picture about the low-energy properties of random two-dimensional antiferromagnets.

Acknowledgment: F.I. is grateful to J.-C. Anglès d’Auriac and G. Fáth for useful discussions. This work has been supported by a German-Hungarian exchange program (DAAD-MÖB), by the German Research Foundation DFG, by the Hungarian National Research Fund under grant No OTKA TO23642, TO25139, TO34183, MO28418 and M36803, by the Ministry of Education under grant No. FKFP 87/2001 and by the Centre of Excellence ICA1-CT-2000-70029. Numerical calculations are partially performed on the Cray-T3E at Forschungszentrum Jülich.


text:
# Breakdown of Fermi-liquid theory in a cuprate superconductor

(December 13, 2001)

## Abstract

The behaviour of electrons in solids is remarkably well described by Landau’s Fermi-liquid theory, which says that even though electrons in a metal interact they can still be treated as well-defined fermions, called “quasiparticles”. At low temperature, the ability of quasiparticles to transport heat is strictly given by their ability to transport charge, via a universal relation known as the Wiedemann-Franz law, which no material in nature has been known to violate. High-temperature superconductors have long been thought to fall outside the realm of Fermi-liquid theory, as suggested by several anomalous properties, but this has yet to be shown conclusively. Here we report on the first experimental test of the Wiedemann-Franz law in a cuprate superconductor, (Pr,Ce)2CuO4. Our study reveals a clear departure from the universal law and provides compelling evidence for the breakdown of Fermi-liquid theory in high-temperature superconductors.

INTRODUCTION

Landau’s Fermi-liquid theory is the definitive theory of electrons in metals Landau , or more generally fermions in condensed matter, and a major landmark of 20th century physics. For example, it is the necessary foundation for the theory of superconductivity by Bardeen, Cooper and Schrieffer (BCS) BCS . In essence, it says that even in the presence of interactions the low-energy excitations of a system of mobile fermions can still be described in terms of well-defined fermionic particles, called “quasiparticles”, with charge $`e`$, spin $`\frac{1}{2}`$ and a mass $`m^{}`$, the latter being renormalized by interactions. The Wiedemann-Franz (WF) law is one of the basic properties of a Fermi liquid, reflecting the fact that the ability of a quasiparticle to transport heat is the same as its ability to transport charge, provided it cannot lose energy through collisions. Reported as an empirical observation by Wiedemann and Franz in 1853 WFL , the law states that the heat conductivity $`\kappa `$ and the electrical conductivity $`\sigma `$ of a metal are related by a universal constant:

$$\frac{\kappa }{\sigma T}=\frac{\pi ^2}{3}(\frac{k_B}{e})^2L_0$$
(1)
where $`T`$ is the absolute temperature, $`k_B`$ is Boltzmann’s constant and $`L_0=2.45\times 10^8`$ W $`\mathrm{\Omega }`$ K-2 is Sommerfeld’s value for the Lorenz ratio $`L\kappa /\sigma T`$ Sommerfeld .

The linear power of temperature in Eq. (1) comes from the linear temperature dependence of the fermionic specific heat, through the relation between heat transport and heat capacity. In kinetic theory,

$$\kappa =\frac{1}{3}cvl$$
(2)
where $`c`$ is the specific heat of the carriers, $`v`$ is their average velocity and $`l`$ their mean free path. Provided the mean free path between collisions is independent of temperature, as it is for the strictly elastic processes that operate at $`T0`$, the heat conduction has the same $`T`$ dependence as the specific heat. So for electrons, it is also linear in $`T`$, and given by Eq. (1). By contrast, boson-like excitations such as phonons or magnons give rise to a low-temperature specific heat and a heat conductivity as $`T0`$ which are proportional to $`T^3`$.

Theoretically, electrons are predicted to obey the WF law at $`T0`$ in a very wide range of environments Kearney : in both three dimensions or two dimensions (but not strictly in one dimension), for any strength of disorder and interaction (in the scaling theory of disorder and interaction) Castellani , scattering Chester  and magnetic field Smrcka . Experimentally, the WF law does appear to be universal at $`T0`$: no material has been reported to violate it. (Note that a departure from Eq. (1) has in fact been reported for silver Pobell , but is in contradiction with other measurements Cu1 ; Cu2 , including our own Ag-test .) This is true not only of simple metals like copper Cu1 ; Cu2 , but also of systems with strong electron correlations – such as the heavy fermion compounds CeAl3 Ott , CeCu6 Amato  and UPt3 Suderow  – or highly anisotropic conduction – such as the quasi-2D system Sr2RuO4 Tanatar  (a ruthenate which is isostructural to the cuprate La2CuO4), the quasi-1D organic conductor (TMTSF)2ClO4 Belin , or the 2D electron gas in a MOSFET Pepper . Even in the presence of so-called non-Fermi liquid behaviour, where the electrical resistivity is seen to deviate from the standard $`T^2`$ dependence, the WF law still holds at $`T0`$, as observed in CeNi2Ge2 Kambe . All this strongly suggests that the ground state of every metal investigated thus far is a Fermi liquid. Of course, if the metallic state gives way to a superconducting state at low temperature, then the WF law is entirely violated, as the charge is no longer transported by fermions but by Cooper pairs, which carry no entropy.

In 1986, high-temperature superconductivity was discovered in a class of oxides called cuprates, and fifteen years hence the fundamental question about these materials still remains: are they host to a new state of matter? In particular, are they Fermi liquids in their ground state, once superconductivity is removed (either by application of a magnetic field or by doping)? Anderson proposed early on Anderson  that the cuprates are indeed fundamentally different from other metals in that they are Mott insulators. When a small number of electrons or holes are doped into the CuO2 planes of their crystal structure, these materials can conduct charge reasonably well and also form a superconducting state. It is believed that the basic excitations of a doped Mott insulator are not fermionic quasiparticles as in other metals - with charge, spin and heat all carried by one and the same particle. Instead, the electron is thought to “fractionalize” into a neutral spin-$`\frac{1}{2}`$ fermion called a “spinon” and a spinless charge-$`e`$ boson called a “holon”, or a “chargon” Kivelson , a phenomenon called “spin-charge” separation.

Even though this bold proposal for a fundamentally new state of matter continues to be at the heart of several current theories of the cuprates Fisher , there has been little experimental evidence for such spin-charge separation. On the contrary, for example, a BCS/Fermi-liquid theory of $`d`$-wave quasiparticles appears to work rather well in the superconducting state of hole-doped cuprates, at least at low energy and near optimal doping Millis . Conceptually, a simple way to investigate the possibility of spin-charge separation is to measure the properties of charge transport and compare them to those of either spin or entropy transport. In this Article, we report on the first test of this kind, where both the charge conductivity $`\sigma `$ and the heat conductivity $`\kappa `$ of a cuprate superconductor are measured in the normal state at $`T0`$. We observe a good, metallic-like nearly temperature-independent charge transport at low temperature without the corresponding heat transport expected from the WF law. The normalized Lorenz number $`L/L_0`$ goes from being much less than unity at $`T0`$ to being greater than unity above 0.2 K. This is highly suggestive of spin-charge separation and a compelling demonstration that the ground state of cuprates can fall outside the realm of Fermi-liquid theory.
THE MATERIAL

The cuprate material used for this study is Pr2-xCexCuO4-y (PCCO), with a doping concentration of $`x=0.15`$, which is roughly the optimum value for maximizing the critical temperature for superconductivity, where $`T_c`$ 20 K. The addition of $`x`$ Ce atoms on Pr sites adds $`x`$ electrons to the CuO2 planes of the parent insulating compound, the Mott insulator Pr2CuO4. PCCO is the electron-doped analog of the hole-doped material La2-xSrxCuO4-y (LSCO), wherein the addition of $`x`$ Sr atoms on La sites removes $`x`$ electrons from (adds $`x`$ holes to) the CuO2 planes. In LSCO, the optimum doping is also at approximately $`x=0.15`$, with a maximum $`T_c`$ 40 K. For reasons that are not clear, both materials have critical temperatures that are significantly lower than those of several other cuprates, such as YBa2Cu3O7-δ (Y-123), Bi2Sr2CaCu2O8+δ (Bi-2212) and Tl2Ba2CuO6+δ (Tl-2201), which all have a maximal $`T_c`$ around 90 K. Nevertheless, all cuprates share the same basic crystal structure, namely that of a stack of CuO2 planes, and the same generic dependence on doping. The technical advantage of LSCO and PCCO is that the magnetic field needed to destroy superconductivity is correspondingly lower, with upper critical field values of $``$ 50 T and $``$ 10 T, respectively. Because these fields can be achieved in the laboratory, it is possible to investigate their low-temperature transport properties in the normal state, such as was done for charge conductivity by Boebinger et al. on LSCO Boebinger  and by Fournier et al. on PCCO Fournier .
CRYSTALS

The single crystal of PCCO used in this study was grown with a flux technique described elsewhere Growth1 ; Growth2 , using a Al2O3 crucible and an oxygen reduction treatment at 1000 C. The concentration of cerium was fixed at $`x=0.15`$. Contacts were made with silver epoxy, diffused at 500 C for 1 hour, and were used to measure both electrical resistivity and thermal conductivity. The electrical resistance of contacts was typically $`1\mathrm{\Omega }`$. The crystal was in the shape of a platelet, 37 $`\mu `$m thick and 720 $`\mu `$m wide, with 1.0 mm separation between voltage contacts. The superconducting transition temperature $`T_c`$ was obtained from three different measurements: as the end of the drop in resistivity, the end of the diamagnetic drop in susceptibility and the onset of a small peak in thermal conductivity. In all cases, $`T_c=20`$ K to within less than $`\pm 0.5`$ K. The width of the transition is 6 K in resistivity, 3 K in magnetisation and about 1 K in thermal conductivity. The broad resistive transition, seen both as a function of temperature and magnetic field, is most likely due to an inhomogeneous distribution of oxygen near the surface. The narrower transition obtained in thermal conductivity suggests that this inhomogeneity is confined to a negligible volume of the sample, and therefore does not affect bulk measurements such as heat transport. Note that all results presented in this paper were reproduced on several other single crystals grown in similar conditions, with comparable $`T_c`$ and resistivity.

CHARGE TRANSPORT

The temperature dependence of the electrical resistivity is shown in Fig. 1 for different magnetic fields applied parallel to the $`c`$-axis of the tetragonal crystal structure. The current is made to flow in the CuO2 planes, where the conduction is some 104 times better than perpendicular to the planes (at room temperature). Above 25 K, the temperature dependence is not linear as in most optimally-doped cuprates, but follows a power law $`a+bT^\alpha `$ with $`\alpha 1.7`$, and has a magnitude characteristic of a reasonably good metal: $`a25\mu \mathrm{\Omega }`$ cm and $`\rho `$(300 K) $``$ 140 $`\mu \mathrm{\Omega }`$ cm. The effect of a magnetic field is to rapidly suppress the superconducting transition initially, but then more slowly at high fields, giving rise to a curve $`T_c(H)`$ that has strong positive curvature. From the magnetoresistance at 0.3 K shown in the lower inset, one can see that the entire sample has completed its transition to the normal state by 13.5 T. Note, however, that the bulk of the sample is no longer superconducting above 8 T, the field beyond which the low-temperature heat transport ceases to evolve (see Fig. 2 below).

The overall behaviour of the resistivity in PCCO is similar to that of hole-doped cuprates when overdoped. Indeed, when doped to have a $`T_c`$ of 15 K, Tl-2201 has a resistivity which goes as $`T^{1.75}`$ with values of 10 $`\mu \mathrm{\Omega }`$ cm at low temperature and 180 $`\mu \mathrm{\Omega }`$ cm at room temperature, and a resistive critical field with a strong upward curvature reaching a value of 16 T at $`T0`$ Mackenzie . One difference is the slight upturn seen at low temperature in PCCO and not in Tl-2201. The resistivity in the normal state (at 14 T) increases by about 10% in going from 8 K down to 0.3 K (see Fig. 1). Similar but much larger upturns were observed in Nd2-xCexCuO4 (NCCO) Harus ; Fournier2  and PCCO Fournier2  at lower carrier concentrations, and attributed to weak localization. In support of this interpretation is the suppression of the upturn by a transverse magnetic field, also observed in our samples (see inset of Fig. 1). This negative magnetoresistance eventually flattens to a constant beyond 25 T, equal to 25.2 $`\mu \mathrm{\Omega }`$ cm at 0.5 K Hill .

In summary, once the superconducting order has been completely suppressed throughout the sample, namely in a magnetic field larger than 13.5 T, the charge transport of this cuprate material at low temperature is that of a fairly good quasi-two-dimensional metal, with a residual resistivity $`\rho (T0)=\rho _0=26.8\mu \mathrm{\Omega }`$ cm in 14 T, which corresponds to a conductivity per CuO2 plane of 60 $`e^2/h`$ (i.e. $`k_Fl60`$).
HEAT TRANSPORT

Fifteen years after the discovery of high-temperature superconductivity, very little is known about the normal state of cuprates at low temperature. The ability to suppress superconductivity in optimally-doped PCCO with a field of only 14 T provides a rare opportunity to shed light on the fundamental nature of the electron system in these materials. In the present study, this was done by measuring the transport of heat as $`T0`$. The thermal conductivity $`\kappa (T)`$ of PCCO is shown in Fig. 2 at temperatures below 0.3 K, for heat flowing parallel to the CuO2 planes. The data is plotted as $`\kappa /T`$ vs $`T^2`$ in order to easily separate the contributions of phonons and electrons, using the fact that phonons are expected to have a heat conductivity which varies as $`T^3`$ when their mean free path reaches the size of the crystal at sufficiently low temperature. A straight line extrapolating to zero in $`\kappa /T`$ vs $`T^2`$ is indeed the asymptotic ($`T0`$) behaviour observed in insulators Thacher , including the Mott insulator YBa2Cu3O6 (i.e. Y-123 without any doped carriers) Taillefer . This is also the behaviour of conventional ($`s`$-wave) superconductors. The absence of a residual linear term $`\kappa _0/T`$, defined as the value of $`\kappa /T`$ as $`T0`$, means that there are no mobile fermionic excitations at low temperature. In insulators, this is due to the lack of electronic carriers, while in superconductors it is because electrons have all formed Cooper pairs at $`T<<T_c`$. The heat is then conducted entirely by phonons. In contrast, a residual linear term is observed when fermionic excitations are present, as in the following three instances: 1) in metals, with a residual linear term given precisely by the WF law; 2) in the vortex state of superconductors, where a magnetic field induces a residual linear term by generating delocalized quasiparticles Boaknin2 ; 3) in $`d`$-wave superconductors, where zero-energy quasiparticles are induced by impurity scattering Durst .

Superconducting state

In the absence of a magnetic field, there is only a very small residual linear term in the thermal conductivity of PCCO. From data on four different crystals, we find $`\kappa _0/T=0.030.07`$ mW K-2 cm-1. This is considerably smaller than the residual linear term observed in three hole-doped cuprates, at optimal doping: $`\kappa _0/T`$ = 0.14, 0.15 and 0.11 mW K-2 cm-1, in Y-123 Taillefer ; Chiao , Bi-2212 Chiao2 ; Aubin  and LSCO Taillefer2 , respectively. Within BCS theory applied to a $`d`$-wave superconductor, this fermionic residual heat conduction is expected, arising from zero-energy quasiparticles induced by impurity scattering near the nodes in the $`d_{x^2y^2}`$ gap function Durst . In the case of Bi-2212, the excellent quantitative agreement between theory and experiment has been viewed as a strong validation of a Fermi-liquid quasiparticle picture for the superconducting state Millis ; Chiao2 , at least at optimal doping and low energies.

Several tentative explanations may be offered for the weakness of the residual linear term in PCCO. The first possibility is the localization of $`d`$-wave quasiparticles, investigated by several authors Lee . It was invoked recently as a possible cause for the absence of a residual linear term in YBa2Cu4O8 (Y-124) Hussey . However, it is not clear why localization should occur in Y-124 and not in Y-123, given that these two cuprates have comparable structure and properties. It seems more plausible in PCCO, because of the highly two-dimensional nature of its conduction – some 100 times more anisotropic than either Y-124 or LSCO. On the other hand, Bi-2212 is equally anisotropic, yet shows delocalized quasiparticles. A second scenario is the absence of nodes in the gap structure of PCCO. This would eliminate any residual linear term (at least in zero magnetic field). The symmetry of the order parameter need not be $`s`$-wave, but could have the form $`d+ix`$, where $`x`$ is a subdominant component of either $`s`$ or $`d_{xy}`$ symmetry. The possibility of a $`T=0`$ transition in the order parameter from $`d`$ to $`d+ix`$ as a function of doping has been raised in the context of a possible quantum critical point in the phase diagram of cuprates Sachdev . For PCCO, however, this would seem to be in conflict with evidence for a rather pure $`d_{x^2y^2}`$ symmetry as determined in a recent tricrystal experiment Tsuei . The other difficulty is that, as we shall see below, a magnetic field normal to the CuO2 planes never induces a residual linear term, implying that the minimum gap would have to be a sizable fraction of the maximum gap (i.e. $`x`$ comparable to $`d`$). This would have to be reconciled with the penetration depth data lambda1 ; lambda2 . A third possibility, proposed recently by Granath et al. Granath , is the removal of the nodes as a result of static stripe ordering.
Normal state

As seen in Fig. 2, the basic effect of a magnetic field is to rapidly increase the thermal conductivity of PCCO (at finite temperature). Given that the phonon conductivity cannot exceed its value at zero field (where the phonon mean free path has reached its maximum value), this increase must be due to excitations of electronic origin. The field-induced conduction (over and above the zero-field curve) grows rapidly (and approximately linearly) with field at low fields to eventually saturate at high fields, where $`\kappa `$ is absolutely constant above 8 T. This is compelling evidence that the thermodynamic upper critical field in this sample is at most 8 T and the bulk of the crystal is in the normal state beyond that. Indeed, in all known superconductors, whether $`s`$-wave or $`d`$-wave, the electronic thermal conductivity is always affected by the magnetic field when in the vortex state, and seen to saturate above $`H_{c2}`$ (see for example Ref. Belin2 ).

Such an $`H_{c2}`$ agrees reasonably well with the criterion of zero resistance, achieved at about 6 T, and also agrees with the $`H_{c2}`$ values reported previously in thin films of PCCO Fournier ; Alff  and NCCO Osofsky ; Alff  at $`x=0.15`$. A roughly linear growth of $`\kappa `$ with field is also seen, for example, in the borocarbide superconductor LuNi2B2C Boaknin2 , however with a major difference: in LuNi2B2C, the field induces a linear term at $`T0`$. Furthermore, this finite residual linear term ultimately reaches a value in the normal state given precisely by the WF law. In striking contrast, a magnetic field, even as high as 13 T, almost twice $`H_{c2}`$, never induces a residual linear term in PCCO. Given the known value of the electrical resistivity at $`T0`$ and 13 T, namely $`\rho _0=26.8\mu \mathrm{\Omega }`$ cm, the WF law predicts a residual linear term $`\kappa _0/T=L_0/\rho _0=0.91`$ mW K-2 cm-1, as drawn in Fig. 2. (Note that weak localization is not expected to alter the WF law appreciably Castellani , as verified experimentally in layered graphene graphene .)

This complete violation of the WF law shows that the non-superconducting ground state of this cuprate material is not a Fermi liquid. The charge carriers responsible for the good electrical conduction do not display the expected fermionic heat transport.

It is instructive to consider the effect of increasing the temperature above zero. Contributions to the heat transport from the electron system ($`\kappa _e`$) and from the ionic lattice ($`\kappa _{ph}`$) will add to give the measured thermal conductivity: $`\kappa (T)=\kappa _e(T)+\kappa _{ph}(T)`$. These two systems are coupled. It is unambiguous that phonons are scattered by electrons since the crystal conducts heat better at zero field than at 13 T beyond 0.6 K. In other words, as the temperature is raised, inelastic scattering processes become increasingly effective at limiting the phonon heat flow, and we expect the dominant process to be electron-phonon scattering.

Given this observed electron-phonon coupling, the total phonon scattering in field is the sum of whatever scatters phonons in zero field plus the added scattering that comes from the field-induced electronic excitations. The thermal resistivity of phonons due to electron scattering is given by $`W_e^{ph}=BT^2`$ Berman , where the constant $`B`$ depends on the strength of the electron-phonon coupling, the electronic density of states, and various other factors. This means that the phonon conductivity at low $`T`$ is given by $`\kappa _{ph}=\kappa (0)[1+\kappa (0)W_e^{ph}]^1`$, where $`\kappa (0)`$ is the measured zero-field conductivity, assumed to be essentially all phononic. We can put a reasonable lower bound on the electron-phonon coupling parameter $`B`$ by requiring that the resulting $`\kappa _e/T`$ does not decrease with $`T`$. Adjusting $`B`$ such that $`\kappa _e/T`$ is constant above 0.3 K gives the curve shown in Fig. 3 for $`H=13`$ T (full circles). The same can be done for other fields with the resulting values of $`\kappa _e/T`$ = 0.6, 1.2 and 1.9 mW K-2 cm-1 and corresponding values of $`B`$ = 0.22, 0.4, and 0.68 K3 m W-1 for $`H`$ = 2, 4, and 8 (or 13) T, respectively. (In comparison, electron-phonon coupling in copper gives $`B=48`$ K3 m W-1 Berman .) Note the self-consistency of this analysis whereby $`B`$ scales with the value of $`\kappa _e/T`$ (above 0.3 K); in other words, by increasing the field – thereby increasing the density of electronic excitations – one increases both the electronic heat conduction and the electron scattering of phonons.

From Fig. 3, we see that $`\kappa _e(T)/T`$ exceeds the value of $`L_0/\rho `$ appropriate for a Fermi liquid. In other words, the low-energy excitations of the electron system violate the WF law not only at $`T0`$, where $`\kappa _e(T)/TL_0/\rho _0`$, but also at finite temperatures, where $`\kappa _e(T)/T>L_0/\rho `$ (above 0.2 K). It is important to appreciate that qualitatively the latter violation is independent of our choice of $`B`$, in the sense that even if $`B`$ is set to zero, $`\kappa _e/T`$ still exceeds $`L_0/\rho `$, in this case by 30% at 0.25 K. We stress that $`B=0`$ is unphysical, as it would lead to a negative $`\kappa _e/T`$ for $`T>0.6`$ K. It is also independent of our assumption that $`\kappa (0)`$ is entirely phononic; indeed if some part of $`\kappa (0)`$ is in fact electronic, then the violation turns out to be even more pronounced. In other words, while there is no accurate way to extract the electronic contribution at 13 T, the fact that the WF law is violated is independent of our model for the phonon conduction and the electron-phonon scattering. The result $`\kappa _e(T)/T2L_0/\rho _0`$ above 0.3 K is obtained in several crystals, even though $`\rho (T_c)`$ varies in the range 20 to 40 $`\mu \mathrm{\Omega }`$ cm.

We have investigated the possibility that our measurement gradually ceases to detect the electronic heat current as electrons fall out of thermal equilibrium with the phonon bath when the temperature approaches $`T=0`$. One can imagine this happening when the electrical contact resistance between the heater and the sample is too large and the heat is predominantly carried by the phonons. This might then explain the drop in $`\kappa _e/T`$ measured below 0.3 K or so (see Fig. 3). Two facts lead us to rule out electron-phonon decoupling as the main mechanism for the drop. First, identical data is obtained by sending heat directly through the electron system using photons (as in Ref. Decoupling ). Secondly, a similar drop is observed in samples of optimally-doped (La,Sr)2CuO4, where we have achieved electrical contact resistances that are 100 times lower than in our PCCO samples, namely 10 m$`\mathrm{\Omega }`$. We therefore believe this low-temperature drop is intrinsic and not specific to PCCO.
CONCLUSION

The cuprate PCCO is the first material to violate the Wiedemann-Franz law. The breakdown of this robust signature of Fermi-liquid theory suggests that the fundamental entities that carry heat, charge (and spin) in the cuprates are not the usual Landau quasiparticles. The fact that the electron system conducts heat in a way which is largely unrelated to the way it carries charge at low temperature points to the existence of neutral excitations responsible for much of $`\kappa _e`$. If these neutral excitations are fermions, i.e. spinons, they should contribute a constant term to $`\kappa _e/T`$, as may well be the case for $`T>0.3`$ K. The drop seen at the very lowest temperatures then remains to be explained, and the possibility of spinon localization should be considered.

The present study is currently limited to a single carrier concentration, near optimal doping, in the whole phase diagram. It will be interesting to investigate the evolution with doping of this emerging picture. If one speculates that the WF law is satisfied in overdoped cuprates, where Fermi-liquid theory is generally assumed to hold, our results on optimally-doped PCCO suggest that a violation of the law is a property of underdoped cuprates. A comprehensive study will shed light on the gradual breakdown of Fermi-liquid theory in the cuprates as the carrier concentration is reduced towards the Mott insulating state.
Acknowledgements

We thank C. Lupien, E. Boaknin, M. Sutherland, M. Chiao, R. Gagnon, J. Brooks, L. Balicas and B. Brandt for their invaluable help in various aspects of the measurements. This work was supported by the Canadian Institute for Advanced Research and funded by NSERC of Canada. LT ackowledges the support of a Premier’s Research Excellence Award from the Government of Ontario. The work in Maryland was supported by the NSF Division of Condensed Matter Physics.
Correspondence should be addressed to L.T. (Louis.Taillefer@utoronto.ca).
Present address: Laboratoire National des Champs Magnétiques Pulsés, 143 Avenue de Rangueil, BP 4245, 31432 Toulouse, Cedex 04, France.
Present address: Département de Physique, Université de Sherbrooke, Sherbrooke, Québec J1K 2R1, Canada.


text:
# Published in: Europhys. Lett., 59 (5), pp. 754-760 (2002). On the consequences of the uncertainty principle on the superconducting fluctuations well inside the normal state

## Abstract

We first argue that the collective behaviour of the Cooper pairs created by thermal fluctuations well above the superconducting transition temperature, $`T_C`$, is dominated by the uncertainty principle which, in particular, leads to a well-defined temperature, $`T^C`$, above which the superconducting coherence vanishes. On the grounds of the BCS approach, the corresponding reduced-temperature, $`\epsilon ^C\mathrm{ln}(T^C/T_C)`$, is estimated to be around $`0.55`$, i.e., above $`T^C1.7T_C`$ coherent Cooper pairs cannot exist. The implications of these proposals on the superfluid density are then examined using the Gaussian-Ginzburg-Landau approximation. Then we present new measurements of the thermal fluctuation effects on the electrical conductivity and on the magnetization in different low- and high-$`T_C`$ superconductors with different dopings which are in excellent agreement with these proposals and that demonstrate the universality of $`\epsilon ^C`$.
74.20.-z Theories and models of superconducting state
74.20.De Phenomenological theories (two-fluid, Ginzburg-Landau, etc.)
74.40.+k Fluctuations (noise, chaos, nonequilibrium superconductivity, localization, etc.)

The behaviour of the superconducting fluctuations well inside the normal state, when the superconducting coherence length, $`\xi (T)`$, becomes of the order of its amplitude extrapolated at $`T=0`$ K, $`\xi (0)`$, is a long-standing open problem which interest has been considerably enhanced by the discovery of the high temperature cuprate superconductors. Recent measurements of the superconducting fluctuations above $`T_C`$ in various high-$`T_C`$ and low-$`T_C`$ superconductors suggest the existence of a well-defined reduced-temperature, $`\epsilon ^C\mathrm{ln}(T^C/T_C)`$, above which the fluctuation effects vanish. These results were explained phenomenologically by introducing in the Gaussian-Ginzburg-Landau (GGL) approach a so-called “total-energy” cutoff, instead of the conventional momentum cutoff always used until now. The first aim of this Letter is to analyze the physical origin of such a total-energy cutoff. We will see here that it can be easily understood in terms of the uncertainty principle, which imposes a limit to the shrinkage above $`T_C`$ of the superconducting wave function when the temperature increases. Then, we will probe experimentally the universality of $`\epsilon ^C`$ by extending our previous measurements of the fluctuation effects in the high reduced-temperature region to very different low- and high-$`T_C`$ superconductors with different dopings, including for the first time a type-I superconductor.

The Heisenberg uncertainty principle was applied in 1953 to superconductors by Pippard to relate the size of the “wave packet formed by the electronic states”, $`\xi _0`$, to the normal-superconducting transition temperature, $`T_C`$ . In terms of the BCS approach, the Pippard proposal suggests that the minimum size of a Cooper pair is of the order of $`\xi _0`$. By taking into account that the superconducting coherence length, $`\xi (T)`$, is the characteristic distance over which the density of Cooper pairs may vary, it may be concluded that even above $`T_C`$, where the Cooper pairs are created by thermal fluctuations, $`\xi (T)`$ must verify

$$\xi (T)\stackrel{>}{_{}}\xi _0,$$
(1)
where $`\xi _0`$ is the actual superconducting coherence length at $`T=0`$ K. Equation (1) provides then a constraint for the existence and behaviour of coherent Cooper pairs which must apply to any theoretical description of the superconducting state formation, including those non-BCS-like which are being proposed for cuprate superconductors . In fact, this condition may be directly obtained by applying the uncertainty principle to the Cooper pairs localized in a coherent volume. In other words, Eq. (1) accounts for the limits imposed by the uncertainty principle to the shrinkage, when the temperature increases, of the superconducting wave function.

The most outstanding consequence of Eq. (1) is that it naturally leads to a reduced-temperature, $`\epsilon ^C`$, determined by $`\xi (\epsilon ^C)\xi _0`$, above which coherent Cooper pairs cannot exist. The value of $`\epsilon ^C`$ will depend on each particular approach through the $`\epsilon `$-dependence of $`\xi (\epsilon )`$, where $`\epsilon \mathrm{ln}(T/T_C)`$ is the reduced-temperature. For instance, by using the mean-field reduced-temperature dependence of the coherence length, $`\xi (\epsilon )=\xi (0)\epsilon ^{1/2}`$, then $`\epsilon ^C(\xi (0)/\xi _0)^2`$. On the grounds of the BCS approach in the clean limit, $`\xi (0)=0.74\xi _0`$, and so $`\epsilon ^C0.55`$ in these superconductors. In fact, this striking result probably also holds at a qualitative level in moderately dirty BCS superconductors (when $`\mathrm{}\stackrel{<}{_{}}\xi _0`$, $`\mathrm{}`$ being the mean free path of the normal carriers) because one may expect that both the Ginzburg-Landau (GL) coherence length amplitude and the actual superconducting coherence length at $`T=0`$ K will be affected by impurities to a similar extent (see, e.g., Ref. , § 7-2).

What consequences has Eq. (1) on the collective behaviour of the Cooper pairs at reduced-temperatures below $`\epsilon ^C`$? Probably the simplest way to address this question at a qualitative level is to introduce Eq. (1) in the conventional GGL framework, in spite that the latter formally applies only when $`\epsilon 1`$. In fact, another central point in this Letter will be to probe experimentally if the introduction of Eq. (1) in the GGL approximation extends its applicability up to $`\epsilon ^C`$. On the grounds of the GGL approach, Eq. (1) leads to

$$\xi ^2(\epsilon )+k^2\stackrel{<}{_{}}\xi _0^2,$$
(2)
where the left-hand term is the GGL total energy per superconducting carrier (in units of $`\mathrm{}^2/2m^{}`$, where $`m^{}`$ is the superconducting carriers effective mass) of the fluctuating mode with wave vector k. Actually, as stressed before for Eq. (1), one may directly obtain Eq. (2) by naïvely applying the uncertainty principle to the spatial extension of the superconducting fluctuations and taking into account that at finite temperatures the energy balance when creating the fluctuations must include both the uncertainty principle and the thermal agitation. This crude reasoning is to some extent similar to the well-known textbook procedure used to estimate the minimum size of atoms by balancing the Coulomb and the Heisenberg localization energies. Note that for $`\epsilon \epsilon ^C`$ \[and using $`\xi (0)`$ instead of $`\xi _0`$\] Eq. (2) reduces to the widely used kinetic-energy or momentum cutoff condition $`k^2c\xi ^2(0)`$, where $`c`$ is a cutoff constant of the order of unity . Note also that any cutoff condition is not built-in in the standard GGL equations, and it must be added to them “by hand”. Adequate extensions of the standard GGL equations to further Gor’kov perturbative orders could perhaps reproduce the total-energy cutoff, but we are not aware of any successful attempt of this.

The deep influence of Eq. (2) on the superconducting fluctuations in the normal state below $`\epsilon ^C`$ is well illustrated by the reduced-temperature dependence of the superfluid density, $`n_s(\epsilon )`$, on which any observable will depend. $`n_s(\epsilon )`$ is defined here on the grounds of the conventional GL approach as the spatially- and thermally-averaged squared modulus of the GL wave function :

$$n_s(\epsilon )\left|\mathrm{\Psi }\right|^2=\underset{𝐤}{}\left|\mathrm{\Psi }_𝐤\right|^2,$$
(3)
where $`\mathrm{\Psi }_𝐤`$ is the wave function of the fluctuating mode with wave vector $`𝐤`$. On the grounds of the Gaussian approximation for the fluctuations of both the amplitude and phase of the order parameter, and for zero applied magnetic field, $`<\left|\mathrm{\Psi }_𝐤\right|^2>`$ is given by the well-known result (see, e.g., Eq. (8.27) of Ref. ):

$$\left|\mathrm{\Psi }_𝐤\right|^2=\frac{2m^{}\xi ^2(0)}{\mathrm{}^2}\frac{k_\mathrm{B}T}{\epsilon +k^2\xi ^2(0)}.$$
(4)
This familiar expression of the amplitude average of each fluctuating mode already illustrates the need of a total-energy cutoff: $`<\left|\mathrm{\Psi }_𝐤\right|^2>`$ increases (instead of decreasing) when the temperature increases well above $`T_C`$. This nonphysical behaviour appears for any $`k`$-value at reduced-temperatures above $`\epsilon +k^2\xi ^2(0)=1`$. It cannot be eliminated, therefore, by the momentum cutoff condition. In contrast, a total-energy cutoff will remove, if $`\epsilon ^C1`$, this nonphysical behaviour (see also later).

From Eqs. (3) and (4) the superfluid density for any cutoff criterion may be directly calculated by just imposing on the $`𝐤`$-summation the corresponding limits for the modulus of $`𝐤`$. Such a limit is infinity for no cutoff, $`\sqrt{(\epsilon ^C\epsilon )}/\xi (0)`$ for the total-energy cutoff, and $`\sqrt{c}/\xi (0)`$ for the momentum cutoff. As it is well known, without cutoff the above integrations diverge at every temperature . With the total-energy cutoff, we get for 2D-films of thickness $`d`$ (and also for extremely anisotropic layered superconductors with effective interlayer separation $`d`$):

$$n_s(\epsilon )_E^{2\mathrm{D}}=\frac{m^{}k_\mathrm{B}T}{2\pi \mathrm{}^2d}\mathrm{ln}\left(\frac{\epsilon ^C}{\epsilon }\right),$$
(5)
and for 3D-bulk isotropic superconductors:

$$n_s(\epsilon )_E^{3\mathrm{D}}=\frac{m^{}k_\mathrm{B}T\sqrt{\epsilon }}{\pi ^2\mathrm{}^2\xi (0)}\left(\sqrt{\frac{\epsilon ^C\epsilon }{\epsilon }}\mathrm{arctan}\sqrt{\frac{\epsilon ^C\epsilon }{\epsilon }}\right).$$
(6)
The corresponding expressions under a momentum cutoff may be obtained from Eqs. (5) and (6) by replacing $`\epsilon ^C`$ by $`c+\epsilon `$.

The reduced-temperature dependence of the superfluid density under these different cutoff conditions is shown in Fig. 1(a). We have chosen for representation $`\epsilon ^C=0.55`$ as it results from the simplest estimate using the BCS theory in the clean limit (or, in the case of the momentum cutoff, $`c=0.55`$). All the other parameters entering in Eqs. (5) and (6), including $`\xi (0)`$, are absorbed by the normalization chosen in the plot. As clearly illustrated by the figure, the conventional momentum cutoff predicts a nonphysical increase of the superfluid density at high $`\epsilon `$’s, which is a consequence of the high-$`T`$ divergence of Eq. (4). In contrast, under the total-energy cutoff $`n_s(\epsilon )`$ vanishes at $`\epsilon =\epsilon ^C`$. The corresponding fall-off is remarkably sharp, following in the close vicinity of $`\epsilon ^C`$ a power law-like behaviour with respect to $`|\stackrel{~}{\epsilon }|`$, with $`\stackrel{~}{\epsilon }\mathrm{ln}(T/T^C)=\epsilon \epsilon ^C`$: In the 2D superconductors $`n_s(\epsilon )_E^{2D}\stackrel{}{_{}}|\stackrel{~}{\epsilon }|`$, and in the 3D superconductors $`n_s(\epsilon )_E^{3D}\stackrel{}{_{}}|\stackrel{~}{\epsilon }|^{1.5}`$, in both cases with 5% or better accuracy for $`|\stackrel{~}{\epsilon }|0.1`$ if $`\epsilon ^C0.3`$. Also noticeable is that such a rapid fall-off occurs when the coherence length competes with the size of the individual Cooper pairs, as illustrated by the $`\xi (\epsilon )/\xi _0`$ scale shown in Fig. 1(a) (whose numerical values correspond to the BCS clean limit): When $`\xi (\epsilon )\stackrel{>}{_{}}2\xi _0`$, which roughly corresponds to $`\epsilon \stackrel{<}{_{}}0.15`$, the consequences of the uncertainty principle on the superconducting fluctuations are inappreciable, and the momentum cutoff condition provides a good approximation to $`n_s(\epsilon )`$. However, for $`2\xi _0\stackrel{>}{_{}}\xi (\epsilon )\stackrel{>}{_{}}\xi _0`$ (corresponding to $`0.15\stackrel{<}{_{}}\epsilon \stackrel{<}{_{}}\epsilon ^C`$), i.e., when $`\xi (\epsilon )`$ competes with the size of the individual Cooper pairs, the uncertainty principle will dominate the collective behaviour of these Cooper pairs.

The above results strongly suggest, therefore, that any superconducting fluctuation effect in the normal state will vanish above $`\epsilon ^C`$. However, probably the best way to probe these results is to extend our first experiments on the fluctuation effects in the high-$`\epsilon `$ region  to different superconducting materials with different $`\xi (0)`$ values and also with various pairing states and maybe different pairing mechanisms. Some examples of the fluctuation effects on the magnetization \[the so-called fluctuation magnetization, $`\mathrm{\Delta }M`$\] and on the electrical conductivity \[the so-called paraconductivity, $`\mathrm{\Delta }\sigma (\epsilon )`$\] obtained in different low- and high-$`T_C`$ superconductors are presented in Fig. 1(b). The experimental setups and procedures used in our present experiments are similar to those described in Refs.  and . Other aspects, including the preparation of the samples, are going to be published elsewhere. Let us stress here, however, that the samples used in the paraconductivity experiments were single crystals and epitaxial thin films. The electrical resistivity versus temperature was measured with a four-terminal arrangement by using a conventional low-frequency (37 Hz) ac lock-in amplifier phase sensitive technique. To be able to determine $`\mathrm{\Delta }M`$ in the high-$`\epsilon `$ region, the magnetization measurements were performed with a SQUID magnetometer (Quantum Design, model MPMS) and by using quite big polycrystalline samples (with masses up to a few grams). Let us also note here that in analyzing all these measurements the background fitting region was always localized well above $`\epsilon ^C`$. So, the results presented in Fig. 1(b) are only moderately affected by the background uncertainties. These measurements cover almost two orders of magnitude in reduced magnetic fields $`hH/H_{c2}(0)`$, where $`H_{c2}(0)`$ is the upper critical magnetic field amplitude (extrapolated to $`T=0`$ K). In fact, they cover both the zero field limit ($`h\epsilon `$) and the finite field regime. In this last case the $`\mathrm{\Delta }M(\epsilon )_\text{h}`$ data could be also affected by dynamic and non-local electrodynamic effects . These examples also cover quite different superconductors, including moderately dirty (PbIn8%, i.e., Pb-8 at. % In) and clean (all the others), type I (Pb) and II (all the others), 3D-bulk low-$`T_C`$ (isotropic PbIn8% and Pb; moderately anisotropic MgB2) and 2D-layered high-$`T_C`$ (the optimally-doped Bi-2212, i.e., Bi2Sr2CaCu2O8+δ with $`\delta 0.16`$, and in the inset the underdoped LaSCO/0.1, i.e., La1.9Sr0.1CuO4).

The hallmark of the suppression of the superfluid density by the total-energy cutoff, i.e., the rapid fall-off at a well-defined reduced-temperature, $`\epsilon ^C`$, of the superconducting fluctuation effects, is present in all the experimental curves in Fig. 1(b). The dashed and the solid lines in the main Fig. 1(b) and in its inset correspond to the GGL predictions in the zero-field limit under a conventional momentum cutoff and, respectively, a total-energy cutoff. The corresponding formulas may be found in Refs. . Note that for our present purposes we must substitute $`c`$ by $`\epsilon ^C`$ in the expressions under the total-energy cutoff, and that in the case of the 2D-multilayered superconductors studied here we must multiply the corresponding single-layered expressions by $`N`$, the number of superconducting layers per periodicity length. The $`\xi (\epsilon )/\xi _0`$ scales in Fig. 1(b) and in its inset illustrate that the behaviour of the superconducting fluctuations is dominated by the localization energy when the superconducting coherence competes with $`\xi _0`$, the size of the Cooper pairs. The comparison between the two $`\mathrm{\Delta }M(\epsilon )_\text{h}`$-curves for PbIn8% in Fig. 1(b) shows that the data for $`h=0.1`$ are, below $`\epsilon 0.1`$, appreciably affected by finite-field (or Prange) effects, but their $`\epsilon ^C`$ still remains unchanged well within the experimental uncertainties. A more detailed comparison with the theoretical results in this finite-field regime will be published elsewhere.

The $`\epsilon ^C`$-values for all the compounds studied here, included those of Fig. 1(b) and also the ones measured in Refs. , are presented in Fig. 2 as a function of $`\xi (0)`$. In this figure, Tl-2223 and Y-123 stand for the optimally-doped Tl2Ba2Ca2Cu3O10 and Y1Ba2Cu3O7-δ with $`\delta 0.05`$, LaSCO/0.14 and 0.25 stand for the optimally-doped La1.86Sr0.14CuO4 and, respectively, overdoped La1.75Sr0.25CuO4, and PbIn18% stands for the Pb-18at.%In alloy. As it may be clearly seen, $`\epsilon ^C`$ varies less than a factor 3, while these measurements cover almost two orders of magnitude in coherence lengths, in amplitudes of the fluctuation effects at $`\epsilon =0.01`$ (on both $`\mathrm{\Delta }M`$ and $`\mathrm{\Delta }\sigma `$), or (in the case of $`\mathrm{\Delta }M`$) in applied reduced magnetic fields \[$`hH/H_{c2}(0)`$ covers in these experiments the range $`2\times 10^3\stackrel{<}{_{}}h\stackrel{<}{_{}}2\times 10^1`$\]. Therefore, these results provide strong experimental evidence that the suppression of the superconducting coherence above a well-defined temperature $`T^C`$ in the normal state is due to a universal mechanism. These results do not exclude, indeed, a possible variation of $`\epsilon ^C`$ in extremely dirty superconductors or in the high reduced magnetic field region (when $`h1`$), where different non-local and pair-breaking effects could appear .

In conclusion, the experimental results and the analyses presented here suggest that the behaviour of the superconducting fluctuations at high reduced-temperatures is dominated by the uncertainty principle, which imposes a limit to the shrinkage of the superconducting wave function. These ideas provide a physical meaning to the “total-energy” cutoff heuristically introduced before to extend the applicability of the mean-field–like approximations to describe the superconducting fluctuations above $`T_C`$ from $`\epsilon 1`$ up to $`\epsilon ^C`$. It would be also interesting to extend these analyses to other superconductors, very in particular to the heavy fermions whose superconducting state coupling is based on antiferromagnetic spin fluctuations. Our present results may also have implications beyond the superconducting fluctuations issue. For instance, the striking fact that even in cuprates with different dopings (including the underdoped) $`\epsilon ^C`$ takes the value that we have directly obtained by using the BCS relationship between $`\xi (0)`$ and $`\xi _0`$ provides a constraint to any theoretical description of the superconducting state formation in these compounds, whose implications will deserve further analysis. The possible implications of these results on the so-called zero-dimensional superconductors, when $`\xi (T)`$ becomes bigger than the dimensions of the material in all directions, will also deserve further analysis. In fact, our present results suggest that the uncertainty principle constraint on the superconducting wave function will provide the last limit to the smallness of an isolated superconductor. They also suggest that the uncertainty principle must be taken into account when describing the short-wavelength thermal fluctuations around any phase transition with a quantum order parameter, so that the classical cutoff condition, $`k\stackrel{<}{_{}}\xi ^1(0)`$, must be substituted by a total-energy cutoff which takes into account the shrinkage at high reduced-temperatures of the quantum wave function.

This work is dedicated to the memory of Victoriano Reinoso, President of Unión Fenosa, whose support through a grant of Unión Fenosa (No. 0666-98) is gratefully acknowledged. Some of the data points summarized in Fig. 2 were obtained in samples supplied by J.A. Campá, A. Maignan, I. Rasines, A. Revcolevschi, and P. Wagner.