# Limits on Phase Separation for Two-Dimensional Strongly Correlated Electrons

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## Abstract

From calculations of the high temperature series for the free energy of the two-dimensional $`t`$-$`J`$ model we constuct series for ratios of the free energy per hole. The ratios can be extrapolated very accurately to low temperatures and used to investigate phase separation. Our results confirm that phase separation occurs only for $`J/t1.2`$. Also, the phase transition into the phase separated state has $`T_c0.25J`$ for large $`J/t`$.

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The Hubbard and $`t`$-$`J`$ models, though widely used to investigate high temperature superconductors, remain controversial when doped away from one electron per site. The possibility that doped holes do not form a uniform phase but instead phase separate into distinct high and low density regions on the lattice is an important issue that has proved difficult to settle. Phase separation for physical choices of model parameters would imply more complicated models of 2D strongly correlated electrons are required to describe high temperature superconductors. Stability of a uniform density phase would leave open the possibility that simple models contain the relevant physics without additional terms.

While experiments have clearly observed phase separation in a few high-$`T_c`$ systems, notably oxygen overdoped La<sub>2</sub>CuO<sub>4+δ</sub> with mobile interstitial oxygen atoms, phase separation does not seem to be a universal feature of the cuprates. However, the mechanism of phase separation causes holes to feel a net attraction, a possible precursor for the formation of stripe phases or superconductivity. Finding an attractive interaction for holes in models that have predominantly strong repulsive interactions is not easy, and all known possibilities deserve thorough investigation.

To investigate the properties of phase separation we have calculated the high temperature series for the 2D $`t`$-$`J`$ model free energy to 10th order in inverse temperature. The Hamiltonian for the $`t`$-$`J`$ model is

$$H=t\underset{ij,\sigma }{}\left(c_{i\sigma }^{}c_{j\sigma }+c_{j\sigma }^{}c_{i\sigma }\right)+J\underset{ij}{}\left(𝐒_i𝐒_j\frac{1}{4}n_in_j\right),$$
(1)   
where the sums are over pairs of nearest neighbor sites and the Hilbert space is restricted to states with no doubly occupied sites. The series is generated for a 2D square lattice.

To determine the stability of the uniform phase we would like to investigate the ground state energy per hole given by

$$e(\delta )=\frac{E_0(\delta )E_0^{AF}}{\delta },$$
(2)   
introduced by Emery, Kivelson and Lin. Here $`E_0(\delta )`$ is the ground state energy per site of the uniform phase for hole doping $`\delta `$ and $`E_0^{AF}=1.16944J`$ is the ground state energy per site for the Heisenberg model where $`\delta =0`$. If $`e(\delta )`$ is a monotonically increasing function of $`\delta `$ the uniform phase is stable. If $`e(\delta )`$ is constant or decreasing for a range of dopings the uniform phase is unstable for those values of $`\delta `$.

There are two main difficulties encountered in calculating $`e(\delta )`$ from numerical measurements (exact diagonalization, quantum Monte Carlo or Green’s function Monte Carlo) of $`E_0(\delta )`$. The first is that $`e(\delta )`$ requires the subtraction of two large numbers $`E_0(\delta )`$ and $`E_0^{AF}`$ to determine a small number which is then divided by $`\delta `$, another small number. Given statistical uncertainty in numerically determining $`E_0(\delta )`$ ($`E_0^{AF}`$ is essentially exact in comparison) this is a difficult task, especially for $`\delta 1`$. The second difficulty is that numerical calculations are done on small clusters. Systematic errors in $`E_0(\delta )`$ are tough to estimate without knowing the finite size scaling of the data and whether the cluster sizes considered are large enough to be in the scaling limit. In addition to these difficulties, phase separation is favored on small clusters for $`\delta 1`$. The reduction in ground state energy due to the kinetic energy of the holes, which disfavors phase separation, is not as large on a small cluster as it is for an infinite lattice. On a small cluster the electron system reduces its energy more through local interactions, which for the $`t`$-$`J`$ model are attractive interactions for antiparallel spins due to the $`J`$ term in the Hamiltonian.

High temperature series provide a means to avoid these difficulties. We generalize $`e(\delta )`$ to $`T>0`$ by

$$f(\delta ,T)=\frac{F(\delta ,T)F^{AF}(T)}{\delta },$$
(3)   
where we have replaced the ground state energy per site by the free energy per site and $`lim_{T0}f(\delta ,T)=e(\delta )`$. This replaces the difficulties mentioned above by the need to analytically continue the series to low temperatures. For $`J/t<1`$ and $`\delta 1`$ we find ratios $`f(\delta _2)/f(\delta _1)`$ for two closely spaced dopings $`\delta _1`$ and $`\delta _2`$ are the best quantities to extrapolate. Series for ratios can be calculated exactly from the series for $`F`$, avoiding the need to subtract two large approximate numbers. The series coefficients are also exact for an infinite lattice so we have no explicit finite size effects. The ratios are extrapolated using standard Padé approximants, but only after the exact series for a given ratio is calculated. The doping spacing we use is $`\mathrm{\Delta }\delta =0.025`$.

By extrapolating $`f(\delta _2)/f(\delta _1)`$ to $`T=0`$ we obtain estimates for $`e(\delta _2)/e(\delta _1)`$ in the uniform phase. Since high temperature series start at infinite temperature and only have information for the phase above a nonzero $`T_c`$, all of our results are for the uniform phase. A description of what happens if we try to extrapolate below $`T_c>0`$ is given below. Results for a range of dopings and $`J/t`$ values are shown in Fig. 1. For the parameters considered here $`e(\delta )<0`$ so that if $`\delta _2>\delta _1`$ and the system phase separates we should find $`e(\delta _2)/e(\delta _1)>1`$ if $`T_c>0`$ or $`e(\delta _2)/e(\delta _1)=1`$ if $`T_c=0`$. If the uniform phase is stable we have $`e(\delta _2)/e(\delta _1)<1`$. The 2D $`t`$-$`J`$ model phase separates into a phase with $`\delta =0`$ and a doped phase with $`\delta =\delta _0`$. For phase separation we therefore expect $`e(\delta )/e(0.01)1`$ immediately upon doping.

In Fig. 1, $`e(\delta )/e(0.01)<1`$ and falls monotonically with increasing $`\delta `$ for all $`J/t`$ shown, indicating no instability towards phase separation in the 2D $`t`$-$`J`$ model for $`J/t<1.2`$.

In Ref.  a variational argument is used to support the presence of phase separation for $`J/t1`$. A variational phase separated state was constructed from two pieces occupying different parts of the lattice: a Heisenberg antiferromagnet for the $`\delta =0`$ phase and a gas of spinless fermions for the $`\delta =\delta _0`$ phase. The energy of this state is then minimized with respect to $`\delta `$, giving $`E_0(\delta )=E_0^{AF}4t\delta (1\sqrt{B\pi J/t})`$ for the phase separated state and $`\delta _0=\sqrt{BJ/\pi t}`$, where $`B=1.16944/2=0.58472`$. This energy was then compared to ground state energy estimates for the uniform phase found by considering a single hole in an antiferromagnet. The energy for the phase separated state was found to lie below the unform state energy for small enough $`J/t`$, and since the variational energy lies above the true ground state energy the conclusion of Ref.  was that the phase separated state is stable. Extrapolating the result for a single hole to a finite density of holes assumes the energy bands remain rigid, a feature not obvious for a strongly correlated system.

In Fig. 2 we compare our estimates for the uniform ground state energy to the phase separated variational ground state energy at $`J/t=0.01`$. We find that our energies lie below the variational energy for $`\delta <\delta _0`$. Note that from this result we cannot conclude that the uniform state is stable, but only that the variational state discussed in Ref.  is not sufficient to show phase separation at $`J/t1`$.

In Fig. 3 we show the temperature dependence of $`f(0.02)/f(0.01)`$ for a range of $`J/t`$ values. Estimating the low $`T`$ behavior of this function is our only approximation. The weak temperature dependence for the ratio leads us to believe our results are reliable. The general trends of the data shown in Figs. 1 and 3 are due to the minimum in $`E_0(\delta )`$ moving to smaller $`\delta `$ as $`J/t`$ is increased, causing $`e(\delta )`$ to decrease in magnitude faster than $`e(0.01)`$, though for the parameters shown $`e(\delta )`$ and $`e(0.01)`$ remain negative. For values of $`J/t`$ larger than shown in Figs. 1 and 3 the ratio $`f(\delta _2)/f(\delta _1)`$ develops a spurious pole due to the crossing of $`F^{AF}`$ and $`F(\delta _1)`$ at $`T>0`$. This pole greatly degrades the accuracy of extrapolations of the ratios at lower temperatures. To investigate larger $`J/t`$ we need another method.

The chemical potential $`\mu =F/\delta `$ provides another means to investigate phase separation. We typically find $`\mu `$ is more difficult to extrapolate than $`f(\delta _2)/f(\delta _1)`$, with the error in the extrapolations for $`\mu `$ considerably larger than for the ratio. For $`J/t1.2`$ we do see $`\mu (\delta )`$ becoming quite flat for $`\delta 1`$, as expected for a first order phase transition into a phase separated state. As the temperature is lowered, $`\mu `$ near the critical point (critical doping $`\delta _c`$ and temperature $`T_c`$) becomes flat, giving a diverging compressibility $`\kappa `$ at the critical point. Results for $`\mu `$ are shown in Fig. 4. The flat region found in $`\mu (\delta )`$ can be used to estimate the boundary for phase separation. However, for larger $`\delta `$ distinguishing where the flat region ends is difficult, leading to errors in the position of the phase separation boundary.

Further evidence of phase separation at large $`J/t`$ can be found by directly extrapolating $`F(\delta ,T)`$ to estimate $`E_0(\delta )`$. Fig. 5 shows results for $`J/t=2.0`$. The characteristic signature of phase separation is the reversed curvature observed from $`\delta =0`$ to $`\delta 0.45`$. The reversed curvature of $`E_0(\delta )`$ (giving an unphysical negative compressibility) results from extrapolating the high temperature uniform phase $`F(\delta ,T)`$ through the $`T_c>0`$ phase transition for phase separation. If $`T_c=0`$ we would find instead that $`E_0(\delta )`$ became linear in $`\delta `$ in the phase separated region.

The reversed curvature shown in Fig. 5 indicates $`T_c>0`$, but $`T_c`$ is probably quite low. An indirect estimate of $`T_c`$ can be made at large $`J/t`$, above $`J/t=3.4367`$ where the 2D $`t`$-$`J`$ model phase separates at all densities into regions with $`\delta =0`$ and $`\delta =1`$. Here we know $`E_0(\delta )`$ for all $`\delta `$, since $`E_0(\delta )`$ is the linear interpolation between $`E_0(0)=1.16944J`$ and $`E_0(1)=0`$.

The ground state chemical potential in this parameter range is the constant slope of $`E_0(\delta )`$ with the value $`\mu /t=1.16944J/t`$. The chemical potential hits the bottom of the tight binding band at $`J/t=3.4367`$ and as $`J/t`$ is further reduced the gain in kinetic energy eventually limits the phase separated state to $`J/t1.2`$. In Fig. 6 we compare $`E_0`$ to $`F(T)`$ in the limit $`J/t\mathrm{}`$ with $`\delta =0.5`$.

Comparing the extrapolated $`F(T)`$ to $`E_0`$ we see they tend to cross at $`T0.25J`$. Since $`F(T)`$ must be less than $`E_0`$ and a monotonic function of $`T`$ this crossing cannot occur. We interpret the tendency to cross as a phase transition to phase separation with $`T_c0.25J`$.

Calculations for the 2D $`t`$-$`J`$ model currently give a wide range of minimum $`J/t`$ values for the presence of phase separation. Minimum $`J/t`$ values reported in the literature are 0, 0.5–0.6, and our result of 1.2. The latter results are in qualitative agreement in that there is a minimum $`J/t>0`$ for phase separation. The reasons for these differences are not clear at present. However, while statistical errors are well under control, systematic errors in ground state energy calculations due to small cluster sizes are much more difficult to control. Calculations investigating phase separation in the 2D Hubbard model find $`e(\delta )`$ equal to a constant for a range of dopings near half filling for the $`U=0`$ tight binding model. This spurious indication of phase separation is due to finite size effects and is reduced for larger clusters. Resolving the different reported results for phase sepraration will probably require significantly larger cluster sizes.

In conclusion, by using an analysis of the high temperature series for the free energy per hole $`f(\delta )`$ at different values of $`J/t`$ we find that phase sepration in the $`t`$-$`J`$ model is limited to $`J/t1.2`$. In addition, we find by indirect arguments that $`T_c0.25J`$ for the first order phase transition into the phase separated state. Combining this with the demonstration that phase separation can only occur at $`T=0`$ for the 2D Hubbard model on a square lattice supports the conjecture that the 2D Hubbard model does not phase separate for any positive $`U`$. Our results suggest phase separation in the 2D $`t`$-$`J`$ model is a classical phase transition similar to a lattice gas with an attractive interaction and that phase separation is not important for physical choices of the $`t`$-$`J`$ model parameters.

This work was supported in part by a faculty travel grant from the Office of International Studies at The Ohio State University (WOP), the Swiss National Science Foundation (WOP) and by EPSRC Grant No. GR/L86852 (MUL). WOP thanks the ETH-Zürich for hospitality while part of this work was being completed.

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