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# Pathology of Schwinger boson mean field theory for Heisenberg spin models

## I Introduction

Schwinger boson representation is by now a well known tool in the study of quantum spin systems . In this method, each spin operator is represented by two Schwinger bosons. In contrast to Holstein-Primakoff bosons , the Schwinger boson representation of spin operators does not involve square roots. Furthermore, while the vacuum state of Holstein-Primakoff bosons has to be a broken symmetry state, this is not the case for Schwinger bosons. Instead, long-ranged order (LRO) is a result of condensation of the Schwinger bosons . Thus, using Schwinger bosons allows one to naturally address both the magnetically disordered and ordered states.

Using the Schwinger boson representation, the quantum spin Hamiltonian is mapped onto an interacting boson Hamiltonian, which can then be approximated by a self-consistent non-interacting Hamiltonian using mean field theory (MFT). In such a mean field theory, a non-zero mean field amplitude corresponds to short-ranged order (SRO). Long range order exists only if for a given temperature, the mean field Hamiltonian gives rise to Bose condensation. The ability of the mean field theory to address both short-ranged and long-ranged order is perhaps its most appealing feature, especially for 1D and 2D systems, where exact solutions has shown that LRO is destroyed at any finite temperature. For the Heisenberg ferromagnetic or antiferromagnetic Hamiltonian on a d-dimensional hypercubic lattice, the results reported in literature are briefly summarized as follows. In both 1D and 2D, in agreement with exact results, there is no LRO at any finite temperature. However, SRO persists until a certain temperature is exceeded . In 3D, LRO is stable at low temperature, and there is a continuous phase transition into the SRO state at some critical temperature. Within Schwinger boson MFT (SBMFT), the order-disorder transition has the usual mean field exponents .

In this paper, we re-examine the SBMFT for the Heisenberg spin Hamiltonian on the 3D cubic lattice. We find that, provided the spin $`S`$ is greater than some critical value $`S_c`$ $`(<1/2),`$ the previously reported mean field solution that exhibits a continuous phase transition for magnetic LRO is actually an unstable solution corresponding to a local maximum of the free energy. Instead, the minimum free energy solution shows a first order transition. Since it is well established that the Heisenberg Hamiltonian has a continuous transition in 3D, our analysis raises serious question about the applicability of the SBMFT in 3D. Furthermore, the first order transition is into a state with zero mean field amplitude, i.e., without any correlation. Thus, the supposed advantage of SBMFT of being able to describe SRO does not actually exist. These pathologies of the SBMFT are not restricted to 3D, but should appear whenever the LRO can be destroyed by tuning some parameter. An example of which is the bilayered Heisenberg antiferromagnet at $`T=0`$ where as the inter-layer coupling is increased, SBMFT also shows a first order transition into the uncorrelated state .

The rest of this paper is organized as follows. In Section II and III, we will discuss the SBMFT solutions for the Heisenberg ferromagnet and antiferromagnet separately, showing that the same pathologies are seen in both cases. These results will be summarized in Section IV, where we will also discuss their relevance to the bilayered Heisenberg antiferromagnet.

## II Ferromagnetic Heisenberg Model

In this section we discuss the SBMFT for the FM Heisenberg model. We first briefly review the Schwinger boson representation and its mean field equations . We then discuss the mean field solutions of the model with emphasis on 3D.

We study a spin-S Heisenberg ferromagnet in a d-dimensional hypercubic lattice with periodic boundary conditions,

$`H=J{\displaystyle \underset{<i,j>}{}}S_iS_j,`$ (1)
where the exchange constant $`J>0`$ and the sum is over all the nearest-neighbor pairs on the lattice. In the Schwinger boson representation, a spin operator is represented by two types of bosons,

$`S_i^z={\displaystyle \frac{1}{2}}(a_i^{}a_ia_i^{}a_i),`$ (2)
$`S_i^+=a_i^{}a_i,S_i^{}=a_i^{}a_i,`$ (3)
These bosons should satisfy the constraints in their Fock space as follows, $`_\sigma a_{i\sigma }^{}a_{i\sigma }=2S`$, with $`2S=1,\mathrm{\hspace{0.17em}2},\mathrm{}`$ for physical systems. By introducing a bond operator, $`B_{ij}^{}=\frac{1}{2}_\sigma a_{i\sigma }^{}a_{j\sigma }`$, the SU(2) FM Heisenberg Hamiltonian can be written as,

$`H_{FMB}=2J{\displaystyle \underset{<ij>}{}}:B_{ij}^{}B_{ij}:+{\displaystyle \frac{NzJ}{2}}S^2+{\displaystyle \underset{i}{}}\lambda _i({\displaystyle \underset{\sigma }{}}a_{i\sigma }^{}a_{i\sigma }2S).`$ (4)
In the above Eqn., $`::`$ denotes a normal ordering of the bosonic operators, N is the number of sites in the lattice, and $`z=2d`$ is the nearest neighbor coordinate. A Lagrangian multiplier field $`\lambda _i`$ for the constraint on site $`i`$ is introduced. Note that the FM Heisenberg model is now transformed to an interacting boson model.

To proceed further, a bond mean field amplitude $`B=<B_{ij}^+>=<B_{ij}>`$, assumed to be real and uniform, is introduced. Neglecting fluctuations, the following non-interacting mean field Hamiltonian is obtained.,

$`H_{MF}=\lambda {\displaystyle \underset{i}{}}({\displaystyle \underset{\sigma }{}}a_{i\sigma }^{}a_{i\sigma }2S)2J{\displaystyle \underset{ij}{}}B(B_{ij}^{}+B_{ij})+{\displaystyle \frac{NzJ}{2}}S^2+NzJB^2,`$ (5)
In $`H_{MF}`$ the local constraint at every site is replaced by a global one, and a non-zero value of B indicates  short-range spin-spin correlation. The mean field Hamiltonian can be diagonalized, and we obtain

$`H_{MF}={\displaystyle \frac{NzJ}{2}}S^2+NzJB^22S\lambda N+{\displaystyle \underset{\stackrel{}{k},\sigma }{}}\omega _\stackrel{}{k}a_{\stackrel{}{k}\sigma }^{}a_{\stackrel{}{k}\sigma },`$ (6)
where the energy dispersion is given by $`\omega _\stackrel{}{k}=JzB(ϵ_\stackrel{}{k}+\mathrm{\Lambda })`$, with $`ϵ_\stackrel{}{k}=\frac{1}{z}_\stackrel{}{\delta }(1e^{i\stackrel{}{k}.\stackrel{}{\delta }})`$, and $`\mathrm{\Lambda }=\frac{\lambda }{JBz}1.`$

The free energy per site is then given by

$`f={\displaystyle \frac{JS^2z}{2}}+zJB^22S\lambda {\displaystyle \frac{2}{\beta N}}{\displaystyle \underset{\stackrel{}{k}}{}}\mathrm{log}({\displaystyle \frac{1}{1e^{\beta \omega _\stackrel{}{k}}}}),`$ (7)
where $`\beta =\frac{1}{k_BT}`$, with $`k_B`$ the Boltzmann constant and $`T`$ the temperature. The amplitudes of the mean fields $`B`$ and $`\lambda `$ are obtained by minimizing the free energy, which leads to two coupled mean field eqns.,

$`S={\displaystyle \frac{1}{N}}{\displaystyle \underset{\stackrel{}{k}}{}}{\displaystyle \frac{1}{e^{\stackrel{~}{\beta }(ϵ_\stackrel{}{k}+\mathrm{\Lambda })}1}},`$ (8)
$`B^2={\displaystyle \frac{B}{N}}{\displaystyle \underset{\stackrel{}{k}}{}}{\displaystyle \frac{1ϵ_\stackrel{}{k}}{e^{\stackrel{~}{\beta }(ϵ_\stackrel{}{k}+\mathrm{\Lambda })}1}},`$ (9)
where $`\stackrel{~}{\beta }=1/k_B\stackrel{~}{T}`$, and $`\stackrel{~}{T}=T/(JzB)`$ acts as an effective temperature. In these eqns., $`\mathrm{\Lambda }`$ may be viewed as an effective chemical potential. Since $`ϵ_\stackrel{}{k}0`$, we have $`\mathrm{\Lambda }0`$. Magnetic long range order corresponds to Schwinger boson condensation at $`\stackrel{}{k}=0`$ . Since bosons do not condense at finite temperature in 1D or 2D, the 1D model and the 2D model are disordered at any temperature. In three and higher dimensions, one expects a finite critical temperature $`T_C`$, below which SBMFT gives a magnetic ordered state.

To study the possible magnetically ordered phase, the Schwinger boson condensate density $`\rho =<a_{\stackrel{}{k}=0,\sigma }^{}a_{\stackrel{}{k}=0,\sigma }>/N`$ is introduced, and the coupled mean field eqns. are rewritten as,

$`S=\rho +{\displaystyle \frac{d^d\stackrel{}{k}}{(2\pi )^d}\frac{1}{e^{\stackrel{~}{\beta }(ϵ_\stackrel{}{k}+\mathrm{\Lambda })}1}},`$ (10)
$`B^2=B(S{\displaystyle \frac{d^d\stackrel{}{k}}{(2\pi )^d}\frac{ϵ_\stackrel{}{k}}{e^{\stackrel{~}{\beta }(ϵ_\stackrel{}{k}+\mathrm{\Lambda })}1}}).`$ (11)
In the Bose condensed state, $`\rho >0`$, $`\mathrm{\Lambda }=0`$, and $`B0`$; In the disordered state, $`\rho =0`$, and $`\mathrm{\Lambda }>0`$. Sarker et al.  determined the critical temperature by requiring $`\mathrm{\Lambda }=0`$ and $`\rho =0`$. This transition point will be labeled as $`\mathrm{`}\mathrm{`}a\mathrm{`}\mathrm{`}`$, with the effective temperature $`\stackrel{~}{T}_a`$. By expanding equations 10 and 11 about $`\stackrel{~}{T}_a`$, the transition was determined to be continuous with mean field exponents. Upon re-examination of the mean field equations, we have, however, found the transition point $`\stackrel{~}{T}_a`$ to be physically inaccessible if the spin $`S`$ is greater than some $`S_C`$. To understand this, we note that these equations are well-behaved in term of $`\stackrel{~}{T}`$. For example, the quantity $`B`$ is smooth and monotomically decreasing as $`\stackrel{~}{T}`$ increases as one would expect. This is shown in fig. 1 for the case of $`S=1/2`$. At $`\stackrel{~}{T}=0`$, $`B`$ is finite, and $`\mathrm{\Lambda }=0`$. As $`\stackrel{~}{T}`$ increases, $`B`$ decreases monotonously. For $`\stackrel{~}{T}>\stackrel{~}{T}_a`$, the state is disordered with $`\rho =0`$; And at $`\stackrel{~}{T}<\stackrel{~}{T}_a`$, the state is ordered with $`\rho >0`$. On the other hand, the physical temperature $`T=JzB\stackrel{~}{T}`$, and since $`B`$ decreases with increasing with $`\stackrel{~}{T}`$, it is possible for $`T`$ to decrease as $`\stackrel{~}{T}`$ increases. This is shown in fig. 2. This would mean for example that $`B`$ would increase with increasing $`T`$, which is physically nonsensical. If the second order transition point $`\stackrel{~}{T}_a`$ belongs to such an unphysical $`\stackrel{~}{T}`$, it will not be accessible.

In ref.2, it was implicitly assumed that the mean field eqns. 9 and 10 have a two branch structure, so that at high $`T`$, $`B=0`$ is the only solution, but below some $`T^{}`$, a second solution with $`B0`$ appears. Instead, mean field eqns. actually have three branches of solutions for $`B`$ or $`\stackrel{~}{T}`$ as functions of $`T`$. One is the trivial solution (upper branch), $`B=0`$, or $`\stackrel{~}{T}\mathrm{}`$ at all $`T`$. The second branch solutions (lower branch) exist for all $`T<T_t`$, with $`\stackrel{~}{T}`$ monotomically increasing with $`T`$. For $`T_g<T<T_t`$, there is yet a third branch of solutions (middle branch), where $`\stackrel{~}{T}`$ goes to $`\mathrm{}`$ at $`T=T_g`$ and decreases as $`T`$ increases until it merges and terminates with the second branch at $`T=T_t`$.

The solutions to the mean field equations correspond to extrema of the free energy. For $`T<T_t,`$ there are more than one solutions, and the one giving the lowest free energy should be chosen. From the structure of the $`\stackrel{~}{T}`$ vs. $`T`$ curve, we can deduce that as $`T`$ is reduced, the free energy functional should behave as follows. For $`T>T_t,`$ there is only one extremum, which is at $`B=0.`$ Between $`T_t`$ and $`T_g,`$ where there are three solutions, there is a local minimum at $`B=0,`$ a local maximum at $`B=B_3`$ (middle branch) and a secondary local minimum at $`B=B_2`$ (lower branch), with $`B_2>B_3.`$ As $`T`$ decreases in the regime, $`B_3`$ moves towards $`0`$ and at $`T=T_g,`$ the curvature at $`B=0`$ changes sign and becomes a local maximum below $`T_{g,}`$ leaving $`B_2`$ as the only minimum. Given this, at some temperature $`T_b`$ between $`T_g`$ and $`T_t,`$ the free energy at $`B_2`$ will become lower than at $`B=0.`$ Thus, at $`T_{b,}`$ $`B`$ will take a jump from $`0`$ to a finite value of $`B_2.`$ In Figs. 3-5, we show plots of free energy $`f`$ vs. $`B`$ to illustrate the above. In these plots, the $`f(B)`$ is calculated by solving eq. 10 for $`\mathrm{\Lambda }`$ with $`B`$ as a variable and then evaluating $`f`$ in eq. 7.

Thus, we see that in general, SBMFT gives a first order transition in $`B.`$ Since $`B`$ is a measure of the short range order, the transition in $`B`$ is fictitious and whether it is first order or continuous is not of any real significance. More importantly is where the Bose condensation transition occurs relative to this transition. Since in terms of $`\stackrel{~}{T},`$ eq. 10 is just that for Bose-Einstein condensation, $`\stackrel{~}{T}_aS^{2/d}`$ for $`d>2`$, as $`S0,`$ and hence so does the physical temperature $`T_a`$. Thus for small $`S,`$ Bose condensation occurs at a temperature where the lowest branch is the stable solution, and the continuous transition at $`\stackrel{~}{T}_a`$ accessible within SBMFT. As $`S`$ increases, however, $`\stackrel{~}{T}_a`$ continues to increase and for $`S>S_c0.15,`$ $`\stackrel{~}{T}_a>\stackrel{~}{T}_b,`$ where the solution at the lower branch becomes meta-stable. At even larger $`S`$ (e.g. $`S=1/2`$), $`\stackrel{~}{T}_a`$ becomes $`>\stackrel{~}{T}_t,`$ and the solution becomes unstable. Either way, for $`S>S_c,`$ as the temperature increases from zero, the system undergoes a discontinuous transition at $`T_b`$ from the LRO state with finite condensate density to the uncorrelated state with $`B=0.`$ There are two problems with this. The first is that result of a first order transition in magnetic long range order for the Heisenberg model in 3D is wrong. The second is that one of the major advantages of SBMFT is supposedly its applicability to both LRO and SRO state. But in fact, the stable solution is either completely uncorrelated or has LRO, just like standard Bethe-Weiss MFT.

## III Antiferromagnetic Heisenberg Model

In this section, we discuss the SBMFT for the AFM Heisenberg model described by the Hamiltonian,

$`H=J{\displaystyle \underset{<i,j>}{}}S_iS_j,`$ (12)
where $`J>0`$, and all other notations are the same as in the previous section for the FM case. We find that the same pathologies in the SBMFT solution for FM model are present also in the AFM model.

The hypercubic lattice is divided into two sub-lattices A and B. In a nearest neighbor pair $`<ij>`$, $`iA`$ and $`jB`$. As in the FM model, two Schwinger bosons $`a_{i\sigma }`$ with $`\sigma =\pm 1`$, at each site $`i`$, and a bond field $`A_{ij}^{}=\frac{1}{2}_\sigma \sigma a_{i\sigma }^{}a_{j\sigma }^{}`$ are introduced. $`A_{ij}`$ is anti-symmetric with respect to the interchange of $`i`$ and $`j`$. A spin rotation by $`\pi `$ about the y-axis is made at all the sites $`j`$ on the sub-lattice B, so that $`a_ja_j`$, $`a_ja_j`$. The bond operator is then transformed as $`A_{ij}^{}A_{ij}^{}=\frac{1}{2}_\sigma a_{i\sigma }^{}a_{j\sigma }^{}`$. This canonical transformation preserves the constraint $`_\sigma a_{i\sigma }^{}a_{i\sigma }=2S=0,1,2,\mathrm{}..`$

In terms of bosonic operators, the AFM Heisenberg model reads,

$`H={\displaystyle \frac{J}{2}}{\displaystyle \underset{<ij>}{}}(A_{ij}^{}A_{ij}2S^2).`$ (13)
The mean field equations of the AFM model may be derived similarly to the FM model. A global Lagrangian multiplier $`\lambda `$ to replace the constraint on every site, and a real and uniform mean field amplitude $`<A_{ij}>=<A_{ij}^{}>=A`$ are introduced. $`A0`$ describes short-range AFM correlations. After some algebra, the mean field Hamiltonian can be written as:

$`H_{MF}=E_0+\lambda {\displaystyle \underset{k,\sigma }{}}a_{k\sigma }^{}a_{k\sigma }{\displaystyle \frac{JAz}{2}}{\displaystyle \underset{k,\sigma }{}}\gamma _k(a_{k\sigma }^{}a_{k\sigma }^{}+h.c),`$ (14)
with $`\gamma _\stackrel{}{k}=\frac{1}{z}_\delta e^{i\stackrel{}{k}\stackrel{}{\delta }}=1ϵ_\stackrel{}{k}`$, and $`E_0=\frac{1}{2}NzJS^22\lambda NS+JA^2Nz`$.

$`H_{MF}`$ is diagonalized by using the standard Bogoliubov transformation, yielding

$`H_{MF}=E_0\lambda N+{\displaystyle \underset{k}{}}\omega _k(\alpha _k^{}\alpha _k+\beta _k^{}\beta _k+1),`$ (15)
where $`\omega _\stackrel{}{k}=(\lambda ^2(JzA\gamma _\stackrel{}{k})^2)^{1/2}`$. To find the optimal values of the mean fields, the free energy is differentiated with respect to $`A`$ and $`\lambda `$, and the SBMFT equations for the AFM model are obtained,

$`S+{\displaystyle \frac{1}{2}}={\displaystyle \frac{1}{N}}{\displaystyle \underset{k}{}}{\displaystyle \frac{\mu }{(\mu ^2\gamma _k^2)^{1/2}}}\left({\displaystyle \frac{1}{e^{\stackrel{~}{\beta }(\mu ^2\gamma _k^2)^{1/2}}1}}+{\displaystyle \frac{1}{2}}\right),`$ (16)
$`A^2={\displaystyle \frac{A}{N}}{\displaystyle \underset{k}{}}{\displaystyle \frac{\gamma _k^2}{(\mu ^2\gamma _k^2)^{1/2}}}\left({\displaystyle \frac{1}{e^{\stackrel{~}{\beta }(\mu ^2\gamma _k^2)^{1/2}}1}}+{\displaystyle \frac{1}{2}}\right),`$ (17)
where we have defined an effective inverse temperature $`\stackrel{~}{\beta }=JAz\beta `$ and an effective chemical potential $`\mu =\frac{\lambda }{JAz}`$. To describe the possible Schwinger boson condensed state, condensation density $`\rho `$ is introduced similar to that in the FM model, and the summations are replaced by integrals. The mean field eqns. become,

$`S+{\displaystyle \frac{1}{2}}=\rho +{\displaystyle \frac{d^d\stackrel{}{k}}{(2\pi )^d}\frac{1}{(\mu ^2\gamma _\stackrel{}{k}^2)^{1/2}}\left(\frac{1}{e^{\stackrel{~}{\beta }(\mu ^2\gamma _k^2)^{1/2}}1}+\frac{1}{2}\right)},`$ (18)
$`A^2=A(\rho +{\displaystyle \frac{d^d\stackrel{}{k}}{(2\pi )^d}\frac{\gamma _\stackrel{}{k}^2}{(\mu ^2\gamma _\stackrel{}{k}^2)^{1/2}}\left(\frac{1}{e^{\stackrel{~}{\beta }(\mu ^2\gamma _\stackrel{}{k}^2)^{1/2}}1}+\frac{1}{2}\right)}).`$ (19)
We now discuss the solutions of these eqns. Note that $`\gamma _\stackrel{}{k}^21`$, so we have $`\mu 1`$. Similar to the FM case, $`\rho =0`$ and $`\mu >1`$ in the disordered phase, and $`\rho >0`$ and $`\mu =1`$ in the Schwinger boson condensation state, which corresponds to the Neel ordering phase of the spin system. The results are very similar to those for the 3D FM model.

The solutions for the mean field equations are smooth and monotonic functions of the effective temperature $`\stackrel{~}{T}`$, but not of the physical temperature $`T`$. In Fig. 6, we show the calculated $`\stackrel{~}{T}`$ as a function of $`T`$ from the mean field eqns. for a typical spin $`S=1/2`$. There are three branches of solutions in $`\stackrel{~}{T}`$. The $`A=0`$ branch, and a middle and a lower branches. The Bose condensation point $`\mathrm{`}\mathrm{`}a\mathrm{`}\mathrm{`}`$ (where $`\mu =1`$ and $`\rho =0`$) is again on the upper branch corresponding to a maximum in the free energy. We have calculated the free energy and found that the stable mean field solution jumps from a high $`T`$ phase in the $`A=0`$ branch to a low $`T`$ phase in the lower branch with a finite condensation density at a temperature $`T=T_b<T_a`$. Therefore, the transition for LRO is first order. The qualitative feature of the free energy as a function of $`A`$ is similar to those in Fig. 3-5 for the FM case. The critical spin for which $`T_a=T_b`$ for the AFM model is found to be $`S_C0.32`$, larger than that in the FM model, but still substantially smaller than $`1/2`$. For $`S>S_C`$ the ordering transition within SBMFT is first order and for $`S<S_C`$, the transition is second order.

## IV Conclusions

We have re-examined the Schwinger boson MFT for quantum spin systems and found that for both the FM and AFM Heisenberg Hamiltonian, the mean field equations possess in general three branches of solutions in the intermediate temperature regime. As a consequence, the system in 3D undergoes a first order transition from the ordered state to the completely uncorrelated state unless the spin $`S`$ is very small. In addition to erroneously predicting a first order transition in magnetic ordering, there is no stable solution with finite SRO without LRO, the existence of which is supposed to be one of the advantages of SBMFT over Bethe-Weiss MFT or spin wave theory.

The three branch structure of the mean field solutions is not restricted to 3D. It is the origin of the reported discontinuous jump in the short-range MF amplitude $`A`$ for the Heisenberg AFM on 2D square lattice as the temperature is increased . For the 2D square lattice, however, the effective temperature for Bose condensation $`\stackrel{~}{T}_a=0,`$ which means $`\stackrel{~}{T}_a<\stackrel{~}{T}_b`$ for all $`S.`$ As a result, SBMFT is capable in that case of describing the SRO state at low temperature. It should not be assumed though that the pathologies associated with SBMFT reported in this paper is only relevant for $`d>2.`$ In fact, it will apply whenever the LRO state is destroyed by tuning some parameter if that parameter is sufficiently large. One example of this is the bilayered Heisenberg AFM Hamiltonian in 2D, which received interest a few years ago due to its relevance to YBCO . In the bilayered system, the in-plane AF magnetic LRO is destroyed by sufficiently large inter-layer coupling which favors having inter-plane neighbors forming singlets . Using SBMFT, Ng et al  found for $`S>S_c0.35`$, the transition is first order from finite condensate density to the state of disconnected inter-plane singlets with zero in-plane correlations. This result contradicted the hypothesis that the 2D bilayered AFM at $`T=0`$ is in the same universality class as the 3D non-linear sigma model at finite $`T`$, a hypothesis partially confirmed by finite sized numerical calculations for $`S=1/2`$ . One possibility is that SBMFT is qualitatively correct, but that the value of $`S_c`$ calculated is too small. Subsequently, Gelfand et al  provided further evidence that the transition for arbitrary $`S`$ is continuous and that the SBMFT prediction of first order transition is incorrect. However, it was not clear why SBMFT gave such a qualitatively incorrect result. From the present work, we can now understand that the first order transition reported there is an artifact of the same pathologies of the SBMFT reported in this paper.

Finally, while we have focused on SU(2) Heisenberg Hamiltonian in this paper, the results are a consequence of the structure of the mean field equations, and therefore will be valid for SU(N) generalization of the Heisenberg Hamiltonian for which the SBMFT approach above  can be applied.

## V Acknowledgments

We acknowledge useful discussions with T. K. Ng and K. K. Ng. This work was supported in part by DOE grant No. DE/FG 03-01ER 45687 and by Chinese Academy of Science.


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# Structural, magnetic and electrical properties of single crystalline La1-xSrxMnO3 for 0.4 < x < 0.85

## I Introduction

The fascinating phase diagrams of the doped maganites result from a subtle interplay of spin, charge, orbital and lattice degrees of freedom. In La1-xSrxMnO3 the main body of experimental investigations has been carried out for Sr concentrations $`x<0.5`$. This partly has been due to the fact that colossal magnetoresistance effects vonHelm93\_Chah93  show up around $`x=0.3`$, which in the beginning of the research seemed to be rather promising for application. On the other hand single crystals for $`x>0.5`$ are hard to grow and hence, only rarely have been investigated.

Already at low concentrations ($`x<0.5`$) a rather complex phase diagram evolves, which is due to the fact that in addition to super-exchange (SE) and double-exchange (DE) interactions, charge order (CO) and structural effects via orbital ordering are of outstanding importance. For $`x<0.2`$, a long-range cooperative Jahn-Teller (JT) effect establishes orbital order (OO), which finally determines the antiferromagnetic (AFM) spin state of A-type in the pure compound at low temperatures. With increasing Sr doping $`(x<0.1)`$ a ferromagnetic (FM) component evolves in addition to the AFM order of subsequent planes which is explained in terms of electronic phase separation Dagot01  or, following the time-honored ideas of de Gennes deGen60 , in terms of a canted AFM (CA) state. However, within this model of competing SE and DE interactions clearly the importance of lattice distortions has to be taken into account.Millis  On further increasing $`x`$ $`(0.1x0.17)`$, it seems clear that a new type of orbital order, probably connected with CO, determines the low-temperature insulating ferromagnet (FM) around $`x=0.125`$.Endoh99 ; Parask00 ; Niem99  Finally, for Sr concentrations $`x>0.17`$ the long-range JT distortions become suppressed and a ferromagnetic metal evolves below the FM phase transition which is stable almost up to half filling.

After the early work on La:SrMnO3 which is summarized by Goodenough and LongoGoode70 , the complex phase diagram has been studied by many groups and a more or less coherent picture can be deduced from the variety of experimental results reported.Parask00 ; Urus95 ; Yama96 ; Kawa96 ; Zhou97  From the systems with narrower bandwidth (e.g. $`L_{1x}A_x`$MnO3 with $`L`$ = Nd, Pr, Sm and $`A`$ = Ca, Sr Maez98 ; Mart99 ) an extreme asymmetry between the hole and electron doped regimes is well known and it seems highly interesting also to investigate the electron doped La1-xSrxMnO3. However, for $`x>0.5`$ much less experimental information is available.

Structural, resistivity and magnetization results for $`x=0.5`$ and 0.54 were reported by Akimoto et al. Akim98  For $`x=0.54`$ they reported an orthorhombic ($`Pbnm`$) nuclear and an A-type AFM structure at 10 K. Results for similar Sr concentrations $`0.5<x<0.6`$ were published by Moritomo et al. Morit98  On increasing $`x`$, the crystal symmetry changes from rhombohedral ($`R3c`$) to pseudotetragonal at $`x=0.54`$ with $`ab<c\sqrt{2}`$. For concentrations around $`x=0.55`$, a metallic AFM phase, with A-type spin structure at low temperatures, is followed by a FM metallic (M) state at elevated temperatures.Morit98  Polycrystalline La1-xSrxMnO3 has been investigated by Fujishiro et al. Fuji98  by magnetization, electrical resistivity and ultrasonic techniques. They arrive at a different phase diagram, with an insulating (I) state for all concentrations $`x>0.5`$. Similar findings were reported by Patil et al. Patil00  who also investigated ceramic samples for $`0.46x0.53`$. They found a sequence of magnetic and charge-order transitions and interpreted their results in terms of electronic phase separation.

Further interest in the overdoped manganites arises from the fact that for the insulating regions of the phase diagram electronic phase separation in form of stripes Rada99  or bistripes Mori98  has been reported. This special form of CO certainly is driven by OO.Khom01  Also theoretically the phase diagrams of the doped manganites have been investigated in great detail.Dagot01 ; Maez98 ; Khom01 ; Held98 ; Brink99  Specifically in Ref. Brink99  the overdoped regime was investigated using DE within degenerate orbitals. Depending on the bandwidth, on increasing electron doping a sequence of spin structures of type A, C, A and F has been predicted.Brink99 ; Good63

In order to clarify the situation and to shed some light on the complex and complete ($`x,T`$)-phase diagram in La1-xSrxMnO3 we grew a series of single crystals for concentrations ($`0.4<x<0.85`$). We were not able to grow crystals with higher Sr concentrations. The reason seems to be rather clear as SrMnO3 reveals a hexagonal crystal structure and obviously there exists a miscibility gap for concentrations close to pure SrMnO3. In the following we present detailed structural, magnetic susceptibility, magnetization and electrical resistivity results for the complete series of crystals. From the results we construct a detailed phase diagram. Polycrystalline SrMnO3 has been investigated to complete the phase diagram. These experiments are a continuation of earlier work on crystals with low Sr doping levels which has been published previously Parask00  and has been included to present the complete ($`x,T`$)-phase diagram of La1-xSrxMnO3 for $`0x1`$.

## II Experimental Details

La1-xSrxMnO3 single crystals were grown by a floating-zone method with radiation heating similar to the techniques as described in Ref.Balba96  For these crystals with Sr concentrations $`x0.5`$, different atmospheric conditions ranging from air atmosphere to excess oxygen pressure up to 50 atm were tested to optimize the growth process. Nevertheless an uncertainty in the control of the concentration $`x`$ of up to 2% cannot be ruled out. To complement the phase diagram pure SrMnO3 has been grown using standard ceramic techniques. Powder x-ray diffraction measurements were performed utilizing Cu-Kα radiation with $`\lambda =0.1541`$ nm.

The magnetic susceptibility and magnetization were measured using a commercial superconducting quantum interference device (SQUID) magnetometer ($`1.5<T<400`$ K, $`H50`$ kOe) and an ac-magnetometer which operates up to magnetic fields of $`H=140`$ kOe. The electrical resistance has been measured using standard four-probe techniques in home-built cryostats and ovens from 1.5 K to 600 K.

## III Results and discussion

### III.1 X-ray diffraction

To demonstrate the quality of the single crystals under investigation, we powdered pieces of the single crystals used for magnetic and transport measurements and performed detailed Rietveld refinements of the diffraction profiles for samples with Sr concentrations $`0.55x0.85`$ at room temperature. Fig. 1 shows the diffraction profiles, the refinement and the difference pattern for $`x=0.55`$ (upper panel) and $`x=0.75`$ (lower panel). First of all we want to stress that all reflections can be indexed and no impurity phases are apparent above the background level, even no spurious amount of SrMnO3 which has been reported in all previous investigations.Goode70 ; Akim98 ; Morit98 ; Fuji98  At first sight one recognizes that with increasing Sr concentration $`x`$ the crystals almost approach cubic symmetry which is expected for concentrations with a tolerance factor close to 1. This is demonstrated by the insets in Fig. 1, showing the splitting of the 220/004 reflections which provides direct experimental evidence of the $`c/a`$ ratio and hence on the tetragonal distortion. For $`x=0.55`$ a clear splitting of the reflections can be detected, while for $`x=0.75`$ no apparent splitting is visible and a splitting can only be derived via the broadening of the reflection in a detailed Rietveld refinement with well defined resolution parameters. Hence the samples near $`x=0.8`$ are very close to cubic symmetry.

From the Rietfeld refinement we determined the lattice constants of the samples under investigation. The results are listed in Tab. 1. At room temperature the structure changes from rhombohedral (R) at $`x=0.5`$ to tetragonal (T) at $`x=0.55`$ and finally to hexagonal (H) close to pure SrMnO3. We would like to recall that SrMnO3 was only prepared in ceramic form and we were not able to grow crystals beyond strontium concentrations $`x=0.85`$. The room-temperature tetragonal phase extends over a broad concentration range, with a significant change of the tetragonal distortion. For $`x=0.55`$ we find a value of $`c/\sqrt{2}a1.01`$. Note that for this concentration ferromagnetism is established already at room temperature. On increasing $`x`$ this ratio is reduced yielding values close to 1, however now in the paramagnetic phase, but still on the verge of magnetic order. It is clear that the $`c/a`$ ratio will strongly depend on the orbital structure, i.e. whether the orbitals are aligned as $`d_{x^2y^2}`$ or as $`d_{3z^2r^2}`$. However, systematic temperature dependent x-ray diffraction measurements are needed to arrive at final conclusions. From preliminary temperature-dependent x-ray diffraction experiments (down to 80 K) we found that for $`0.5<x<0.7`$ the symmetry is lowered and the structure changes into a monoclinic (Mc) phase characterized by space group $`P2_1/m`$. Fig. 2 illustrates the evolution of superlattice reflections for $`x=0.6`$ due to the monoclinic distortion on cooling. At the boundaries of this monoclinic low-temperature phase for $`x0.5`$ and $`x0.7`$ we suggest that the system enters into a structurally mixed phase where the Mc phase coexists with a R and T phase, respectively. However a more detailed evaluation is necessary to analyze these two-phase regions. A detailed report on the structural properties will be given elsewhere.Krim02  It should be noticed that a low-temperature monoclinic phase with space group $`P2_1/m`$ has been established in the doped manganites La0.5Ca0.5MnO3 and Pr0.6(Ca1-xSrx)0.4MnO3, as well as in Pr0.5Sr0.5MnO3.Rad97 ; Lee98 ; Kawa97  Furthermore, the presence of monoclinic domains within an orthorombic matrix has been reported for Pr0.7Ca0.25Sr0.05MnO3 and Pr0.75Sr0.25MnO3 on the basis of high-resolution microscopy.Her96

### III.2 Transport properties

Fig. 3 shows the temperature dependence of the electrical resistivity below room temperature. Clearly La1-xSrxMnO3 reveals a metallic conductivity for $`0.4<x<0.6`$. These findings differ from those reported by Patil et al. Patil00  for concentrations close to $`x=0.5`$ obtained from ceramic samples, where the resistivity increases towards low temperatures. From optical measurements these authors find indications for an anisotropy of the conductivity. This fact together with possible grain effects in ceramic samples could explain the different results.

For Sr concentrations $`x=0.625`$ and 0.7 a significant increase of the resistivity occurs below 250 K. Finally in the samples with $`x>0.7`$ this feature is sharper and denotes the transition from the paramagnetic to the antiferromagnetic state. Towards low temperatures a purely semiconducting behavior can be found. It seems that the samples with Sr concentration $`x0.7`$ belong to a two-phase region separating metallic and insulating regimes. At the same time the system is close to a phase boundary between the monoclinic and tetragonal crystal structures. Nevertheless, the sample with $`x=0.7`$ remains a candidate for the occurrence of electronic phase separation for $`T<200`$ K. To investigate also the high-temperature electronic behavior, we measured the electrical resistance for some representative samples up to 600 K. The results for $`x=0.5`$ and $`0.75`$ are shown in the inset. For $`x=0.5`$ the metallic behavior at low temperatures changes into the temperature characteristics of a bad metal at elevated temperatures. For $`x>0.7`$ a bad metallic behavior for $`T>250`$ K changes into strongly semiconducting temperature characteristics below. The low-temperature resistivity as a function of Sr concentration exhibits a maximum around $`x0.75`$. This may indicate a CO state at electronic quarter filling of the $`e_g`$ bands.

### III.3 Magnetization and magnetic susceptibility

The magnetic dc-susceptibility (M/H measured at 1 kOe) of La1-xSrxMnO3 is shown in Fig. 4 in the upper frame. For $`x=0.4`$, at 370 K we find the pure ferromagnetic phase transition, which is driven by DE interactions and is characteristic for the materials showing a colossal magneto-resistance (CMR) effect. For $`x=0.5`$ and 0.6 the magnetization decreases below 250 K indicating that the ferromagnetic moments become reduced at low temperatures. This may be due to a slight canting of the spins or due to electronic phase-separation effects. Similar findings for $`0.46x0.53`$ were interpreted in terms of phase separation within a charge ordered state.Patil00  We would like to recall that for $`x0.5`$ we found indications of a two-phase region of a rhombohedral and a monoclinic structure. At the moment it is unclear, whether this is a structural two-phase region, or whether the groundstate can be explained in terms of electronic phase separation between FM and AFM regions including scenarios like stripe or bistripe formation.

Well defined cusps appear for $`x=0.65`$ and 0.7 which indicate the vanishing of a spontaneous ferromagnetic moment and the presence of a nearly completely antiferromagnetic (AFM) spin-structure at low temperatures. It is important to note that we observed a pronounced temperature hysteresis at these cusps typical for a first-order magnetic transition. Finally for $`x>0.7`$ the characteristics of purely antiferromagnetic phase transitions are detected. From the inverse susceptibilities, which are shown in the lower frame of Fig. 4, we can deduce the Curie-Weiss (CW) temperatures, which continuously decrease while the Sr concentration increases from $`x=0.4`$ to $`x=0.7`$ (cf. Tab. 1). Beyond this concentration a significant decrease of the CW temperatures appears and finally, for $`x=0.85`$, a negative CW temperature can be read off. For the concentrations $`0.55x0.7`$ in addition a distinct deviation from the CW behavior can be detected well above the magnetic ordering temperature indicating the presence of strong spin fluctuations or even of short-range magnetic order.

To further elucidate the low-temperature magnetic properties of La1-xSrxMnO3, Fig. 5 shows the magnetization at 5 K for a series of crystals with concentrations $`0.5<x<0.65`$. An almost pure antiferromagnet at $`x=0.65`$ is followed by an increasing ferromagnetic component on decreasing $`x`$. But even at $`x=0.5`$ only 2/3 of the full possible ferromagnetic magnetization is observed at low fields, and on increasing external field the magnetization increases strictly linearly, which can be explained in terms of a canted antiferromagnet, whose canting angle becomes reduced in increasing fields, or in terms of electronic phase separation. Including earlier published resultsParask00 , the lower inset of Fig. 5 demonstrates, how the ferromagnetic moment evolves in the complete concentration regime. The expected spin-only FM moment only evolves for Sr concentrations $`0.2<x<0.4`$ and approaches values close to zero for lower and higher Sr concentrations. The upper inset of Fig. 5 compares the field dependence of the magnetization for the concentrations $`x=0.55`$, 0.6, and 0.65 at $`T=290`$ K. The representation $`M_n^2`$ vs. $`H/M_n`$ (Arrot-plotArro67 ) demonstrates the presence of a spontaneous FM component (i.e. finite $`M^2`$ at $`H=0`$) for $`x=0.55`$. At the same temperature the behavior of $`x=0.65`$ is purely paramagnetic (i.e. $`H/M`$ is constant). The curve for $`x=0.6`$ exhibits an intermediate behavior, denoting the presence of strong FM fluctuations or short-range order (SR). This corresponds to the strong deviations from the Curie-Weiss behavior discussed earlier (see Fig. 4).

In what follows, we wanted to study the magnetic anisotropy close to half filling in more detail. Around $`x=0.55`$ the ferromagnetic phase at elevated temperatures is followed by a further magnetic phase transition which significantly reduces the magnetization (see Fig. 4). To elucidate the temperature evolution of this weak ferromagnetic regime in more detail, Fig. 6 shows the magnetization vs. external field in La0.45Sr0.55MnO3 for a series of temperatures. At 250 K, just below the FM phase transition a strong ferromagnetic hysteresis evolves and, taking into account the elevated temperature, almost the full saturated moment of Mn3+/Mn4+ can be detected. However, below 200 K the magnetization at moderate fields becomes significantly reduced and reveals a strictly linear increase of $`M`$ as function of field. Finally at 5 K the FM component amounts approximately 0.5 $`\mu _B`$ only.

To study the anisotropy of this magnetic ground state, the data were taken for two different orientations of the sample with respect to the external field. The upper inset of Fig. 6 shows the angular dependence of the magnetization as observed at $`T=100`$ K when the sample was rotated around an axis approximately within the $`a,b`$-plane. From this a hard and an easy axis were defined, which differ by almost a factor of 2.5 in the magnetization values. The lower inset of Fig. 6 shows the temperature dependence of the magnetic susceptibility measured for these both orientations. The distinct evolution of anisotropic behavior below $`T250`$ K can be observed. This behavior clearly is different from the anisotropy observed for strontium concentrations of $`x=0.05`$ where the magnetization is zero along $`a`$ and $`b`$ and finite along $`c`$, indicating a slight canting of the moments out of the $`a,b`$-plane.Parask00  It seems that for $`x=0.55`$ the AFM structure at low temperatures is certainly more complex. Nevertheless, it has to be stated, that neither a considerable uncertainty concerning the determination of the $`a,b`$-plane nor possible twinning of the sample can be ruled out. However, as observed for $`x=0.05`$Parask00  the paramagnetic susceptibility again is fully isotropic for temperatures above the magnetically ordered regime. It is interesting to note that the anisotropy changes in the (canted) antiferromagnetic state. These results indicate either a canted spin structure or phase separation assuming ferromagnetic clusters within an antiferromagnetic matrix. But, of course, we cannot exclude more complex phase-separation scenarios.Rada99 ; Mori98  It also should be kept in mind that the sample under consideration still behaves metallic, in the paramagnetic (PM), the FM, and the canted AFM state, respectively.

### III.4 Phase diagram

Finally in Fig. 7 we present the phase diagram for the complete concentration regime $`0x0.85`$ where mixed single crystals can be grown. We included the results from earlier work Parask00  ($`0x0.3`$). The complex sequence of magnetic phases at low concentrations is highly influenced by the cooperative JT distortion of the O’ phase and by the orbital order of the O” phase.Endoh99  For $`x>0.2`$ a large ferromagnetic regime evolves which reveals a rhombohedral structure and shows CMR effects throughout. For $`x>0.5`$ a tetragonal phase appears which is a FM metal. On decreasing temperature it undergoes a transition into a monoclinic antiferromagnetic state, but still exhibits metallic behavior. We would like to recall that in Pr0.5Sr0.5MnO3 and Nd0.5Sr0.5MnO3 the FM and M phase is followed by an insulating AFM phase, which reveals a CE-type spin structure for the Nd and an A-type layered spin structure for the Pr compound.Kawa97  The latter shows no clear signs of CO.Kawa97  However, for Nd0.45Sr0.55MnO3 a metallic behavior has been detected within the ferromagnetic layers, while the resistivity along c revealed a semiconducting characteristic.Kuwa99  It seems that in the La:Sr series of the manganites this two dimensional metallic phase, which is antiferromagnetic, evolves for $`x0.6`$. There the resistivity remains fully metallic ($`d\rho /dT>0`$) for all temperatures (see Fig. 3) and at $`T=5`$ K only a weak ferromagnetic moment can be detected (Fig. 5).

This metallic and AFM state is monoclinic and is embedded into structurally different regions (R for $`x<0.5`$ and T for $`x>0.7`$), depicted schematically by vertical dashed lines in Fig. 7. It seems naturally to assume that this exotic phase also is characterized by a new orbital order. Close to $`x=0.5`$ it seems that the M/FM phase coexists with the M/AFM phase. According to preliminary diffraction experiments indeed also the crystallographic phases coexist. We would like to recall that from observations in conventional ferromagnets a variety of domain structures can be formed in multicomponent systems, including cluster or stripe formation. Whether in this case a description in terms of electronic phase separation is adequate, has to be proven in detailed experiments. At present it is also unclear how the observation of stripes Rada99  or bistripes Mori98  is compatible with the observed magnetic anisotropy. For concentrations $`x0.7`$ metallic and insulating domains cannot be ruled out. This we conclude from the temperature dependence of the resistivity. At the moment it remains an open question, whether a T/I/AFM phase coexists with an Mc/M/AFM state or whether in this region electronic phase separation evolves out of the structurally pure phase.

A further interesting phenomenon in this concentration range is the fact, that the AFM metallic phase evolves out of a ferromagnetic metal. Probably double-exchange interactions drive the ferromagnet, while superexchange interactions are responsible for the AFM state. This can only be explained, if the orbital order changes as a function of temperature.

For concentrations $`x>0.75`$ a purely AFM and insulating state evolves within a nearly cubic structure. For these concentrations the tolerance factor is close to 1. For further increasing concentrations the ABO3 perovskite structure is unstable and no mixed crystals can be grown. SrMnO3-δ reveals a layered perovskite structure.

## IV Conclusion

What did we learn from these experiments in addition to the existing enormous amount of knowledge on the doped manganites? To summarize, we were able to grow high-quality single crystals of La1-xSrxMnO3 for $`0x0.85`$ with no parasitic phases like SrMnO3. We constructed a rather complete ($`x,T`$) phase diagram (Fig. 7), which reveals the well established asymmetry between the hole doped $`(x<0.5)`$ and the electron doped $`(x>0.5)`$ regime. Of course, an essential part of this asymmetry is driven by geometrical constraints via the tolerance factor, which increases from $`t=0.89`$ for $`x=0`$ to $`t=1.01`$ for $`x=1`$. Hence, on increasing concentration, La1-xSrxMnO3 reveals a decreasing buckling of the MnO6 octahedra. But partly this asymmetry also is driven by orbital degeneracy. Close to $`x=0`$ strong JT distortions reveal orbital order which concomitantly determines the A-type spin structure. For higher Sr concentrations and in the crystals with a high symmetry at the Mn site, orbital degeneracy will play an essential role, yielding completely different spin ground states.

In Fig. 7 the combined influence of the concentration dependence of the tolerance factor and the increasing importance of orbital degeneracy as $`x`$ increases is nicely documented in the sequence of structural phases: At room temperature and for $`0x0.85`$ we find the crystallographic phases O’ orthorhombic, O orthorhombic, rhombohedral and tetragonal. The corresponding series of electronic ground-state properties is insulating/spin A-type AFM, insulating/spin FM, metallic/spin FM, metallic/spin A-type AFM; insulating/spin C-type AFM, and finally insulating/spin G-type for $`x=1`$. So far we did not investigate the spin structures of the magnetic phases for $`x1`$. Theoretically, taking SE, DE and orbital degeneracy into account the sequence of spin structures A-F-A-C-G has been predicted.Maez98  We want to stress that a pure insulating AFM state appears in all phase diagrams at high doping levels and that a G-type antiferromagnet is stable for $`x=1`$. The spin structure close to $`x=0.8`$ (AFM, C-type) has been taken in analogy to other doped manganites and to the existing literature. For this concentration regime around $`x=0.8`$ evidence for charge order can be found due to the sharp increase of the resistivity at $`T_N`$, possibly in the form of stripe or bistripe structures as it has been suggested in literature.Mori98  Close to $`x=0.6`$ it has been proposed that the orbitals are strictly aligned within the $`a,b`$-plane forcing an A-type spin structure.Maez98  La0.4Sr0.6MnO3 reveals antiferromagnetic order with a FM component, which is of the order of $`0.1\mu _B`$ at low fields. It is this concentration regime where also two-dimensional metallic behavior is expected.

In what follows we would like to compare the phase diagram of La1-xSrxMnO3 as observed in the present investigations with published phase diagrams of other manganites and with theoretical predictions. This discussion is based on experiments covering the hole and electron doped regime of the phase diagram and investigating the half-doped case in detail. Experimental phase diagrams are available for La:Sr Niem99 , La:Ca Schiff95  , Pr:Sr Maez98 ; Mart99 ; Kawa97 , Pr:Ca Mart99 ; Tomi96 , Nd:Sr Maez98 ; Kawa97 , Sm:Sr and Sm:Ca Mart99  manganite. From these results a generic electronic phase diagram can be deduced, which yields the sequence of AFM (A-type)/I, FM/I, FM/M and AFM/I (C-type). The latter spin structure dominates a broad region in the electron doped ($`x>0.5`$) crystals. It is clear that these spin structures and electronic properties are closely linked with the orbital degrees of freedom, and the orbital order for most of these phases has been theoretically proposed by Maezono et al. Maez98 , Khomskii Khom01 , van den Brink et al. Brin99  and by Solovyev and Terakura.Solo99

It is worth mentioning that there are some noticeable exceptions from this universal phase diagram: e.g. the Sm:Ca Mart99  and the Pr:Ca Mart99 ; Tomi96  compounds do not exhibit a typical CMR regime with a ferromagnetic and insulating ground state for $`x<0.5`$. This fact probably results from geometrical constraints. In addition peculiarities show up close to half filling: In the Nd:Sr and Pr:Sr compounds close to $`x=0.5`$ charge ordered antiferromagnetic phases were found.Kawa97  Magnetically these systems form ferromagnetic zig-zag chains which are coupled antiferromagnetically. This CE-type of magnetic structure results from charge and orbital order and has been explained theoretically in detail.Solo99 ; Brin99  The FM zig-zag chains with their concomitant charge order can easily be molten by the application of moderate magnetic fields.Kuwa95  In addition, van den Brink et al. Brin99  have shown that for doping $`x<0.5`$ the CE structure is unstable against phase separation. This CE-type spin structure with a checkerboard-type CO is not observed in the La:Sr compound under investigation. In our high-quality samples we find an AFM and metallic ground state with no signs of charge order. Hence we do not expect to find a CE-type magnetic structure. A metallic AFM spin A-type phase has been predicted by Maezono et al.Maez98  which reveals an (x2 \- y2) orbital structure. In this structure hopping along c is forbidden and the metallic conductivity is strictly two dimensional and indeed this type of behavior has been observed in Nd0.45Sr0.55MnO3.Kuwa99  We believe that this type of spin and orbital structure may also be present in La1-xSrxMnO3 for $`x0.6`$. Measurements of the magnetic structure and of the anisotropy of the electronic transport still have to be performed. It remains a puzzle why in Nd0.45Sr0.55MnO3, which reveals a metallic, spin A-type phase, Kuwahara et al.Kuwa99  observed a significant anisotropy in the resistivity but not in the magnetic susceptibility. In contrast La0.45Sr0.55MnO3 exhibits a pronounced anisotropy both in the FM and in the AFM states (cf. Fig. 6). It seems clear that the FM metallic state at elevated temperatures still is driven by double exchange, and perhaps the low-temperature metallic state indicates electronic phase separation where the FM metallic paths still percolate. The occurrence of a FM metal followed by an AFM metallic state for concentrations close to $`x=0.6`$ still is a puzzle and further experimental work is needed to elucidate this strange phase.

###### Acknowledgements.

This work was supported by the Bundesministerium für Bildung und Forschung (BMBF) via VDI/EKM, FKZ 13N6917, by the Deutsche Forschungsgemeinschaft via SFB 484 (Augsburg), and by INTAS via project 97-30850.