Stabilization of Long-Range Order by Additional Anisotropic Spins in Two-Dimensional Isotropic Heisenberg Antiferromagnets —A Possible Model of an Organic Compound with Magnetic Anions—

Abstract

We examine a two-dimensional (2D) coupled antiferromagnetic (AF) Heisenberg model that consists of two subsystems: an isotropic S = 1/2 spin subsystem with strong AF exchange interactions (main system), and a uniaxial S = 5/2 spin subsystem with weak exchange interactions. This model is an example in which additional semiclassical degrees of freedom affect a quantum system; it also describes a possible stabilization mechanism of AF long-range order (LRO) in the 2D organic compound λ-(BETS)2FeCl4, where BETS stands for bis(ethylenedithio)tetraselenafulvalene. Previous experimental studies have revealed that 3d spins on FeCl4 anions passively follow the AF LRO of the π-electron system in the BETS layers, although the AF LRO is stabilized by the 3d spins themselves. To explain this paradoxical behavior, we examine a scenario in which the uniaxial anisotropy of the 3d spins stabilizes the AF LRO on an isotropic 2D π-spin system. We extend Green’s function theory, called the Tyablikov approximation, to the present system, which describes spin-wave excitations and is consistent with the Mermin–Wagner theorem. It is shown that even extremely weak interactions with the uniaxial subsystem efficiently stabilize the AF LRO in the main system, even in the absence of AF exchange interactions in the uniaxial subsystem. The AF LRO is triggered by the uniaxial subsystem, but the sublattice magnetization remains smaller than that of the main system in the high-temperature region. These results are consistent with experimental data for λ-(BETS)2FeCl4 and λ-(BETS)2GaCl4; the latter does not have the 3d spins and does not exhibit the AF LRO.