Magnetic interactions in disordered perovskite PbFe_{1/2}Nb_{1/2}O_3 and related compounds. Dominance of nearest-neighbor interaction

TL;DR

This paper models the magnetism of disordered double perovskites using the Heisenberg model, highlighting the dominance of nearest-neighbor interactions and the influence of chemical ordering on magnetic properties.

Contribution

It demonstrates that magnetic interactions are primarily governed by nearest-neighbor exchange and links chemical ordering patterns to magnetic behavior in double perovskites.

Findings

J_1 is over 20 times J_2, with J_2 defining the magnetic energy scale.

Chemical ordering influences magnetic properties and transition temperatures.

Certain ordering types can lead to ferrimagnetism and superparamagnetism.

Abstract

We show that the magnetism of double perovskite AFe_{1/2}M_{1/2}O_3 systems may be described by the Heisenberg model on the simple cubic lattice, where only half of sites are occupied by localized magnetic moments. The nearest-neighbor interaction J_1 is more than 20 times the next-nearest neighbor interaction J_2, the third-nearest interaction along the space diagonal of the cube being negligible. We argue that the variety of magnetic properties observed in different systems is connected with the variety of chemical ordering in them. We analyze six possible types of the chemical ordering in 2x2x2 supercell, and argue that the probability to find them in a real compound does not correspond to a random occupation of lattice sites by magnetic ions. The exchange J_2 rather than J_1 define the magnetic energy scale of most double perovskite compounds that means the enhanced probability of 1:1 short range ordering. Two multiferroic compounds PbFe_{1/2}M_{1/2}O_3 (M=Nb, Ta) are exceptions. We show that the relatively high temperature of antiferromagnetic transition is compatible with a layered short-range chemical order, which was recently shown to be most stable for these two compounds [I. P. Raevski, {\em et al.}, Phys.\ Rev.\ B \textbf{85}, 224412 (2012)]. We show also that one of the types of ordering has ferrimagnetic ground state. The clusters with short-range order of this type may be responsible for a room-temperature superparamagnetism, and may form the cluster glass at low temperatures.