Evidence of strong antiferromagnetic coupling between localized and itinerant electrons in ferromagnetic Sr2FeMoO6

TL;DR

This study investigates the magnetic interactions in Sr2FeMoO6, revealing strong antiferromagnetic coupling between localized Fe3+ ions and itinerant electrons, challenging traditional superexchange models and supporting a novel magnetic mechanism.

Contribution

It provides experimental evidence of strong antiferromagnetic coupling between localized and itinerant electrons in Sr2FeMoO6, supporting a new mechanism for magnetic order in double perovskites.

Findings

Curie-Weiss behavior with ferromagnetic $ heta$

Reduced effective magnetic moment due to AFM coupling

ESR spectrum described by Bloch-Hasegawa equations

Abstract

Magnetic dc susceptibility ($\chi$) and electron spin resonance (ESR) measurements in the paramagnetic regime, are presented. We found a Curie-Weiss (CW) behavior for $\chi$(T) with a ferromagnetic $\Theta = 446(5)$ K and $\mu_{eff} = 4.72(9) \mu_{B}/f.u.$, this being lower than that expected for either $Fe^{3+}(5.9\mu_{B})$ or $Fe^{2+}(4.9\mu_{B})$ ions. The ESR g-factor $g = 2.01(2)$, is associated with $Fe^{3+}$. We obtained an excellent description of the experiments in terms of two interacting sublattices: the localized $Fe^{3+}$ ($3d^{5}$) cores and the delocalized electrons. The coupled equations were solved in a mean-field approximation, assuming for the itinerant electrons a bare susceptibility independent on $T$. We obtained $\chi_{e}^{0} = 3.7$ $10^{-4}$ emu/mol. We show that the reduction of $\mu_{eff}$ for $Fe^{3+}$ arises from the strong antiferromagnetic (AFM) interaction between the two sublattices. At variance with classical ferrimagnets, we found that $\Theta$ is ferromagnetic. Within the same model, we show that the ESR spectrum can be described by Bloch-Hasegawa type equations. Bottleneck is evidenced by the absence of a $g$-shift. Surprisingly, as observed in CMR manganites, no narrowing effects of the ESR linewidth is detected in spite of the presence of the strong magnetic coupling. These results provide evidence that the magnetic order in $Sr_{2}FeMoO_{6}$ does not originates in superexchange interactions, but from a novel mechanism recently proposed for double perovskites.