Abstract

The monometallic pseudo-octahedral complex, [Co(H2O)2(CH3COO)2(C5H5N)2], is shown to exhibit slow magnetic relaxation under an applied field of 1500 Oe. The compound is examined by a combination of experimental and computational techniques in order to elucidate the nature of its electronic structure and slow magnetic relaxation. We demonstrate that any sensible model of the electronic structure must include a proper treatment of the first-order orbital angular momentum, and we find that the slow magnetic relaxation can be well described by a two-phonon Raman process dominating at high temperature, with a temperature independent quantum tunnelling pathway being most efficient at low temperature.

Highlights

  • The study of paramagnetic molecules exhibiting a measurably slow relaxation of their magnetisation is a field that has been growing since the observation of so-called single-molecule magnet (SMM) behaviour in a dodecametallic mixed-valence manganese cluster just over two decades ago [1]

  • The main reason for this is the complexity that arises from spin-orbit coupling, one of the necessary prerequisites for slow magnetic relaxation

  • We report slow magnetic relaxation behaviour in the monometallic pseudo-octahedral cobalt(II) compound, [Co(H2O)2(CH3COO)2(C5H5N)2], and further we examine the nature of the relaxation barrier in the context of a model that accounts for the first-order orbital angular momentum

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Summary

Introduction

The study of paramagnetic molecules exhibiting a measurably slow relaxation of their magnetisation is a field that has been growing since the observation of so-called single-molecule magnet (SMM) behaviour in a dodecametallic mixed-valence manganese cluster just over two decades ago [1]. The main reason for this is the complexity that arises from spin-orbit coupling, one of the necessary prerequisites for slow magnetic relaxation.

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