Issue 5, 2024

Multistep transitions in spin crossover materials without long-range spin state order from dimensional reduction

Abstract

Most theories of multistep spin crossover (SCO) have focused on intermediate phases with long-range spin state order. However, disordered intermediate phases have also been observed experimentally. Here we show that the interplay of crystallographically inequivalent SCO centres with elastic interactions between SCO centres can lead to an effective reduction in the dimensionality of the system. This is highly analogous to dimensional reduction in quantum magnetism. The resulting quasi-one-dimensional and quasi-zero-dimensional models naturally result in disorder at non-zero temperatures, explaining the absence of long-range spin state order in our calculations. Furthermore, the low effective dimensionality can strongly suppress short-range correlations and hence diffuse scattering should not necessarily be expected to be observed experimentally in these disordered phases. Our model contains parameter regimes where disordered intermediate phases give rise to diffuse scattering and other regimes where disordered intermediate phases do not. Our results are in good agreement with experiments on [FeII3(saltrz)6(MII(CN)4)3]·8(H2O) [Sciortino et al., Chem. Sci., 2017, 8, 701].

Graphical abstract: Multistep transitions in spin crossover materials without long-range spin state order from dimensional reduction

Article information

Article type
Paper
Submitted
29 Nov 2023
Accepted
14 Jan 2024
First published
17 Jan 2024
This article is Open Access
Creative Commons BY-NC license

Mater. Adv., 2024,5, 2057-2068

Multistep transitions in spin crossover materials without long-range spin state order from dimensional reduction

G. Ruzzi, J. Cruddas and B. J. Powell, Mater. Adv., 2024, 5, 2057 DOI: 10.1039/D3MA01057K

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