Interplay of electronic correlations and chemical bonding in FeN${}_2$ under pressure

Abstract

We report a theoretical study of the effects of electronic correlations, magnetic properties, and chemical bonding in the recently synthesized high-pressure orthorhombic phase of FeN${}_2$ using the DFT+dynamical mean-field theory approach. Our analysis documents a complex crystal-chemical behavior of FeN${}_2$ characterized by the formation of a strongly covalent N-N bond with an unexpected valence state of Fe ions $3+$ (paramagnetic ferric Fe${}^{3+}$ ions in the low-spin state), in agreement with available experimental data. Our results reveal weak (orbital-dependent) correlation effects, which are complicated by the possible emergence of multiple spin density wave states on a microscopic level. This suggests the importance of antiferromagnetic spin fluctuations to explain the properties of FeN${}_2$ under pressure.

9 pages, 6 figures

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