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

TL;DR

This study uses advanced theoretical methods to explore how electronic correlations and chemical bonding influence the magnetic and structural properties of high-pressure FeN₂, revealing complex covalent bonds and magnetic states.

Contribution

It provides a detailed theoretical analysis of FeN₂ under pressure, highlighting the role of electronic correlations and magnetic fluctuations in its behavior.

Findings

Formation of strongly covalent N-N bonds

Fe ions in a +3 valence state with low-spin configuration

Presence of multiple spin density wave states

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.