Exploration of the spin-phonon coupling in the noncollinear antiferromagnetic antiperovskite Mn$_3$NiN

TL;DR

This study uses first-principles calculations to investigate the spin-phonon coupling in Mn3NiN, revealing strong spin-lattice interactions and unstable vibrational modes linked to magnetic ordering changes.

Contribution

It provides the first detailed theoretical analysis of spin-phonon coupling in Mn3NiN, highlighting the influence of magnetic structure and exchange-correlation schemes.

Findings

Strong spin-lattice coupling observed.

Unstable vibrational modes at M and R points.

Magnetic ordering affects phonon stability.

Abstract

Antiferromagnetic antiperovskites, of the form Mn$_3B$N ($B$ = Ni, Cu, Zn, Sn, Ir, and Pt), have shown an outstanding behavior in which, giant negative thermal expansion and chiral magnetic structures are intertwined. As such, aiming to shed light on the magnetostructural behavior, related to the magnetic ordering and structure of this type of materials, we studied by theoretical first-principles calculations the spin-phonon coupling in the Manganese-based antiperovskite Mn$_3$NiN, as a prototype in the Mn$_3B$N family. We found a strong spin-lattice coupling by means of the understanding of the phonon-dispersion curves obtained when including the chiral noncollinear magnetic structure. To do so, we highlight the importance of the exchange-correlation scheme selected and its influence on the electronic, structural, and vibrational degrees of freedom. Finally, we found two unstable vibrational modes at the $M$- and $R$-points when the magnetic ordering is switched to ferromagnetic from the chiral $\Gamma_{4g}$ and $\Gamma_{5g}$. The latter coupling was observed as a key signature of the strong spin-lattice interaction.