Magnetic anisotropy and low-energy spin dynamics in the van der Waals compounds Mn$_{2}$P$_{2}$S$_{6}$ and MnNiP$_{2}$S$_{6}$

TL;DR

This study uses high-field electron spin resonance to explore magnetic anisotropy and low-energy spin dynamics in van der Waals compounds Mn2P2S6 and MnNiP2S6, revealing how Ni content influences magnetic excitations and fluctuations.

Contribution

It provides detailed insights into the magnetic anisotropy, spin fluctuations, and the crossover of spin wave behavior in these compounds, highlighting the role of Ni in magnetic stabilization.

Findings

Ni increases magnon gap and g-factor anisotropy.

MnNiP2S6 exhibits stronger spin fluctuations and short-range order.

Spin wave excitations in Mn2P2S6 show a crossover from 3D to 2D XY regime.

Abstract

We report the detailed high-field and high-frequency electron spin resonance (HF-ESR) spectroscopic study of the single-crystalline van der Waals compounds Mn$_{2}$P$_{2}$S$_{6}$ and MnNiP$_{2}$S$_{6}$. Analysis of magnetic excitations shows that in comparison to Mn$_{2}$P$_{2}$S$_{6}$ increasing the Ni content yields a larger magnon gap in the ordered state and a larger g-factor value and its anisotropy in the paramagnetic state. The studied compounds are found to be strongly anisotropic having each the unique ground state and type of magnetic order. Stronger deviation of the g-factor from the free electron value in the samples containing Ni suggests that the anisotropy of the exchange is an important contributor to the stabilization of a certain type of magnetic order with particular anisotropy. At temperatures above the magnetic order, we have analyzed the spin-spin correlations resulting in a development of slowly fluctuating short-range order. They are much stronger pronounced in MnNiP$_{2}$S$_{6}$ compared to Mn$_{2}$P$_{2}$S$_{6}$. The enhanced spin fluctuations in MnNiP$_{2}$S$_{6}$ are attributed to the competition of different types of magnetic order. Finally, the analysis of the temperature dependent critical behavior of the magnon gaps below the ordering temperature in Mn$_{2}$P$_{2}$S$_{6}$ suggests that the character of the spin wave excitations in this compound undergoes a field induced crossover from a 3D-like towards 2D XY regime.