Quantum Fluctuations in the van der Walls material $\rm NiPS_3$

TL;DR

This paper investigates the quantum magnetic excitation spectrum of NiPS3, revealing multiple magnon modes, the effects of anisotropy, and potential hidden nematic orders, using advanced spin wave theory.

Contribution

It introduces a multi-boson generalized spin wave theory for S=1 systems to analyze NiPS3's magnetic excitations, including bilinear and biquadratic interactions, and explores quantum corrections and instabilities.

Findings

Identified a single magnon mode consistent with experiments.

Discovered a gapped flat band of two-magnon fluctuations.

Linked higher energy dispersions to quadrupolar fluctuations.

Abstract

We present the magnetic excitation spectrum of the quantum magnet $\rm NiPS_3$ near the zig-zag ground state of a minimal honeycomb spin Hamiltonian that includes bilinear and biquadratic spin interactions. Our analysis, using a multi-boson generalized spin wave theory suited for spin S=1 systems, revealed two normal modes at the linear level. The one at lower energy corresponds to a single magnon mode, consistent with results from spectroscopy experiments. Without single-ion anisotropy, this mode features a Goldstone mode at the corner of the Brillouin zone. When single ion anisotropy is introduced, the zig-zag phase's global U(1) invariance is broken, resulting in a gap. The higher energy mode corresponds to two-magnon fluctuations, which appear at the harmonic level in the generalized spin wave theory. This mode forms a gapped flat band due to bilinear spin interactions and becomes dispersive when biquadratic interactions are considered. The higher energy dispersion is related to quadrupolar fluctuations, which are feasible in magnets where the order parameter fluctuates in the SU(3) space. The spectrum analysis yielded quantum corrections to the order parameter and detected instabilities in the $\rm NiPS_3$ dipolar phases. Identifying the highest energy branch in experiments could provide insight into hidden nematic orders in $\rm NiPS_3$ and other van der Waals magnets.