Stabilization of zigzag order in NiPS$_3$ via positive biquadratic interaction

TL;DR

This paper investigates the spin interactions in NiPS$_3$, revealing a positive biquadratic exchange term that stabilizes its zigzag magnetic order, combining density functional theory and advanced computational methods.

Contribution

It identifies and quantifies a positive biquadratic interaction in NiPS$_3$, demonstrating its role in stabilizing zigzag order, which clarifies previous uncertainties about its spin Hamiltonian.

Findings

Positive biquadratic interaction with B/J_3 ≈ 0.44

Biquadratic term stabilizes zigzag order

Ground state well-described by minimal J1-J3-B model

Abstract

Despite extensive research, the precise spin Hamiltonian of the van der Waals antiferromagnet NiPS$_3$ -- which hosts a zigzag-ordered ground state -- remains debated. While consensus has emerged on ferromagnetic nearest-neighbor ($J_1$) and antiferromagnetic third-nearest-neighbor ($J_3$) Heisenberg interactions, recent studies suggest a biquadratic ($B$) exchange term may also play a role, though its estimated magnitude varies widely. To address this controversy, we perform density functional theory calculations and extract a positive biquadratic interaction with $B/J_3 \approx 0.44$. Within the minimal $J_1$-$J_3$-$B$ model, we show that these parameters naturally stabilize zigzag ordering using minimally augmented spin-wave theory. Density-matrix renormalization group calculations further validate our extracted parameters as a reasonable description of the ground state. Although fully resolving the spin Hamiltonian of NiPS$_3$ requires further investigation, our findings provide new insights into its biquadratic interaction.