Correlation-Driven Spin Reorientation via Competing Anisotropy Channels in CrPS4

TL;DR

This paper uncovers a correlation-driven mechanism for temperature-induced spin reorientation in CrPS4, linking local correlations with competing anisotropy channels to explain magnetic behavior.

Contribution

It demonstrates how local magnetic correlations influence anisotropy channels and induce spin reorientation, advancing understanding of low-dimensional magnetic systems.

Findings

Ferromagnetic intrachain correlations persist above TN.

Competing single-ion and exchange anisotropy channels drive reorientation.

Differential renormalization of anisotropy channels explains spin canting.

Abstract

We identify a correlation-driven mechanism for the temperature-induced spin reorientation in the quasi-one-dimensional van der Waals antiferromagnet CrPS4. Magnetic pair distribution function (mPDF) analysis resolves the local spin direction and shows that ferromagnetic intrachain correlations persist far above TN. Combining these correlations with a DFT-derived spin Hamiltonian reveals competing single-ion and exchange-anisotropy channels, with single-ion anisotropy remaining local while exchange anisotropy is renormalized as intersite correlations decay. This differential renormalization rotates the effective easy axis and captures the ordered-state canting. Above TN, the continued rotation beyond the model prediction delineates the limits of the dominant-chain approximation. These results establish mPDF-derived correlations as direct inputs to microscopic Hamiltonians and show how low-dimensional correlations can control magnetic anisotropy.