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Crystal-Field-Tuned Spin-Flip Luminescence in NiPS_{3}.

Léonard Schué¹, Nashra Pistawala², Hebatalla Elnaggar³

¹Institut Polytechnique de Paris, Ecole Polytechnique, CNRS, Laboratoire de Physique de la Matière Condensée, 91120 Palaiseau, France.

Physical Review Letters

|June 26, 2026

Summary

Researchers investigated nickel thiophosphate (NiPS3) and its photoluminescence. They found the luminescence is localized at the Ni site and not directly correlated with magnetic ordering, challenging its magnetic origin.

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Area of Science:

Condensed Matter Physics
Materials Science
Quantum Magnetism

Background:

Layered magnetic materials offer unique platforms for studying 2D magnetism.
Nickel thiophosphate (NiPS3) is an antiferromagnetic material exhibiting photoluminescence linked to spin states.

Purpose of the Study:

To elucidate the origin of photoluminescence in NiPS3.
To investigate the relationship between magnetic transitions and optical properties.
To determine if the observed excitation is linked to magnetism.

Main Methods:

Synthesis of NiPS3 with metal and ligand substitutions.
Temperature-dependent photoluminescence spectroscopy.
Crystal field and charge transfer multiplet calculations.
Phonon side band analysis.

Main Results:

Photoluminescence originates from Ni crystal field levels, identified as spin-flip luminescence.
Luminescence is localized at the Ni site, confirmed by phonon side bands.
Alloying with Zn and Se showed no correlation between luminescence temperature dependence and Néel temperature.

Conclusions:

The photoluminescence in NiPS3 is a localized spin-flip excitation at the Ni site.
The observed optical properties are not fundamentally linked to the magnetic ordering temperature.
This challenges the proposed magnetic origin of the excitation in NiPS3.