Strong Neel ordering and luminescence correlation in a two-dimensional antiferromagnet

TL;DR

This study reveals strong light-magnetic interactions in 2D antiferromagnetic MnPS3 through a novel near-infrared photoluminescence mode that correlates with Neel ordering and persists in monolayers, enabling new magneto-optical insights.

Contribution

It uncovers a new in-gap photoluminescence mode in 2D MnPS3 that correlates with magnetic order and can be tuned, advancing understanding of light-magnetism interactions in 2D antiferromagnets.

Findings

The in-gap PL mode strongly correlates with Neel ordering.

The PL mode persists down to monolayer thickness.

Ultraviolet-ozone treatment enhances PL strength.

Abstract

Magneto-optical effect has been widely used in light modulation, optical sensing and information storage. Recently discovered two-dimensional (2D) van der Waals layered magnets are considered as promising platforms for investigating novel magneto-optical phenomena and devices, due to the long-range magnetic ordering down to atomically-thin thickness, rich species and tunable properties. However, majority 2D antiferromagnets suffer from low luminescence efficiency which hinders their magneto-optical investigations and applications. Here, we uncover strong light-magnetic ordering interactions in 2D antiferromagnetic MnPS3 utilizing a newly-emerged near-infrared photoluminescence (PL) mode far below its intrinsic bandgap. This ingap PL mode shows strong correlation with the Neel ordering and persists down to monolayer thickness. Combining the DFT, STEM and XPS, we illustrate the origin of the PL mode and its correlation with Neel ordering, which can be attributed to the oxygen ion-mediated states. Moreover, the PL strength can be further tuned and enhanced using ultraviolet-ozone treatment. Our studies offer an effective approach to investigate light-magnetic ordering interactions in 2D antiferromagnetic semiconductors.