Electronic band structure changes across the antiferromagnetic phase transition of exfoliated MnPS$_3$ probed by $\mu$-ARPES

TL;DR

This study uses micron-scale angle-resolved photoelectron spectroscopy to investigate how the electronic band structure of exfoliated MnPS3 changes across its antiferromagnetic transition, revealing orbital-specific modifications and the 2D nature of the material.

Contribution

It provides the first direct probing of the electronic band structure of exfoliated MnPS3 across the N{\'e}el temperature using $bc$-ARPES, linking experimental observations with density functional theory.

Findings

Pronounced band structure changes across the N{\'e}el temperature.

Orbital character identified as Mn 3d and S 3p levels.

Minor differences between monolayer and thicker films.

Abstract

Exfoliated magnetic 2D materials enable versatile tuning of magnetization, e.g., by gating or providing proximity-induced exchange interaction. However, their electronic band structure after exfoliation has not been probed, most likely due to their photochemical sensitivity. Here, we provide micron-scale angle-resolved photoelectron spectroscopy of the exfoliated intralayer antiferromagnet MnPS$_3$ above and below the N\'{e}el temperature down to one monolayer. The favorable comparison with density functional theory calculations enables to identify the orbital character of the observed bands. Consistently, we find pronounced changes across the N\'{e}el temperature for bands that consist of Mn 3d and 3p levels of adjacent S atoms. The deduced orbital mixture indicates that the superexchange is relevant for the magnetic interaction. There are only minor changes between monolayer and thicker films demonstrating the predominant 2D character of MnPS$_3$. The novel access is transferable to other MPX$_3$ materials (M: transition metal, P: phosphorus, X: chalcogenide) providing a multitude of antiferromagnetic arrangements.