Raman and first-principles study of the pressure induced Mott-insulator to metal transition in bulk FePS$_3$

TL;DR

This study investigates how pressure induces phase transitions in FePS3, a 2D Mott insulator, transforming it into a metal through Raman spectroscopy and first-principles calculations, revealing two key structural changes at specific pressures.

Contribution

It provides a combined experimental and theoretical analysis of pressure-induced phase transitions and electronic changes in FePS3, a novel 2D Mott insulator.

Findings

Phase transitions at 4.6 GPa and 12 GPa identified by Raman spectroscopy.

Transition from monoclinic to metallic trigonal phase under pressure.

Band gap reduction from 1.54 eV to 0.1 eV before metallization.

Abstract

Recently discovered class of 2D materials based on transition metal phosphorous trichalcogenides exhibit antiferromagnetic ground state, with potential applications in spintronics. Amongst them, FePS$ _{3} $ is a Mott insulator with a band gap of $\sim$ 1.5 eV. This study using Raman spectroscopy along with first-principles density functional theoretical analysis examines the stability of its structure and electronic properties under pressure. Raman spectroscopy reveals two phase transitions at 4.6 GPa and 12 GPa marked by the changes in pressure coefficients of the mode frequencies and the number of symmetry allowed modes. FePS$_3$ transforms from the ambient monoclinic C2/m phase with a band gap of 1.54 eV to another monoclinic C2/m (band gap of 0.1 eV) phase at 4.6 GPa, followed by another transition at 12 GPa to the metallic trigonal P-31m phase. Our work complements recently reported high pressure X-ray diffraction studies.