Large Disparity Between Optical and Fundamental Band Gaps in Layered In2Se3

TL;DR

This study uses first-principles calculations to analyze various layered In2Se3 structures, revealing significant differences between their fundamental and optical band gaps, and providing insights into their stability and electronic properties.

Contribution

It offers a detailed theoretical investigation of layered In2Se3 phases, clarifying their stability, band gap nature, and optical properties, which addresses previous inconsistencies in experimental data.

Findings

Large disparities between fundamental and optical gaps.

High absorption coefficients comparable to direct-gap semiconductors.

Tendency towards n-type conductivity in band alignment.

Abstract

In$_2$Se$_3$ is a semiconductor material that can be stabilized in different crystal structures (at least one 3D and several 2D layered structures have been reported) with diverse electrical and optical properties. This feature has plagued its characterization over the years, with reported band gaps varying in an unacceptable range of 1 eV. Using first-principles calculations based on density functional theory and the HSE06 hybrid functional, we investigated the structural and electronic properties of four layered phases of In$_2$Se$_3$, addressing their relative stability and the nature of their fundamental band gaps, i.e., direct {\em versus} indirect. Our results show large disparities between fundamental and optical gaps. The absorption coefficients are found to be as high as that in direct-gap III-V semiconductors. The band alignment with respect to conventional semiconductors indicate a tendency to $n$-type conductivity, explaining recent experimental observations.