Opening band gaps of low-dimensional materials at the meta-GGA level of density functional approximations

TL;DR

This paper introduces a modified meta-GGA functional, mTASK, that improves band gap predictions for low-dimensional materials, achieving accuracy comparable to hybrid functionals while maintaining efficiency for bulk systems.

Contribution

The authors modify the TASK functional to better predict band gaps of low-dimensional materials, demonstrating significant improvements over the original functional.

Findings

mTASK enhances band gap accuracy for 2D and 1D materials.

mTASK maintains original TASK accuracy for bulk 3D materials.

The functional performs well on TMD nanoribbons under bending.

Abstract

The recent TASK meta-GGA density functional [Phys. Rev. Research, 1, 033082 (2019)] is constructed with an enhanced nonlocality in the generalized Kohn-Sham scheme, and therefore harbors great opportunities for band gap prediction. Although this approximation was found to yield excellent band gaps of bulk solids, this accuracy cannot be straightforwardly transferred to low-dimensional materials. The reduced screening of these materials results in larger band gaps compared to their bulk counterparts, as an additional barrier to overcome. In this work, we demonstrate how the alteration of exact physical constraints in this functional affects the band gaps of monolayers and nanoribbons, and present accurate band gaps competing with the HSE06 approximation. In order to achieve this goal, we have modified the TASK functional (a) by changing the tight upper-bound for one or two-electron systems ($h_X^0$) from 1.174 to 1.29 (b) by changing the limit of interpolation function $f_X (\alpha \rightarrow \infty$) of the TASK functional that interpolates the exchange enhancement factor $F_X (s,\alpha)$ from $\alpha=$ 0 to 1. The resulting modified TASK (mTASK) was tested for various materials from 3D to 2D to 1D (nanoribbons), and was compared with the results of the higher-level hybrid functional HSE06 or with the G$_0$W$_0$ approximation within many-body perturbation theory. We find that mTASK greatly improves the band gaps and band structures of 2D and 1D systems, without significantly affecting the accuracy of the original TASK for the bulk 3D materials, when compared to the PBE-GGA and SCAN meta-GGA. We further demonstrate the applicability of mTASK by assessing the band structures of TMD nanoribbons with respect to various bending curvatures.