Predicting Fundamental Gaps of Chromium-Based 2D Materials Using GW Methods

TL;DR

This study evaluates various GW computational methods for accurately predicting the fundamental electronic gaps of chromium-based 2D materials, highlighting their strengths, limitations, and the importance of input choices.

Contribution

It systematically compares GW variants built on different DFT inputs for 2D materials, especially chromium-based, revealing insights into their predictivity and reliability.

Findings

Single-shot G₀W₀@PBE provides reasonable gap estimates with caution.

Vertex corrections impact quasiparticle correction behavior.

G₀W₀@HSE06 may overestimate gaps in some cases.

Abstract

Precise and accurate predictions of the two-dimensional (2D) material's fundamental gap are crucial for next-generation flexible electronic and photonic devices. We, therefore, evaluated the predictivity of the GW approach in its several variants built on various density functional theory (DFT) inputs. We identified reasons for significant discrepancies between generalized gradient approximation and hybrid DFT results for intricate cases of 2D materials containing chromium and evaluated the diverse behavior of subsequent quasiparticle corrections. We examined the impact of omitted vertex corrections using the more computationally intensive quasiparticle self-consistent QPGW and partially self-consistent QPGW$_0$ methodologies. We observed consistent trends across Cr-based and other 2D materials compared by advanced GW calculations, suggesting that single-shot G$_0$W$_0$@PBE can provide reasonable estimates of fundamental gaps when applied with caution. While this approach shows promise for a variety of 2D materials, including complicated antiferromagnetic chromium-based transition metal carbides (MXenes), further research is required to validate its reliability for strongly correlated systems. In contrast, the G$_0$W$_0$@HSE06 approach may strongly overestimate gaps in some cases.