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

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 the 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 QPGW₀ methodologies. We observed consistent trends across Cr-based and other 2D materials compared by advanced GW calculations, suggesting that single-shot G₀W₀@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 G₀W₀@HSE06 approach may strongly overestimate gaps in some cases.