Quasiparticle band structure engineering in van der Waals heterostructures via dielectric screening

TL;DR

This paper introduces a computational method to predict how dielectric screening in van der Waals heterostructures affects the band gaps of 2D materials, enabling precise band structure engineering.

Contribution

It presents a general, efficient GΔW method using the QEH model to accurately calculate band gap renormalization in 2D heterostructures, surpassing traditional DFT approaches.

Findings

Band gap reduction scales inversely with 2D material polarizability.

The method accurately matches full GW calculations.

Dielectric engineering effectively tailors 2D material properties.

Abstract

The idea of combining different two-dimensional (2D) crystals in van der Waals heterostructures (vdWHs) has led to a new paradigm for band structure engineering with atomic precision. Due to the weak interlayer couplings, the band structures of the individual 2D crystals are largely preserved upon formation of the heterostructure. However, regardless of the details of the interlayer hybridisation, the size of the 2D crystal band gaps are always reduced due to the enhanced dielectric screening provided by the surrounding layers. The effect can be on the order of electron volts, but its precise magnitude is non-trivial to predict because of the non-local nature of the screening in quasi-2D materials, and it is not captured by effective single-particle methods such as density functional theory. Here we present an efficient and general method for calculating the band gap renormalization of a 2D material embedded in an arbitrary vdWH. The method evaluates the change in the GW self-energy of the 2D material from the change in the screened Coulomb interaction. The latter is obtained using the quantum-electrostatic heterostructure (QEH) model. We benchmark the G$\Delta$W method against full first-principles GW calculations and use it to unravel the importance of screening-induced band structure renormalisation in various vdWHs. A main result is the observation that the size of the band gap reduction of a given 2D material when inserted into a heterostructure scales inversely with the polarisability of the 2D material. Our work demonstrates that dielectric engineering \emph{via} van der Waals heterostructuring represents a promising strategy for tailoring the band structure of 2D materials.