A method to restore the intrinsic dielectric functions of 2D materials in periodic calculations and its applications to the dielectric and optical properties of ultrathin h-BN and MoS2

TL;DR

This paper introduces a method to accurately determine the intrinsic dielectric functions of 2D materials in periodic calculations, correcting for vacuum spacing effects, and applies it to study ultrathin h-BN and MoS2.

Contribution

The authors present a novel approach to restore the intrinsic dielectric functions of 2D materials, improving the accuracy of dielectric and optical property predictions in computational models.

Findings

Out-of-plane dielectric constants increase with layer number.

In-plane dielectric properties remain unchanged with layer number.

The method yields results in better agreement with experimental data.

Abstract

Previous calculations of the dielectric and optical properties of 2D materials often overlooked or circumvented the influence of vacuum spacing introduced in periodic calculations, which gave rise to mispredictions of the intrinsic properties of 2D materials or merely qualitative results. We first elucidate the relationship between the vacuum spacing and the dielectric and optical properties of 2D materials in periodic calculations, and then bring forward an effective method to accurately predict the dielectric and optical properties of 2D materials by restoring the intrinsic dielectric functions of 2D materials independent of the additional vacuum spacing. As examples, the intrinsic dielectric and optical properties of ultrathin h-BN and MoS2 from monolayer to pentalayer, including dielectric functions, optical absorption coefficients, refraction indexes, reflectivities, extinction coefficients, and energy loss functions, have been calculated by our method. Our calculations reveal that the out-of-plane optical dielectric constants, static refraction indexes, and static reflectivities of 2D h-BN and MoS2 increase as the number of layers increases, while the in-plane counterparts remain unchanged. Excitonic frequency-dependent optical properties of h-BN and MoS2 from monolayer to bulk are also calculated by solving the Bethe-Salpeter equation and show strong anisotropy. In better agreement with experimental results than previous calculations, the presented method demonstrates enormous potential to investigate the dielectric and optical properties of other 2D materials extensively and quantitively.