Optical properties of metallic MXene multilayers through advanced first-principles calculations

Abstract

Having a strong electromagnetic absorption, MXene multilayers are readily envisaged for applications in electromagnetic shields and related prospective technology. However, an $\mathit{ab}$ initio characterization of the optical properties of MXenes is still lacking, due in part to major difficulties with the treatment of metallicity in the first-principles approaches. Here we addressed the latter challenge, after a careful treatment of intraband transitions, to present a thorough analysis of the electronic and optical properties of a selected set of metallic MXene layers based on density functional theory (DFT) and many-body perturbation theory calculations. Our results reveal that the $\mathit{GW}$ corrections are particularly important in regions of the band structure where $\mathit{d}$ and $\mathit{p}$ states hybridize. For some systems, we show that $\mathit{GW}$ corrections open a gap between occupied states, resulting in a band structure that closely resembles that of an intrinsic transparent conductor, thereby opening an additional line of prospective applications for the MXenes family. Nevertheless, $\mathit{GW}$ and Bethe-Salpeter corrections have a minimal influence on the absorption spectra, in contrast to what is typically observed in semiconductor layers. Our present results suggest that calculations within the independent particle approximation (IPA) calculations are sufficiently accurate for assessing the optical characteristics of bulk-layered MXene materials. Finally, our calculated dielectric properties and absorption spectra, in agreement with existing experimental data, confirm the potential of MXenes as effective infrared emitters.