Resonant Raman signatures of two-dimensional layered materials from first-principles calculations

Two-dimensional layered materials (2DMs) continue to attract increased research interest as promising building blocks for novel electronic devices. Their electronic properties can be tuned via varying parameters like the number of layers, the layer-stacking order, or applying tensile strain. With such great tunability, exact property control is a key challenge. Raman spectroscopy is a nondestructive tool that is sensitive to subtle structural and electronic changes. Resonant Raman spectroscopy with varying wavelengths of the excitation laser allows for additional insights into the electronic transitions of the studied system. While straightforward experimentally, theoretical modeling of resonant Raman spectra requires the application and efficient implementation of the third-order time-dependent perturbation theory. Here, we present a Density Functional Theory based study of the resonant Raman spectra of various systems including graphene nanoribbons and transition metal dichalcogenides. We discuss the agreement with experimentally available data and provide pathways to property identification from resonant Raman fingerprints.