Theory of absorption lineshape in monolayers of transition metal dichalcogenides

Abstract

The linear absorption spectra in monolayers of transition metal dichalcogenides show pronounced signatures of the exceptionally strong exciton-phonon interaction in these materials. To account for both exciton and phonon physics in such optical signals, we compare different theoretical methods to calculate the absorption spectra using the example of $\mathrm{MoS}{\mathrm{e}}_2$. In this paper, we derive the equations of motion for the polarization either using a correlation expansion up to 4th Born approximation or a time convolutionless master equation. We show that the Born approximation might become problematic when not treated in high enough order, especially at high temperatures. In contrast, the time convolutionless formulation gives surprisingly good results despite its simplicity when compared to higher-order corrrelation expansion and therefore provides a powerful tool to calculate the lineshape of linear absorption spectra in the very popular monolayer materials.

to be published in Physical Review B

References in corpus (6)

• Computational 2D Materials Database: Electronic Structure of Transition-Metal Dichalcogenides and Oxides
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• Dark excitons in transition metal dichalcogenides
• Phonon Sidebands in Transition Metal Dichalcogenides
• Influence of the effective layer thickness on the groundstate and excitonic properties of transition-metal dichalcogenide systems
• Density-matrix theory of the optical dynamics and transport in quantum cascade structures: The role of coherence

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