Phonon-assisted photoluminescence of bilayer MoS$_2$ from first principles

Abstract

In indirect band gap materials, phonon-assisted processes are key mechanisms for photoluminescence (PL). Using a first-principles many-body approach, we systematically investigate the phonon-assisted PL in bilayer MoS$_2$ and its dependence on temperature and external tensile strain. The effects of phonons are accounted for using a supercell approach: we identify the phonon momenta that are important to PL, construct supercells that are commensurate with these phonons, and examine the changes in the optical absorption after explicit displacements of atoms along each phonon mode. The PL intensity is then obtained via the van Roosbroeck-Shockley relationship from the optical absorption spectra. This approach enables us to investigate phonon-absorption and phonon-emission processes separately and how each process depends on temperature. Our results reveal that optical phonons associated with out-of-plane vibrations of S atoms and in-plane vibrations of Mo atoms contribute most to the indirect PL for unstrained bilayer MoS$_2$. Additionally, we also discuss how the PL spectra and the phonon contributions evolve with strain. In particular, we show that at high strain, additional phonon channels become available due to the modulation of the electronic band structure.