November 6, 2013 | Diana Y. Qiu, Felipe H. da Jornada, and Steven G. Louie*
The paper presents first-principles calculations of the optical response of monolayer molybdenum disulfide (MoS$_2$) using the GW-Bethe Salpeter equation (GW-BSE) approach, including self-energy, excitonic, and electron-phonon effects. The authors identify a large and diverse number of strongly bound excitonic states with novel k-space characteristics, which were not previously observed experimentally or theoretically. The absorption spectrum is dominated by excitonic states with binding energies close to 1 eV and strong electron-phonon broadening in the visible to ultraviolet range. The study explains recent experimental measurements and resolves inconsistencies between previous GW-BSE calculations. The authors emphasize the importance of fine k-space sampling for accurate description of excitonic states and the need for a high energy cutoff and a large number of bands in the calculations. They also discuss the impact of electron-phonon interactions on the absorption spectrum, showing that the region between 2.2 and 2.8 eV contains multiple bright and dark excitonic states. The findings suggest that MoS$_2$ could be an excellent candidate for exploring inter- and intra-excitonic processes, and that variations in temperature, dielectric screening, and mechanical strain could affect the optical absorption in this region.The paper presents first-principles calculations of the optical response of monolayer molybdenum disulfide (MoS$_2$) using the GW-Bethe Salpeter equation (GW-BSE) approach, including self-energy, excitonic, and electron-phonon effects. The authors identify a large and diverse number of strongly bound excitonic states with novel k-space characteristics, which were not previously observed experimentally or theoretically. The absorption spectrum is dominated by excitonic states with binding energies close to 1 eV and strong electron-phonon broadening in the visible to ultraviolet range. The study explains recent experimental measurements and resolves inconsistencies between previous GW-BSE calculations. The authors emphasize the importance of fine k-space sampling for accurate description of excitonic states and the need for a high energy cutoff and a large number of bands in the calculations. They also discuss the impact of electron-phonon interactions on the absorption spectrum, showing that the region between 2.2 and 2.8 eV contains multiple bright and dark excitonic states. The findings suggest that MoS$_2$ could be an excellent candidate for exploring inter- and intra-excitonic processes, and that variations in temperature, dielectric screening, and mechanical strain could affect the optical absorption in this region.