Optical spectrum of MoS2: many-body effects and diversity of exciton states

Phys Rev Lett. 2013 Nov 22;111(21):216805. doi: 10.1103/PhysRevLett.111.216805. Epub 2013 Nov 20.


We present first-principles calculations of the optical response of monolayer molybdenum disulfide employing the GW-Bethe-Salpeter equation (GW-BSE) approach including self-energy, excitonic, and electron-phonon effects. We show that monolayer MoS2 possesses a large and diverse number of strongly bound excitonic states with novel k-space characteristics that were not previously seen experimentally or theoretically. The absorption spectrum is shown to be dominated by excitonic states with a binding energy close to 1 eV and by strong electron-phonon broadening in the visible to ultraviolet range. Our results explain recent experimental measurements and resolve inconsistencies between previous GW-BSE calculations.