No abstract

We present converged ab initio calculations of the optical absorption spectra of single-layer, double-layer, and bulk MoS 2 . Both the quasiparticle-energy calculations (on the level of the GW approximation ) and the calculation of the absorption spectra (on the level of the Bethe-Salpeter equation) explicitly include spin-orbit coupling, using the full spinorial Kohn-Sham wave functions as input. Without excitonic effects, the absorption spectra would have the form of a step function, corresponding to the joint density of states of a parabolic band dispersion in two dimensions. This profile is deformed by a pronounced bound excitonic peak below the continuum onset. The peak is split by spin-orbit interaction in the case of single-layer and (mostly) by interlayer interaction in the case of double-layer and bulk MoS 2 . The resulting absorption spectra are thus very similar in the three cases, but the interpretation of the spectra is different. Differences in the spectra can be seen in the shape of the absorption spectra at 3 eV where the spectra of the single and double layers are dominated by a strongly bound exciton.

Transition metal dichalcogenides (TMDs) are emerging as promising two-dimensional (2D) semiconductors for optoelectronic and flexible devices. However, a microscopic explanation of their photophysics, of pivotal importance for the understanding and optimization of device operation, is still lacking. Here, we use femtosecond transient absorption spectroscopy, with pump pulse tunability and broadband probing, to monitor the relaxation dynamics of single-layer MoS2 over the entire visible range, upon photoexcitation of different excitonic transitions. We find that, irrespective of excitation photon energy, the transient absorption spectrum shows the simultaneous bleaching of all excitonic transitions and corresponding red-shifted photoinduced absorption bands. First-principle modeling of the ultrafast optical response reveals that a transient bandgap renormalization, caused by the presence of photoexcited carriers, is primarily responsible for the observed features. Our results demonstrate the strong impact of many-body effects in the transient optical response of TMDs even in the low-excitation-density regime.