Three-particle states and brightening of intervalley excitons in a doped MoS2 monolayer

Optical spectra of two-dimensional transition-metal dichalcogenides (TMDC) are influenced by complex multiparticle excitonic states. Their theoretical analysis requires solving the many-body problem, which in most cases, is prohibitively complicated. In this work, we calculate the optical spectra by exact diagonalization of the three-particle Hamiltonian within the Tamm-Dancoff approximation where the doping effects are accounted for via the Pauli blocking mechanism, modelled by a discretized mesh in the momentum space. The single-particle basis is extracted from the ab initio calculations. Obtained three-particle eigenstates and the corresponding transition dipole matrix elements are used to calculate the linear absorption spectra as a function of the doping level. Results for negatively doped MoS2 monolayer (ML) are in excellent quantitative agreement with the available experimental data, validating our approach. The results predict additional spectral features due to the intervalley exciton that is optically dark in an undoped ML but is brightened by the doping. Our approach can be applied to a plethora of other atomically thin semiconductors, where the doping induced brightening of the many-particle states is also anticipated..