Photon Upconversion of Defect-Bound Excitons in hBN-Encapsulated MoS Monolayer.

Atomic defects associated with vacancies in two-dimensional transition metal dichalcogenide monolayers efficiently trap charged carriers and strongly localize excitons. Defects in semiconducting monolayers are seldomly utilized for enhancing optical phenomena, although they may provide resonant intermediate states within the energy band gap for applications with multiphoton excitations, like highly efficient and thermally robust photon upconversion. In an MoS monolayer encapsulated by hBN with high defect and resident electron densities, we observe an upconversion of localized exciton (X) emission with a huge energy gain of up to 290 meV.

Upconversion photoluminescence excitation reveals exciton-trion and exciton-biexciton coupling in hBN/WS[Formula: see text]/hBN van der Waals heterostructures.

Monolayers of transition-metal dichalcogenides with direct band gap located at the binary [Formula: see text] points of the Brillouin zone are promising materials for applications in opto- and spin-electronics due to strongly enhanced Coulomb interactions and specific spin-valley properties. They furthermore represent a unique platform to study electron-electron and electron-phonon interactions in diverse exciton complexes. Here, we demonstrate processes in which the neutral biexciton and two negative trions, namely the spin-triplet and spin-singlet trions, upconvert light into a bright intravalley exciton in an hBN-encapsulated WS[Formula: see text] monolayer.