Upconversion photoluminescence excitation reveals exciton-trion and exciton-biexciton coupling in hBN/WS2/hBN van derWaals heterostructures

Monolayers of transition-metal dichalcogenides with direct band gap located at the binaryK(-)/K+ 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 WS2 monolayer. We propose that the energy gains required in the polarized upconversion photoluminescence originate from different interactions including resonant optical phonons, a cooling of resident electrons and a non-local and an anisotropic electron-hole exchange, respectively. The temperature dependence (7-120 K) of the excitonic upconversion intensity obtained at excitation energies corresponding to the biexciton and trions provides insight into an increasing phonon population as well as a thermally enhanced electron scattering. Our study sheds new light on the understanding of excitonic spin and valley properties of van derWaals heterostructures and improves the understanding of photonic upconversion mechanisms in two-dimensional quantum materials.

Automated summary

Monolayers of transition-metal dichalcogenides with direct band gap located at specific points in the Brillouin zone show promising applications in opto- and spin-electronics due to enhanced Coulomb interactions and specific spin-valley properties. Processes demonstrating the upconversion of light into bright intravalley excitons in WS2 monolayers provide insight into various interactions, including resonant optical phonons, cooling of resident electrons, and non-local electron-hole exchange. Temperature-dependent studies on excitonic upconversion intensity suggest increased phonon population and thermally enhanced electron scattering in two-dimensional quantum materials, shedding new light on excitonic properties and photonic upconversion mechanisms in van der Waals heterostructures.