Phonon-assisted upconversion in twisted two-dimensional semiconductors

Phonon-assisted photon upconversion (UPC) is an anti-Stokes process in which incident photons achieve higher energy emission by absorbing phonons. This letter studies phonon-assisted UPC in twisted 2D semiconductors, in which an inverted contrast between UPC and conventional photoluminescence (PL) of WSe2 twisted bilayer is emergent. A 4-fold UPC enhancement is achieved in 5.5° twisted bilayer while PL weakens by half. Reduced interlayer exciton conversion efficiency driven by lattice relaxation, along with enhanced pump efficiency resulting from spectral redshift, lead to the rotation-angle-dependent UPC enhancement. The counterintuitive phenomenon provides a novel insight into a unique way that twisted angle affects UPC and light-matter interactions in 2D semiconductors. Furthermore, the UPC enhancement platform with various superimposable means offers an effective method for lighting bilayers and expanding the application prospect of 2D stacked van der Waals devices.