Phonon-assisted upconverted emission is the heart of energy harvesting, bioimaging, optical cryptography, and optical refrigeration. It has been demonstrated that emerging two-dimensional (2D) semiconductors can provide an excellent platform for efficient phonon-assisted upconversion due to the enhanced optical transition strength and phonon-exciton interaction of 2D excitons. However, there is little research on the further enhancement of excitonic upconverted emission in 2D semiconductors. Here, we report the enhanced multiphoton upconverted emission of 2D excitons in doubly resonant plasmonic nanocavities. Owing to the enhanced light collection, enhanced excitation rate, and quantum efficiency enhancement arising from the Purcell effect, an upconverted emission amplification of >1000-fold and a decrease of 2~3 orders of magnitude in the saturated excitation power are achieved. These findings pave the way for the development of excitonic upconversion lasing, nanoscopic thermometry, and sensing, revealing the possibility of optical refrigeration in future 2D electronic or excitonic devices.

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.