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Emerging photo-induced excitonic processes in transition metal dichalcogenide(TMD) heterobilayers, e.g., coupling, dephasing, and energy transfer of intra-and inter-layer excitons, allow new opportunities for ultrathin photonicdevices. Yet, with the associated large degree of spatial heterogeneity,understanding and controlling their complex competing interactions at thenanoscale remains a challenge. Here, we present an all-round dynamic control ofintra- and inter-layer excitonic processes in aWSe$_2$/Mo$_{0.5}$W$_{0.5}$Se$_2$ heterobilayer using multifunctionaltip-enhanced photoluminescence (TEPL) spectroscopy. Specifically, we controlthe radiative recombination path and emission rate, electronic bandgap energy,and neutral to charged exciton conversion with <20 nm spatial resolution in areversible manner. It is achieved through the tip-induced engineering of Autip-heterobilayer distance and interlayer distance, GPa scale local pressure,and plasmonic hot-electron injection respectively, with simultaneousspectroscopic TEPL measurements. This unique nano-opto-electro-mechanicalcontrol approach provides new strategies for developing versatilenano-excitonic devices based on TMD heterobilayers.

Dynamical Control of Interlayer Excitons and Trions in WSe$_2$/Mo$_{0.5}$W$_{0.5}$Se$_2$ Heterobilayer via Tunable Near-Field Cavity