Tunable interlayer excitons and switchable interlayer trions via dynamic near-field cavity

Emerging photo-induced excitonic processes in transition metal dichalcogenide (TMD) heterobilayers, e.g., interplay of intra- and inter-layer excitons and conversion of excitons to trions, allow new opportunities for ultrathin hybrid photonic devices. However, with the associated large degree of spatial heterogeneity, understanding and controlling their complex competing interactions in TMD heterobilayers at the nanoscale remains a challenge. Here, we present an all-round dynamic control of interlayer-excitons and -trions in a WSe₂/Mo_0.5 W_0.5 Se₂ heterobilayer using multifunctional tip-enhanced photoluminescence (TEPL) spectroscopy with <20 nm spatial resolution. Specifically, we demonstrate the bandgap tunable interlayer excitons and the dynamic interconversion between interlayer-trions and -excitons, through the combinational tip-induced engineering of GPa-scale pressure and plasmonic hot electron injection, with simultaneous spectroscopic TEPL measurements. This unique nano-opto-electro-mechanical control approach provides new strategies for developing versatile nano-excitonic/trionic devices using TMD heterobilayers.