Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect

Abstract

Excitons, Coulomb-bound electron-hole pairs, are elementary photo-excitations in semiconductors that can couple to light through radiative relaxation. In contrast, dark excitons (X_D) show anti-parallel spin configuration with generally forbidden radiative emission. Because of their long lifetimes, these dark excitons are appealing candidates for quantum computing and optoelectronics. However, optical read-out and control of X_D states has remained challenging due to their decoupling from light. Here, we present a tip-enhanced nano-optical approach to induce, switch and programmably modulate the X_D emission at room temperature. Using a monolayer transition metal dichalcogenide (TMD) WSe₂ on a gold substrate, we demonstrate ~6 × 10⁵-fold enhancement in dark exciton photoluminescence quantum yield achieved through coupling of the antenna-tip to the dark exciton out-of-plane optical dipole moment, with a large Purcell factor of ≥2 × 10³ of the tip-sample nano-cavity. Our approach provides a facile way to harness excitonic properties in low-dimensional semiconductors offering new strategies for quantum optoelectronics.