Twist-Dependent Tuning of Excitonic Emissions in Bilayer WSe₂

Monolayer (ML) transition metal dichalcogenides (TMDCs) have been rigorously studied to comprehend their rich spin and valley physics, exceptional optical properties, and ability to open new avenues in fundamental research and technology. However, intricate analysis of twisted homobilayer (t-BL) systems is highly required due to the intriguing twist angle (t-angle)-dependent interlayer effects on optical and electrical properties. Here, we report the evolution of the interlayer effect on artificially stacked BL WSe₂, grown using chemical vapor deposition (CVD), with t-angle in the range of 0 ≤ θ ≤ 60°. Systematic analyses based on Raman and photoluminescence (PL) spectroscopies suggest intriguing deviations in the interlayer interactions, higher-energy exciton transitions (in the range of ∼1.6-1.7 eV), and stacking. In contrast to previous observations, we demonstrate a red shift in the PL spectra with t-angle. Density functional theory (DFT) is employed to understand the band-gap variations with t-angle. Exciton radiative lifetime has been estimated theoretically using temperature-dependent PL measurements, which shows an increase with t-angle that agrees with our experimental observations. This study presents the groundwork for further investigation of the evolution of various interlayer excitons and their dynamics with t-angle in homobilayer systems, critical for optoelectronic applications.