Anomalous redshift in interlayer exciton emission with increasing twist angle in WSe₂/MoSe₂ heterostructures

Abstract Van der Waals heterostructures utilizing semiconducting transition metal dichalcogenide (TMDC) monolayers have surfaced as compelling candidates due to their intriguing optical characteristics, which can be effectively controlled by the manipulation of the stacking twist angle. This study investigates the intricate correlation between twist angle, band offset, and interlayer exciton emission within twisted WSe2/MoSe2 heterostructures. Our findings suggest a crucial influence of monolayer stacking order on the band offset and the dipole orientation in twisted heterostructures that leads to either blueshift or redshift in emission energy. Herein, we fabricate heterobilayers with twist angles varying from 1° to 56° and observe an anomalous redshift energy of 100 meV in the interlayer exciton emission. Additionally, photoluminescence excitation spectroscopy measurements highlight the systematic twist angle dependence of intralayer exciton resonances, indicating significant angle dependent effects on individual monolayer bandgaps and on the interlayer coupling strength. Our fundamental study of exciton resonances provides comprehensive insights into the nuanced interplay between twist angle, dipole orientation, and dielectric asymmetry, providing a deeper understanding of the factors governing the optical properties of layered TMDC heterostructures.