Polarons shape the interlayer exciton emission of MoSe2/WSe2 heterobilayers

Abstract

Abstract We present evidence for the strong participation of hot phonons in the photo-physics of interlayer excitons (IXs) in 2H − and 3R − stacked MoSe2/WSe2 heterobilayers. Photoluminescence (PL) excitation spectroscopy reveals that excess energy associated with relaxation of intra-layer excitons towards IXs profoundly shapes the overall IX-PL lineshape, while the energy of the spectrally narrow discrete emission lines conventionally associated with trapped moiré IXs remain unaffected. A strikingly uniform line-spacing of the discrete emission lines is observed, along with characteristic temperature and excitation level dependence. Results suggest an entirely new picture of the discrete IX emission in which non-thermal phonons play a crucial role in shaping the spectrum. Excitation power and time resolved data indicate that these features are most likely polaronic in nature. Our findings extend the understanding of the photophysics of IXs beyond current interpretations based primarily on moiré-trapped IXs.