2023/05/07 by Galit Cohen, Cohen, Galit, Jonah B. Haber +7 · 2 citations
Engineering · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #Computational Physics (physics.comp-ph) #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Perovskite Materials and Applications #Semiconductor Quantum Structures and Devices #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2305.04223
openalex publication_date 2023/05/07 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/01
Non-radiative exciton relaxation processes are critical for energy transduction efficiencies in optoelectronic materials, but how these processes are connected to the underlying crystal structure and its associated electron, exciton, and phonon band structures is poorly understood. Here, we present a first-principles approach to explore exciton relaxation pathways in pentacene, a paradigmatic molecular crystal and optoelectronic semiconductor. We compute the momentum- and band-resolved exciton-phonon interactions, and use them to analyse key scattering channels. We find that exciton intraband transitions on femtosecond timescales leading to dark-state occupation is a dominant nonradiative relaxation channel in pentacene. We further show how the nature of real-time propagation of the exciton wavepacket is connected with the longitudinal-transverse exciton splitting, stemming from crystal anisotropy, and concomitant anisotropic exciton and phonon dispersions. Our results provide a framework for understanding time-resolved exciton propagation and energy transfer in molecular crystals and beyond.