Exciton-Phonon Interaction and Relaxation Times from First Principles

Chen, Hsiao-Yi; Sangalli, Davide; Bernardi, Marco

doi:10.1103/physrevlett.125.107401

Exciton-Phonon Interaction and Relaxation Times from First Principles

Journal Article · Mon Aug 31 00:00:00 EDT 2020 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.125.107401· OSTI ID:1803599

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California Institute of Technology (CalTech), Pasadena, CA (United States); OSTI
Consiglio Nazionale delle Ricerche (CNR), Monterotondo Scalo (Italy). Institute of Structure of Matter (ISM); Universita degli Studi di Milano (Italy)
California Institute of Technology (CalTech), Pasadena, CA (United States)

Electron-phonon interactions are key to understanding the dynamics of electrons in materials and can be modeled accurately from first principles. However, when electrons and holes form Coulomb-bound states (excitons), quantifying their interactions and scattering processes with phonons remains an open challenge. Here we show a rigorous approach for computing exciton-phonon (ex-ph) interactions and the associated exciton dynamical processes from first principles. Starting from the ab initio Bethe-Salpeter equation, we derive expressions for the ex-ph matrix elements and relaxation times. Finally, we apply our method to bulk hexagonal boron nitride, for which we map the ex-ph relaxation times as a function of exciton momentum and energy, analyze the temperature and phonon-mode dependence of the ex-ph scattering processes, and accurately predict the phonon-assisted photoluminescence. The approach introduced in this work is general and provides a framework for investigating exciton dynamics in a wide range of materials.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: European Union’s Horizon 2020; Ministry of Education, University and Research (MIUR); National Science Foundation (NSF); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; SC0019166

OSTI ID:: 1803599

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 10 Vol. 125; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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