𝐴𝑏 initio density-matrix approach to exciton coherence: Phonon scattering, Coulomb interactions, and radiative recombination

Amit, Tomer; Vosco, Guy; Ben, Mauro Del; Refaely-Abramson, Sivan

doi:10.1103/phvn-cd52

𝐴𝑏 initio density-matrix approach to exciton coherence: Phonon scattering, Coulomb interactions, and radiative recombination

Journal Article · Sun Sep 28 20:00:00 EDT 2025 · Physical Review. B

DOI:https://doi.org/10.1103/phvn-cd52· OSTI ID:3007579

^[1]; ^[1]; Ben, Mauro Del ^[2]; ^[1]

Weizmann Institute of Science, Rehovot (Israel)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Relaxation processes following light excitation in semiconductors are key in materials-based quantum technology applications. These processes are broadly studied in atomically thin transition-metal dichalcogenides, quasi-two-dimensional excitonic semiconductors in which atomistic design allows for tunable excited-state properties, such as relaxation lifetimes and photoinduced coherence. In this work, we present a density-matrix-based approach to compute exciton relaxation within a many-body ab initio perspective. We expand our previously developed Lindblad density-matrix formalism to capture multichannel electron-hole pair relaxation processes, including phonon and Coulomb scattering as well as radiative recombination, and we study their effect on the time-resolved excited-state propagation. Using monolayer MoSe₂ as a prototypical example, we examine many-body effects on the time-dependent dynamics of photoactive excitations, exploring how the electron-hole pair interactions are reflected in variations of the excitation energy, spectral signature, and state coherence. In conclusion, our method supplies a detailed understanding of exciton relaxation mechanisms in realistic materials, offering a previously unexplored pathway to study excited-state dynamics in semiconductors from first principles.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Minerva Foundation; Israel Science Foundation; H2020 European Research Council

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 3007579

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 11 Vol. 112; ISSN 2469-9950; ISSN 2469-9969

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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𝐴𝑏 initio density-matrix approach to exciton coherence: Phonon scattering, Coulomb interactions, and radiative recombination

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