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arxiv 2505.07021 v1 pith:2D2YUCSE submitted 2025-05-11 cond-mat.mtrl-sci

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

classification cond-mat.mtrl-sci
keywords relaxationcoherenceexcited-stateexcitonprocessessemiconductorsapproachcoulomb
verification ladder T0 review T1 audit T2 compute T3 formal T4 reserved
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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 (TMDs), quasi-two-dimensional excitonic semiconductors in which atomistic design allows for tunable excited-state properties, such as relaxation lifetimes and photo-induced 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 multi-channel electron-hole pair relaxation processes, including phonon and Coulomb scattering as well as radiative recombination, and study their effect on the time-resolved excited-state propagation. Using monolayer MoSe$_2$ 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. 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.

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