arXiv · 2607.18183
Excitonic effects in the photocarriers dynamics of two-dimensional materials
Abstract
We investigate the role of excitonic correlations in shaping the ultrafast dynamics of photoexcited carriers in semiconductors. Conventional approaches describe relaxation within single-particle frameworks, where electron-electron and electron-phonon scattering drive thermalization toward Fermi-Dirac distributions, neglecting electron-hole correlations that dominate near band edges. We introduce a two-particle framework based on excitonic Bloch equations (XBE) that captures carrier-phonon scattering and explicitly accounts for exciton formation. Applying this approach to non-resonantly photoexcited WSe$_2$ monolayers, we reveal qualitatively different carrier relaxation pathways: in contrast to state-of-the-art methods, XBE predict enhanced intervalley scattering and dominant carrier population in Q valleys over K valleys, in agreement with time-resolved ARPES experiments. Moreover, the momentum distribution of thermalized carriers is shaped by exciton wavefunctions rather than by Fermi-Dirac statistics, signaling the formation of a correlated nonequilibrium state. These results establish excitonic correlations as a key mechanism governing photocarrier dynamics in excitonic materials.
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Carlos Betancur, Gianluca Stefanucci, Enrico Perfetto. 2026-07-20. Excitonic effects in the photocarriers dynamics of two-dimensional materials. https://doi.org/10.1021/acs.nanolett.6c01651
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