Many-body enhancement of high-harmonic generation in monolayer MoS2

Victor Chang Lee, Lun Yue, Mette B. Gaarde, Yang-hao Chan () and Diana Y. Qiu ()
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Victor Chang Lee: Yale University
Lun Yue: Louisiana State University
Mette B. Gaarde: Louisiana State University
Yang-hao Chan: Academia Sinica
Diana Y. Qiu: Yale University

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract Many-body effects play an important role in enhancing and modifying optical absorption and other excited-state properties of solids in the perturbative regime, but their role in high harmonic generation (HHG) and other nonlinear response beyond the perturbative regime is not well-understood. We develop here an ab initio many-body method to study nonperturbative HHG based on the real-time propagation of the non-equilibrium Green’s function with the GW self energy. We calculate the HHG of monolayer MoS2 and obtain good agreement with experiment, including the reproduction of characteristic patterns of monotonic and nonmonotonic harmonic yield in the parallel and perpendicular responses, respectively. Here, we show that many-body effects are especially important to accurately reproduce the spectral features in the perpendicular response, which reflect a complex interplay of electron-hole interactions (or exciton effects) in tandem with the many-body renormalization and Berry curvature of the independent quasiparticle bandstructure.

Date: 2024
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DOI: 10.1038/s41467-024-50534-3

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