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• W2977127564 abstract "When short and intense laser pulses interact with nanosystems which include plasmonic nanoparticles (NPs) and molecules, the laser induced spatially inhomogeneous near-fields modify the molecule's electron dynamics. Consequently, this affects the high-order harmonic generation (HHG) processes. Although a lot of experimental and theoretical work have been devoted to study the plasmon-driven HHG processes of atoms or diatomic molecules, there are no clear pictures to show how the electronic trajectories and spectral characters vary with the locations of polyatomic molecules. Here we perform a comprehensive theoretical study on the coupled dynamics between the spatially inhomogeneous fields and matter by combining the computational electrodynamic model with the time-dependent density functional theory. The plasmon-driven electron dynamics and HHG spectra of a benzene molecule in the vicinity of a gold nanosphere or in the gap of a pair of nanospheres have been investigated. The unique phenomena arisen from the surface-enhanced near-field are described and the underlying mechanism which determines the salient features of plasmon-driven HHG is presented. Our study demonstrates that the HHG spectral features are sensitive to the molecule-NP's distance and the incident light's polarization, and that the intensities of lower-order harmonics follow an exponentially decay with the molecule-NP's distance and the laser's polarization direction. Additionally, we find that when the incident light frequency is resonant with plasmon excitation, the obvious phase difference between the x- and y -components of near fields makes the electronic trajectories obviously follow elliptical paths. However, that elliptically polarized light does not generate the strikingly different spectra due to the near field's spatial inhomogeneity." @default.
• W2977127564 created "2019-10-03" @default.
• W2977127564 creator A5001497356 @default.
• W2977127564 creator A5030409288 @default.
• W2977127564 date "2019-10-14" @default.
• W2977127564 modified "2023-10-16" @default.
• W2977127564 title "Plasmon-driven high harmonic generation of benzene: effect of spatial inhomogenity of near field" @default.
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• W2977127564 doi "https://doi.org/10.1088/2516-1075/ab47ef" @default.
• W2977127564 hasPublicationYear "2019" @default.
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