Abstract
This work explores the interplay of electronic band structure, Coulomb interactions, and optical resonances that triggers high-harmonic generation in condensed matter systems driven by intense and ultrashort optical pulses. The authors results are in qualitative agreement with atomistic simulations of quasi one dimensional carbon nanotubes and provide a roadmap to identify material platforms for solid-state high-harmonic generation
Highlights
High-harmonic generation (HHG) is perhaps the most striking example of a nonlinear optical process and its ability to spectrally and temporally disperse intense laser light [1,2]
Concise theoretical explanations of the underlying physics were developed shortly thereafter, culminating in the celebrated three-step model of an atom interacting with a single cycle of an intense impinging optical field: tunnel ionization triggered by the driving electric field liberates an electron from the atom that gains additional kinetic energy as it is driven away
Seeking to optimize high-order harmonic generation (HHG) yields in condensed-matter systems, we explore the synergy between electronic band structure and optical resonances in finite SSH chains, which constitute a convenient, computationally inexpensive model that has already been demonstrated to qualitatively describe HHG predicted in the more rigorous time-dependent density functional theory (TDDFT) simulations of related 1D systems [33,34]
Summary
High-harmonic generation (HHG) is perhaps the most striking example of a nonlinear optical process and its ability to spectrally and temporally disperse intense laser light [1,2]. Theoretical proposals considered a three-step-like model in which an electron undergoes Bloch oscillations within an electronic band (either valence or conduction after interband tunneling) as a consequence of the change in direction of acceleration after half an optical cycle of the driving electric field [19,20,21]; the excited electron subsequently scatters within its band (i.e., intraband HHG) or recombines with the parent hole or ion (i.e., interband HHG) to recollide with the first- and second-nearest holes or ions This simplified description does not explain the role of electronelectron correlations, and available experiments and numerical simulations often do not elucidate the specific origin of generated harmonics (e.g., from interband or intraband charge-carrier motion); the generation of even-order harmonics, the existence of atto-chirps, the formation of a well-defined high-energy cutoff, and numerous aspects of the electronic band structure still remain underexplored in the context of solid-state HHG [22,23,24,25]. Our findings elucidate the roles of these features intrinsic to different solid-state systems, providing a road map for the identification and engineering of next-generation solid-state nonlinear optical devices capable of producing XUV light and/or attosecond pulses
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