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arXiv · 2504.02567

High harmonic generation in monolayer MoS2 controlled by resonant and near-resonant pulses on ultrashort time scales

Pavel Peterka·Artur O. Slobodeniuk·Tomáš Novotný·Pawan Suthar·Miroslav Bartoš·František Trojánek·Petr Malý·Martin Kozák
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Abstract

We report on experimental investigation of nonperturbative high harmonic generation (HHG) in monolayer MoS2 in the ultraviolet spectral region driven by mid-infrared light. We study how the HHG is influenced by pre-excitation of the monolayer using resonant and near-resonant pulses in a pump-probe-like scheme. The resonant light creates high density exciton population. Due to ultrafast dephasing caused by electron-electron scattering, the HHG is suppressed in the presence of pre-excited carriers. In the case of near-resonant excitation with photon energy below the exciton transition, the dynamics of the observed suppression of the HHG yield contains a fast component which is a consequence of momentum scattering at carriers, which are excited by two-photon transition when the two pulses temporally overlap in the sample. This interpretation is supported by comparison of the experimental data with theoretical calculations of two-photon absorption spectrum of MoS2 monolayer. This work demonstrates a possibility to control HHG in lowdimensional materials on ultrashort timescales by combining the driving strong-field pulse with a weak near-resonant light.

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Pavel Peterka, Artur O. Slobodeniuk, Tomáš Novotný, Pawan Suthar, Miroslav Bartoš, František Trojánek, Petr Malý, Martin Kozák. 2025-04-03. High harmonic generation in monolayer MoS2 controlled by resonant and near-resonant pulses on ultrashort time scales. https://doi.org/10.1063/5.0158995

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