Extraction of higher-order nonlinear electronic response in solids using high harmonic generation

Seunghwoi Han, Lisa Ortmann, Hyunwoong Kim, Yong Woo Kim, Takashi Oka, Alexis Chacon, Brent Doran, Marcelo Ciappina, Maciej Lewenstein, Seung-Woo Kim (), Seungchul Kim () and Alexandra S. Landsman
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Seunghwoi Han: Korea Advanced Institute of Science and Technology (KAIST)
Lisa Ortmann: Max Planck Institute for the Physics of Complex Systems
Hyunwoong Kim: Korea Advanced Institute of Science and Technology (KAIST)
Yong Woo Kim: Korea Advanced Institute of Science and Technology (KAIST)
Takashi Oka: Max Planck Institute for the Physics of Complex Systems
Alexis Chacon: Physics and Chemistry of Materials T1-Division, Los Alamos National Laboratory
Brent Doran: University of Oxford
Marcelo Ciappina: Institute of Physics of the ASCR, ELI-Beamlines
Maciej Lewenstein: ICFO – Institut de Ciències Fotòniques, The Barcelona Institute of Science and Technology
Seung-Woo Kim: Korea Advanced Institute of Science and Technology (KAIST)
Seungchul Kim: Pusan National University
Alexandra S. Landsman: Max Planck Institute for the Physics of Complex Systems

Nature Communications, 2019, vol. 10, issue 1, 1-6

Abstract: Abstract Nonlinear susceptibilities are key to ultrafast lightwave driven optoelectronics, allowing petahertz scaling manipulation of the signal. Recent experiments retrieved a 3rd order nonlinear susceptibility by comparing the nonlinear response induced by a strong laser field to a linear response induced by the otherwise identical weak field. The highly nonlinear nature of high harmonic generation (HHG) has the potential to extract even higher order nonlinear susceptibility terms. However, up till now, such characterization has been elusive due to a lack of direct correspondence between high harmonics and nonlinear susceptibilities. Here, we demonstrate a regime where such correspondence can be clearly made, extracting nonlinear susceptibilities (7th, 9th, and 11th) from sapphire of the same order as the measured high harmonics. The extracted high order susceptibilities show angular-resolved periodicities arising from variation in the band structure with crystal orientation. Our results open a door to multi-channel signal processing, controlled by laser polarization.

Date: 2019
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DOI: 10.1038/s41467-019-11096-x

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