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

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...

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Bibliographic Details
Published in:Nature communications 2019-07, Vol.10 (1), p.3272-6, Article 3272
Main Authors: Han, Seunghwoi, Ortmann, Lisa, Kim, Hyunwoong, Kim, Yong Woo, Oka, Takashi, Chacon, Alexis, Doran, Brent, Ciappina, Marcelo, Lewenstein, Maciej, Kim, Seung-Woo, Kim, Seungchul, Landsman, Alexandra S.
Format: Article
Language:English
Subjects:
140/125
639/624/400/3923
639/624/400/584
Crystal structure
ENGINEERING
Harmonic generations
Humanities and Social Sciences
Lasers
multidisciplinary
Nonlinear response
Optoelectronics
Physics
Sapphire
Scaling
Science
Science & Technology - Other Topics
Science (multidisciplinary)
Signal processing
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Summary: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. Characterizing higher order nonlinearities and responses to optical excitations in materials is challenging. Here, the authors use high harmonic generation in sapphire crystals to extract higher order susceptibilities and characterize the nonlinear electronic response directly from experimental measurements.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-019-11096-x