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; Alexandra S. Landsman

doi:10.1038/s41467-019-11096-x

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, Alexandra S. Landsman

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

34 Scopus citations

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.

Original language	English
Article number	3272
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-11096-x
State	Published - 1 Dec 2019
Externally published	Yes

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title = "Extraction of higher-order nonlinear electronic response in solids using high harmonic generation",

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.",

author = "Seunghwoi Han and Lisa Ortmann and Hyunwoong Kim and Kim, {Yong Woo} and Takashi Oka and Alexis Chacon and Brent Doran and Marcelo Ciappina and Maciej Lewenstein and Kim, {Seung Woo} and Seungchul Kim and Landsman, {Alexandra S.}",

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doi = "10.1038/s41467-019-11096-x",

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AU - Han, Seunghwoi

AU - Ortmann, Lisa

AU - Kim, Hyunwoong

AU - Kim, Yong Woo

AU - Oka, Takashi

AU - Chacon, Alexis

AU - Doran, Brent

AU - Ciappina, Marcelo

AU - Lewenstein, Maciej

AU - Kim, Seung Woo

AU - Kim, Seungchul

AU - Landsman, Alexandra S.

PY - 2019/12/1

Y1 - 2019/12/1

N2 - 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.

AB - 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.

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

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