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.

Authors:

Han, Seunghwoi ^[1]; Ortmann, Lisa ^[2]; Kim, Hyunwoong  ^[3];

• Search DOE PAGES for author "Kim, Hyunwoong"
• Search DOE PAGES for ORCID "0000-0002-7253-5114"

Kim, Yong Woo ^[3]; Oka, Takashi ^[4]; Chacon, Alexis ^[5]; Doran, Brent ^[6]; Ciappina, Marcelo  ^[7];

• Search DOE PAGES for author "Ciappina, Marcelo"
• Search DOE PAGES for ORCID "0000-0002-1123-6460"

Lewenstein, Maciej ^[8]; Kim, Seung-Woo  ^[3];

• Search DOE PAGES for author "Kim, Seung-Woo"
• Search DOE PAGES for ORCID "0000-0003-0235-1739"

Kim, Seungchul  ^[9];

• Search DOE PAGES for author "Kim, Seungchul"
• Search DOE PAGES for ORCID "0000-0002-6765-2471"

Landsman, Alexandra S. ^[2]

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+ Show Author Affiliations

1. Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Mechanical Engineering; Univ. of Central Florida, Orlando, FL (United States), Institute for the Frontier of Attosecond Science and Technology, CREOL and Department of Physics
2. Max Planck Inst. for the Physics of Complex Systems, Dresden (Germany)
3. Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Mechanical Engineering
4. Max Planck Inst. for the Physics of Complex Systems, Dresden (Germany); Max Planck Inst. for Chemical Physics of Solids, Dresden (Germany)
5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Nonlinear Studies, Physics and Chemistry of Materials
6. Univ. of Oxford (United Kingdom). Mathematical Institute
7. Institute of Physics of the ASCR, Prague (Czechia)
8. ICFO – Institut de Ciències Fotòniques, The Barcelona Institute of Science and Technology, Castelldefels (Barcelona) (Spain) ICREA – Institució Catalana de Recerca i Estudis Avançats, Barcelona (Spain)
9. Pusan National Univ., Busan (Korea, Republic of). Dept. of Optics and Mechatronics Engineering, College of Nanoscience and Nanotechnology

Publication Date:

Mon Jul 22 00:00:00 EDT 2019

Research Org.:

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Org.:

USDOE Office of Science (SC)

OSTI Identifier:

1624172

Grant/Contract Number:  

AC52-06NA25396; RF-2012R1A3A1050386; NRF-2017M3D1A1039287; NRF-2018R1A4A1025623

Resource Type:

Accepted Manuscript

Journal Name:

Nature Communications

Additional Journal Information:

Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:

Nature Publishing Group

Country of Publication:

United States

Language:

English

Subject:

42 ENGINEERING; Science & Technology - Other Topics