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

Journal Article · · Nature Communications
 [1];  [2]; ORCiD logo [3];  [3];  [4];  [5];  [6]; ORCiD logo [7];  [8]; ORCiD logo [3]; ORCiD logo [9];  [2]
  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

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.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC52-06NA25396; RF-2012R1A3A1050386; NRF-2017M3D1A1039287; NRF-2018R1A4A1025623
OSTI ID:
1624172
Journal Information:
Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 28 works
Citation information provided by
Web of Science

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