Uncovering extreme nonlinear dynamics in solids through time-domain field analysis

Journal Article · 02 February 2023 · Physical Review. B

DOI: https://doi.org/10.1103/physrevb.107.054302 · OSTI ID:2004999

Keathley, P. D.  ^[1]; Jensen, S. V. B.  ^[2]; Yeung, M. ^[3]; Bionta, M. R.  ^[4]; Madsen, L. Bojer  ^[2]

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1. Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); SLAC
2. Aarhus University (Denmark)
3. Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)
4. Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)

Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Furthermore, time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters.

• Research Organization: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
• Sponsoring Organization: USDOE Office of Science (SC); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
• Grant/Contract Number: AC02-76SF00515
• OSTI ID: 2004999
• Journal Information: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 5 Vol. 107; ISSN 2469-9950
• Publisher: American Physical Society (APS)Copyright Statement
• Country of Publication: United States
• Language: English