Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy
Abstract
Attosecond four-wave mixing (FWM) spectroscopy using an extreme ultraviolet (XUV) pulse and two noncollinear near-infrared (NIR) pulses is employed to measure Rydberg wave packet dynamics resulting from XUV excitation of a 3s electron in atomic argon into a series of autoionizing 3s–1np Rydberg states ~29 eV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the FWM emission signals of each individually detected state. A wave packet decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcited 3s–1 (n + 1) p states to the observed 3s–1np Rydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. Finally, the theory highlights that coherent amplitude transfer is driven nonresonantly to the 3s–1np states by the NIR light through 3s–1 (n + 1)s and 3s–1 (n – 1)d dark states during the FWM process.
- Authors:
-
[1];
[3];
[1];
[4];
[1]
- University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Princeton University, NJ (United States); University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- University of California, Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- University of Chicago, IL (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
- OSTI Identifier:
- 2004590
- Alternate Identifier(s):
- OSTI ID: 2234189
- Grant/Contract Number:
- AC02-76SF00515; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 107; Journal Issue: 2; Journal ID: ISSN 2469-9926
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; atomic orbital; autoionization & auger processes; light-matter interaction; optical coherence; four-wave mixing; high-harmonic generation
Citation Formats
Gaynor, James D., Fidler, Ashley P., Kobayashi, Yuki, Lin, Yen-Cheng, Keenan, Clare L., Neumark, Daniel M., and Leone, Stephen R. Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy. United States: N. p., 2023.
Web. doi:10.1103/physreva.107.023526.
Gaynor, James D., Fidler, Ashley P., Kobayashi, Yuki, Lin, Yen-Cheng, Keenan, Clare L., Neumark, Daniel M., & Leone, Stephen R. Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy. United States. https://doi.org/10.1103/physreva.107.023526
Gaynor, James D., Fidler, Ashley P., Kobayashi, Yuki, Lin, Yen-Cheng, Keenan, Clare L., Neumark, Daniel M., and Leone, Stephen R. Tue .
"Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy". United States. https://doi.org/10.1103/physreva.107.023526. https://www.osti.gov/servlets/purl/2004590.
@article{osti_2004590,
title = {Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy},
author = {Gaynor, James D. and Fidler, Ashley P. and Kobayashi, Yuki and Lin, Yen-Cheng and Keenan, Clare L. and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Attosecond four-wave mixing (FWM) spectroscopy using an extreme ultraviolet (XUV) pulse and two noncollinear near-infrared (NIR) pulses is employed to measure Rydberg wave packet dynamics resulting from XUV excitation of a 3s electron in atomic argon into a series of autoionizing 3s–1np Rydberg states ~29 eV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the FWM emission signals of each individually detected state. A wave packet decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcited 3s–1 (n + 1) p states to the observed 3s–1np Rydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. Finally, the theory highlights that coherent amplitude transfer is driven nonresonantly to the 3s–1np states by the NIR light through 3s–1 (n + 1)s and 3s–1 (n – 1)d dark states during the FWM process.},
doi = {10.1103/physreva.107.023526},
journal = {Physical Review A},
number = 2,
volume = 107,
place = {United States},
year = {Tue Feb 28 00:00:00 EST 2023},
month = {Tue Feb 28 00:00:00 EST 2023}
}
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