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Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy

Journal Article · · Physical Review A
 [1];  [2];  [3];  [4];  [5];  [4];  [4]
  1. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC
  2. Princeton University, NJ (United States); University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  3. University of California, Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  4. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  5. University of Chicago, IL (United States)
+ Show Author Affiliations
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.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-05CH11231; AC02-76SF00515
OSTI ID:
2004590
Alternate ID(s):
OSTI ID: 2234189
Journal Information:
Physical Review A, Journal Name: Physical Review A Journal Issue: 2 Vol. 107; ISSN 2469-9926
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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