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

James D. Gaynor, Ashley P. Fidler, Yuki Kobayashi, Yen Cheng Lin, Clare L. Keenan, Daniel M. Neumark*, Stephen R. Leone*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

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. 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.

Original languageEnglish (US)
Article number023526
JournalPhysical Review A
Volume107
Issue number2
DOIs
StatePublished - Feb 2023

Funding

Work for this paper was performed by personnel and equipment supported by the Office of Science, Office of Basic Energy Sciences through the Atomic, Molecular and Optical Sciences Program of the Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at LBNL under Contract No. DE-AC02-05CH11231. J.D.G. is grateful to the Arnold and Mabel Beckman Foundation for support as an Arnold O. Beckman Postdoctoral Fellow. A.P.F. acknowledges support from the National Science Foundation (NSF) Graduate Research Fellowship Program, and Y.K. and S.R.L. acknowledge NSF Grant No. CHE-1951317 and No. 2243756 for program support that led to the calculational aspect of the research. Y.-C.L. acknowledges financial support from the Taiwan Ministry of Education. Y.K. also acknowledges the support from the Urbanek-Chorodow Fellowship at Stanford University. C.L.K. acknowledges support from the NSF Research Experience for Undergraduates (REU) program Grants No. EEC-1461231 and No. EEC-1852537. The authors are grateful to Dr. Kenneth Schafer and Dr. Mette Gaarde for helpful discussions of nonresonant light matter interactions.

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

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