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Title: Autoionization dynamics of (2 P 1/2) ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses

Abstract

The autoionization dynamics of the (2P1/2)ns/d Rydberg states in krypton are investigated using spatially isolated wave-mixing signals generated with a short train of subfemtosecond extreme ultraviolet (XUV) pulses and noncollinear, few-cycle near infrared pulses. Despite ubiquitous quantum beat oscillations from XUV-induced coherences within the excited-state manifold, these wave-mixing spectra allow for the simultaneous evaluation of autoionization lifetimes from a series of Rydberg states above the first ionization potential. Experimentally measured lifetimes of 22 ± 8 fs, 33 ± 6 fs, and 49 ± 6 fs for the wave-mixing signals emitting from the (2P1/2)6d/8s, (2P1/2)7d/9s, and (2P1/2)8d/10s resonances compare favorably with lifetimes for the (2P1/2)6d, 7d, and 8d Rydberg states determined from spectral linewidths. Analysis of the quantum beats reveals that the enhancement of wave-mixing pathways that couple the (2P1/2)nd states to themselves leads to individual reporter state-dependent decays in the wave-mixing signals. Lastly, the results demonstrate the promise of wave-mixing spectroscopies with subfemtosecond XUV pulses to provide valuable insights into processes governed by electronic dynamics.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [2];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1580916
Alternate Identifier(s):
OSTI ID: 1562580
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 11; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; Wave-mixing; autoionization; attosecond; nonlinear optics; lifetimes

Citation Formats

Fidler, Ashley P., Marroux, Hugo J. B., Warrick, Erika R., Bloch, Etienne, Cao, Wei, Leone, Stephen R., and Neumark, Daniel M. Autoionization dynamics of (2 P 1/2) ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses. United States: N. p., 2019. Web. https://doi.org/10.1063/1.5113912.
Fidler, Ashley P., Marroux, Hugo J. B., Warrick, Erika R., Bloch, Etienne, Cao, Wei, Leone, Stephen R., & Neumark, Daniel M. Autoionization dynamics of (2 P 1/2) ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses. United States. https://doi.org/10.1063/1.5113912
Fidler, Ashley P., Marroux, Hugo J. B., Warrick, Erika R., Bloch, Etienne, Cao, Wei, Leone, Stephen R., and Neumark, Daniel M. Wed . "Autoionization dynamics of (2 P 1/2) ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses". United States. https://doi.org/10.1063/1.5113912. https://www.osti.gov/servlets/purl/1580916.
@article{osti_1580916,
title = {Autoionization dynamics of (2 P 1/2) ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses},
author = {Fidler, Ashley P. and Marroux, Hugo J. B. and Warrick, Erika R. and Bloch, Etienne and Cao, Wei and Leone, Stephen R. and Neumark, Daniel M.},
abstractNote = {The autoionization dynamics of the (2P1/2)ns/d Rydberg states in krypton are investigated using spatially isolated wave-mixing signals generated with a short train of subfemtosecond extreme ultraviolet (XUV) pulses and noncollinear, few-cycle near infrared pulses. Despite ubiquitous quantum beat oscillations from XUV-induced coherences within the excited-state manifold, these wave-mixing spectra allow for the simultaneous evaluation of autoionization lifetimes from a series of Rydberg states above the first ionization potential. Experimentally measured lifetimes of 22 ± 8 fs, 33 ± 6 fs, and 49 ± 6 fs for the wave-mixing signals emitting from the (2P1/2)6d/8s, (2P1/2)7d/9s, and (2P1/2)8d/10s resonances compare favorably with lifetimes for the (2P1/2)6d, 7d, and 8d Rydberg states determined from spectral linewidths. Analysis of the quantum beats reveals that the enhancement of wave-mixing pathways that couple the (2P1/2)nd states to themselves leads to individual reporter state-dependent decays in the wave-mixing signals. Lastly, the results demonstrate the promise of wave-mixing spectroscopies with subfemtosecond XUV pulses to provide valuable insights into processes governed by electronic dynamics.},
doi = {10.1063/1.5113912},
journal = {Journal of Chemical Physics},
number = 11,
volume = 151,
place = {United States},
year = {2019},
month = {9}
}

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