Excited-state vibronic wave-packet dynamics in H2 probed by XUV transient four-wave mixing
Abstract
The complex behavior of a molecular wave packet initiated by an extreme ultraviolet (XUV) pulse is investigated with noncollinear wave mixing spectroscopy. A broadband XUV pulse spanning 12-16 eV launches a wave packet in H2 comprising a coherent superposition of multiple electronic and vibrational levels. The molecular wave packet evolves freely until a delayed few-cycle optical laser pulse arrives to induce nonlinear signals in the XUV via four-wave mixing (FWM). The angularly resolved FWM signals encode rich energy exchange processes between the optical laser field and the XUV-excited molecule. The noncollinear geometry enables spatial separation of ladder and V- or Λ-type transitions induced by the optical field. Ladder transitions, in which the energy exchange with the optical field is around 3 eV, appear off axis from the incident XUV beam. Each vibrationally revolved FWM line probes a different part of the wave packet in energy, serving as a promising tool for energetic tomography of molecular wave packets. V- or Λ-type transitions, in which the energy exchange is well under 1 eV, result in on-axis nonlinear signals. The first-order versus third-order interference of the on-axis signal serves as a mapping tool of the energy flow pathways. Intra- and interelectronic potential energymore »
- Authors:
-
- Univ. of Science and Technology, Wuhan (China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), 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:
- 1580207
- Alternate Identifier(s):
- OSTI ID: 1419095
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 97; 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
Citation Formats
Cao, Wei, Warrick, Erika R., Fidler, Ashley, Leone, Stephen R., and Neumark, Daniel M. Excited-state vibronic wave-packet dynamics in H2 probed by XUV transient four-wave mixing. United States: N. p., 2018.
Web. doi:10.1103/physreva.97.023401.
Cao, Wei, Warrick, Erika R., Fidler, Ashley, Leone, Stephen R., & Neumark, Daniel M. Excited-state vibronic wave-packet dynamics in H2 probed by XUV transient four-wave mixing. United States. https://doi.org/10.1103/physreva.97.023401
Cao, Wei, Warrick, Erika R., Fidler, Ashley, Leone, Stephen R., and Neumark, Daniel M. Thu .
"Excited-state vibronic wave-packet dynamics in H2 probed by XUV transient four-wave mixing". United States. https://doi.org/10.1103/physreva.97.023401. https://www.osti.gov/servlets/purl/1580207.
@article{osti_1580207,
title = {Excited-state vibronic wave-packet dynamics in H2 probed by XUV transient four-wave mixing},
author = {Cao, Wei and Warrick, Erika R. and Fidler, Ashley and Leone, Stephen R. and Neumark, Daniel M.},
abstractNote = {The complex behavior of a molecular wave packet initiated by an extreme ultraviolet (XUV) pulse is investigated with noncollinear wave mixing spectroscopy. A broadband XUV pulse spanning 12-16 eV launches a wave packet in H2 comprising a coherent superposition of multiple electronic and vibrational levels. The molecular wave packet evolves freely until a delayed few-cycle optical laser pulse arrives to induce nonlinear signals in the XUV via four-wave mixing (FWM). The angularly resolved FWM signals encode rich energy exchange processes between the optical laser field and the XUV-excited molecule. The noncollinear geometry enables spatial separation of ladder and V- or Λ-type transitions induced by the optical field. Ladder transitions, in which the energy exchange with the optical field is around 3 eV, appear off axis from the incident XUV beam. Each vibrationally revolved FWM line probes a different part of the wave packet in energy, serving as a promising tool for energetic tomography of molecular wave packets. V- or Λ-type transitions, in which the energy exchange is well under 1 eV, result in on-axis nonlinear signals. The first-order versus third-order interference of the on-axis signal serves as a mapping tool of the energy flow pathways. Intra- and interelectronic potential energy curve transitions are decisively identified. The current study opens possibilities for accessing complete dynamic information in XUV-excited complex systems.},
doi = {10.1103/physreva.97.023401},
journal = {Physical Review A},
number = 2,
volume = 97,
place = {United States},
year = {Thu Feb 01 00:00:00 EST 2018},
month = {Thu Feb 01 00:00:00 EST 2018}
}
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Works referencing / citing this record:
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