Title: Wave packet dynamics and control in excited states of molecular nitrogen

Journal Article · · Journal of Chemical Physics
DOI: https://doi.org/10.1063/5.0188182 · OSTI ID:2481413
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  1. Nagoya Univ. (Japan)
  2. Tohoku Univ., Sendai (Japan)
  3. Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada). Energie, Matériaux et Télécommunications
  4. Argonne National Laboratory (ANL), Argonne, IL (United States)
  5. Lund Univ. (Sweden)
  6. Technische Univ. Wien (Austria)
  7. Stefan-Albert-Ludwigs-Universität Freiburg (Germany)
  8. ELI-HU Research and Development Non-Profit Ltd., Szeged (Hungary). ELI-ALPS Research Institute
  9. Elettra Sincrotrone Trieste (Italy)
  10. Nagoya Univ. (Japan); Elettra Sincrotrone Trieste (Italy)

Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N2. Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ~ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
German Research Foundation (DFG); Japan Society for the Promotion of Science (JSPS) - KAKENHI; Knut and Alice Wallenberg Foundation (KAWF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2481413
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 10 Vol. 160; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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