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Title: Strongly coupled intermediate electronic states in one-color two-photon single valence ionization of O2

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/5.0128846· OSTI ID:1960025
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [3]
  1. Graduate Group in Applied Science and Technology, University of California, Berkeley, California 94720, USA;Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA;Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University Autonoma de Madrid (Spain)
  3. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  4. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Davis, CA (United States)
+ Show Author Affiliations

Here, we present an experimental and theoretical energy- and angle-resolved investigation on the non-dissociative photoionization dynamics of near-resonant, one-color, two-photon, single valence ionization of neutral O2 molecules. Using 9.3 eV femtosecond pulses produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and O$$^{+}_{2}$$ cations produced from one-color, two-photon ionization in coincidence. The measured and calculated photoelectron angular distributions show agreement, which indicates that a superposition of two intermediate electronic states is dominantly involved and that wavepacket motion on those near-resonantly populated intermediate states does not play a significant role in the measured two-photon ionization dynamics. Here, we find greater utility in the diabatic representation compared to the adiabatic representation, where invoking a single valence-character diabat is sufficient to describe the underlying two-photon ionization mechanism.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Energy Research Scientific Computing Center (NERSC); USDOE
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231; BES-ERCAP-0020143; BES-ERCAP-0019776
OSTI ID:
1960025
Alternate ID(s):
OSTI ID: 1908855; OSTI ID: 1924471
Journal Information:
Journal of Chemical Physics, Vol. 158, Issue 2; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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