Strongly coupled intermediate electronic states in one-color two-photon single valence ionization of O2
- 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
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University Autonoma de Madrid (Spain)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Davis, CA (United States)
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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