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Title: The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields

Much of our intuition about strong-field processes is built upon studies of diatomic molecules, which typically have electronic states that are relatively well separated in energy. In polyatomic molecules, however, the electronic states are closer together, leading to more complex interactions. A combined experimental and theoretical investigation of strong-field ionization followed by hydrogen elimination in the hydrocarbon series C 2D 2, C 2D 4 and C 2D 6 reveals that the photofragment angular distributions can only be understood when the field-dressed orbitals rather than the field-free orbitals are considered. Our measured angular distributions and intensity dependence show that these field-dressed orbitals can have strong Rydberg character for certain orientations of the molecule relative to the laser polarization and that they may contribute significantly to the hydrogen elimination dissociative ionization yield. Thus, these findings suggest that Rydberg contributions to field-dressed orbitals should be routinely considered when studying polyatomic molecules in intense laser fields.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [3] ;  [3] ;  [1] ;  [1] ;  [1] ;  [4] ;  [3] ;  [1] ;  [4] ;  [1] ;  [3] ;  [2]
  1. Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab. and Dept. of Physics
  2. Ludwig Maximilian Univ., Munich (Germany). Dept. of Chemistry
  3. Augustana College, Sioux Falls, SD (United States). Dept. of Physics
  4. Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab. and Dept. of Physics; Ludwig Maximilian Univ., Munich (Germany). Dept. of Physics
Publication Date:
Grant/Contract Number:
FG02-09ER16115; SC0002378
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Kansas State Univ., Manhattan, KS (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Oak Ridge Institute for Science and Education (ORISE), Oak Ridge, TN (United States); National Science Foundation (NSF); German Science Foundation (DFG)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 74 ATOMIC AND MOLECULAR PHYSICS
OSTI Identifier:
1418580