The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields
Abstract
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 C2D2, C2D4 and C2D6 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:
-
- Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab. and Dept. of Physics
- Ludwig Maximilian Univ., Munich (Germany). Dept. of Chemistry
- Augustana College, Sioux Falls, SD (United States). Dept. of Physics
- 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:
- Research Org.:
- Kansas State Univ., Manhattan, KS (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Oak Ridge Institute for Science and Education (ORISE), Oak Ridge, TN (United States); National Science Foundation (NSF); German Science Foundation (DFG)
- OSTI Identifier:
- 1418580
- Grant/Contract Number:
- FG02-09ER16115; SC0002378
- Resource 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
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Jochim, Bethany, Siemering, R., Zohrabi, M., Voznyuk, O., Mahowald, J. B., Schmitz, D. G., Betsch, K. J., Berry, Ben, Severt, T., Kling, Nora G., Burwitz, T. G., Carnes, K. D., Kling, M. F., Ben-Itzhak, I., Wells, E., and de Vivie-Riedle, R. The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields. United States: N. p., 2017.
Web. doi:10.1038/s41598-017-04638-0.
Jochim, Bethany, Siemering, R., Zohrabi, M., Voznyuk, O., Mahowald, J. B., Schmitz, D. G., Betsch, K. J., Berry, Ben, Severt, T., Kling, Nora G., Burwitz, T. G., Carnes, K. D., Kling, M. F., Ben-Itzhak, I., Wells, E., & de Vivie-Riedle, R. The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields. United States. https://doi.org/10.1038/s41598-017-04638-0
Jochim, Bethany, Siemering, R., Zohrabi, M., Voznyuk, O., Mahowald, J. B., Schmitz, D. G., Betsch, K. J., Berry, Ben, Severt, T., Kling, Nora G., Burwitz, T. G., Carnes, K. D., Kling, M. F., Ben-Itzhak, I., Wells, E., and de Vivie-Riedle, R. Fri .
"The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields". United States. https://doi.org/10.1038/s41598-017-04638-0. https://www.osti.gov/servlets/purl/1418580.
@article{osti_1418580,
title = {The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields},
author = {Jochim, Bethany and Siemering, R. and Zohrabi, M. and Voznyuk, O. and Mahowald, J. B. and Schmitz, D. G. and Betsch, K. J. and Berry, Ben and Severt, T. and Kling, Nora G. and Burwitz, T. G. and Carnes, K. D. and Kling, M. F. and Ben-Itzhak, I. and Wells, E. and de Vivie-Riedle, R.},
abstractNote = {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 C2D2, C2D4 and C2D6 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.},
doi = {10.1038/s41598-017-04638-0},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Fri Jun 30 00:00:00 EDT 2017},
month = {Fri Jun 30 00:00:00 EDT 2017}
}
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