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

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.

doi:10.1038/s41598-017-04638-0

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

Journal Article · Fri Jun 30 00:00:00 EDT 2017 · Scientific Reports

DOI:https://doi.org/10.1038/s41598-017-04638-0· OSTI ID:1418580

Jochim, Bethany ^[1]; Siemering, R. ^[2]; Zohrabi, M. ^[3]; Voznyuk, O. ^[4]; Mahowald, J. B. ^[4]; Schmitz, D. G. ^[4]; Betsch, K. J. ^[3]; Berry, Ben ^[3]; Severt, T. ^[3]; Kling, Nora G. ^[5]; Burwitz, T. G. ^[4]; Carnes, K. D. ^[3]; Kling, M. F. ^[5]; Ben-Itzhak, I. ^[3]; Wells, E. ^[4]; de Vivie-Riedle, R. ^[2]

Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab. and Dept. of Physics; OSTI
Ludwig Maximilian Univ., Munich (Germany). Dept. of Chemistry
Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab. and Dept. of Physics
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

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.

View Accepted Manuscript (DOE)

Research Organization:: Kansas State Univ., Manhattan, KS (United States)

Sponsoring Organization:: German Science Foundation (DFG); National Science Foundation (NSF); Oak Ridge Institute for Science and Education (ORISE), Oak Ridge, TN (United States); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0002378

OSTI ID:: 1418580

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 7; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Theory of Tunnel Ionization in Complex Systems Brabec, Thomas; Côté, Michel; Boulanger, Paul Physical Review Letters, Vol. 95, Issue 7 https://doi.org/10.1103/PhysRevLett.95.073001	journal	August 2005
Strong-Field Molecular Ionization from Multiple Orbitals Kotur, Marija; Weinacht, Thomas C.; Zhou, Congyi Physical Review X, Vol. 1, Issue 2 https://doi.org/10.1103/PhysRevX.1.021010	journal	November 2011
Electronic Predetermination of Ethylene Fragmentation Dynamics Xie, Xinhua; Roither, Stefan; Schöffler, Markus Physical Review X, Vol. 4, Issue 2 https://doi.org/10.1103/PhysRevX.4.021005	journal	April 2014
Attosecond physics Krausz, Ferenc; Ivanov, Misha Reviews of Modern Physics, Vol. 81, Issue 1 https://doi.org/10.1103/RevModPhys.81.163	journal	February 2009
Laser Tunnel Ionization from Multiple Orbitals in HCl Akagi, H.; Otobe, T.; Staudte, A. Science, Vol. 325, Issue 5946 https://doi.org/10.1126/science.1175253	journal	September 2009
Fundamentals of Attosecond Optics Chang, Zenghu CRC Press https://doi.org/10.1201/b10402	book	April 2016
Real-time pulse length measurement of few-cycle laser pulses using above-threshold ionization Sayler, A. M.; Rathje, Tim; Müller, W. Optics Express, Vol. 19, Issue 5 https://doi.org/10.1364/OE.19.004464	journal	January 2011

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Deformation of an inner valence molecular orbital in ethanol by an intense laser field Akagi, Hiroshi; Otobe, Tomohito; Itakura, Ryuji Science Advances, Vol. 5, Issue 5 https://doi.org/10.1126/sciadv.aaw1885	journal	May 2019

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