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

Autor: Jochim B; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA., Siemering R; Department für Chemie, Ludwig-Maximilians-Universität München, Butenandt-Strasse 11, D-81377, München, Germany., Zohrabi M; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA., Voznyuk O; Department of Physics, Augustana University, Sioux Falls, SD 57197, USA., Mahowald JB; Department of Physics, Augustana University, Sioux Falls, SD 57197, USA., Schmitz DG; Department of Physics, Augustana University, Sioux Falls, SD 57197, USA., Betsch KJ; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA., Berry B; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA., Severt T; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA., Kling NG; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA.; Department für Physik, Ludwig-Maximilians-Universität München, Am Coulombwall 1, D-85748, Garching, Germany., Burwitz TG; Department of Physics, Augustana University, Sioux Falls, SD 57197, USA., Carnes KD; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA., Kling MF; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA.; Department für Physik, Ludwig-Maximilians-Universität München, Am Coulombwall 1, D-85748, Garching, Germany., Ben-Itzhak I; J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA., Wells E; Department of Physics, Augustana University, Sioux Falls, SD 57197, USA. eric.wells@augie.edu., de Vivie-Riedle R; Department für Chemie, Ludwig-Maximilians-Universität München, Butenandt-Strasse 11, D-81377, München, Germany. Regina.de_Vivie@cup.uni-muenchen.de.
Jazyk: angličtina
Zdroj: Scientific reports [Sci Rep] 2017 Jun 30; Vol. 7 (1), pp. 4441. Date of Electronic Publication: 2017 Jun 30.
DOI: 10.1038/s41598-017-04638-0
Abstrakt: 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 2 D 2 , C 2 D 4 and C 2 D 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. These findings suggest that Rydberg contributions to field-dressed orbitals should be routinely considered when studying polyatomic molecules in intense laser fields.
Databáze: MEDLINE