Strong-field dissociation of CS$^{2+}$ via a pump/dump-like mechanism

ORAL

Abstract

Laser-induced dissociation of the quasi-bound electronic ground state of CS$^{2+}$ is investigated in intense laser pulses ($<$55 fs, $<$10$^{16}$ W/cm$^2$). Photodissociation is observed to be the dominant dissociation pathway; however, a more curious feature in the kinetic energy release spectrum suggests no significant energy gain from the initial states. We propose a pump/dump-like mechanism to explain this observed feature. Contrary to the conventional pump/dump control scheme, this process occurs within a single laser pulse, where the time delay is caused by the molecular structure. The process begins when the vibrational wavepacket in the electronic ground state of CS$^{2+}$ is pumped into the electronic first excited state's continuum by a single photon. After a period of stretching at an energy above the potential barrier, the emission of a second photon is stimulated by the same laser pulse, most likely at the Condon point.

*Supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy, Grants DE-FG02-86ER13491 and DE-FG02-09ER16115. TU supported by GACR and MetaCentrum.

Authors

  • Travis Severt

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
    • J. R. Macdonald Laboratory, Department of Physics, Kansas State University
    • J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506 USA
    • J. R. Macdonald Laboratory, Physics Dept., Kansas State University, Manhattan, KS, USA
  • M. Zohrabi

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • K.J. Betsch

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • U. Ablikim

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • Bethany Jochim

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • K.D. Carnes

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • S. Zeng

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • B.D. Esry

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • I. Ben-Itzhak

    • J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506, USA
  • T. Uhl\&#039;{I}kov\&#039;{a}

    • Department of Analytical Chemistry, Institute of Chemical Technology, Prague Technick\&#039;{a}, Czech Republic