Neutral-Ionic State Correlations in Strong-Field Molecular Ionization

Marija Kotur, Congyi Zhou, Spiridoula Matsika, Serguei Patchkovskii, Michael Spanner, and Thomas C. Weinacht

Phys. Rev. Lett. 109, 203007 – Published 14 November 2012

Abstract

We study correlations between neutral and ionic states in strong-field molecular ionization. We compare predictions based on Dyson orbital norms and quasistatic semiclassical tunneling theories (Keldysh and molecular orbital Ammosov-Delone-Krainov) with more detailed calculations of strong-field ionization which take into account (i) the Coulomb interaction between the outgoing continuum electron wave packet and the remaining bound electrons and (ii) electron-core interactions that cause distortions of the electronic continuum states during the ionization event. Our results highlight the prominence of electronic rearrangement effects in strong-field ionization with intense ultrafast laser pulses, where the outgoing continuum electron can cause electronic transitions in the parent ion. Calculations and measurements for excited uracil molecules reveal the breakdown of Keldysh-weighted Dyson norm predictions for ionization to different states of the molecular cation in the strong-field regime.

Received 18 April 2012

DOI:https://doi.org/10.1103/PhysRevLett.109.203007

Authors & Affiliations

Marija Kotur¹, Congyi Zhou², Spiridoula Matsika², Serguei Patchkovskii³, Michael Spanner³, and Thomas C. Weinacht¹

¹Department of Physics and Astronomy, Stony Brook University, Stony Brook, New York 11794, USA
²Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, USA
³Steacie Institute for Molecular Sciences, National Research Council of Canada, Ottawa, Ontario, Canada K1A 0R6