Abstract
We investigate strong-field XUV-IR pump-probe dissociative ionization of CO2 by solving the Schrödinger equation for the nuclear motion in full dimensionality on the lowest five coupled Oppenheimer (BO) potential-energy surfaces. Applying a multi-configurational self-consistent-field quantum-chemistry code to calculate ab initio non-BO, laser dipole, and spin-orbit couplings between adiabatic electronic states, we provide kinetic energy release (KER) spectra for the O(3Pg) + CO+( X2Σ+) and O+(4Su) + CO(X1Σ+) dissociation channels and their branching ratio. Our KER spectra identify the vibrational excitations of CO+ fragments along a dominant 3ω dissociation paths. Mediated by the nuclear dynamics near the conical intersection of the CO2+ A2∏u and B2Σu+ states, we reproduce a core-hole oscillation period 115 fs, in good agreement with the experiment of Timmers et al. [1]. In addition, we find 62 fs oscil-lations in the CO+ fragmentation channel due to quantum beats between specific vibrational and electronic CO2+ states.
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