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Abstract:
We report fully differential photoelectron spectra from an ab initio coupled-channels treatment of CO2. Photoionization by laser pulses centered at wavelengths of 400 and 800 nm is considered, with arbitrary molecular alignment and polarization (linear and elliptic). Calculations reveal significant excited-state channel contributions that are, at certain molecular orientations, an order of magnitude larger than the ground-state channel in the rescattering plateau. A partial washout of the multiphoton structure in the above threshold ionization spectra and of the nodal features in angle-resolved spectra is observed due to ionization to excited-state channels. The qualitative nature of the spectra is determined by ionization thresholds, orbital symmetries, and interchannel coupling, in order of precedence.