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Ultrafast dynamics of the lowest-lying neutral states in carbon dioxide

  • Author(s): Wright, TW;
  • Champenois, EG;
  • Cryan, JP;
  • Shivaram, N;
  • Yang, CS;
  • Belkacem, A
  • et al.
Abstract

We present a study of the ultrafast dissociation dynamics of the lowest-lying electronic excited states in CO2 by using ultraviolet (UV) and extreme-ultraviolet (XUV) pulses from high-order harmonic generation. We observe two primary dissociation channels: a direct dissociation channel along the Πg1 electronically excited manifold, and a second channel which results from the mixing of electronic states. The direct dissociation channel is found to have a lifetime which is shorter than our experimental resolution, whereas the second channel has a significantly longer lifetime of nearly 200 fs. In this long-lived channel we observe a beating of the vibrational populations with a period of ∼133 fs.

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