Communication: Tracking molecular structure deformation and relaxation in real time.

The CH3I structural deformation induced by strong laser fields is revealed by time- and frequency-resolved ro-vibrational spectra. The experimental results show that the CH3I molecule undergoes ultrafast structural deformation of CH3 "umbrella-closing" induced by the strong fs laser field (more than 10(11) W/cm(2)) and followed by a structural relaxation of "umbrella-opening" within an exponential decay time scale of ∼620 fs. This study provides a first glimpse of the immense potential of the time- and frequency-resolved vibrational spectra in studying molecular deformation dynamics.