Spatiotemporal imaging of ultrafast molecular motion: collapse and revival of the D+2 nuclear wave packet

Phys Rev Lett. 2006 Nov 10;97(19):193001. doi: 10.1103/PhysRevLett.97.193001. Epub 2006 Nov 6.

Abstract

We report on a real-time imaging of the ultrafast D(+)2 rovibrational nuclear wave-packet motion performed using a combination of a pump-probe setup with 7 fs laser pulses and a "reaction-microscope" spectrometer. We observe fast dephasing (collapse) of the vibrational wave packet and its subsequent revival and prove rotational excitation in ultrashort laser pulses. Channel-selective Fourier analysis of the wave packet's long-term (approximately 3000 fs) evolution allows us to resolve its individual constituents, revealing unique information on the mechanisms of strong-field ionization and dissociation.