UC Berkeley

The ground-state vibrational wave packet produced by strong-field ionization of Br2 is characterized by femtosecond high-harmonic transient absorption spectroscopy. Vibrational motion is observed in time by a change in the 3d core-level transition energy with bond length 0.14 eV/pm to higher energies at shorter bond lengths. The wave packet has the expected period of 104 fs for the predominant v0v1 vibrational quantum beat, which is prepared near the outer turning point with a phase of 0.21π±0.05π due to the preferential ionization at short bond lengths. Simultaneous observation of a wave packet on the Br2+2Π g,3/2 ground state, prepared at the equilibrium bond distance of the ion, confirms preferential ionization near the inner turning point of the neutral. The Br2 ground-state wave packet has a degree of coherence ranging between 0.19 and 0.24, where unity is perfect coherence. The results utilize the sensitivity of core-level transient absorption spectroscopy to bond length and charge state, providing a means to analyze the formation and evolution of vibrational wave packets. © 2013 American Physical Society.