Direct Coulomb explosion imaging of coherent rotational dynamics induced by few-cycle laser pulses in light and heavy hydrogen

Irina Bocharova, Maia Magrakvelidze, Predrag Ranitovic, Dipanwita Ray, Lewis Cocke, Igor Litvinyuk
James R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS, USA

We followed fast evolution of angular distributions for H2 and D2 molecules after their interaction with 8 fs 800 nm laser pulses. The rotating molecules were exploded by another few-cycle probe pulse time-delayed for up to 10 ps in respect to the pump. For neutral molecules we observed coherent rotational dynamics characterized by periodic revivals without noticeable decoherence within the 10 ps time-scale. For D2 up to 4 rotational states were involved in the wavepackets for each of the two spin isomers. In light hydrogen the resulting dynamics was dominated by beating of just two rotational states. The experimental data are in excellent agreement with our numerical simulations obtained by solving time-dependent Schrödinger equation. For molecules that were ionized by the pump pulse we observed both vibrational and rotational dynamics. Time-dependent angular distributions for the molecular ions exhibit transient alignment only soon after the pulse (20 fs for H2+ and 40 fs for D2+ with no consequent revivals within the next 10 ps.

This work was supported by the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy, and by the National Science Foundation.

Presented at DAMOP, May 2008, in State College, PA.


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