High Harmonic Generation in SF$_{6}$: Raman-excited Vibrational Quantum Beats

Details High Harmonic Generation in SF$_{6}$: Raman-excited Vibrational Quantum Beats High Harmonic Generation in SF$_{6}$: Raman-excited Vibrational Quantum Beats

2007-01-09

arxiv.org/abs/physics/0701113v1

Physics

Atomic Physics

submitted to PRL

Scientific paper

10.1088/0953-4075/40/18/F01

In a recent experiment (N. Wagner et al., PNAS v103, p13279) on SF$_{6}$, a high-harmonic generating laser pulse is preceded by a pump pulse which stimulates Raman-active modes in the molecule. Varying the time delay between the two pulses modulates high harmonic intensity, with frequencies equal to the vibration frequencies of the Raman-active modes. We propose an explanation of this modulation as a quantum interference between competing pathways that occur via adjacent vibrational states of the molecule. The Raman and high harmonic processes act as beamsplitters, producing vibrational quantum beats among the Raman-active vibrational modes that are excited by the first pulse. We introduce a rigorous treatment of the electron-ion recombination process and the effect of the ionic Coulomb field in the electron propagation outside the molecule, improving over the widely-used three-step model.

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