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Volume 171, 2014
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The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics

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Abstract

The sensitivities of high-harmonic generation (HHG) and strong-field ionization (SFI) to coupled electronic and nuclear dynamics are studied, using the nitric oxide (NO) molecule as an example. A coherent superposition of electronic and rotational states of NO is prepared by impulsive stimulated Raman scattering and probed by simultaneous detection of HHG and SFI yields. We observe a fourfold higher sensitivity of high-harmonic generation to electronic dynamics and attribute it to the presence of inelastic quantum paths connecting coherently related electronic states [Kraus et al., Phys. Rev. Lett.111, 243005 (2013)]. Whereas different harmonic orders display very different sensitivities to rotational or electronic dynamics, strong-field ionization is found to be most sensitive to electronic motion. We introduce a general theoretical formalism for high-harmonic generation from coupled nuclear-electronic wave packets. We show that the unequal sensitivities of different harmonic orders to electronic or rotational dynamics result from the angle dependence of the photorecombination matrix elements which encode several autoionizing and shape resonances in the photoionization continuum of NO. We further study the dependence of rotational and electronic coherences on the intensity of the excitation pulse and support the observations with calculations.

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Publication details

The article was received on 21 Feb 2014, accepted on 14 Apr 2014 and first published on 14 Apr 2014


Article type: Paper
DOI: 10.1039/C4FD00018H
Author version available: Download Author version (PDF)
Citation: Faraday Discuss., 2014,171, 113-132
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    The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics

    D. Baykusheva, P. M. Kraus, S. B. Zhang, N. Rohringer and H. J. Wörner, Faraday Discuss., 2014, 171, 113
    DOI: 10.1039/C4FD00018H

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