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Multiple pulse coherent dynamics and wave packet control of the N2 a" 1Σg+ dark state by attosecond four wave mixing

Abstract

Nonlinear multidimensional spectroscopy is ubiquitous in the optical and radio-frequency regimes as a powerful tool to access structure and dynamics. The extension of this technique into the extreme ultraviolet (XUV) with attosecond pulses holds the promise of probing electronic dynamics and correlations with unprecedented time and spatial resolution. In this work, we use noncollinear four-wave mixing of a weak XUV attosecond pulse train (11-17 eV) and few- femtosecond NIR pulses (800 nm) to spectroscopically and dynamically probe the dipole-forbidden double-well potential of the a" 1Σg+ electronic state of nitrogen. The results demonstrate optical coupling of the inner and outer limits of the initially XUV-prepared vibrational wave packet in the valence character b' 1u+ state to the inner and outer wells, respectively, of the a" 1Σg+ double well state by 800 nm light. Two four-wave mixing schemes with different pulse timing sequences and noncollinear beam geometries are used (one NIR pulse collinear and one NIR pulse noncollinear versus both NIR pulses noncollinear to the XUV) to measure the a" dark state energetic structure and to control the dynamical preparation and motion of a dark state wave packet by selective population of either the inner Rydberg or outer valence-character potential well. Experimental measurements of the a" 1Σg+ outer well vibrational spacing and anharmonicity closely match the values theoretically predicted for this previously unobserved state.

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Publication details

The article was received on 11 Apr 2018, accepted on 08 May 2018 and first published on 08 May 2018


Article type: Paper
DOI: 10.1039/C8FD00074C
Citation: Faraday Discuss., 2018, Accepted Manuscript
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    Multiple pulse coherent dynamics and wave packet control of the N2 a" 1Σg+ dark state by attosecond four wave mixing

    E. R. Warrick, A. Fidler, W. Cao, E. Bloch, D. M. Neumark and S. R. Leone, Faraday Discuss., 2018, Accepted Manuscript , DOI: 10.1039/C8FD00074C

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