Attosecond Probing of Nuclear Dynamics with Trajectory-Resolved High-Harmonic Spectroscopy

Attosecond Probing of Nuclear Dynamics with Trajectory-Resolved High-Harmonic Spectroscopy We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajectories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H2 and D2 are used simultaneously to retrieve the nuclear dynamics on the attosecond and ångström scale. Compared to using only short trajectories, this extends the temporal range of the measurement to one optical cycle. The experiment is also applied to methane and ammonia molecules. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Physical Review Letters American Physical Society (APS)

Attosecond Probing of Nuclear Dynamics with Trajectory-Resolved High-Harmonic Spectroscopy

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Attosecond Probing of Nuclear Dynamics with Trajectory-Resolved High-Harmonic Spectroscopy

Abstract

We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajectories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H2 and D2 are used simultaneously to retrieve the nuclear dynamics on the attosecond and ångström scale. Compared to using only short trajectories, this extends the temporal range of the measurement to one optical cycle. The experiment is also applied to methane and ammonia molecules.
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Publisher
The American Physical Society
Copyright
Copyright © © 2017 American Physical Society
ISSN
0031-9007
eISSN
1079-7114
D.O.I.
10.1103/PhysRevLett.119.033201
Publisher site
See Article on Publisher Site

Abstract

We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajectories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H2 and D2 are used simultaneously to retrieve the nuclear dynamics on the attosecond and ångström scale. Compared to using only short trajectories, this extends the temporal range of the measurement to one optical cycle. The experiment is also applied to methane and ammonia molecules.

Journal

Physical Review LettersAmerican Physical Society (APS)

Published: Jul 21, 2017

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