Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra

Austin DR, Johnson AS, Mcgrath F, Wood D, Miseikis L, Siegel T, Hawkins P, Harvey A, Masin Z, Patchkovskii S, Vacher M, Malhado JP, Ivanov MY, Smirnova O, Marangos JP (2021)

Publication Type: Journal article

Publication year: 2021

Journal

Scientific Reports Nature Publishing Group: Open Access Journals - Option B

Book Volume: 11

Article Number: 2485

Journal Issue: 1

DOI: 10.1038/s41598-021-82232-1

Abstract

We present a new methodology for measuring few-femtosecond electronic and nuclear dynamics in both atoms and polyatomic molecules using multidimensional high harmonic generation (HHG) spectroscopy measurements, in which the spectra are recorded as a function of the laser intensity to form a two-dimensional data set. The method is applied to xenon atoms and to benzene molecules, the latter exhibiting significant fast nuclear dynamics following ionization. We uncover the signature of the sub-cycle evolution of the returning electron flux in strong-field ionized xenon atoms, implicit in the strong field approximation but not previously observed directly. We furthermore extract the nuclear autocorrelation function in strong field ionized benzene cations, which is determined to have a decay of τ= 4 ± 1 fs, in good agreement with the τ= 3.5 fs obtained from direct dynamics variational multi-configuration Gaussian calculations. Our method requires minimal assumptions about the system, and is applicable even to un-aligned polyatomic molecules.

Involved external institutions

Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie im Forschungsverbund Berlin e.V. / Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy DE Germany (DE) Imperial College London / The Imperial College of Science, Technology and Medicine GB United Kingdom (GB)

How to cite

APA:

Austin, D.R., Johnson, A.S., Mcgrath, F., Wood, D., Miseikis, L., Siegel, T.,... Marangos, J.P. (2021). Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra. Scientific Reports, 11(1). https://doi.org/10.1038/s41598-021-82232-1

MLA:

Austin, Dane R., et al. "Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra." Scientific Reports 11.1 (2021).

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