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Article Dans Une Revue Scientific Reports Année : 2021

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

Allan Johnson
  • Fonction : Auteur
Felicity Mcgrath
  • Fonction : Auteur
David Wood
  • Fonction : Auteur
Lukas Miseikis
  • Fonction : Auteur
Thomas Siegel
  • Fonction : Auteur
Zdeněk Mašín
  • Fonction : Auteur
Morgane Vacher
João Pedro Malhado
  • Fonction : Auteur
Misha Ivanov
  • Fonction : Auteur
Olga Smirnova
  • Fonction : Auteur
Jon Marangos
  • Fonction : Auteur

Résumé

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 $$\tau _0 = 4 \pm 1$$ τ 0 = 4 ± 1 fs, in good agreement with the $$ \tau _0 = 3.5$$ τ 0 = 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.

Dates et versions

hal-03370996 , version 1 (08-10-2021)

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Dane Austin, Allan Johnson, Felicity Mcgrath, David Wood, Lukas Miseikis, et al.. Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra. Scientific Reports, 2021, 11 (1), ⟨10.1038/s41598-021-82232-1⟩. ⟨hal-03370996⟩
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