Exposing the role of electron correlation in strong-field double ionization: X-ray transient absorption of orbital alignment in Xe+ and Xe2+

Scott Sayres, Erik R. Hosler, Stephen R. Leone

Research output: Contribution to journalArticle

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Abstract

Orbital alignment measurements and theory are used to examine the role of electron correlation during atomic strong-field double ionization (795 nm, (1-5) × 1014 W cm-2). High-order harmonic, transient absorption spectroscopy is used to measure the angular distributions of singly and doubly tunnel-ionized xenon atomic states via 4d core to 5p valence shell transitions between 55 and 60 eV. The experimental MJ alignment distributions are compared to results of a rate-equation model based on sequential ionization, previously developed for coherent electron motion, and now applied to account for the alignment prepared by tunneling ionization. The hole generated in the 2P3/2 state of Xe+ is measured to be entirely composed of |MJ| = 1/2, in agreement with theory. The result is a higher degree of alignment than previously reported. Because the model neglects effects of electron-ion recollision, the theory predicts a high degree of alignment in both spin-parallel (triplet) and antiparallel (singlet) terms of Xe2+. However, the alignment generated with linearly polarized light is observed to be spin-state dependent. The measured alignments for triplet spin states (3P2 has |MJ| = [0: 1: 2] of [27±6: 45±11: 29±0] and 3P1 has |MJ| = [0: 1] of [56±2: 44±2]) are in good agreement with the expectations of theory, which are [33: 53: 14] and [66: 33], respectively. The results validate the rate equation model for sequential tunnel ionization. However, the alignment extracted for a singlet state is greatly diminished: 1D2 is measured to be [18±1: 39±2: 43 ± 2] compared to theoretical expectation of [60: 39: 1] for |MJ| = [0: 1: 2]. The poor agreement with the sequential ionization model suggests that the alignment of 1D2 is strongly influenced by the high propensity for the liberated first electron to return to and recollide with its parent atomic orbital. Therefore, although the influence of electron recollision appears minor in the triplet states and suggests sequential ionization, electron correlation between the ionic core and the first ionized electron cannot be ignored in the singlet state. Singlet states are likely to be generated through nonsequential double ionization over the intensity range where the experiments are performed.

Original languageEnglish (US)
Pages (from-to)8614-8624
Number of pages11
JournalJournal of Physical Chemistry A
Volume118
Issue number37
DOIs
StatePublished - Sep 18 2014
Externally publishedYes

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Electron correlations
Ionization
alignment
ionization
X rays
orbitals
electrons
x rays
Electrons
tunnels
Tunnels
Xenon
Angular distribution
Light polarization
Absorption spectroscopy
xenon
polarized light
atomic energy levels
absorption spectroscopy
angular distribution

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Exposing the role of electron correlation in strong-field double ionization : X-ray transient absorption of orbital alignment in Xe+ and Xe2+. / Sayres, Scott; Hosler, Erik R.; Leone, Stephen R.

In: Journal of Physical Chemistry A, Vol. 118, No. 37, 18.09.2014, p. 8614-8624.

Research output: Contribution to journalArticle

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N2 - Orbital alignment measurements and theory are used to examine the role of electron correlation during atomic strong-field double ionization (795 nm, (1-5) × 1014 W cm-2). High-order harmonic, transient absorption spectroscopy is used to measure the angular distributions of singly and doubly tunnel-ionized xenon atomic states via 4d core to 5p valence shell transitions between 55 and 60 eV. The experimental MJ alignment distributions are compared to results of a rate-equation model based on sequential ionization, previously developed for coherent electron motion, and now applied to account for the alignment prepared by tunneling ionization. The hole generated in the 2P3/2 state of Xe+ is measured to be entirely composed of |MJ| = 1/2, in agreement with theory. The result is a higher degree of alignment than previously reported. Because the model neglects effects of electron-ion recollision, the theory predicts a high degree of alignment in both spin-parallel (triplet) and antiparallel (singlet) terms of Xe2+. However, the alignment generated with linearly polarized light is observed to be spin-state dependent. The measured alignments for triplet spin states (3P2 has |MJ| = [0: 1: 2] of [27±6: 45±11: 29±0] and 3P1 has |MJ| = [0: 1] of [56±2: 44±2]) are in good agreement with the expectations of theory, which are [33: 53: 14] and [66: 33], respectively. The results validate the rate equation model for sequential tunnel ionization. However, the alignment extracted for a singlet state is greatly diminished: 1D2 is measured to be [18±1: 39±2: 43 ± 2] compared to theoretical expectation of [60: 39: 1] for |MJ| = [0: 1: 2]. The poor agreement with the sequential ionization model suggests that the alignment of 1D2 is strongly influenced by the high propensity for the liberated first electron to return to and recollide with its parent atomic orbital. Therefore, although the influence of electron recollision appears minor in the triplet states and suggests sequential ionization, electron correlation between the ionic core and the first ionized electron cannot be ignored in the singlet state. Singlet states are likely to be generated through nonsequential double ionization over the intensity range where the experiments are performed.

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