Angular momentum dependence in multiphoton ionization and attosecond time delays

Multiphoton interference measurements in attosecond physics, e.g., the reconstruction of attosecond beating by interference of two-photon transitions (RABITT), are the typical methods of choice to experimentally access the photoionization delay in atoms and molecules. The exact relation between the measurable multiphoton delays and the theoretical single-photon delays is typically modeled by correction terms, continuum-continuum delays, obtained from a high-energy limit of the theory. However, these are unreliable at photoelectron kinetic energies smaller than about 10 eV, and do not have photoemission angular dependence. In this work we develop an accurate analytic alternative that gives accurate correction terms even at very low energies. Our method is computationally very straightforward, predicts correct multiphoton photoelectron angular distributions as well as the expected angular dependence of the continuum-continuum delay. We validate the approach theoretically against state-of-the-art ab initio calculations as well as experimentally with a two-harmonic RABITT setup, which properly separates different higher-order multiphoton pathways and offers a promising way of analyzing congested molecular photoionization spectra.

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Publication Details

Journal
Physical review. A/Physical review, A
Published
2025-01-16
DOI
https://doi.org/10.1103/physreva.111.013110
Citations
4
Primary Topic
Laser-Matter Interactions and Applications
Type
article
Field-Weighted Citation Impact
4.99

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article

Angular momentum dependence in multiphoton ionization and attosecond time delays

F. Lépine, Jakub Benda, V. Loriot, Zdeněk Mašín et al.
4 citations
Physical review. A/Physical review, A
Laser-Matter Interactions and Applications
4.99
article

Angular momentum dependence in multiphoton ionization and attosecond time delays

F. Lépine, Jakub Benda, V. Loriot, Zdeněk Mašín, Saikat Nandi, Sreelakshmi Palakkal
article en
4 citations

Abstract

Multiphoton interference measurements in attosecond physics, e.g., the reconstruction of attosecond beating by interference of two-photon transitions (RABITT), are the typical methods of choice to experimentally access the photoionization delay in atoms and molecules. The exact relation between the measurable multiphoton delays and the theoretical single-photon delays is typically modeled by correction terms, continuum-continuum delays, obtained from a high-energy limit of the theory. However, these are unreliable at photoelectron kinetic energies smaller than about 10 eV, and do not have photoemission angular dependence. In this work we develop an accurate analytic alternative that gives accurate correction terms even at very low energies. Our method is computationally very straightforward, predicts correct multiphoton photoelectron angular distributions as well as the expected angular dependence of the continuum-continuum delay. We validate the approach theoretically against state-of-the-art ab initio calculations as well as experimentally with a two-harmonic RABITT setup, which properly separates different higher-order multiphoton pathways and offers a promising way of analyzing congested molecular photoionization spectra.

Physical review. A/Physical review, AVol. 111(1)
Université Claude Bernard Lyon 1 (FR), Charles University (CZ), Institut Lumière Matière (FR)
Univerzita Karlova v Praze, Ministerstvo Školství, Mládeže a Tělovýchovy, Grantová Agentura České Republiky, Institut national des sciences de l'Univers
Openalex Percentile: Top 6%
Laser-Matter Interactions and Applications
4.99
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Angular momentum dependence in multiphoton ionization and attosecond time delays — F. Lépine, Jakub Benda, et al. · Physical review. A/Physical review, A (2025) | TGRS Research Map | TGRS