Bond-length dependence of attosecond ionization delays in O 2 arising from electron correlation to a shape resonance.

Autor: Hammerland D; ETH Zürich, Laboratorium für Physikalische Chemie, Zürich, Switzerland., Berglitsch T; ETH Zürich, Laboratorium für Physikalische Chemie, Zürich, Switzerland., Zhang P; ETH Zürich, Laboratorium für Physikalische Chemie, Zürich, Switzerland., Luu TT; Department of Physics, The University of Hong Kong, SAR Hong Kong, China., Ueda K; ETH Zürich, Laboratorium für Physikalische Chemie, Zürich, Switzerland.; Department of Chemistry, Tohoku University, Sendai, Japan., Lucchese RR; Lawrence Berkeley National Laboratory, Berkeley, USA., Wörner HJ; ETH Zürich, Laboratorium für Physikalische Chemie, Zürich, Switzerland.
Jazyk: angličtina
Zdroj: Science advances [Sci Adv] 2024 Mar 29; Vol. 10 (13), pp. eadl3810. Date of Electronic Publication: 2024 Mar 27.
DOI: 10.1126/sciadv.adl3810
Abstrakt: We experimentally and theoretically demonstrate that electron correlation can cause the bond-length sensitivity of a shape resonance to induce an unexpected vibrational state-dependent ionization delay in a nonresonant channel. This discovery was enabled by a high-resolution attosecond-interferometry experiment based on a 400-nm driving and dressing wavelength. The short-wavelength driver results in a 6.2-electron volt separation between harmonics, markedly reducing the spectral overlap in the measured interferogram. We demonstrate the promise of this method on O 2 , a system characterized by broad vibrational progressions and a dense photoelectron spectrum. We measure a 40-attosecond variation of the photoionization delays over the X 2 Π g vibrational progression. Multichannel calculations show that this variation originates from a strong bond-length dependence of the energetic position of a shape resonance in the [Formula: see text] channel, which translates to the observed effects through electron correlation. The unprecedented energy resolution and delay accuracies demonstrate the promise of visible-light-driven molecular attosecond interferometry.
Databáze: MEDLINE
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