4.6 Article

Few-Femtosecond Isotope Effect in Polyatomic Molecules Ionized by Extreme Ultraviolet Attosecond Pulse Trains

期刊

JOURNAL OF PHYSICAL CHEMISTRY A
卷 126, 期 34, 页码 5692-5701

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.2c03487

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资金

  1. Agence Nationale de la Recherche (ANR Circe) [ANR-16-CE30-0012]
  2. COST ATTOCHEM
  3. EUR LUMOMAT project
  4. Investments for the Future program [ANR-18-EURE-0012]
  5. GENCI - IDRIS [101124, 101353]
  6. CCIPL (Le centre de calcul intensif des Pays de la Loire)
  7. CNRS
  8. Federation de Recherche Andre Marie Ampe`re (FRAMA)
  9. Agence Nationale de la Recherche (ANR) [ANR-16-CE30-0012, ANR-18-EURE-0012] Funding Source: Agence Nationale de la Recherche (ANR)

向作者/读者索取更多资源

In attosecond chemistry, isotope labeling is an effective tool for unraveling relaxation pathways in highly excited photoionized molecules. Through experiments and calculations, it was found that nuclear and electron-nuclear dynamics in ethylene were almost 40% faster compared to its deuterated counterpart.
Following ionization by an extreme ultraviolet (XUV) attosecond pulse train, a polyatomic molecule can be promoted to more-than-one excited states of the residual ion. The ensuing relaxation dynamics is often facilitated by several reaction coordinates, making them difficult to disentangle by the usual spectroscopic means. Here, we show that in atto-chemistry isotope labeling can be an efficient tool for unraveling the relaxation pathways in highly excited photoionized molecules. Employing an XUV pump pulse and a near-infrared probe pulse, we found the nuclear as well as coupled electron-nuclear dynamics in ethylene to be almost 40% faster compared to that of its deuterated counterpart. The findings, which are supported by advanced nonadiabatic dynamics calculations, led to the identification of the relevant nuclear coordinates controlling the relaxation. Our experiment highlights the relevance of ultrashort XUV pulses to capture the isotopic effect in few-femtosecond molecular photodynamics.

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