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Core-Valence Attosecond Transient Absorption Spectroscopy of Polyatomic Molecules

Nikolay V. Golubev* and Jiří Vaníček

Alexander I. Kuleff

  • Laboratory of Theoretical Physical Chemistry, Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

  • Theoretische Chemie, Universität Heidelberg, Im Neuenheimer Feld 229, D-69120 Heidelberg, Germany and ELI-ALPS, Wolfgang Sandner utca 3, H-6728 Szeged, Hungary

  • *nik.v.golubev@gmail.com
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Phys. Rev. Lett. 127, 123001 – Published 16 September, 2021

DOI: https://doi.org/10.1103/PhysRevLett.127.123001

Abstract

Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale which makes real-time observations of electron dynamics in molecules particularly difficult. In this work, we report an extension of the theory underlying the attosecond transient absorption spectroscopy (ATAS) for the case of molecules, including a full account for the coupled electron-nuclear dynamics in the initially created wave packet, and apply it to probe the oscillations of the positive charge created after outer-valence ionization of the propiolic acid molecule. By taking advantage of element-specific core-to-valence transitions induced by x-ray radiation, we show that the resolution of ATAS makes it possible to trace the dynamics of electron density with atomic spatial resolution.

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Phys. Rev. Lett. 127, 123001– Published 16 September, 2021
  • Received 29 October 2020
  • Revised 1 July 2021
  • Accepted 30 July 2021
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