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High Resolution Phonon-assisted Quasi-resonance Fluorescence Spectroscopy
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Quantum-Path-Resolved Attosecond High-Harmonic Spectroscopy.

Antoine Camper1,2, Amélie Ferré3, Valérie Blanchet4

  • 1Université Paris-Saclay, CEA, CNRS, LIDYL, 91191 Gif-sur-Yvette, France.

Physical Review Letters
|March 10, 2023
PubMed
Summary
This summary is machine-generated.

Investigating molecular attosecond dynamics is simplified by resolving quantum paths. This method reveals ultrafast ionic motion, like charge migration, without complex theoretical models.

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Area of Science:

  • Quantum dynamics
  • Molecular physics
  • Attosecond science

Background:

  • Strong-field ionization of molecules releases electrons, leading to high-order harmonic emission.
  • This process also triggers attosecond electronic and vibrational dynamics within the molecular ion.
  • Understanding these subcycle dynamics typically necessitates advanced theoretical modeling.

Purpose of the Study:

  • To demonstrate a method for avoiding complex theoretical modeling in attosecond dynamics studies.
  • To reveal subcycle ionic dynamics by resolving emission from distinct electronic quantum paths.
  • To investigate ultrafast ionic dynamics, including charge migration, using quantum-path-resolved spectroscopy.

Main Methods:

  • Analyzing high-order harmonic emission from strong-field ionized molecules.
  • Resolving emission from two families of electronic quantum paths with identical kinetic energy but different travel times.
  • Measuring harmonic amplitude and phase in aligned CO2 and N2 molecules.

Main Results:

  • Observed strong influence of laser-induced dynamics on a shape resonance and multichannel interference.
  • Demonstrated that quantum-path resolution simplifies the analysis of attosecond electronic and vibrational dynamics.
  • Showcased the potential of attosecond self-probing via quantum path interference.

Conclusions:

  • Quantum-path-resolved spectroscopy offers a direct route to studying ultrafast ionic dynamics.
  • This technique bypasses the need for complex theoretical modeling in many attosecond science applications.
  • Opens new avenues for investigating phenomena like charge migration in molecules.