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Multidimensional high-harmonic echo spectroscopy: Resolving coherent electron dynamics in the EUV regime.

Shicheng Jiang1, Mahesh Gudem2, Markus Kowalewski2

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We introduce a new multidimensional high-harmonic echo spectroscopy to observe electron dynamics in molecules. This technique uses strong optical fields to capture ultrafast valence electron motion with femtosecond resolution.

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Area of Science:

  • Quantum Dynamics
  • Spectroscopy
  • Strong-Field Physics

Background:

  • Observing coherent electron dynamics is crucial for understanding molecular processes.
  • Standard spectroscopic techniques have limitations in resolving ultrafast electron motion over broad energy ranges.

Purpose of the Study:

  • To theoretically propose a novel multidimensional high-harmonic echo spectroscopy technique.
  • To resolve coherent electron dynamics spanning multiple electronvolts with high temporal resolution.

Main Methods:

  • Utilizing strong optical fields and a semi-perturbative approach.
  • Employing phase-matched, well-separated few-cycle strong infrared laser pulses.
  • Analyzing high harmonic echo signals generated from coherent valence electron dynamics.

Main Results:

  • The proposed technique can describe coherent valence electron dynamics driven by laser pulses.
  • It allows direct observation of molecular dynamics via high harmonic echo.
  • Simulations demonstrate ultrafast valence electron dynamics captured with femtosecond resolution.

Conclusions:

  • Multidimensional high-harmonic echo spectroscopy is a promising tool for studying ultrafast electron dynamics.
  • The technique reveals novel ultra-delayed partial rephasing echoes.
  • It offers a new pathway for high-resolution investigation of molecular electronic behavior.