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Molecular recollision interferometry in high harmonic generation.

Xibin Zhou1, Robynne Lock, Wen Li

  • 1JILA and Department of Physics, University of Colorado and NIST, Boulder, Colorado 80309, USA. Xibin.Zhou@colorado.edu

Physical Review Letters
|March 21, 2008
PubMed
Summary
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We observed a phase reversal in high-order harmonic generation from aligned carbon dioxide (CO2) molecules. This quantum interference phenomenon provides insights into electron wave packet dispersion within molecules.

Area of Science:

  • Quantum optics
  • Molecular physics
  • Ultrafast spectroscopy

Background:

  • High-order harmonic generation (HHG) is a nonlinear process where intense laser fields interact with atoms or molecules.
  • Understanding the electron dynamics and quantum interferences in HHG is crucial for attosecond science and molecular imaging.
  • Previous studies have explored HHG in various systems, but detailed phase measurements in aligned molecules remain challenging.

Purpose of the Study:

  • To measure the phase of high-order harmonic generation (HHG) from transiently aligned carbon dioxide (CO2) molecules.
  • To investigate the influence of molecular alignment on the HHG phase.
  • To extract information about the electron wave packet dispersion and molecular potential effects.

Main Methods:

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  • Utilizing extreme-ultraviolet (XUV) interferometry to precisely measure the phase of HHG.
  • Employing transient molecular alignment techniques to control the orientation of CO2 molecules.
  • Analyzing both harmonic intensity and phase information to probe electron dynamics.

    • Main Results:

    • Unambiguously observed a phase reversal in HHG for higher harmonic orders in sufficiently aligned CO2 molecules.
    • The observed phase reversal is attributed to molecular-scale quantum interferences between the electronic wave function and the recolliding electron.
    • Extracted accurate dispersion relation information for the returning electron wave packet, revealing the influence of the molecular potential.

    Conclusions:

    • The study confirms a two-center interference model for HHG in aligned molecules.
    • Phase measurements provide a powerful tool to probe electron wave packet dynamics and molecular potentials.
    • This work advances the understanding of fundamental light-matter interactions in molecules.