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Related Experiment Video

Updated: Jul 12, 2026

Spatial Separation of Molecular Conformers and Clusters

Spatial Separation of Molecular Conformers and Clusters

Published on: January 9, 2014

Quantum interference during high-order harmonic generation from aligned molecules.

Tsuneto Kanai¹, Shinichirou Minemoto, Hirofumi Sakai

¹Department of Physics, Graduate School of Science, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo 113-0033, Japan.

|May 27, 2005

Summary

Quantum interference in high-order harmonic generation (HHG) from aligned CO2 molecules was observed. This finding reveals electron de Broglie wave interference within a single molecule and optical cycle, offering new insights into molecular structure.

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Area of Science:

Atomic, Molecular, and Optical Physics
Quantum Optics
Ultrafast Science

Background:

High-order harmonic generation (HHG) is a process where intense laser fields interact with atoms or molecules to produce high-energy photons.
The three-step model describes HHG involving electron tunneling, acceleration, and recombination.
Aligned molecules offer unique opportunities to study quantum phenomena in HHG due to their inherent symmetries.

Purpose of the Study:

To investigate quantum interference of electron de Broglie waves in the recombination step of HHG.
To explore the use of aligned CO2 molecules for studying HHG dynamics.
To correlate ion yields and harmonic signals to disentangle ionization and recombination contributions.

Main Methods:

Utilizing aligned CO2 molecules in an HHG experiment.
Measuring harmonic signals as a function of pump-probe delay.
Analyzing modulation patterns in harmonic spectra.

Main Results:

Evidence for quantum interference of electron de Broglie waves during HHG recombination in aligned CO2 molecules was found.
Interference occurred within a single molecule and a single optical cycle.
Harmonic signal modulations were explained by molecular valence orbital properties.

Conclusions:

Simultaneous observation of ion yields and harmonic signals provides a novel method for probing instantaneous molecular structure.
The study demonstrates quantum interference as a sensitive probe of molecular electronic structure during HHG.