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Two-Dimensional Frequency Resolved Optomolecular Gating of High-Order Harmonic Generation.

A Ferré¹, H Soifer², O Pedatzur²

¹Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.

Physical Review Letters

|February 20, 2016

Summary

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This summary is machine-generated.

Researchers probed molecular electronic wave functions using advanced high-harmonic spectroscopy. This technique disentangles ionization and recombination steps, offering new insights into molecular dynamics and structure.

Area of Science:

Quantum mechanics
Molecular spectroscopy
Nonlinear optics

Background:

Probing electronic wave functions in polyatomic molecules presents significant challenges.
Laser-molecule interactions are highly nonlinear, coupling various degrees of freedom.
High-harmonic generation (HHG) is a powerful technique for studying electron dynamics.

Purpose of the Study:

To disentangle the ionization and recombination steps in HHG.
To develop advanced schemes for probing molecular electronic wave functions.
To gain insight into the structural and dynamical properties of molecular systems.

Main Methods:

Combining two-dimensional control of electron trajectories with vibrational control of molecules.
Introducing frequency-resolved optomolecular gating (FROG) for temporal resolution of harmonic emission.

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Studying vibrational motion in dinitrogen tetroxide (N_{2}O_{4}).

Main Results:

Successfully disentangled the ionization and recombination phases of HHG.
Resolved the temporal amplitude and phase of harmonic emission from excited molecules.
Demonstrated the capability of advanced schemes to provide unique insights into molecular properties.

Conclusions:

Advanced HHG schemes offer unprecedented control and insight into molecular electronic structure.
Frequency-resolved optomolecular gating is a key development for temporal analysis of HHG.
The study provides a new pathway for understanding molecular dynamics and structural properties.