Journal
PHYSICAL REVIEW LETTERS
Volume 116, Issue 5, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.116.053002
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Funding
- Conseil Regional d'Aquitaine [20091304003 ATTOMOL, 2.1.3-09010502]
- European Union [LASERLAB-EUROPE II 228334, LASERLAB-EUROPE 284464]
- French Agence Nationale pour la Recherche [ANR14-CE32-0014 MISFITS]
- Minerva Foundation
- Israeli Science Foundation
- Israeli Centers of Research Excellence program
- Crown photonics Center
- European Research Council Starting Research Grant MIDAS
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Probing electronic wave functions of polyatomic molecules is one of the major challenges in high-harmonic spectroscopy. The extremely nonlinear nature of the laser-molecule interaction couples the multiple degrees of freedom of the probed system. We combine two-dimensional control of the electron trajectories and vibrational control of the molecules to disentangle the two main steps in high-harmonic generation-ionization and recombination. We introduce a new measurement scheme, frequency-resolved optomolecular gating, which resolves the temporal amplitude and phase of the harmonic emission from excited molecules. Focusing on the study of vibrational motion in N2O4, we show that such advanced schemes provide a unique insight into the structural and dynamical properties of the underlying mechanism.
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