title: Two-Dimensional Frequency Resolved Optomolecular Gating of High-Order Harmonic Generation.
abstract: 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 N_{2}O_{4}, we show that such advanced schemes provide a unique insight into the structural and dynamical properties of the underlying mechanism.
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: A
authors.initials: A
authors.lastname: Ferré
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: H
authors.initials: H
authors.lastname: Soifer
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: O
authors.initials: O
authors.lastname: Pedatzur
authors.affiliation: Synchrotron SOLEIL, Saint Aubin, BP 34, 91192 Gif-sur-Yvette, France.
authors.forename: C
authors.initials: C
authors.lastname: Bourassin-Bouchet
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: B D
authors.initials: BD
authors.lastname: Bruner
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: R
authors.initials: R
authors.lastname: Canonge
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: F
authors.initials: F
authors.lastname: Catoire
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: D
authors.initials: D
authors.lastname: Descamps
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: B
authors.initials: B
authors.lastname: Fabre
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: E
authors.initials: E
authors.lastname: Mével
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: S
authors.initials: S
authors.lastname: Petit
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: N
authors.initials: N
authors.lastname: Dudovich
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: Y
authors.initials: Y
authors.lastname: Mairesse