title: Probing ultrafast dynamics of chiral molecules using time-resolved photoelectron circular dichroism.
abstract: Measuring the ultrafast dynamics of chiral molecules in the gas phase has been a long standing and challenging quest of molecular physics. The main limitation to reach that goal has been the lack of highly sensitive chiroptical measurement. By enabling chiral discrimination with up to several 10% of sensitivity, photoelectron circular dichroism (PECD) offers a solution to this issue. However, tracking ultrafast processes requires measuring PECD with ultrashort light pulses. Here we compare the PECD obtained with different light sources, from the extreme ultraviolet to the mid-infrared range, leading to different ionization regimes: single-photon, resonance-enhanced multiphoton, above-threshold and tunnel ionization. We use single and multiphoton ionization to probe the ultrafast relaxation of fenchone molecules photoexcited in their first Rydberg states. We show that time-resolved PECD enables revealing dynamics much faster than the population decay of the Rydberg states, demonstrating the high sensitivity of this technique to vibronic relaxation.
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr and Institut Natinal de la Recherche Scientifique, Varennes, Québec, Canada.
authors.forename: Samuel
authors.initials: S
authors.lastname: Beaulieu
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Antoine
authors.initials: A
authors.lastname: Comby
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Baptiste
authors.initials: B
authors.lastname: Fabre
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Dominique
authors.initials: D
authors.lastname: Descamps
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Amélie
authors.initials: A
authors.lastname: Ferré
authors.affiliation: Synchrotron SOLEIL, Saint Aubin, BP 34, 91192 Gif-sur-Yvette, France.
authors.forename: Gustavo
authors.initials: G
authors.lastname: Garcia
authors.affiliation: Lidyl, CEA/Saclay, 91191 Gif-sur-Yvette Cedex, France.
authors.forename: Romain
authors.initials: R
authors.lastname: Géneaux
authors.affiliation: Institut Natinal de la Recherche Scientifique, Varennes, Québec, Canada.
authors.forename: Francois
authors.initials: F
authors.lastname: Légaré
authors.affiliation: Synchrotron SOLEIL, Saint Aubin, BP 34, 91192 Gif-sur-Yvette, France.
authors.forename: Laurent
authors.initials: L
authors.lastname: Nahon
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Stéphane
authors.initials: S
authors.lastname: Petit
authors.affiliation: Lidyl, CEA/Saclay, 91191 Gif-sur-Yvette Cedex, France.
authors.forename: Thierry
authors.initials: T
authors.lastname: Ruchon
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Bernard
authors.initials: B
authors.lastname: Pons
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Valérie
authors.initials: V
authors.lastname: Blanchet
authors.affiliation: Université de Bordeaux - CNRS - CEA, CELIA, UMR5107, F33405 Talence, France. yann.mairesse@celia.u-bordeaux.fr.
authors.forename: Yann
authors.initials: Y
authors.lastname: Mairesse