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Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry

Abstract : Unravelling the main initial dynamics responsible for chiral recognition is a key step in the understanding of many biological processes. However this challenging task requires a sensitive enantiospecic probe to investigate molecular dynamics on their natural femtosecond timescale. Here we show that, in the gas phase, the ultrafast relaxation dynamics of photoexcited chiral molecules can be tracked by recording Time-Resolved PhotoElectron Circular Dichroism (TR-PECD) resulting from the photoionisation by a circularly polarized probe pulse. A large forward/backward asymmetry along the probe propagation axis is observed in the photoelectron angular distribution. Its evolution with pump-probe delay reveals ultrafast dynamics that are inaccessible in the angle-integrated photoelectron spectrum nor via the usual electron emission anisotropy parameter (β). PECD, which originates from the electron scattering in the chiral molecular potential, appears as a new sensitive observable for ultrafast molecular dynamics in chiral systems.
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https://hal.archives-ouvertes.fr/hal-01395562
Contributor : Valerie Blanchet <>
Submitted on : Tuesday, November 15, 2016 - 11:24:05 PM
Last modification on : Monday, December 14, 2020 - 5:20:39 PM
Long-term archiving on: : Monday, March 27, 2017 - 9:21:39 AM

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Antoine Comby, Samuel Beaulieu, Martial Boggio-Pasqua, Dominique Descamps, Francois Légaré, et al.. Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry. Journal of Physical Chemistry Letters, American Chemical Society, 2016, 7 (21), pp.4514 - 4519. ⟨10.1021/acs.jpclett.6b02065⟩. ⟨hal-01395562v2⟩

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