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 stepin 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 relaxationdynamics of photoexcited chiral molecules can be tracked by recording Time-ResolvedPhotoElectron Circular Dichroism (TR-PECD) resulting from the photoionisation bya circularly polarized probe pulse. A large forward/backward asymmetry along theprobe propagation axis is observed in the photoelectron angular distribution. Its evolution with pump-probe delay reveals ultrafast dynamics that are inaccessible in theangle-integrated photoelectron spectrum nor via the usual electron emission anisotropyparameter ($\beta$). PECD, which originates from the electron scattering in the chiral molecular potential, appears as a new sensitive observable for ultrafast molecular dynamicsin chiral systems.

References in corpus (1)

• Time-resolved photoelectron spectroscopy of non-adiabatic dynamics in polyatomic molecules

Cited by in corpus (8)

• Attosecond-resolved photoionization of chiral molecules
• Time-resolved high harmonic spectroscopy of dynamical symmetry breaking in bi-circular laser fields
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• Photoelectron circular dichroism of O 1$s$-photoelectrons of uniaxially oriented trifluoromethyloxirane: Energy dependence and sensitivity to molecular configuration
• Photoelectron circular dichroism in angle-resolved photoemission from liquid fenchone
• Observation of photoelectron circular dichroism using a nanosecond laser
• Large circular dichroism in the total photoemission yield of free chiral nanoparticles created by a pure electric dipole effect
• Circular dichroism in the photoelectron angular distribution of achiral molecules