Real-time probing of chirality during a chemical reaction

Abstract

Chiral molecules interact and react differently with other chiral objects, depending on their handedness. Therefore, it is essential to understand and ultimately control the evolution of molecular chirality during chemical reactions. Although highly sophisticated techniques for the controlled synthesis of chiral molecules have been developed, the observation of chirality on the natural femtosecond time scale of a chemical reaction has so far remained out of reach for isolated molecules. Here, we demonstrate a general experimental technique, based on high-harmonic generation in tailored laser fields, and apply it to probe the time evolution of molecular chirality during the photodissociation of 2-iodobutane. These measurements show a change in sign and a pronounced increase in the magnitude of the chiral response over the first 100 fs, followed by its decay within less than 500 fs, revealing the photodissociation to achiral products. The observed time evolution is explained in terms of the variation of the electric and magnetic transition-dipole moments between the lowest electronic states of the cation as a function of the reaction coordinate. These results open the path to investigations of the chirality of molecular reaction pathways, light-induced chirality in chemical processes and the control of molecular chirality through tailored laser pulses.

8 pages, 5 figures

References in corpus (5)

• Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry
• Opportunities for chiral discrimination using high harmonic generation in tailored laser fields
• Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy
• Strong-field control and enhancement of chiral response in bi-elliptical high-order harmonic generation: an analytical model
• Time-domain chirally-sensitive three-pulse coherent probes of vibrational excitons in proteins

Cited by in corpus (15)

• Ultrafast chirality: the road to efficient chiral measurements
• Femtosecond photoelectron circular dichroism of chemical reactions
• The Application of Tailored Fields for Studying Chirality and Symmetry
• Site-specific Interrogation of an Ionic Chiral Fragment During Photolysis Using an X-ray Free-Electron Laser
• Detecting multiple chirality centers in chiral molecules with high harmonic generation
• Probing molecular chirality via laser-induced electronic fluxes
• Imaging charge-migration in chiral molecules using time-resolved x-ray diffraction
• Giant chiro-optical response in high harmonic generation
• Strong chiral dichroism in above threshold ionization and ionization rates from locally-chiral light
• High-harmonic generation in liquids with few-cycle pulses: effect of laser-pulse duration on the cut-off energy
• Machine Learning-Based Optimization of Chiral Photonic Nanostructures: Evolution- and Neural Network-Based Design
• Ultrafast spatiotemporal chiroptical response of dielectric and plasmonic nanospheres
• Effects of electronic correlation on the high harmonic generation in helium: a time-dependent configuration interaction singles vs time-dependent full configuration interaction study
• Circular dichroism in the photoelectron angular distribution of achiral molecules
• Quantum-elevated Chiral Discrimination for Bio-molecules