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Jason B. Greenwood

Publications and source records attributed to Jason B. Greenwood.

2 recordsLinked to original sources

Direct Asymmetric Photochemistry with Synthetic Chiral Light

Circularly polarized light has long been used to distinguish the two mirror images of chiral molecules. Recently, a conceptual breakthrough has predicted that a new form of optical fields - synthetic chiral light - could usher in an 'electric-dipole revolution' in chiroptical interactions. We report the first experimental evidence for this prediction in the optical domain, using a three-dimensional laser electric field synthesized to trace a chiral pattern. The ionization and fragmentation of chiral molecules was found to depend on both the molecular handedness, and the handedness and geometry of the synthetic chiral field. Supported by two theoretical models, our results demonstrate that synthetic chiral light can induce strong chiroptical interactions, opening new horizons for asymmetric photochemistry and chiral analysis.

physics.chem-ph↗

Correlation-driven sub-3 fs charge migration in ionised adenine

Sudden ionisation of a relatively large molecule can initiate a correlation-driven process dubbed charge migration, where the electron density distribution is expected to rapidly change. Capturing this few-femtosecond/attosecond charge redistribution represents the real-time observation of the electron correlation in the molecule. So far, there has been no experimental evidence of this process. Here we report on a time-resolved study of the correlation-driven charge migration process occurring in the bio-relevant molecule adenine after ionisation by a 15-35 eV attosecond pulse . We find that, the production of intact doubly charged adenine - via a shortly-delayed laser-induced second ionisation event - represents the signature of a charge inflation mechanism resulting from the many-body excitation. This conclusion is supported by first-principles time-dependent simulations. Our findings opens new important perspectives for the control of the molecular reactivity at the electronic timescale.

physics.chem-ph↗