Pump-probe spectroscopy of chiral vibrational dynamics

Tikhonov DS, Blech A, Leibscher M, Greenman L, Schnell M, Koch C (2022)

Publication Type: Journal article

Publication year: 2022


Book Volume: 8

Article Number: eade0311

Journal Issue: 49

DOI: 10.1126/sciadv.ade0311


A planar molecule may become chiral upon excitation of an out-of-plane vibration, changing its handedness during half a vibrational period. When exciting such a vibration in an ensemble of randomly oriented molecules with an infrared laser, half of the molecules will undergo the vibration phase-shifted by π compared to the other half, and no net chiral signal is observed. This symmetry can be broken by exciting the vibrational motion with a Raman transition in the presence of a static electric field. Subsequent ionization of the vibrating molecules by an extreme ultraviolet pulse probes the time-dependent net handedness via the photoelectron circular dichroism. Our proposal for pump-probe spectroscopy of molecular chirality, based on quantum-chemical theory and discussed for the example of the carbonyl chlorofluoride molecule, is feasible with current experimental technology.

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How to cite


Tikhonov, D.S., Blech, A., Leibscher, M., Greenman, L., Schnell, M., & Koch, C. (2022). Pump-probe spectroscopy of chiral vibrational dynamics. Science Advances, 8(49). https://dx.doi.org/10.1126/sciadv.ade0311


Tikhonov, Denis S., et al. "Pump-probe spectroscopy of chiral vibrational dynamics." Science Advances 8.49 (2022).

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