Pump-probe spectroscopy of chiral vibrational dynamics
| Autor: | Denis S. Tikhonov, Alexander Blech, Monika Leibscher, Loren Greenman, Melanie Schnell, Christiane P. Koch |
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| Jazyk: | angličtina |
| Rok vydání: | 2022 |
| Předmět: | |
| Zdroj: | Science advances 8(49), eade0311 (2022). doi:10.1126/sciadv.ade0311 |
| Popis: | Science advances 8(49), eade0311 (2022). 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. Published by Assoc., Washington, DC [u.a.] |
| Databáze: | OpenAIRE |
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