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Pump-probe spectroscopy of chiral vibrational dynamics
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-shif...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Association for the Advancement of Science
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9728962/ https://www.ncbi.nlm.nih.gov/pubmed/36475788 http://dx.doi.org/10.1126/sciadv.ade0311 |
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author | Tikhonov, Denis S. Blech, Alexander Leibscher, Monika Greenman, Loren Schnell, Melanie Koch, Christiane P. |
author_facet | Tikhonov, Denis S. Blech, Alexander Leibscher, Monika Greenman, Loren Schnell, Melanie Koch, Christiane P. |
author_sort | Tikhonov, Denis S. |
collection | PubMed |
description | 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. |
format | Online Article Text |
id | pubmed-9728962 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | American Association for the Advancement of Science |
record_format | MEDLINE/PubMed |
spelling | pubmed-97289622022-12-13 Pump-probe spectroscopy of chiral vibrational dynamics Tikhonov, Denis S. Blech, Alexander Leibscher, Monika Greenman, Loren Schnell, Melanie Koch, Christiane P. Sci Adv Physical and Materials Sciences 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. American Association for the Advancement of Science 2022-12-07 /pmc/articles/PMC9728962/ /pubmed/36475788 http://dx.doi.org/10.1126/sciadv.ade0311 Text en Copyright © 2022 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY). https://creativecommons.org/licenses/by/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution license (https://creativecommons.org/licenses/by/4.0/) , which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. |
spellingShingle | Physical and Materials Sciences Tikhonov, Denis S. Blech, Alexander Leibscher, Monika Greenman, Loren Schnell, Melanie Koch, Christiane P. Pump-probe spectroscopy of chiral vibrational dynamics |
title | Pump-probe spectroscopy of chiral vibrational dynamics |
title_full | Pump-probe spectroscopy of chiral vibrational dynamics |
title_fullStr | Pump-probe spectroscopy of chiral vibrational dynamics |
title_full_unstemmed | Pump-probe spectroscopy of chiral vibrational dynamics |
title_short | Pump-probe spectroscopy of chiral vibrational dynamics |
title_sort | pump-probe spectroscopy of chiral vibrational dynamics |
topic | Physical and Materials Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9728962/ https://www.ncbi.nlm.nih.gov/pubmed/36475788 http://dx.doi.org/10.1126/sciadv.ade0311 |
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