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Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields

Chiral molecules with low enantiomer interconversion barriers racemize even at cryogenic temperatures due to quantum tunneling, forming a racemic mixture that is impossible to separate using conventional chemical methods. Here we both experimentally and theoretically demonstrate a method to create a...

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Autores principales: Sun, Wenhao, Tikhonov, Denis S., Singh, Himanshi, Steber, Amanda L., Pérez, Cristóbal, Schnell, Melanie
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9941128/
https://www.ncbi.nlm.nih.gov/pubmed/36807276
http://dx.doi.org/10.1038/s41467-023-36653-3
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author Sun, Wenhao
Tikhonov, Denis S.
Singh, Himanshi
Steber, Amanda L.
Pérez, Cristóbal
Schnell, Melanie
author_facet Sun, Wenhao
Tikhonov, Denis S.
Singh, Himanshi
Steber, Amanda L.
Pérez, Cristóbal
Schnell, Melanie
author_sort Sun, Wenhao
collection PubMed
description Chiral molecules with low enantiomer interconversion barriers racemize even at cryogenic temperatures due to quantum tunneling, forming a racemic mixture that is impossible to separate using conventional chemical methods. Here we both experimentally and theoretically demonstrate a method to create and probe a state-specific enantiomeric enrichment for such molecular systems. The coherent, non-linear, and resonant approach is based on a microwave six-wave mixing scheme and consists of five phase-controlled microwave pulses. The first three pulses induce a chiral wavepacket in a chosen rotational state, while the consecutive two pulses induce a polarization for a particular rotational transition (listen transition) with a magnitude proportional to the enantiomeric excess created. The experiments are performed with the transiently chiral molecule benzyl alcohol, where a chiral molecular response was successfully obtained. This signal demonstrates that enantiomeric excess can be induced in a quantum racemic mixture of a transiently chiral molecule using the developed microwave six-wave mixing scheme, which is an important step towards controlling non-rigid chiral molecular systems.
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spelling pubmed-99411282023-02-22 Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields Sun, Wenhao Tikhonov, Denis S. Singh, Himanshi Steber, Amanda L. Pérez, Cristóbal Schnell, Melanie Nat Commun Article Chiral molecules with low enantiomer interconversion barriers racemize even at cryogenic temperatures due to quantum tunneling, forming a racemic mixture that is impossible to separate using conventional chemical methods. Here we both experimentally and theoretically demonstrate a method to create and probe a state-specific enantiomeric enrichment for such molecular systems. The coherent, non-linear, and resonant approach is based on a microwave six-wave mixing scheme and consists of five phase-controlled microwave pulses. The first three pulses induce a chiral wavepacket in a chosen rotational state, while the consecutive two pulses induce a polarization for a particular rotational transition (listen transition) with a magnitude proportional to the enantiomeric excess created. The experiments are performed with the transiently chiral molecule benzyl alcohol, where a chiral molecular response was successfully obtained. This signal demonstrates that enantiomeric excess can be induced in a quantum racemic mixture of a transiently chiral molecule using the developed microwave six-wave mixing scheme, which is an important step towards controlling non-rigid chiral molecular systems. Nature Publishing Group UK 2023-02-20 /pmc/articles/PMC9941128/ /pubmed/36807276 http://dx.doi.org/10.1038/s41467-023-36653-3 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Sun, Wenhao
Tikhonov, Denis S.
Singh, Himanshi
Steber, Amanda L.
Pérez, Cristóbal
Schnell, Melanie
Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
title Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
title_full Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
title_fullStr Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
title_full_unstemmed Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
title_short Inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
title_sort inducing transient enantiomeric excess in a molecular quantum racemic mixture with microwave fields
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9941128/
https://www.ncbi.nlm.nih.gov/pubmed/36807276
http://dx.doi.org/10.1038/s41467-023-36653-3
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