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Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light

Molecular chirality, a geometric property of utmost importance in biochemistry, is now being investigated in the time-domain. Ultrafast chiral techniques can probe the formation or disappearance of stereogenic centers in molecules. The element-sensitivity of X-rays adds the capability to probe chira...

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Autores principales: Jiang, Xiang, Nam, Yeonsig, Rouxel, Jérémy R., Yong, Haiwang, Mukamel, Shaul
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10583748/
https://www.ncbi.nlm.nih.gov/pubmed/37860657
http://dx.doi.org/10.1039/d3sc02807k
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author Jiang, Xiang
Nam, Yeonsig
Rouxel, Jérémy R.
Yong, Haiwang
Mukamel, Shaul
author_facet Jiang, Xiang
Nam, Yeonsig
Rouxel, Jérémy R.
Yong, Haiwang
Mukamel, Shaul
author_sort Jiang, Xiang
collection PubMed
description Molecular chirality, a geometric property of utmost importance in biochemistry, is now being investigated in the time-domain. Ultrafast chiral techniques can probe the formation or disappearance of stereogenic centers in molecules. The element-sensitivity of X-rays adds the capability to probe chiral nuclear dynamics locally within the molecular system. However, the implementation of ultrafast techniques for measuring transient chirality remains a challenge because of the intrinsic weakness of chiral-sensitive signals based on circularly polarized light. We propose a novel approach for probing the enantiomeric dynamics by using the orbital angular momentum (OAM) of X-ray light, which can directly monitor the real-time chirality of molecules. Our simulations probe the oscillations in excited chiral formamide on different potential energy surfaces and demonstrate that using the X-ray OAM can increase the measured asymmetry ratio. Moreover, combining the OAM and SAM (spin angular momentum) provides stronger dichroic signals than linearly polarized light, and offers a powerful scheme for chiral discrimination.
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spelling pubmed-105837482023-10-19 Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light Jiang, Xiang Nam, Yeonsig Rouxel, Jérémy R. Yong, Haiwang Mukamel, Shaul Chem Sci Chemistry Molecular chirality, a geometric property of utmost importance in biochemistry, is now being investigated in the time-domain. Ultrafast chiral techniques can probe the formation or disappearance of stereogenic centers in molecules. The element-sensitivity of X-rays adds the capability to probe chiral nuclear dynamics locally within the molecular system. However, the implementation of ultrafast techniques for measuring transient chirality remains a challenge because of the intrinsic weakness of chiral-sensitive signals based on circularly polarized light. We propose a novel approach for probing the enantiomeric dynamics by using the orbital angular momentum (OAM) of X-ray light, which can directly monitor the real-time chirality of molecules. Our simulations probe the oscillations in excited chiral formamide on different potential energy surfaces and demonstrate that using the X-ray OAM can increase the measured asymmetry ratio. Moreover, combining the OAM and SAM (spin angular momentum) provides stronger dichroic signals than linearly polarized light, and offers a powerful scheme for chiral discrimination. The Royal Society of Chemistry 2023-09-11 /pmc/articles/PMC10583748/ /pubmed/37860657 http://dx.doi.org/10.1039/d3sc02807k Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Jiang, Xiang
Nam, Yeonsig
Rouxel, Jérémy R.
Yong, Haiwang
Mukamel, Shaul
Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light
title Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light
title_full Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light
title_fullStr Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light
title_full_unstemmed Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light
title_short Time-resolved enantiomer-exchange probed by using the orbital angular momentum of X-ray light
title_sort time-resolved enantiomer-exchange probed by using the orbital angular momentum of x-ray light
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10583748/
https://www.ncbi.nlm.nih.gov/pubmed/37860657
http://dx.doi.org/10.1039/d3sc02807k
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