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Revealing pseudorotation and ring-opening reactions in colloidal organic molecules

Colloids have a rich history of being used as ‘big atoms’ mimicking real atoms to study crystallization, gelation and the glass transition of condensed matter. Emulating the dynamics of molecules, however, has remained elusive. Recent advances in colloid chemistry allow patchy particles to be synthe...

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Autores principales: Swinkels, P. J. M., Stuij, S. G., Gong, Z., Jonas, H., Ruffino, N., Linden, B. van der, Bolhuis, P. G., Sacanna, S., Woutersen, S., Schall, P.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8121934/
https://www.ncbi.nlm.nih.gov/pubmed/33990609
http://dx.doi.org/10.1038/s41467-021-23144-6
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author Swinkels, P. J. M.
Stuij, S. G.
Gong, Z.
Jonas, H.
Ruffino, N.
Linden, B. van der
Bolhuis, P. G.
Sacanna, S.
Woutersen, S.
Schall, P.
author_facet Swinkels, P. J. M.
Stuij, S. G.
Gong, Z.
Jonas, H.
Ruffino, N.
Linden, B. van der
Bolhuis, P. G.
Sacanna, S.
Woutersen, S.
Schall, P.
author_sort Swinkels, P. J. M.
collection PubMed
description Colloids have a rich history of being used as ‘big atoms’ mimicking real atoms to study crystallization, gelation and the glass transition of condensed matter. Emulating the dynamics of molecules, however, has remained elusive. Recent advances in colloid chemistry allow patchy particles to be synthesized with accurate control over shape, functionality and coordination number. Here, we show that colloidal alkanes, specifically colloidal cyclopentane, assembled from tetrameric patchy particles by critical Casimir forces undergo the same chemical transformations as their atomic counterparts, allowing their dynamics to be studied in real time. We directly observe transitions between chair and twist conformations in colloidal cyclopentane, and we elucidate the interplay of bond bending strain and entropy in the molecular transition states and ring-opening reactions. These results open the door to investigate complex molecular kinetics and molecular reactions in the high-temperature classical limit, in which the colloidal analogue becomes a good model.
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spelling pubmed-81219342021-05-18 Revealing pseudorotation and ring-opening reactions in colloidal organic molecules Swinkels, P. J. M. Stuij, S. G. Gong, Z. Jonas, H. Ruffino, N. Linden, B. van der Bolhuis, P. G. Sacanna, S. Woutersen, S. Schall, P. Nat Commun Article Colloids have a rich history of being used as ‘big atoms’ mimicking real atoms to study crystallization, gelation and the glass transition of condensed matter. Emulating the dynamics of molecules, however, has remained elusive. Recent advances in colloid chemistry allow patchy particles to be synthesized with accurate control over shape, functionality and coordination number. Here, we show that colloidal alkanes, specifically colloidal cyclopentane, assembled from tetrameric patchy particles by critical Casimir forces undergo the same chemical transformations as their atomic counterparts, allowing their dynamics to be studied in real time. We directly observe transitions between chair and twist conformations in colloidal cyclopentane, and we elucidate the interplay of bond bending strain and entropy in the molecular transition states and ring-opening reactions. These results open the door to investigate complex molecular kinetics and molecular reactions in the high-temperature classical limit, in which the colloidal analogue becomes a good model. Nature Publishing Group UK 2021-05-14 /pmc/articles/PMC8121934/ /pubmed/33990609 http://dx.doi.org/10.1038/s41467-021-23144-6 Text en © The Author(s) 2021 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
Swinkels, P. J. M.
Stuij, S. G.
Gong, Z.
Jonas, H.
Ruffino, N.
Linden, B. van der
Bolhuis, P. G.
Sacanna, S.
Woutersen, S.
Schall, P.
Revealing pseudorotation and ring-opening reactions in colloidal organic molecules
title Revealing pseudorotation and ring-opening reactions in colloidal organic molecules
title_full Revealing pseudorotation and ring-opening reactions in colloidal organic molecules
title_fullStr Revealing pseudorotation and ring-opening reactions in colloidal organic molecules
title_full_unstemmed Revealing pseudorotation and ring-opening reactions in colloidal organic molecules
title_short Revealing pseudorotation and ring-opening reactions in colloidal organic molecules
title_sort revealing pseudorotation and ring-opening reactions in colloidal organic molecules
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8121934/
https://www.ncbi.nlm.nih.gov/pubmed/33990609
http://dx.doi.org/10.1038/s41467-021-23144-6
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