Revealing pseudorotation and ring-opening reactions in colloidal organic molecules

Abstract

AbstractColloids 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.

Autoren

PJM Swinkels
SG Stuij
Z Gong
H Jonas
N Ruffino
B van der Linden
PG Bolhuis
S Sacanna
S Woutersen
P Schall

DOI

10.1038/s41467-021-23144-6

eISSN

2041-1723

Ausgabe der Veröffentlichung

1

Zeitschrift

Nature Communications

Sprache

en

Artikelnummer

2810

Online publication date

2021

Status

Published online

Herausgeber

Springer Science and Business Media LLC

Herausgeber URL

http://dx.doi.org/10.1038/s41467-021-23144-6

Datum der Datenerfassung

2022

Titel

Revealing pseudorotation and ring-opening reactions in colloidal organic molecules

Ausgabe der Zeitschrift

12

Datenquelle: Crossref

Abstract

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.

Addresses

Institute of Physics, University of Amsterdam, Amsterdam, The Netherlands.

Autoren

PJM Swinkels
SG Stuij
Z Gong
H Jonas
N Ruffino
B van der Linden
PG Bolhuis
S Sacanna
S Woutersen
P Schall

DOI

10.1038/s41467-021-23144-6

eISSN

2041-1723

Externe Identifier

PubMed Identifier: 33990609
PubMed Central ID: PMC8121934

Open access

true

ISSN

2041-1723

Ausgabe der Veröffentlichung

1

Zeitschrift

Nature communications

Sprache

eng

Medium

Electronic

Online publication date

2021

Open access status

Open Access

Paginierung

2810

Datum der Veröffentlichung

2021

Status

Published

Publisher licence

CC BY

Datum der Datenerfassung

2021

Titel

Revealing pseudorotation and ring-opening reactions in colloidal organic molecules.

Sub types

Research Support, Non-U.S. Gov't
research-article
Journal Article

Ausgabe der Zeitschrift

12

Files

https://www.nature.com/articles/s41467-021-23144-6.pdf https://europepmc.org/articles/PMC8121934?pdf=render

Datenquelle: Europe PubMed Central

Abstract

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.

Date of acceptance

2021

Autoren

PJM Swinkels
SG Stuij
Z Gong
H Jonas
N Ruffino
B van der Linden
PG Bolhuis
S Sacanna
S Woutersen
P Schall

Autoren-URL

https://www.ncbi.nlm.nih.gov/pubmed/33990609

DOI

10.1038/s41467-021-23144-6

eISSN

2041-1723

Externe Identifier

PubMed Central ID: PMC8121934

Ausgabe der Veröffentlichung

1

Zeitschrift

Nat Commun

Sprache

eng

Country

England

Paginierung

2810

PII

10.1038/s41467-021-23144-6

Datum der Veröffentlichung

2021

Status

Published online

Datum, an dem der Datensatz öffentlich gemacht wurde

2021

Titel

Revealing pseudorotation and ring-opening reactions in colloidal organic molecules.

Sub types

Journal Article
Research Support, Non-U.S. Gov't

Ausgabe der Zeitschrift

12

Datenquelle: PubMed

Revealing pseudorotation and ring-opening reactions in colloidal organic molecules

Files

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