Ab Initio Liquid Water Dynamics in Aqueous TMAO Solution

Publikationstyp:
Zeitschriftenaufsatz
Metadaten:
Autoren
  • Kota Usui
  • Johannes Hunger
  • Marialore Sulpizi
  • Tatsuhiko Ohto
  • Mischa Bonn
  • Yuki Nagata
Autoren-URL
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000360026400022&DestLinkType=FullRecord&DestApp=WOS_CPL
DOI
10.1021/acs.jpcb.5b02579
eISSN
1520-5207
Externe Identifier
  • Clarivate Analytics Document Solution ID: CP6VN
  • PubMed Identifier: 26172877
ISSN
1520-6106
Ausgabe der Veröffentlichung
33
Zeitschrift
JOURNAL OF PHYSICAL CHEMISTRY B
Paginierung
10597 - 10606
Datum der Veröffentlichung
2015
Status
Published
Titel
<i>Ab Initio</i> Liquid Water Dynamics in Aqueous TMAO Solution
Sub types
  • Article
Ausgabe der Zeitschrift
119

Datenquelle: Web of Science (Lite)

Andere Metadatenquellen:
Autoren
  • Kota Usui
  • Johannes Hunger
  • Marialore Sulpizi
  • Tatsuhiko Ohto
  • Mischa Bonn
  • Yuki Nagata
DOI
10.1021/acs.jpcb.5b02579
eISSN
1520-5207
ISSN
1520-6106
Ausgabe der Veröffentlichung
33
Zeitschrift
The Journal of Physical Chemistry B
Sprache
en
Online publication date
2015
Paginierung
10597 - 10606
Datum der Veröffentlichung
2015
Status
Published
Herausgeber
American Chemical Society (ACS)
Herausgeber URL
http://dx.doi.org/10.1021/acs.jpcb.5b02579
Datum der Datenerfassung
2023
Titel
<i>Ab Initio</i> Liquid Water Dynamics in Aqueous TMAO Solution
Ausgabe der Zeitschrift
119

Datenquelle: Crossref

Abstract
Ab initio molecular dynamics (AIMD) simulations in trimethylamine N-oxide (TMAO)-D2O solution are employed to elucidate the effects of TMAO on the reorientational dynamics of D2O molecules. By decomposing the O-D groups of the D2O molecules into specific subensembles, we reveal that water reorientational dynamics are retarded considerably in the vicinity of the hydrophilic TMAO oxygen (O(TMAO)) atom, due to the O-D···O(TMAO) hydrogen-bond. We find that this reorientational motion is governed by two distinct mechanisms: The O-D group rotates (1) after breaking the O-D···O(TMAO) hydrogen-bond, or (2) together with the TMAO molecule while keeping this hydrogen-bond intact. While the orientational slow-down is prominent in the AIMD simulation, simulations based on force field models exhibit much faster dynamics. The simulated angle-resolved radial distribution functions illustrate that the O-D···O(TMAO) hydrogen-bond has a strong directionality through the sp(3) orbital configuration in the AIMD simulation, and this directionality is not properly accounted for in the force field simulation. These results imply that care must be taken when modeling negatively charged oxygen atoms as single point charges; force field models may not adequately describe the hydration configuration and dynamics.
Addresses
  • †Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany.
Autoren
  • Kota Usui
  • Johannes Hunger
  • Marialore Sulpizi
  • Tatsuhiko Ohto
  • Mischa Bonn
  • Yuki Nagata
DOI
10.1021/acs.jpcb.5b02579
eISSN
1520-5207
Externe Identifier
  • PubMed Identifier: 26172877
Funding acknowledgements
  • Deutsche Forschungsgemeinschaft: TRR 146
  • Max-Planck-Gesellschaft:
Open access
false
ISSN
1520-6106
Ausgabe der Veröffentlichung
33
Zeitschrift
The journal of physical chemistry. B
Sprache
eng
Medium
Print-Electronic
Online publication date
2015
Paginierung
10597 - 10606
Datum der Veröffentlichung
2015
Status
Published
Datum der Datenerfassung
2015
Titel
Ab Initio Liquid Water Dynamics in Aqueous TMAO Solution.
Sub types
  • Journal Article
Ausgabe der Zeitschrift
119

Datenquelle: Europe PubMed Central

Abstract
Ab initio molecular dynamics (AIMD) simulations in trimethylamine N-oxide (TMAO)-D2O solution are employed to elucidate the effects of TMAO on the reorientational dynamics of D2O molecules. By decomposing the O-D groups of the D2O molecules into specific subensembles, we reveal that water reorientational dynamics are retarded considerably in the vicinity of the hydrophilic TMAO oxygen (O(TMAO)) atom, due to the O-D···O(TMAO) hydrogen-bond. We find that this reorientational motion is governed by two distinct mechanisms: The O-D group rotates (1) after breaking the O-D···O(TMAO) hydrogen-bond, or (2) together with the TMAO molecule while keeping this hydrogen-bond intact. While the orientational slow-down is prominent in the AIMD simulation, simulations based on force field models exhibit much faster dynamics. The simulated angle-resolved radial distribution functions illustrate that the O-D···O(TMAO) hydrogen-bond has a strong directionality through the sp(3) orbital configuration in the AIMD simulation, and this directionality is not properly accounted for in the force field simulation. These results imply that care must be taken when modeling negatively charged oxygen atoms as single point charges; force field models may not adequately describe the hydration configuration and dynamics.
Autoren
  • Kota Usui
  • Johannes Hunger
  • Marialore Sulpizi
  • Tatsuhiko Ohto
  • Mischa Bonn
  • Yuki Nagata
Autoren-URL
https://www.ncbi.nlm.nih.gov/pubmed/26172877
DOI
10.1021/acs.jpcb.5b02579
eISSN
1520-5207
Ausgabe der Veröffentlichung
33
Zeitschrift
J Phys Chem B
Sprache
eng
Country
United States
Paginierung
10597 - 10606
Datum der Veröffentlichung
2015
Status
Published
Datum, an dem der Datensatz öffentlich gemacht wurde
2015
Titel
Ab Initio Liquid Water Dynamics in Aqueous TMAO Solution.
Sub types
  • Journal Article
Ausgabe der Zeitschrift
119

Datenquelle: PubMed

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