Surface Charges at the CaF2/Water Interface Allow Very Fast Intermolecular Vibrational-Energy Transfer
- Publication type:
- Journal article
- Metadata:
-
- Autoren
- Dominika Lesnicki
- Zhen Zhang
- Mischa Bonn
- Marialore Sulpizi
- Ellen HG Backus
- Autoren-URL
- https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000535947700001&DestLinkType=FullRecord&DestApp=WOS_CPL
- DOI
- 10.1002/anie.202004686
- eISSN
- 1521-3773
- Externe Identifier
- Clarivate Analytics Document Solution ID: NF1FD
- PubMed Identifier: 32239715
- ISSN
- 1433-7851
- Ausgabe der Veröffentlichung
- 31
- Zeitschrift
- ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
- Schlüsselwörter
- 2D sum-frequency generation
- ab-initio molecular dynamics
- energy transfer
- solid
- liquid interfaces
- Paginierung
- 13116 - 13121
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Titel
- Surface Charges at the CaF<sub>2</sub>/Water Interface Allow Very Fast Intermolecular Vibrational-Energy Transfer
- Sub types
- Article
- Ausgabe der Zeitschrift
- 59
Data source: Web of Science (Lite)
- Other metadata sources:
-
- Abstract
- <jats:title>Abstract</jats:title><jats:p>We investigate the dynamics of water in contact with solid calcium fluoride, where at low pH, localized charges can develop upon fluorite dissolution. We use 2D surface‐specific vibrational spectroscopy to quantify the heterogeneity of the interfacial water (D<jats:sub>2</jats:sub>O) molecules and provide information about the sub‐picosecond vibrational‐energy‐relaxation dynamics at the buried solid/liquid interface. We find that strongly H‐bonded OD groups, with a vibrational frequency below 2500 cm<jats:sup>−1</jats:sup>, display very rapid spectral diffusion and vibrational relaxation; for weakly H‐bonded OD groups, above 2500 cm<jats:sup>−1</jats:sup>, the dynamics slows down substantially. Atomistic simulations based on electronic‐structure theory reveal the molecular origin of energy transport through the local H‐bond network. We conclude that strongly oriented H‐bonded water molecules in the adsorbed layer, whose orientation is pinned by the localized charge defects, can exchange vibrational energy very rapidly due to the strong collective dipole, compensating for a partially missing solvation shell.</jats:p>
- Autoren
- Dominika Lesnicki
- Zhen Zhang
- Mischa Bonn
- Marialore Sulpizi
- Ellen HG Backus
- DOI
- 10.1002/anie.202004686
- eISSN
- 1521-3773
- ISSN
- 1433-7851
- Ausgabe der Veröffentlichung
- 31
- Zeitschrift
- Angewandte Chemie International Edition
- Sprache
- en
- Online publication date
- 2020
- Paginierung
- 13116 - 13121
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Herausgeber
- Wiley
- Herausgeber URL
- http://dx.doi.org/10.1002/anie.202004686
- Datum der Datenerfassung
- 2023
- Titel
- Surface Charges at the CaF<sub>2</sub>/Water Interface Allow Very Fast Intermolecular Vibrational‐Energy Transfer
- Ausgabe der Zeitschrift
- 59
Data source: Crossref
- Abstract
- We investigate the dynamics of water in contact with solid calcium fluoride, where at low pH, localized charges can develop upon fluorite dissolution. We use 2D surface-specific vibrational spectroscopy to quantify the heterogeneity of the interfacial water (D<sub>2</sub> O) molecules and provide information about the sub-picosecond vibrational-energy-relaxation dynamics at the buried solid/liquid interface. We find that strongly H-bonded OD groups, with a vibrational frequency below 2500 cm<sup>-1</sup> , display very rapid spectral diffusion and vibrational relaxation; for weakly H-bonded OD groups, above 2500 cm<sup>-1</sup> , the dynamics slows down substantially. Atomistic simulations based on electronic-structure theory reveal the molecular origin of energy transport through the local H-bond network. We conclude that strongly oriented H-bonded water molecules in the adsorbed layer, whose orientation is pinned by the localized charge defects, can exchange vibrational energy very rapidly due to the strong collective dipole, compensating for a partially missing solvation shell.
- Addresses
- Institute of Physics, Johannes, Gutenberg University Mainz, Staudingerweg 7, 55099, Mainz, Germany.
- Autoren
- Dominika Lesnicki
- Zhen Zhang
- Mischa Bonn
- Marialore Sulpizi
- Ellen HG Backus
- DOI
- 10.1002/anie.202004686
- eISSN
- 1521-3773
- Externe Identifier
- PubMed Identifier: 32239715
- PubMed Central ID: PMC7496624
- Funding acknowledgements
- European Research Council: 336679
- Deutsche Forschungsgemeinschaft: TRR146
- Open access
- true
- ISSN
- 1433-7851
- Ausgabe der Veröffentlichung
- 31
- Zeitschrift
- Angewandte Chemie (International ed. in English)
- Sprache
- eng
- Medium
- Print-Electronic
- Online publication date
- 2020
- Open access status
- Open Access
- Paginierung
- 13116 - 13121
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Publisher licence
- CC BY
- Datum der Datenerfassung
- 2020
- Titel
- Surface Charges at the CaF<sub>2</sub> /Water Interface Allow Very Fast Intermolecular Vibrational-Energy Transfer.
- Sub types
- research-article
- Journal Article
- Ausgabe der Zeitschrift
- 59
Files
https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/anie.202004686 https://europepmc.org/articles/PMC7496624?pdf=render
Data source: Europe PubMed Central
- Abstract
- We investigate the dynamics of water in contact with solid calcium fluoride, where at low pH, localized charges can develop upon fluorite dissolution. We use 2D surface-specific vibrational spectroscopy to quantify the heterogeneity of the interfacial water (D2 O) molecules and provide information about the sub-picosecond vibrational-energy-relaxation dynamics at the buried solid/liquid interface. We find that strongly H-bonded OD groups, with a vibrational frequency below 2500 cm-1 , display very rapid spectral diffusion and vibrational relaxation; for weakly H-bonded OD groups, above 2500 cm-1 , the dynamics slows down substantially. Atomistic simulations based on electronic-structure theory reveal the molecular origin of energy transport through the local H-bond network. We conclude that strongly oriented H-bonded water molecules in the adsorbed layer, whose orientation is pinned by the localized charge defects, can exchange vibrational energy very rapidly due to the strong collective dipole, compensating for a partially missing solvation shell.
- Autoren
- Dominika Lesnicki
- Zhen Zhang
- Mischa Bonn
- Marialore Sulpizi
- Ellen HG Backus
- Autoren-URL
- https://www.ncbi.nlm.nih.gov/pubmed/32239715
- DOI
- 10.1002/anie.202004686
- eISSN
- 1521-3773
- Externe Identifier
- PubMed Central ID: PMC7496624
- Funding acknowledgements
- Deutsche Forschungsgemeinschaft: TRR146
- ERC Starting Grant: 336679
- Ausgabe der Veröffentlichung
- 31
- Zeitschrift
- Angew Chem Int Ed Engl
- Schlüsselwörter
- 2D sum-frequency generation
- ab-initio molecular dynamics
- energy transfer
- solid/liquid interfaces
- Sprache
- eng
- Country
- Germany
- Paginierung
- 13116 - 13121
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Titel
- Surface Charges at the CaF2 /Water Interface Allow Very Fast Intermolecular Vibrational-Energy Transfer.
- Sub types
- Journal Article
- Ausgabe der Zeitschrift
- 59
Data source: PubMed
- Author's licence
- CC-BY
- Autoren
- Dominika Lesnicki
- Zhen Zhang
- Mischa Bonn
- Marialore Sulpizi
- Ellen HG Backus
- Hosting institution
- Universitätsbibliothek Mainz
- Sammlungen
- JGU-Publikationen
- Resource version
- Published version
- DOI
- 10.1002/anie.202004686
- File(s) embargoed
- false
- Open access
- true
- ISSN
- 1521-3773
- Ausgabe der Veröffentlichung
- 31
- Zeitschrift
- Angewandte Chemie
- Schlüsselwörter
- 530 Physik
- 530 Physics
- 540 Chemie
- 540 Chemistry and allied sciences
- Sprache
- eng
- Open access status
- Open Access
- Paginierung
- 13116 - 13121
- Datum der Veröffentlichung
- 2020
- Public URL
- https://openscience.ub.uni-mainz.de/handle/20.500.12030/6261
- Herausgeber
- Wiley-VCH
- Herausgeber URL
- https://doi.org/10.1002/anie.202004686
- Datum der Datenerfassung
- 2021
- Datum, an dem der Datensatz öffentlich gemacht wurde
- 2021
- Zugang
- Public
- Titel
- Surface charges at the CaF2/water interface allow very fast intermolecular vibrational-energy transfer
- Ausgabe der Zeitschrift
- 59
Files
dr._lesnicki_dominika-surface_charge-20210804001010568.pdf
Data source: OPENSCIENCE.UB
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