Gutenberg Open Science: Surface charges at the CaF2/water interface allow very fast intermolecular vibrational-energy transfer

Please use this identifier to cite or link to this item: http://doi.org/10.25358/openscience-6251

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DC Field	Value	Language
dc.contributor.author	Lesnicki, Dominika	-
dc.contributor.author	Zhang, Zhen	-
dc.contributor.author	Bonn, Mischa	-
dc.contributor.author	Sulpizi, Marialore	-
dc.contributor.author	Backus, Ellen H. G.	-
dc.date.accessioned	2021-08-09T09:31:55Z	-
dc.date.available	2021-08-09T09:31:55Z	-
dc.date.issued	2020	-
dc.identifier.uri	https://openscience.ub.uni-mainz.de/handle/20.500.12030/6261	-
dc.description.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 (D2O) 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.	en_GB
dc.language.iso	eng	de
dc.rights	CC BY	*
dc.rights.uri	https://creativecommons.org/licenses/by/4.0/	*
dc.subject.ddc	530 Physik	de_DE
dc.subject.ddc	530 Physics	en_GB
dc.subject.ddc	540 Chemie	de_DE
dc.subject.ddc	540 Chemistry and allied sciences	en_GB
dc.title	Surface charges at the CaF2/water interface allow very fast intermolecular vibrational-energy transfer	en_GB
dc.type	Zeitschriftenaufsatz	de
dc.identifier.doi	http://doi.org/10.25358/openscience-6251	-
jgu.type.dinitype	article	en_GB
jgu.type.version	Published version	de
jgu.type.resource	Text	de
jgu.organisation.department	FB 08 Physik, Mathematik u. Informatik	de
jgu.organisation.number	7940	-
jgu.organisation.name	Johannes Gutenberg-Universität Mainz	-
jgu.rights.accessrights	openAccess	-
jgu.journal.title	Angewandte Chemie	de
jgu.journal.volume	59	de
jgu.journal.issue	31	de
jgu.pages.start	13116	de
jgu.pages.end	13121	de
jgu.publisher.year	2020	-
jgu.publisher.name	Wiley-VCH	de
jgu.publisher.place	Weinheim	de
jgu.publisher.uri	https://doi.org/10.1002/anie.202004686	de
jgu.publisher.issn	1521-3773	de
jgu.organisation.place	Mainz	-
jgu.subject.ddccode	530	de
jgu.subject.ddccode	540	de
jgu.publisher.doi	10.1002/anie.202004686
jgu.organisation.ror	https://ror.org/023b0x485
Appears in collections:	JGU-Publikationen

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