Details
| Original language | English |
|---|---|
| Pages (from-to) | 340-346 |
| Number of pages | 7 |
| Journal | Nano letters |
| Volume | 22 |
| Issue number | 1 |
| Early online date | 27 Dec 2021 |
| Publication status | Published - 12 Jan 2022 |
Abstract
Water diffusion across the surfaces of materials is of importance to disparate processes such as water purification, ice formation, and more. Despite reports of rapid water diffusion on surfaces the molecular level, details of such processes remain unclear. Here, with scanning tunneling microscopy, we observe structural rearrangements and diffusion of water trimers at unexpectedly low temperatures (<10 K) on a copper surface, temperatures at which water monomers or other clusters do not diffuse. Density functional theory calculations reveal a facile trimer diffusion process involving transformations between elongated and almost cyclic conformers in an inchworm-like manner. These subtle intermolecular reorientations maintain an optimal balance of hydrogen-bonding and water–surface interactions throughout the process. This work shows that the diffusion of hydrogen-bonded clusters can occur at exceedingly low temperatures without the need for hydrogen bond breakage or exchange; findings that will influence Ostwald ripening of ice nanoclusters and hydrogen bonded clusters in general.
Keywords
- diffusion, hydrogen-bonding, oligomers, Water
ASJC Scopus subject areas
- Chemical Engineering(all)
- Bioengineering
- Chemistry(all)
- General Chemistry
- Materials Science(all)
- General Materials Science
- Physics and Astronomy(all)
- Condensed Matter Physics
- Engineering(all)
- Mechanical Engineering
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In: Nano letters, Vol. 22, No. 1, 12.01.2022, p. 340-346.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Rapid Water Diffusion at Cryogenic Temperatures through an Inchworm-like Mechanism
AU - Fang, Wei
AU - Meyer auf der Heide, Kastur M.
AU - Zaum, Christopher
AU - Michaelides, Angelos
AU - Morgenstern, Karina
N1 - Funding Information: This work was supported by the Research Training group ‘Confinement-controlled Chemistry’, which is funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - GRK2376/331 085 229 and by the DFG under Germany’s Excellence Strategy - EXC-2033 - Projektnummer 390 677 874 RESOLV. We are grateful to the Materials Chemistry Consortium (funded by EPSRC (EP/L000202)) and to the UK Materials and Molecular Modelling Hub (funded by EPSRC (EP/P020194/1 and EP/T022213/1)) for computational resources.
PY - 2022/1/12
Y1 - 2022/1/12
N2 - Water diffusion across the surfaces of materials is of importance to disparate processes such as water purification, ice formation, and more. Despite reports of rapid water diffusion on surfaces the molecular level, details of such processes remain unclear. Here, with scanning tunneling microscopy, we observe structural rearrangements and diffusion of water trimers at unexpectedly low temperatures (<10 K) on a copper surface, temperatures at which water monomers or other clusters do not diffuse. Density functional theory calculations reveal a facile trimer diffusion process involving transformations between elongated and almost cyclic conformers in an inchworm-like manner. These subtle intermolecular reorientations maintain an optimal balance of hydrogen-bonding and water–surface interactions throughout the process. This work shows that the diffusion of hydrogen-bonded clusters can occur at exceedingly low temperatures without the need for hydrogen bond breakage or exchange; findings that will influence Ostwald ripening of ice nanoclusters and hydrogen bonded clusters in general.
AB - Water diffusion across the surfaces of materials is of importance to disparate processes such as water purification, ice formation, and more. Despite reports of rapid water diffusion on surfaces the molecular level, details of such processes remain unclear. Here, with scanning tunneling microscopy, we observe structural rearrangements and diffusion of water trimers at unexpectedly low temperatures (<10 K) on a copper surface, temperatures at which water monomers or other clusters do not diffuse. Density functional theory calculations reveal a facile trimer diffusion process involving transformations between elongated and almost cyclic conformers in an inchworm-like manner. These subtle intermolecular reorientations maintain an optimal balance of hydrogen-bonding and water–surface interactions throughout the process. This work shows that the diffusion of hydrogen-bonded clusters can occur at exceedingly low temperatures without the need for hydrogen bond breakage or exchange; findings that will influence Ostwald ripening of ice nanoclusters and hydrogen bonded clusters in general.
KW - diffusion
KW - hydrogen-bonding
KW - oligomers
KW - Water
UR - http://www.scopus.com/inward/record.url?scp=85122450398&partnerID=8YFLogxK
U2 - 10.48550/arXiv.2112.13549
DO - 10.48550/arXiv.2112.13549
M3 - Article
C2 - 34958578
AN - SCOPUS:85122450398
VL - 22
SP - 340
EP - 346
JO - Nano letters
JF - Nano letters
SN - 1530-6984
IS - 1
ER -