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Intramolecular water divining: Locating H2O inside a C60 cage

Intramolecular water divining: Locating H2O inside a C60 cage
Intramolecular water divining: Locating H2O inside a C60 cage
We determine the location of an H2O molecule isolated within an adsorbed buckminsterfullerene cage, and compare this to the intrafullerene position of HF. Using normal incidence X-ray standing wave (NIXSW) analysis, coupled with density functional theory and molecular dynamics simulations, we show that both H2O and HF are located at an off-centre position within the fullerene cage, caused by substantial intra-cage electrostatic fields generated by surface adsorption of the fullerene. The atomistic and electronic structure simulations also reveal significant internal rotational motion consistent with the NIXSW data. Despite this substantial intra-cage interaction, we find that neither HF or H2O contribute to the endofullerene frontier orbitals, confirming the chemical isolation of the encapsulated molecules. We also show that our experimental NIXSW measurements and theoretical data are best described by a mixed adsorption site model.
2399-3669
Jarvis, Samuel P
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Sang, Hongqian
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Junqueira, Filipe
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Gordon, Oliver
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Hodgkinson, Jo E. A.
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Saywell, Alex
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Rahe, Philipp
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Mamone, Salvatore
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Taylor, Simon
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Sweetman, Adam
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Leaf, Jeremy
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Duncan, David
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Lee, Tien-Lin
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Thakur, Pardeep K.
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Hoffman, Gabriella
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Whitby, Richard J.
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Levitt, Malcolm H.
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Held, Georg
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Kantorovich, Lev
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Moriarty, Philip
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Jones, Robert G
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Jarvis, Samuel P
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Sang, Hongqian
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Junqueira, Filipe
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Gordon, Oliver
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Hodgkinson, Jo E. A.
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Saywell, Alex
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Rahe, Philipp
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Mamone, Salvatore
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Taylor, Simon
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Sweetman, Adam
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Leaf, Jeremy
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Duncan, David
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Lee, Tien-Lin
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Thakur, Pardeep K.
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Hoffman, Gabriella
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Whitby, Richard J.
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Levitt, Malcolm H.
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Held, Georg
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Kantorovich, Lev
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Moriarty, Philip
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Jones, Robert G
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Jarvis, Samuel P, Sang, Hongqian, Junqueira, Filipe, Gordon, Oliver, Hodgkinson, Jo E. A., Saywell, Alex, Rahe, Philipp, Mamone, Salvatore, Taylor, Simon, Sweetman, Adam, Leaf, Jeremy, Duncan, David, Lee, Tien-Lin, Thakur, Pardeep K., Hoffman, Gabriella, Whitby, Richard J., Levitt, Malcolm H., Held, Georg, Kantorovich, Lev, Moriarty, Philip and Jones, Robert G (2021) Intramolecular water divining: Locating H2O inside a C60 cage. Communications Chemistry. (In Press)

Record type: Article

Abstract

We determine the location of an H2O molecule isolated within an adsorbed buckminsterfullerene cage, and compare this to the intrafullerene position of HF. Using normal incidence X-ray standing wave (NIXSW) analysis, coupled with density functional theory and molecular dynamics simulations, we show that both H2O and HF are located at an off-centre position within the fullerene cage, caused by substantial intra-cage electrostatic fields generated by surface adsorption of the fullerene. The atomistic and electronic structure simulations also reveal significant internal rotational motion consistent with the NIXSW data. Despite this substantial intra-cage interaction, we find that neither HF or H2O contribute to the endofullerene frontier orbitals, confirming the chemical isolation of the encapsulated molecules. We also show that our experimental NIXSW measurements and theoretical data are best described by a mixed adsorption site model.

Text
H2O_C60_accepted - Accepted Manuscript
Restricted to Repository staff only until 30 August 2022.
Available under License Creative Commons Attribution.
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Accepted/In Press date: 20 July 2021

Identifiers

Local EPrints ID: 450887
URI: http://eprints.soton.ac.uk/id/eprint/450887
ISSN: 2399-3669
PURE UUID: c3e43ce4-c059-4e71-800e-48249c71b9a8
ORCID for Richard J. Whitby: ORCID iD orcid.org/0000-0002-9891-5502
ORCID for Malcolm H. Levitt: ORCID iD orcid.org/0000-0001-9878-1180

Catalogue record

Date deposited: 18 Aug 2021 16:32
Last modified: 19 Aug 2021 01:37

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Contributors

Author: Samuel P Jarvis
Author: Hongqian Sang
Author: Filipe Junqueira
Author: Oliver Gordon
Author: Jo E. A. Hodgkinson
Author: Alex Saywell
Author: Philipp Rahe
Author: Salvatore Mamone
Author: Simon Taylor
Author: Adam Sweetman
Author: Jeremy Leaf
Author: David Duncan
Author: Tien-Lin Lee
Author: Pardeep K. Thakur
Author: Gabriella Hoffman
Author: Georg Held
Author: Lev Kantorovich
Author: Philip Moriarty
Author: Robert G Jones

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