Davidson, ER;
Klimeš, J;
Alfè, D;
Michaelides, A;
(2014)
Cooperative interplay of van der Waals forces and quantum nuclear effects on adsorption: H at graphene and at coronene.
ACS Nano
, 8
(10)
9905 - 9913.
10.1021/nn505578x.
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Abstract
The energetic barriers that atoms and molecules often experience when binding to surfaces are incredibly important to a myriad of chemical and physical processes. However, these barriers are difficult to describe accurately with current computer simulation approaches. Two prominent contemporary challenges faced by simulation are the role of van der Waals forces and nuclear quantum effects. Here we examine the widely studied model systems of hydrogen on graphene and coronene using a van der Waals inclusive density functional theory approach together with path integral molecular dynamics at 50 K. We find that both van der Waals and quantum nuclear effects work together in a cooperative manner to dramatically reduce the barriers for hydrogen atoms to adsorb. This suggests that the low temperature hydrogenation of graphene is easier than previously thought and in more general terms that the combined roles of van der Waals and quantum tunnelling can lead to qualitative changes in adsorption.
| Type: | Article |
|---|---|
| Title: | Cooperative interplay of van der Waals forces and quantum nuclear effects on adsorption: H at graphene and at coronene |
| Location: | United States |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/nn505578x |
| Publisher version: | http://dx.doi.org/10.1021/nn505578x |
| Language: | English |
| Additional information: | This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in ACS Nano, copyright © American Chemical Society after peer review. To access the final edited and published work see http://dx.doi.org/10.1021/nn505578x |
| Keywords: | density functional theory, path integral molecular dynamics, quantum nuclear effects, van der Waals forces |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Earth Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy |
| URI: | https://discovery.ucl.ac.uk/id/eprint/1462175 |
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