Permanent URL to this publication: http://dx.doi.org/10.5167/uzh-51642
Watkins, M; Pan, D; Wang, E G; Michaelides, A; VandeVondele, J; Slater, B (2011). Large variation of vacancy formation energies in the surface of crystalline ice. Nature Materials, 10(10):794-798.
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Resolving the atomic structure of the surface of ice particles within clouds, over the temperature range encountered in the atmosphere and relevant to understanding heterogeneous catalysis on ice, remains an experimental challenge. By using first-principles calculations, we show that the surface of crystalline ice exhibits a remarkable variance in vacancy formation energies, akin to an amorphous material. We find vacancy formation energies as low as similar to 0.1-0.2 eV, which leads to a higher than expected vacancy concentration. Because a vacancy's reactivity correlates with its formation energy, ice particles may be more reactive than previously thought. We also show that vacancies significantly reduce the formation energy of neighbouring vacancies, thus facilitating pitting and contributing to pre-melting and quasi-liquid layer formation. These surface properties arise from proton disorder and the relaxation of geometric constraints, which suggests that other frustrated materials may possess unusual surface characteristics.
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|Item Type:||Journal Article, refereed, original work|
|Communities & Collections:||07 Faculty of Science > Department of Chemistry|
|Deposited On:||08 Jan 2012 20:52|
|Last Modified:||11 Jun 2014 23:48|
|Publisher:||Nature Publishing Group|
|Other Identification Number:||ISI:000295155200017|
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