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The role of nuclear quantum effects in the relative stability of hexagonal and cubic ice
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Buxton, Samuel J., Quigley, David and Habershon, Scott (2019) The role of nuclear quantum effects in the relative stability of hexagonal and cubic ice. The Journal of Chemical Physics, 151 (14). 144503. doi:10.1063/1.5123992
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WRAP-role-nuclear-quantum-effects-relative-stability-hexagonal-cubic-2019.pdf - Accepted Version - Requires a PDF viewer. Download (915Kb) | Preview |
Official URL: http://dx.doi.org/10.1063/1.5123992
Abstract
At atmospheric pressure, hexagonal ice (Ih) is thermodynamically stable relative to cubic ice (Ic), although the magnitude and underlying physical origin of this stability difference are not well defined. Pure Ic crystals are not accessible experimentally, and hence computer simulations have often been used to interrogate the relative stabilities of Ih and Ic; however, these simulations are dominated by molecular interaction models that ignore the intramolecular flexibility of individual water molecules, do not describe intermolecular hydrogen-bonding with sufficient accuracy, or ignore the role of nuclear quantum effects (NQEs) such as zero-point energy. Here, we show that when comparing the relative stability of Ih and Ic using a flexible, anharmonic molecular interaction model, while also accurately accounting for NQEs, a new picture emerges: Ih is stabilized relative to Ic as a result of subtle differences in the intramolecular geometries and intermolecular interactions of water molecules which are modulated by NQEs. Our simulations hence suggest that NQEs are a major contributor to the stabilization of Ih under terrestrial conditions and thus contribute to the well-known hexagonal (sixfold) symmetry of ice crystals.
| Item Type: | Journal Article | ||||||||
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| Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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| Divisions: | Faculty of Science > Chemistry Faculty of Science > Physics |
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| Library of Congress Subject Headings (LCSH): | Quantum theory , Nuclear physics, Ice crystals -- Growth, Computational chemistry , Nucleation | ||||||||
| Journal or Publication Title: | The Journal of Chemical Physics | ||||||||
| Publisher: | AIP | ||||||||
| ISSN: | 0021-9606 | ||||||||
| Official Date: | 14 October 2019 | ||||||||
| Dates: |
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| Volume: | 151 | ||||||||
| Number: | 14 | ||||||||
| Article Number: | 144503 | ||||||||
| DOI: | 10.1063/1.5123992 | ||||||||
| Status: | Peer Reviewed | ||||||||
| Publication Status: | Published | ||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||
| RIOXX Funder/Project Grant: |
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