The Library
The role of nuclear quantum effects in the relative stability of hexagonal and cubic ice
Tools
Tools
Tools
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 ISSN 0021-9606.
|
PDF
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 | ||||||||
|---|---|---|---|---|---|---|---|---|---|
| Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
||||||||
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Science > Physics |
||||||||
| 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: |
|
||||||||
| 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 | ||||||||
| Date of first compliant deposit: | 25 March 2021 | ||||||||
| Date of first compliant Open Access: | 25 March 2021 | ||||||||
| RIOXX Funder/Project Grant: |
|
||||||||
| Related URLs: |
Request changes or add full text files to a record
Repository staff actions (login required)
 |
View Item |
Downloads
Downloads per month over past year
