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Accuracy of buffered-force QM/MM simulations of silica
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Peguiron, Anke, Ciacchi, Lucio Colombi, De Vita, Alessandro, Kermode, James R. and Moras, Gianpietro (2015) Accuracy of buffered-force QM/MM simulations of silica. Journal of Chemical Physics, 142 . 064116. doi:10.1063/1.4907786 ISSN 0021-9606.
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Official URL: http://dx.doi.org/10.1063/1.4907786
Abstract
We report comparisons between energy-based quantum mechanics/molecular mechanics (QM/MM) and buffered force-based QM/MM simulations in silica. Local quantities—such as density of states, charges, forces, and geometries—calculated with both QM/MM approaches are compared to the results of full QM simulations. We find the length scale over which forces computed using a finite QM region converge to reference values obtained in full quantum-mechanical calculations is ∼10 Å rather than the ∼5 Å previously reported for covalent materials such as silicon. Electrostatic embedding of the QM region in the surrounding classical point charges gives only a minor contribution to the force convergence. While the energy-based approach provides accurate results in geometry optimizations of point defects, we find that the removal of large force errors at the QM/MM boundary provided by the buffered force-based scheme is necessary for accurate constrained geometry optimizations where Si–O bonds are elongated and for finite-temperature molecular dynamics simulations of crack propagation. Moreover, the buffered approach allows for more flexibility, since special-purpose QM/MM coupling terms that link QM and MM atoms are not required and the region that is treated at the QM level can be adaptively redefined during the course of a dynamical simulation.
| 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, Engineering and Medicine > Engineering > Engineering | |||||||||||||||
| Library of Congress Subject Headings (LCSH): | Quantum theory, Silica | |||||||||||||||
| Journal or Publication Title: | Journal of Chemical Physics | |||||||||||||||
| Publisher: | American Institute of Physics | |||||||||||||||
| ISSN: | 0021-9606 | |||||||||||||||
| Official Date: | 12 February 2015 | |||||||||||||||
| Dates: |
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| Volume: | 142 | |||||||||||||||
| Number of Pages: | 13 | |||||||||||||||
| Article Number: | 064116 | |||||||||||||||
| DOI: | 10.1063/1.4907786 | |||||||||||||||
| Status: | Peer Reviewed | |||||||||||||||
| Publication Status: | Published | |||||||||||||||
| Access rights to Published version: | Restricted or Subscription Access | |||||||||||||||
| Description: | Argonne Leadership Computing Facility at Argonne National Laboratory is supported by the Office of Science of the U.S. Department of Energy under contract DE-AC02-06CH11357. |
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| Date of first compliant deposit: | 29 December 2015 | |||||||||||||||
| Date of first compliant Open Access: | 29 December 2015 | |||||||||||||||
| Funder: | Seventh Framework Programme (European Commission) (FP7), Engineering and Physical Sciences Research Council (EPSRC), Imperial College, London. Rio Tinto Centre for Advanced Mineral Recovery, Deutsche Forschungsgemeinschaft (DFG) | |||||||||||||||
| Grant number: | 229205 (FP7), EP/L014742/1 (EPSRC), EP/L027682/1 (EPSRC), CI 144/2 (DFG) | |||||||||||||||
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