期刊
JOURNAL OF PHYSICS-CONDENSED MATTER
卷 22, 期 7, 页码 -出版社
IOP Publishing Ltd
DOI: 10.1088/0953-8984/22/7/074203
关键词
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资金
- EURYI
- EPSRC [EP/F067496]
- Royal Society
- Office of Science and Technology
- Engineering and Physical Sciences Research Council [EP/F067496/1, EP/E503969/1] Funding Source: researchfish
- EPSRC [EP/E503969/1, EP/F067496/1] Funding Source: UKRI
The performance of a variety of techniques for locating transition states on potential energy surfaces is evaluated within the density functional theory framework. Diffusion of a water molecule across NaCl(001) and HCl bond breaking on the same surface are treated as general test cases; the former is an example of a low barrier diffusion process and the latter an example of a relatively high barrier covalent bond rupture event. The methods considered include the nudged elastic band (NEB), Dewar, Healy and Stewart (DHS), dimer, constrained optimization (CO), activation-relaxation technique (ART) and one-side growing string (OGS) as well as novel combinations of the DHS with growing string (DHS + GS) and DHS plus climbing image (CI-DHS). A key conclusion to come from this study is that the NEB method is relatively fast, especially when just a single (climbing) image is used. Indeed, using more images represents an unnecessary computational burden for our set of processes. The dimer method exhibits variable performance; being poor for the water diffusion processes, which have small activation energies, but much more efficient for the HCl bond breaking process which has a higher barrier. When only a poor initial guess of the transition state geometry is available, the CI-DHS scheme is one of the most efficient techniques considered. And as a means to quickly establish an approximate minimum energy pathway the DHS + GS scheme offers some potential.
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