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Full Record Details
Persistent URL
http://purl.org/net/epubs/work/41690
Record Status
Checked
Record Id
41690
Title
Superlinearly converging dimer method for transition state search
Contributors
J Kaestner (Science and Technology Facilities Council)
,
P Sherwood (Science and Technology Facilities Council)
Abstract
Algorithmic improvements of the dimer method [G. Henkelman and H. Jónsson, J. Chem. Phys. 111, 7010 (1999)] are described in this paper. Using the limited memory Broyden-Fletcher-Goldfarb-Shanno (L-BFGS) optimizer for the dimer translation greatly improves the convergence compared to the previously used conjugate gradient algorithm. It also saves one energy and gradient calculation per dimer iteration. Extrapolation of the gradient during repeated dimer rotations reduces the computational cost to one gradient calculation per dimer rotation. The L-BFGS algorithm also improves convergence of the rotation. Thus, three to four energy and gradient evaluations are needed per iteration at the beginning of a transition state search, while only two are required close to convergence. Moreover, we apply the dimer method in internal coordinates to reduce coupling between the degrees of freedom. Weighting the coordinates can be used to apply chemical knowledge about the system and restrict the transition state search to only part of the system while minimizing the remainder. These improvements led to an efficient method for the location of transition states without the need to calculate the Hessian. Thus, it is especially useful in large systems with expensive gradient evaluations.
Organisation
CSE
,
CSE-CCG
,
CSE-BIO
,
STFC
Keywords
Physics
,
Chemistry
Funding Information
Related Research Object(s):
Licence Information:
Language
English (EN)
Type
Details
URI(s)
Local file(s)
Year
Journal Article
J Phys Chem
128 (2008): 014106.
doi:10.1063/1.2815812
2008
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