Nudged elastic band calculations accelerated with Gaussian process regression

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dc.contributor Aalto-yliopisto fi
dc.contributor Aalto University en Koistinen, Olli-Pekka Dagbjartsdóttir, Freyja B. Ásgeirsson, Vilhjálmur Vehtari, Aki Jonsson, Hannes 2018-08-01T12:43:00Z 2018-08-01T12:43:00Z 2017-10-21
dc.identifier.citation Koistinen , O-P , Dagbjartsdóttir , F B , Ásgeirsson , V , Vehtari , A & Jonsson , H 2017 , ' Nudged elastic band calculations accelerated with Gaussian process regression ' Journal of Chemical Physics , vol 147 , no. 15 , 152720 , pp. 1-14 . DOI: 10.1063/1.4986787 en
dc.identifier.issn 0021-9606
dc.identifier.issn 1089-7690
dc.identifier.other PURE UUID: 59149a6b-08a3-4ff3-b0a5-52c7067bed0b
dc.identifier.other PURE ITEMURL:
dc.identifier.other PURE LINK:
dc.identifier.other PURE FILEURL:
dc.description.abstract Minimum energy paths for transitions such as atomic and/or spin rearrangements in thermalized systems are the transition paths of largest statistical weight. Such paths are frequently calculated using the nudged elastic band method, where an initial path is iteratively shifted to the nearest minimum energy path. The computational effort can be large, especially when ab initio or electron density functional calculations are used to evaluate the energy and atomic forces. Here, we show how the number of such evaluations can be reduced by an order of magnitude using a Gaussian process regression approach where an approximate energy surface is generated and refined in each iteration. When the goal is to evaluate the transition rate within harmonic transition state theory, the evaluation of the Hessian matrix at the initial and final state minima can be carried out beforehand and used as input in the minimum energy path calculation, thereby improving stability and reducing the number of iterations needed for convergence. A Gaussian process model also provides an uncertainty estimate for the approximate energy surface, and this can be used to focus the calculations on the lesser-known part of the path, thereby reducing the number of needed energy and force evaluations to a half in the present calculations. The methodology is illustrated using the two-dimensional Müller-Brown potential surface and performance assessed on an established benchmark involving 13 rearrangement transitions of a heptamer island on a solid surface. en
dc.format.extent 1-14
dc.format.mimetype application/pdf
dc.language.iso en en
dc.relation.ispartofseries Journal of Chemical Physics en
dc.relation.ispartofseries Volume 147, issue 15 en
dc.rights openAccess en
dc.subject.other 113 Computer and information sciences en
dc.title Nudged elastic band calculations accelerated with Gaussian process regression en
dc.type A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä fi
dc.description.version Peer reviewed en
dc.contributor.department Department of Computer Science
dc.contributor.department University of Iceland
dc.contributor.department Department of Applied Physics
dc.subject.keyword 113 Computer and information sciences
dc.identifier.urn URN:NBN:fi:aalto-201808014174
dc.identifier.doi 10.1063/1.4986787 info:eu-repo/date/embargoEnd/2018-09-21

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