Behler, Jörg

[["dc.bibliographiccitation.firstpage","2957"],["dc.bibliographiccitation.issue","11"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry Letters"],["dc.bibliographiccitation.lastpage","2962"],["dc.bibliographiccitation.volume","10"],["dc.contributor.author","Spiering, Paul"],["dc.contributor.author","Shakouri, Khosrow"],["dc.contributor.author","Behler, Jörg"],["dc.contributor.author","Kroes, Geert-Jan"],["dc.contributor.author","Meyer, Jörg"],["dc.date.accessioned","2019-07-09T11:51:55Z"],["dc.date.available","2019-07-09T11:51:55Z"],["dc.date.issued","2019"],["dc.description.abstract","Electron-hole pair (ehp) excitation is thought to substantially affect the dynamics of molecules on metal surfaces, but it is not clear whether this can be better addressed by orbital-dependent friction (ODF) or the local density friction approximation (LDFA). We investigate the effect of ehp excitation on the dissociative chemisorption of N2 on and its inelastic scattering from Ru(0001), which is the benchmark system of highly activated dissociation, with these two different models. ODF is in better agreement with the best experimental estimates for the reaction probabilities than LDFA, yields results for vibrational excitation in better agreement with experiment, but slightly overestimates the translational energy loss during scattering. N2 on Ru(0001) is thus the first system for which the ODF and LDFA approaches are shown to yield substantially different results for easily accessible experimental observables, including reaction probabilities."],["dc.identifier.doi","10.1021/acs.jpclett.9b00523"],["dc.identifier.pmid","31088059"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/16229"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/60041"],["dc.language.iso","en"],["dc.notes.intern","Merged from goescholar"],["dc.relation","info:eu-repo/grantAgreement/EC/FP7/338580/EU//REACTIONBARRIOMETRY"],["dc.rights","CC BY-NC-ND 4.0"],["dc.rights.uri","https://creativecommons.org/licenses/by-nc-nd/4.0"],["dc.subject.ddc","540"],["dc.title","Orbital-Dependent Electronic Friction Significantly Affects the Description of Reactive Scattering of N 2 from Ru(0001)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","23470"],["dc.bibliographiccitation.issue","41"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry. C, Nanomaterials and Interfaces"],["dc.bibliographiccitation.lastpage","23480"],["dc.bibliographiccitation.volume","122"],["dc.contributor.author","Shakouri, Khosrow"],["dc.contributor.author","Behler, Jörg"],["dc.contributor.author","Meyer, Jörg"],["dc.contributor.author","Kroes, Geert-Jan"],["dc.date.accessioned","2019-07-09T11:46:04Z"],["dc.date.available","2019-07-09T11:46:04Z"],["dc.date.issued","2018"],["dc.description.abstract","The excitation of electron-hole pairs in reactive scattering of molecules at metal surfaces often affects the physical and dynamical observables of interest, including the reaction probability. Here, we study the influence of electron-hole pair excitation on the dissociative chemisorption of N2 on Ru(0001) using the local density friction approximation method. The effect of surface atom motion has also been taken into account by a high-dimensional neural network potential. Our nonadiabatic molecular dynamics simulations with electronic friction show that the reaction of N2 is more strongly affected by the energy transfer to surface phonons than by the energy loss to electron-hole pairs. The discrepancy between the computed reaction probabilities and experimental results is within the experimental error both with and without friction; however, the incorporation of electron-hole pairs yields somewhat better agreement with experiments, especially at high collision energies. We also calculate the vibrational efficacy for the N2 + Ru(0001) reaction and demonstrate that the N2 reaction is more enhanced by exciting the molecular vibrations than by adding an equivalent amount of energy into translation."],["dc.identifier.doi","10.1021/acs.jpcc.8b06729"],["dc.identifier.pmid","30364480"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/15390"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/59374"],["dc.language.iso","en"],["dc.notes.intern","Merged from goescholar"],["dc.relation","info:eu-repo/grantAgreement/EC/FP7/338580/EU//REACTIONBARRIOMETRY"],["dc.relation.issn","1932-7447"],["dc.rights","CC BY-NC-ND 4.0"],["dc.rights.uri","http://creativecommons.org/licenses/by-nc-nd/4.0/"],["dc.subject.ddc","540"],["dc.title","Analysis of Energy Dissipation Channels in a Benchmark System of Activated Dissociation: N2 on Ru(0001)."],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","1763"],["dc.bibliographiccitation.issue","8"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry Letters"],["dc.bibliographiccitation.lastpage","1768"],["dc.bibliographiccitation.volume","10"],["dc.contributor.author","Gerrits, N."],["dc.contributor.author","Shakouri, Khosrow"],["dc.contributor.author","Behler, Jörg"],["dc.contributor.author","Kroes, Geert-Jan"],["dc.date.accessioned","2019-07-09T11:51:24Z"],["dc.date.available","2019-07-09T11:51:24Z"],["dc.date.issued","2019"],["dc.description.abstract","An accurate description of reactive scattering of molecules on metal surfaces often requires the modeling of energy transfer between the molecule and the surface phonons. Although ab initio molecular dynamics (AIMD) can describe this energy transfer, AIMD is at present untractable for reactions with reaction probabilities smaller than 1%. Here, we show that it is possible to use a neural network potential to describe a polyatomic molecule reacting on a mobile metal surface with considerably reduced computational effort compared to AIMD. The highly activated reaction of CHD3 on Cu(111) is used as a test case for this method. It is observed that the reaction probability is influenced considerably by dynamical effects such as the bobsled effect and surface recoil. A special dynamical effect for CHD3 + Cu(111) is that a higher vibrational efficacy is obtained for two quanta in the CH stretch mode than for a single quantum."],["dc.identifier.doi","10.1021/acs.jpclett.9b00560"],["dc.identifier.pmid","30922058"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/16121"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/59942"],["dc.language.iso","en"],["dc.notes.intern","Merged from goescholar"],["dc.relation","info:eu-repo/grantAgreement/EC/FP7/338580/EU//REACTIONBARRIOMETRY"],["dc.rights","CC BY-NC-ND 4.0"],["dc.rights.uri","https://creativecommons.org/licenses/by-nc-nd/4.0"],["dc.subject.ddc","540"],["dc.title","Accurate Probabilities for Highly Activated Reaction of Polyatomic Molecules on Surfaces Using a High-Dimensional Neural Network Potential: CHD 3 + Cu(111)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","2131"],["dc.bibliographiccitation.issue","10"],["dc.bibliographiccitation.journal","The Journal of Physical Chemistry Letters"],["dc.bibliographiccitation.lastpage","2136"],["dc.bibliographiccitation.volume","8"],["dc.contributor.author","Shakouri, Khosrow"],["dc.contributor.author","Behler, Joerg"],["dc.contributor.author","Meyer, Joerg"],["dc.contributor.author","Kroes, Geert-Jan"],["dc.date.accessioned","2018-11-07T10:23:44Z"],["dc.date.available","2018-11-07T10:23:44Z"],["dc.date.issued","2017"],["dc.description.abstract","Ab initio molecular dynamics (AIMD) simulations enable the accurate description of reactive molecule-surface scattering especially if energy transfer involving surface phonons is important. However, presently, the computational expense of AIMD rules out its application to systems where reaction probabilities are smaller than about 1%. Here we show that this problem can be overcome by a high-dimensional neural network fit of the molecule-surface interaction potential, which also incorporates the dependence on phonons by taking into account all degrees of freedom of the surface explicitly. As shown for N-2 + Ru(0001), which is a prototypical case for highly activated dissociative chemisorption, the method allows an accurate description of the coupling of molecular and surface atom motion and accurately accounts for vibrational properties of the employed slab model of Ru(0001). The neural network potential allows reaction probabilities as low as 10(-5) to be computed, showing good agreement with experimental results."],["dc.identifier.doi","10.1021/acs.jpclett.7b00784"],["dc.identifier.isi","000402026500005"],["dc.identifier.pmid","28441867"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/14721"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/42520"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","PUB_WoS_Import"],["dc.publisher","Amer Chemical Soc"],["dc.relation.issn","1948-7185"],["dc.rights","CC BY-NC-ND 4.0"],["dc.rights.uri","https://creativecommons.org/licenses/by-nc-nd/4.0"],["dc.title","Accurate Neural Network Description of Surface Phonons in Reactive Gas-Surface Dynamics: N-2 + Ru(0001)"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.status","published"],["dspace.entity.type","Publication"]]