Behler, Jörg

[["dc.bibliographiccitation.issue","20"],["dc.bibliographiccitation.journal","Physical Review B"],["dc.bibliographiccitation.volume","101"],["dc.contributor.author","Eckhoff, Marco"],["dc.contributor.author","Blöchl, Peter E."],["dc.contributor.author","Behler, Jörg"],["dc.date.accessioned","2020-12-10T18:20:23Z"],["dc.date.available","2020-12-10T18:20:23Z"],["dc.date.issued","2020"],["dc.identifier.doi","10.1103/PhysRevB.101.205113"],["dc.identifier.eissn","2469-9969"],["dc.identifier.issn","2469-9950"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/75546"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area B | B03 Relaxation, Thermalisierung, Transport und Kondensation in hochangeregten Festkörpern"],["dc.relation","SFB 1073 | Topical Area C | C03 Vom Elektronentransfer zur chemischen Energiespeicherung: ab-initio Untersuchungen korrelierter Prozesse"],["dc.title","Hybrid density functional theory benchmark study on lithium manganese oxides"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","244703"],["dc.bibliographiccitation.issue","24"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","155"],["dc.contributor.author","Eckhoff, Marco"],["dc.contributor.author","Behler, Jörg"],["dc.date.accessioned","2022-04-01T10:00:40Z"],["dc.date.available","2022-04-01T10:00:40Z"],["dc.date.issued","2021"],["dc.description.abstract","Unraveling the atomistic and the electronic structure of solid-liquid interfaces is the key to the design of new materials for many important applications, from heterogeneous catalysis to battery technology. Density functional theory (DFT) calculations can, in principle, provide a reliable description of such interfaces, but the high computational costs severely restrict the accessible time and length scales. Here, we report machine learning-driven simulations of various interfaces between water and lithium manganese oxide (LixMn2O4), an important electrode material in lithium ion batteries and a catalyst for the oxygen evolution reaction. We employ a high-dimensional neural network potential to compute the energies and forces several orders of magnitude faster than DFT without loss in accuracy. In addition, a high-dimensional neural network for spin prediction is utilized to analyze the electronic structure of the manganese ions. Combining these methods, a series of interfaces is investigated by large-scale molecular dynamics. The simulations allow us to gain insights into a variety of properties, such as the dissociation of water molecules, proton transfer processes, and hydrogen bonds, as well as the geometric and electronic structure of the solid surfaces, including the manganese oxidation state distribution, Jahn-Teller distortions, and electron hopping."],["dc.identifier.doi","10.1063/5.0073449"],["dc.identifier.pmid","34972388"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/105483"],["dc.identifier.url","https://publications.goettingen-research-online.de/handle/2/105483"],["dc.language.iso","en"],["dc.notes.intern","DOI-Import GROB-530"],["dc.relation","SFB 1073 | Topical Area C | C03 Vom Elektronentransfer zur chemischen Energiespeicherung: ab-initio Untersuchungen korrelierter Prozesse"],["dc.relation","SFB 1073 | Topical Area C: Photonen- und elektronengetriebene Reaktionen"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation.eissn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.title","Insights into lithium manganese oxide–water interfaces using machine learning potentials"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","164107"],["dc.bibliographiccitation.issue","16"],["dc.bibliographiccitation.journal","The Journal of Chemical Physics"],["dc.bibliographiccitation.volume","153"],["dc.contributor.author","Eckhoff, Marco"],["dc.contributor.author","Lausch, Knut Nikolas"],["dc.contributor.author","Blöchl, Peter E."],["dc.contributor.author","Behler, Jörg"],["dc.date.accessioned","2021-04-14T08:31:42Z"],["dc.date.available","2021-04-14T08:31:42Z"],["dc.date.issued","2020"],["dc.identifier.doi","10.1063/5.0021452"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/83687"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-399"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C03 Vom Elektronentransfer zur chemischen Energiespeicherung: ab-initio Untersuchungen korrelierter Prozesse"],["dc.relation.eissn","1089-7690"],["dc.relation.issn","0021-9606"],["dc.title","Predicting oxidation and spin states by high-dimensional neural networks: Applications to lithium manganese oxide spinels"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.issue","17"],["dc.bibliographiccitation.journal","Physical Review B"],["dc.bibliographiccitation.volume","102"],["dc.contributor.author","Eckhoff, Marco"],["dc.contributor.author","Schönewald, Florian"],["dc.contributor.author","Risch, Marcel"],["dc.contributor.author","Volkert, Cynthia A."],["dc.contributor.author","Blöchl, Peter E."],["dc.contributor.author","Behler, Jörg"],["dc.date.accessioned","2021-04-14T08:31:34Z"],["dc.date.available","2021-04-14T08:31:34Z"],["dc.date.issued","2020"],["dc.identifier.doi","10.1103/PhysRevB.102.174102"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/83639"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-399"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C03 Vom Elektronentransfer zur chemischen Energiespeicherung: ab-initio Untersuchungen korrelierter Prozesse"],["dc.relation","SFB 1073 | Topical Area C | C05 Kontrolle Elektronen-getriebener Chemie durch Interkalation"],["dc.relation.eissn","2469-9969"],["dc.relation.issn","2469-9950"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.title","Closing the gap between theory and experiment for lithium manganese oxide spinels using a high-dimensional neural network potential"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]

[["dc.contributor.author","Schönewald, Florian"],["dc.contributor.author","Eckhoff, Marco"],["dc.contributor.author","Baumung, Max"],["dc.contributor.author","Risch, Marcel"],["dc.contributor.author","Blöchl, Peter E."],["dc.contributor.author","Behler, Jörg"],["dc.contributor.author","Volkert, Cynthia A."],["dc.date.accessioned","2021-10-15T10:22:40Z"],["dc.date.available","2021-10-15T10:22:40Z"],["dc.date.issued","2020-07-08"],["dc.description.abstract","We investigate the effect of the surface electronic structure and composition of LiMn$ nanoparticles on the electrocatalytic oxygen evolution reaction (OER). Scanning transmission electron microscopy (STEM) electron energy loss spectroscopy (EELS) studies combined with density functional theory (DFT) based simulations of the EEL spectra reveal in pristine nanoparticles a 4 nm thick surface layer with reduced average Mn oxidation state and increased Mn concentration. This is attributed to Mn$^{2+}$ partially replacing Li$^+$ at the tetrahedral sites of the spinel lattice accompanied by Mn 3d-state filling of octahedrally coordinated Mn. During electrocatalytic OER cycling, this near-surface tetrahedral Mn is leached out, thereby increasing the oxidation state of octahedrally coordinated Mn. Using rotating ring-disc electrode (RRDE) based detection of O and Mn during the OER, we show that the oxygen evolution remains constant while the Mn$^{2+}$ is removed, revealing that near-surface tetrahedrally coordinated Mn has no effect on the OER activity of LiMn$. This is surprising since the e$ occupancy of Mn in octahedral sites, which is widely used as a descriptor of OER activity, changes significantly in the surface layer during cycling. The fact that e$ emptying fails to correlate with OER activity here indicates that octahedral cation valence is not a fundamental measure of activity, either because the active surface state is not affected by tetrahedral Mn or because other details of the band structure or metal-oxygen bonding character, more strongly regulate the rate-limiting steps for OER."],["dc.identifier.arxiv","2007.04217v1"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/90947"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C03 Vom Elektronentransfer zur chemischen Energiespeicherung: ab-initio Untersuchungen korrelierter Prozesse"],["dc.relation","SFB 1073 | Topical Area C | C05 Kontrolle Elektronen-getriebener Chemie durch Interkalation"],["dc.title","A criticial view on e$ occupancy as a descriptor for oxygen evolution catalytic activity in LiMn$ nanoparticles"],["dc.type","preprint"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]

[["dc.bibliographiccitation.firstpage","3793"],["dc.bibliographiccitation.issue","6"],["dc.bibliographiccitation.journal","Journal of Chemical Theory and Computation"],["dc.bibliographiccitation.lastpage","3809"],["dc.bibliographiccitation.volume","15"],["dc.contributor.author","Eckhoff, Marco"],["dc.contributor.author","Behler, Jörg"],["dc.date.accessioned","2020-12-10T15:22:40Z"],["dc.date.available","2020-12-10T15:22:40Z"],["dc.date.issued","2019"],["dc.identifier.doi","10.1021/acs.jctc.8b01288"],["dc.identifier.eissn","1549-9626"],["dc.identifier.issn","1549-9618"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/73491"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.title","From Molecular Fragments to the Bulk: Development of a Neural Network Potential for MOF-5"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dspace.entity.type","Publication"]]