title: Global Materials Structure Search with Chemically Motivated Coordinates.
abstract: Identification of relevant reaction pathways in ever more complex composite materials and nanostructures poses a central challenge to computational materials discovery. Efficient global structure search, tailored to identify chemically relevant intermediates, could provide the necessary first-principles atomistic insight to enable a rational process design. In this work we modify a common feature of global geometry optimization schemes by employing automatically generated collective curvilinear coordinates. The similarity of these coordinates to molecular vibrations enhances the generation of chemically meaningful trial structures for covalently bound systems. In the application to hydrogenated Si clusters, we concomitantly observe a significantly increased efficiency in identifying low-energy structures and exploit it for an extensive sampling of potential products of silicon-cluster soft landing on Si(001) surfaces.
authors.affiliation: Department Chemie, Technische Universität München , Lichtenbergstr. 4, D-85748 Garching, Germany.
authors.forename: Chiara
authors.initials: C
authors.lastname: Panosetti
authors.affiliation: Department Chemie, Technische Universität München , Lichtenbergstr. 4, D-85748 Garching, Germany.
authors.forename: Konstantin
authors.initials: K
authors.lastname: Krautgasser
authors.affiliation: Physical and Theoretical Chemistry Laboratory, Department of Chemistry, University of Oxford , South Parks Road, Oxford, OX1 3QZ, United Kingdom.
authors.forename: Dennis
authors.initials: D
authors.lastname: Palagin
authors.affiliation: Department Chemie, Technische Universität München , Lichtenbergstr. 4, D-85748 Garching, Germany.
authors.forename: Karsten
authors.initials: K
authors.lastname: Reuter
authors.affiliation: Department of Chemistry, Yale University , New Haven, Connecticut 06520, United States.
authors.forename: Reinhard J
authors.initials: RJ
authors.lastname: Maurer
keywords: Basin hopping; adsorbate structure search; curvilinear coordinates; delocalized internals; global optimization