title: Analytical gradients for subsystem density functional theory within the slater-function-based amsterdam density functional program.
abstract: We present a new implementation of analytical gradients for subsystem density-functional theory (sDFT) and frozen-density embedding (FDE) into the Amsterdam Density Functional program (ADF). The underlying theory and necessary expressions for the implementation are derived and discussed in detail for various FDE and sDFT setups. The parallel implementation is numerically verified and geometry optimizations with different functional combinations (LDA/TF and PW91/PW91K) are conducted and compared to reference data. Our results confirm that sDFT-LDA/TF yields good equilibrium distances for the systems studied here (mean absolute deviation: 0.09 Å) compared to reference wave-function theory results. However, sDFT-PW91/PW91k quite consistently yields smaller equilibrium distances (mean absolute deviation: 0.23 Å). The flexibility of our new implementation is demonstrated for an HCN-trimer test system, for which several different setups are applied. © 2016 Wiley Periodicals, Inc.
authors.affiliation: Theoretische Organische Chemie, Organisch-Chemisches Institut and Center for Multiscale Theory and Computation, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, Münster, 48149, Germany.
authors.forename: Danny
authors.initials: D
authors.lastname: Schlüns
authors.affiliation: Amsterdam Center for Multiscale Modeling, Vrije Universiteit Amsterdam, De Boelelaan 1083, HV Amsterdam, 1081, The Netherlands.|Scientific Computing & Modelling NV, Vrije Universiteit, Theoretical Chemistry, De Boelelaan 1083, HV Amsterdam, 1081, The Netherlands.
authors.forename: Mirko
authors.initials: M
authors.lastname: Franchini
authors.affiliation: San Diego Supercomputer Center, University of California San Diego, 9500 Gilman Drive, La Jolla, California, 92093-0505, USA.
authors.forename: Andreas W
authors.identifier: 0000-0002-8048-6906
authors.initials: AW
authors.lastname: Götz
authors.affiliation: Theoretische Organische Chemie, Organisch-Chemisches Institut and Center for Multiscale Theory and Computation, Westfälische Wilhelms-Universität Münster, Corrensstraße 40, Münster, 48149, Germany.
authors.forename: Johannes
authors.initials: J
authors.lastname: Neugebauer
authors.affiliation: Institute of Physical and Theoretical Chemistry, TU Braunschweig, Hans-Sommer-Straße 10, Braunschweig, 38106, Germany.
authors.forename: Christoph R
authors.initials: CR
authors.lastname: Jacob
authors.affiliation: Amsterdam Center for Multiscale Modeling, Vrije Universiteit Amsterdam, De Boelelaan 1083, HV Amsterdam, 1081, The Netherlands.
authors.forename: Lucas
authors.initials: L
authors.lastname: Visscher
mesh_terms: D000465:Algorithms; D003198:Computer Simulation; D008956:Models, Chemical; D008958:Models, Molecular; D021281:Quantitative Structure-Activity Relationship
keywords: analytical gradients; geometry optimization; subsystem density functional theory