Berlin 2015 – wissenschaftliches Programm
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TT: Fachverband Tiefe Temperaturen
TT 38: Frontiers of Electronic Structure Theory: Nuclear Dynamics, Methods (jointly with O, HL)
TT 38.2: Vortrag
Dienstag, 17. März 2015, 11:00–11:15, MA 004
Towards First-Principles Modeling of Electrolytic Solvent Effects in Photo-Catalytic Water Splitting — •Stefan Ringe1, Sebastian Matera2, Harald Oberhofer1, and Karsten Reuter1 — 1Technische Universität München — 2Freie Universität Berlin
Due to the complexity of the physical processes underlying photo-catalytic surface reactions, ab-initio computational approaches have to overcome major challenges concerning accuracy and computational costs. In particular, an efficient description of electrolytic solvent effects—which are crucial for charge driven reactions—is highly necessary.
We present an implementation of the modified Poisson-Boltzmann (MPB) model in the highly parallel and numerically efficient all-electron DFT code FHI-aims. In contrast to most implicit solvent models, this technique combines nonlinear dielectric solvent response with a statistical description of solvated finite-sized ions. This has been shown to capture a majority of electrochemical solvent effects appearing in heterogeneous photo-catalysis.[1]
We developed a self-consistent function-space oriented solution scheme for Poisson-Boltzmann-like equations which in contrast to common multi-grid solvers is able to exploit the specialized grids and optimized integration schemes of FHI-aims. We demonstrate the approach and its efficiency for the linearized Poisson-Boltzmann equation and a range of molecular systems. Finally, we discuss how the methodology can be employed for the solution of non-linear problems. [1] Kilic,M.S., Bazant, M.Z., Phys. Rev. E, 75, 2007, 021502.