Dresden 2014 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 7: Focussed Session: Frontiers of Electronic Structure Theory - Non-equilibrium Phenomena at the Nano-scale
O 7.7: Vortrag
Montag, 31. März 2014, 12:45–13:00, TRE Ma
Towards a combined QM/MM and implicit solvent description of photoelectrochemical processes — •Markus Sinstein1, Daniel Berger1, Ran Jia2, Volker Blum3, Harald Oberhofer1, and Karsten Reuter1 — 1Technische Universität München, Germany — 2Jilin University, P.R. China — 3Duke University, USA
Photoelectrochemical systems are widely explored to drive energy-relevant redox reactions like water splitting or CO2 reduction. The detailed analysis of the involved elementary processes via first-principles calculations is challenged by the necessity to simultaneously account for the extended semiconductor photocatalyst and the liquid electrolyte. Especially for charge (proton and/or electron) transfer steps traditionally employed periodic boundary condition approaches involve charged supercells with difficult to control finite size errors. To this end, we present a solid state QM/MM embedding approach, in which only a finite cluster model of the photocatalyst surface is treated quantum mechanically and the correct Madelung potential of the periodic system is obtained by embedding into a charge field. For the efficient modeling of photoelectrochemical processes we combine this approach with an implicit solvation scheme within the DFT package FHI-aims. Finally, we also show early test results of the combined QM/MM implicit solvent model.