Dresden 2014 – wissenschaftliches Programm

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TT: Fachverband Tiefe Temperaturen

TT 15: Focus Session: Frontiers of Electronic Structure Theory - Non-Equilibrium Phenomena at the Nano-Scale (organized by O)

TT 15.7: 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.