Berlin 2024 – scientific programme

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O: Fachverband Oberflächenphysik

O 47: Metal Substrates I

O 47.2: Talk

Wednesday, March 20, 2024, 10:45–11:00, MA 043

Electronic Structure Benchmark Calculations for CO2 Reduction Products on Cu(111)-Clusters from Projection-Based Embedding Theory — •Elena Kolodzeiski and Christopher Stein — TU Munich, TUM School of Natural Sciences, Department of Chemistry, Lichtenbergstr. 4, 85748 Garching, Germany

Copper surfaces are promising catalysts for the conversion of carbon dioxide. Despite the immense interest in such systems, current theoretical approaches have limitations either in numerical cost or accuracy. We propose the use of a cluster model described by the projection-based embedding theory (PBET) as a balanced compromise. This approach involves partitioning the system into an active system and an environmental, focusing the computational efforts on the active subsystem. The system partitioning is based on our recently developed ACE-of-SPADE algorithm, which has been proven to enable consistent active orbital space selection even for such challenging systems as transition metal clusters. Here, we present a benchmark study validating the accuracy of the cluster embedding approach for calculating the binding energy of a series of CO2 reduction products on Cu(111)-clusters. The cluster approach is first verified by comparison to PBE plane-wave calculations and then extensively validated regarding the impact of different cluster models. We showed that the proposed QM/QM embedding strategy considerably improves the accuracy compared to PBE plane-wave calculations. PBET, in combination with the ACE-of-SPADE algorithm, provides a highly accurate method for studying chemical reactions on cluster models of metal surfaces.

Keywords: Embedding Calculations