Regensburg 2025 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 84: Gerhard Ertl Young Investigator Award Competition

O 84.4: Vortrag

Donnerstag, 20. März 2025, 12:00–12:30, H24

Towards Understanding Surface Restructuring: Automatic Process Exploration and Local Environment Analysis — •Patricia Poths, King Chun Lai, Francesco Cannizzaro, Christoph Scheurer, Sebastian Matera, and Karsten Reuter — Fritz-Haber-Institut der MPG, Berlin

The formation of surface oxides on the Pd(100) surface is a prototypical example of catalyst surface restructuring under operando conditions. Despite extensive investigation of this process, its mechanism and corresponding time scales remain unknown. By combining a Machine-Learned Interatomic Potential with our newly-developed Automatic Process Explorer (APE) [1], we study the O-induced restructuring of the Pd(410) vicinal surface as an example for step-edge initiation of oxide formation. We identify ∼3,000 unique elementary processes. Taking first steps towards a comprehensive mechanism, we analyze this rich library of processes utilizing a fuzzy classification methodology [2]. Many identified pathways involve non-intuitive complex collective motion of several atoms. These pathways can explain experimentally-observed restructuring, such as step bunching or microfaceting. Furthermore, the time scales of the majority of restructuring pathways are comparable to those of catalytic processes, implying significant coupling between surface restructuring and catalysis [3].

[1] Lai et al., ChemRxiv, DOI:10.26434/chemrxiv-2024-jbzr7 .

[2] Lai et al., J. Chem. Phys. 159, 024129 (2023).

[3] Poths et al., ChemRxiv, DOI:10.26434/chemrxiv-2024-36l28 .

Keywords: Automatic process exploration; surface restructuring; catalysis