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Regensburg 2022 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 38: Solid-Liquid Interfaces 4: Reactions and Electrochemistry

O 38.5: Vortrag

Mittwoch, 7. September 2022, 11:45–12:00, H4

Enter the Void: Cavity Formation at Metal-Water Interfaces — •Thorben Eggert1,2, Nicolas G. Hörmann1, and Karsten Reuter11Fritz-Haber-Institut der Max-Planck-Gesellschaft, Berlin, Germany — 2Technical University of Munich, Munich, Germany

Cavity formation is an important concept when rationalizing the solvation of ions. However, most studies analyze cavities only in bulk liquids, omitting that their properties may change dramatically at solid-liquid interfaces.

Here, we study cavities at interfaces, particularly their free energy of formation based on molecular dynamics simulations. Specifically, we use a particle insertion approach, as well as the Multistate Bennett Acceptance Ratio method. We demonstrate that cavity formation at interfaces is dependent on the substrate material, which can be partially rationalized by the substrate-specific interfacial water structure. Furthermore, we observe stabilized cavities behind the first solvation layer of water.

These results might on the one hand rationalize recent theoretical suggestions of a non-electrostatic, attractive force on ions near interfaces, and on the other hand enable the improvement of implicit solvation models, which typically neglect substrate-specificity in their description.

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