Berlin 2024 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 60: Solid-Liquid Interfaces III: Reactions and Electrochemistry
O 60.9: Vortrag
Mittwoch, 20. März 2024, 17:15–17:30, MA 042
Extracting free energy charge transfer paths of solvated ions from molecular dynamic simulations — •Zhenyu Wang, Mira Todorova, Christoph Freysoldt, and Jörg Neugebauer — Max-Planck-Institut für Eisenforschung GmbH, Max-Planck-Str.-1, D-40237, Düsseldorf, Germany
The Marcus theory is indispensable for understanding and predicting electron transfer reactions, which are fundamental in various chemical and biological systems. While solvation shells play a key role in stabilizing ions in solution, a quantitative approach to assess charge transfer intricacies is currently absent. This study introduces a quantitative model to elucidate solvation shell formation precisely. In our model, ions’ charges (qcore) serve as generalized coordinates, and we derive free energy profiles as functions of qcore. We present a systematic workflow for generating solvation configurations around ions with varying charges. Thermodynamic integration aligns the free energy of ions in different charge states. Our approach successfully reproduces Marcus parabolas, revealing a pivotal transition in the solvation mode at qcore ≈ 0.5 e. This model significantly enhances our ability to quantitatively analyze charge transfer complexities, providing fresh insights into solvation shell dynamics. The outcomes of this work holds promise for advancing the understanding of electron transfer reactions in chemical and biological contexts.
Keywords: Marcus theory; electron transfer reaction; solvation configuration; molecular dynamics simulation