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Item type:Publication, Access status: with files , Effect of anion hydrophobicity on the oxidation of ferrocene-terminated monolayersSelf-assembled monolayers (SAMs) terminated with ferrocene ((Formula presented.)) moieties are a popular model system for electron transfer processes at solid-liquid interfaces. Numerous experimental studies have found a correlation between the hydrophobicity of anions in the electrolyte and the redox potential. In this computational study, the redox potential is calculated for various anion species and SAM configurations using classical molecular dynamics. Thermodynamic integration and the constrained charge method are used to determine the redox potential as the free energy change associated with electron transfers from the (Formula presented.) moieties to the electrodes. The results show the anticipated lower redox potentials for hydrophobic anions and allow the study of changes at the solid-liquid interface at the atomistic level.Publicationtype: Journal Article57 53 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Efficient treatment of long-range electrostatics in charge equilibration approaches(American Institute of Physics (AIP), 2025-05-07); ; ; ; A charge equilibration method based on real-space Gaussians as charge densities is presented. The implementation is part of the Electrode package available in the Large-scale Atomic/Molecular Massively Parallel Simulator and benefits from its efficient particle-mesh Ewald approach. A simple strategy required to switch from the previously used Slater-type orbital (STO) shielding to Gaussians is provided by fitting the Coulomb energy of two Gaussian charge distributions to the repulsion between two STOs. Their widths were optimized for O, Si, and Ti species, obtaining results consistent with previous studies using STOs in the case of SiO2 polymorphs. In the limit of sufficiently narrow Gaussians, it is shown that the implementation converges to electronegativity equalization method results for the case of Ti/TiOx interfaces. The method presented is implemented in a way that is potentially beneficial for the application of modern machine-learning force fields that include long-range electrostatic interactions.Publicationtype: Journal Article36 74