Related papers: Ions at electrochemical interfaces: from explicit …
The organic salt $\alpha$-(BEDT-TTF)$_2$I$_3$ is considered a model system for metal-insulator transition due to electronic charge ordering at $T_{\rm CO}=135$~K. The optical properties obtained from polarized reflection measurements above…
Fundamental understanding of interatomic forces in molecules must emerge from quantum mechanics, yet widely used empirical force fields rely on simplified mechanistic approximations that often fail to capture the complexity of many-body…
Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in…
Understanding ion adsorption at electrified metal-electrolyte interfaces is essential for accurate modeling of electrochemical systems. Here, we systematically investigate the free energy profiles of Na$^+$, Cl$^-$, and F$^-$ ions at the…
Battery electrode surfaces are generally coated with electronically insulating solid films of thickness 1-50 nm. Both electrons and Li+ can move at the electrode-surface film interface in response to the voltage, which adds complexity to…
Using non-equilibrium molecular dynamics simulations and a coarse grained model of ionic liquids, we have investigated the impact that the shape and the intramolecular charge distribution of the ions have on the electrotuneable friction…
Many key industrial processes, from electricity production, conversion and storage to electrocatalysis or electrochemistry in general, rely on physical mechanisms occurring at the interface between a metallic electrode and an electrolyte…
The ion distribution of electrolytes near interfaces with dielectric contrast has important consequences for electrochemical processes and many other applications. To date, most studies of such systems have focused on geometrically simple…
Atomistic simulations of electrochemical interfaces remain challenging due to the long time scales required to adequately sample the structure of the electric double layer. The emergence of efficient, short-range machine learning…
As a first step to meet the challenge to calculate the electronic structure and total energy of charged states of atoms and molecules adsorbed on ultrathin-insulating films supported by a metallic substrate using density functional theory…
Accurate modelling of electrostatic interactions and charge transfer is fundamental to computational chemistry, yet most machine learning interatomic potentials (MLIPs) rely on local atomic descriptors that cannot capture long-range…
Organo-metallic molecular structures where a single metallic atom is embedded in the organic backbone are ideal systems to study the effect of strong correlations on their electronic structure. In this work we calculate the electronic and…
Alkali salt-doped ionic liquids are emerging as promising electrolyte systems for energy applications, owing to their excellent interfacial stability. To address their limited ionic conductivity, various strategies have been proposed,…
The influence of inner electrons on the ionization dynamics in strong laser fields is investigated in a wavelength regime where the inner electron dynamics is usually assumed to be negligible. The role of inner electrons is of particular…
A crucial aspect in the simulation of electrochemical interfaces consists in treating the distribution of electronic charge of electrode materials that are put in contact with an electrolyte solution. Recently, it has been shown how a…
Dense plasma environment affects the electronic structure of ions via variations of the microscopic electrical fields, also known as plasma screening. This effect can be either estimated by simplified analytical models, or by…
We have recently developed a method based on relativistic time-dependent density functional theory (TD-DFT) that allows the calculation of electronic spectra in solution (Creutzberg, Hedeg{\aa}rd, J. Chem. Theory Comput.18, 2022, 3671).…
While fluids near a solid surface are at the core of applications in energy storage/conversion, electrochemistry/electrowetting and adsorption/catalysis, their nanoscale behavior remains only partially deciphered. Beyond conventional…
While first-principles calculations of electrode-molecule binding play an indispensable role in obtaining atomic-level understanding in surface science and electrochemistry, a significant challenge remains because the adsorption energy is…
The electrostatic interaction between two non-identical, moderately charged colloids situated in close proximity of each other at a fluid interface is studied. By resorting to a well-justified model system, this problem is analytically…