Related papers: First-principles theory of electrochemical capacit…
The renewable energy sector critically needs low-cost and environmentally neutral energy storage solutions throughout the entire device life cycle. However, the limited performance of standard water-based electrochemical systems prevents…
First-principles calculations combining density-functional theory and continuum solvation models enable realistic theoretical modeling and design of electrochemical systems. When a reaction proceeds in such systems, the number of electrons…
Understanding the electrodes' surface morphology influence on the ions' distribution is essential for designing the supercapacitors with enhanced energy density characteristics. We develop a model for the structure of electrolytes near the…
The Bragg-Williams free energy is used to incorporate nearest-neighbor interactions into the lattice gas model of a solvent-free ionic liquid near a planar electrode. We calculate the differential capacitance from solutions of the…
Constant-potential molecular dynamics (MD) simulations are indispensable for understanding the capacitance, structure, and dynamics of electrical double layers (EDLs) at the atomistic level. However, the classical constant-potential method,…
The interface plays a critical role in electrochemical systems, driving the development of various theories to investigate properties at nanoscale and microscale levels, including the electrictrochemical double layer (EDL) theory and…
Modeling microstructure evolution in electrochemical systems is vital for understanding the mechanism of various electrochemical processes. In this work, we propose a general phase field framework that is fully variational and thus…
Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…
In all theoretical treatments of electron transport through single molecules between two metal electrodes, a clear distinction has to be made between a coherent transport regime with a strong coupling throughout the junction and a Coulomb…
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…
Implicit solvation is an effective, highly coarse-grained approach in atomic-scale simulations to account for a surrounding liquid electrolyte on the level of a continuous polarizable medium. Originating in molecular chemistry with finite…
Electrode-electrolyte interfaces are crucial for electrochemical energy conversion and storage. At these interfaces, the liquid electrolytes form electrical double layers (EDLs). However, despite more than a century of active research, the…
The electrical double layer (EDL) is fundamental to the operation of devices for electrochemical energy storage and conversion. Existing models of EDL in solid electrolytes focus predominantly on the space charge layer and lack a complete…
The coupled quantum dynamics of electrons and protons is ubiquitous in many dynamical processes involving light-matter interaction, such as solar energy conversion in chemical systems and photosynthesis. A first-principles description of…
We show that classical molecular density functional theory (MDFT), here in the homogeneous reference fluid approximation in which the functional is inferred from the properties of the bulk solvent, is a powerful new tool to study, at a…
In order to obtain a reasonably accurate and easily implemented approach to many-electron calculations, we will develop a new Density Functional Theory (DFT). Specifically, we derive an approximation to electron density, the first term of…
We develop a new density functional theory (DFT) and formalism for correlated electron systems by taking as reference an interacting electron system that has a ground state wavefunction which obeys exactly the Gutzwiller approximation for…
The capacitance of an arbitrarily shaped object is calculated with the same second-kind integral equation method used for computing static and dynamic polarizabilities. The capacitance is simply the dielectric permittivity multiplied by the…
The self consistent version of the density functional theory (DFT) is presented, which allows to calculate the ground state and dynamic properties of finite multi-electron systems such as atoms, molecules and clusters. The exact functional…
Combining classical density functional theory (cDFT) with quantum mechanics (QM) methods offers a computationally efficient alternative to traditional QM/molecular mechanics (MM) approaches for modeling mixed quantum-classical systems at…