Related papers: First-principles theory of electrochemical capacit…
Ab initio techniques have revolutionised the way in which theory can help practitioners to explore critical mechanisms that govern reactions or properties, and to develop new strategies for materials discovery and design. Yet, their…
This work explores the use of joint density-functional theory, a new form of density-functional theory for the ab initio description of electronic systems in thermodynamic equilibrium with a liquid environment, to describe electrochemical…
In this work we theoretically study the differential capacitance of an aqueous electrolyte in contact with a planar electrode, using classical Density Functional Theory, and show how this measurable quantity can be used as a probe to better…
The ab initio simulation of charged interfaces in the framework of density functional theory (DFT) is heavily employed for the study of electrochemical energy conversion processes. The capacitance is the primary descriptor for the response…
The distribution of electric fields within the electrochemical double layer depends on both the electrode and electrolyte in complex ways. These fields strongly influence chemical dynamics in the electrode-electrolyte interface, but cannot…
Impressive progress in the control of atomically thin crystals is now enabling the realization of gated structures in which two electrodes are separated by atomic scale distances. The electrical capacitance of these structures is determined…
Most of the performances of electrochemical devices are governed by molecular processes taking place at the solution-electrode interfaces and molecular simulation are the main way to study these processes. Aqueous electrochemical systems…
Electromechanics in fluids describes the response of the number density to electric fields, and thus provides a powerful means by which to control the behavior of liquids. While continuum approaches have proven successful in describing…
Quantum-chemical processes in liquid environments impact broad areas of science, from molecular biology to geology to electrochemistry. While density-functional theory (DFT) has enabled efficient quantum-mechanical calculations which…
A diffuse interface (phase field) model for an electrochemical system is developed. We describe the minimal set of components needed to model an electrochemical interface and present a variational derivation of the governing equations. With…
We formulate a general mean-field theory of a flat electric double layer in ionic liquids and electrolyte solutions with ions possessing static polarizability and a permanent dipole moment on a charged electrode. We establish a new…
The electric double layer (EDL) governs electrocatalysis, energy conversion, and storage, yet its atomic structure, capacitance, and reactivity remain elusive. Here we introduce a machine learning interatomic potential framework that…
The electrical double layer (EDL) at aqueous solution-metal oxide interfaces critically affects many fundamental processes in electrochemistry, geology and biology, yet understanding its microscopic structure is challenging for both theory…
We present a study of the structure and differential capacitance of electric double layers of aqueous electrolytes. We consider Electric Double Layer Capacitors (EDLC) composed of spherical cations and anions in a dielectric continuum…
Density functional theory is used to describe electrolyte solutions in contact with electrodes of planar or spherical shape. For the electrolyte solutions we consider the so-called civilized model, in which all species present are treated…
Molecules can form myriad crystalline polymorphs, each with distinct properties affecting their performance across diverse applications, from pharmaceuticals to functional materials and more. Predicting the thermodynamically most stable…
As interest in nanomaterials grows, ab initio simulations play a crucial role in designing electrochemical catalysts. Electrochemical reactions depend on electrode potential, highlighting the importance of the grand canonical…
Computational chemistry has become an indispensable tool for generating data and insights, pervading all branches of experimental chemistry. Its most central concept is the potential energy hypersurface, key to all chemistry and materials…
To improve the understanding of the relation between electrode curvature and energy storage mechanisms, a systematic investigation of the correlation between convex and concave electrode surfaces and the differential capacitance of an…
We introduce a combined density functional theory (DFT) and non-equilibrium Green's function (NEGF) framework to compute the capacitance of nanocapacitors and directly extract the dielectric response of a sub-nanometer dielectric under…