Related papers: Electrolytes structure near electrodes with molecu…
We analyze a model problem representing a multi-electronic molecule sitting on a metal surface. Working with a reduced configuration interaction Hamiltonian, we show that one can extract very accurate ground state wavefunctions as compared…
Whether or not specific ion effects determine the charge storage properties of aqueous graphene and graphite-based supercapacitors remains a highly debated topic. In this work we present a multiscale quantum mechanics classical molecular…
Progress in electrochemical applications of ionic liquids builds on an understanding of electrical double-layer. This computational study focuses on structure-determined quantities -- maximum packing density, potentials and capacitances --…
We use Monte Carlo simulations to examine the simplest model of an ionic liquid, called the restricted primitive model, at a metal surface. We find that at moderately low temperatures the capacitance of the metal/ionic liquid interface is…
The structure of the double-layer formed at the surface of carbon electrodes is governed by the interactions between the electrode and the electrolyte species. However, carbon is notoriously difficult to simulate accurately, even with…
We study the response of a model micro-electrochemical cell to a large ac voltage of frequency comparable to the inverse cell relaxation time. To bring out the basic physics, we consider the simplest possible model of a symmetric binary…
Quantum dots (QDs), embedded in supercapacitors (S-C) cells exhibited capacitance amplification that peaked at certain QD concentration. More than 2.5 peak amplification was demonstrated with cyclic voltammetry (C-V) at a scan rate of 0.1…
We investigate active electrolytes within the mean-field level of description. The focus is on how the double-layer structure of passive, thermalized charges is affected by active dynamics of all constituting ions. One feature of active…
We introduce a new form of density functional theory for the {\em ab initio} description of electronic systems in contact with a molecular liquid environment. This theory rigorously joins an electron density-functional for the electrons of…
We review recent ab initio molecular dynamics studies of electrode/electrolyte interfaces in lithium ion batteries. Our goals are to introduce experimentalists to simulation techniques applicable to models which are arguably most faithful…
A solid ionic conductor with cation conductivity in the interelectrode region is studied. Due to their large size, the anions are considered fixed and form a homogeneous neutralizing electric background. The model can be used to describe…
The quest for safe high-energy batteries with "5V-class" cathodes and lithium metal anodes drives research into solid electrolytes. However, reasons for the large charge transfer resistances -- the major bottleneck of all-solid-state…
An application of quantum size carbon structures--graphenes as electrodes of supercapacitors is studied. A fundamental limit of energy and power density arising from quantum nature of objects due to singularity in graphene density of states…
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…
Electrolyte gating is a powerful technique for accumulating large carrier densities in surface two-dimensional electron systems (2DES). Yet this approach suffers from significant sources of disorder: electrochemical reactions can damage or…
We investigate the complexation of a highly charged sphere with a long flexible polyelectrolyte, \textit{both negatively charged} in salt free environment. Electroneutrality is insured by the presence of divalent counterions. Using…
We theoretically study electrostatic properties of electric double layer using a generalized Poisson-Boltzmann approach taking into account the orientational ordering of water dipoles and the excluded volume effect of water molecules as…
The properties of rechargeable lithium-ion batteries are determined by the electrochemical and kinetic properties of their constituent materials as well as by their underlying microstructure. Microstructural design can be leveraged to…
As a class of electron-rich materials, electrides demonstrate promising applications in many fields. However, the required high pressure restricts the practical applications to some extent. This study reveals that the unique feature of…
We propose a framework to study the spatio-temporal evolution of liquid-liquid phase separation of weak polyelectrolytes in ionic solutions. Unlike strong polyelectrolytes, which carry a fixed charge, the charge state of weak…