Related papers: Interfacial water asymmetry at ideal electrochemic…
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 electric double layer is an important structure that appears at charged liquid interfaces, and it determines the performance of various electrochemical devices such as supercapacitors and electrokinetic energy converters. Here the…
The interactions of a hydrophilic surface with water can significantly influence the characteristics of the liquid water interface. In this manuscript, we explore this influence by studying the molecular structure of liquid water at a…
The atomic-scale response of inhomogeneous fluids at interfaces and surrounding solute particles plays a critical role in governing chemical, electrochemical and biological processes at such interfaces. Classical molecular dynamics…
A major challenge in modelling interfacial processes in electrochemical (EC) devices is performing simulations at constant potential. This requires an open-boundary description of the electrons, so that they can enter and leave the…
Ion hydration and interfacial water play crucial roles in numerous phenomena ranging from biological to industrial systems. Although biologically relevant (and mostly smaller) ions have been studied extensively in this context, very little…
In this thesis we study the lateral electrostatic interaction between a pair of non-identical, moderately charged colloidal particles trapped at an electrolyte interface in the limit of short inter-particle separations. Using a simplified…
There is a growing interest in the study of coupled plasma-liquid systems because of their applications to biomedicine, biological and chemical disinfection, agriculture, and other areas. Without an understanding of the near-surface gas…
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…
The notion that large electric fields at the air-water interface catalyze spontaneous chemical reactions has sparked significant debate, with far reaching implications for atmospheric chemistry and interfacial reactivity. Using vibrational…
Spurred by the increasing needs in electrochemical energy storage devices, the electrode/electrolyte interface has received a lot of interest in recent years. Molecular dynamics simulations play a proeminent role in this field since they…
Studies of the thermodynamics of complex coacervation of pairs of symmetric, strongly ionizable, oppositely charged polyelectrolyte chains are abundant. To generalize such understanding to asymmetric chain lengths and variable ionizability…
Quantum-mechanical methods are widely used for understanding molecular interactions throughout biology, chemistry, and materials science. Quantum diffusion Monte Carlo (DMC) and coupled cluster with single, double, and perturbative triple…
It has been widely reported that as water contacts hydrophobic materials such as air or hydrocarbons (liquid or solid), the interfaces acquire a negative charge. It is not entirely clear whether this occurs due to the nature of water, or…
The electrostatic interaction between colloidal particles trapped at the interface between two immiscible electrolyte solutions is studied in the limit of small inter-particle distances. Within an appropriate model exact analytic…
Dipolar susceptibility of interfacial water and the corresponding interface dielectric constant were calculated from numerical molecular dynamics simulations for neutral and charged states of buckminsterfullerene C$_{60}$. Dielectric…
We report a detailed theoretical investigation on electrochemical capacitance of a nanoscale capacitor where there is a DC coupling between the two conductors. For this ``leaky'' quantum capacitor, we have derived general analytic…
Water molecules are traditionally regarded as passive dielectric media in electrochemical systems. In this work, we challenge this conventional perspective using molecular dynamics simulations and theoretical analysis. We show that…
A statistical mechanical distance constraint model (DCM) is presented that explicitly accounts for network rigidity among constraints present within a system. Constraints are characterized by local microscopic free energy functions.…
We investigate the solvation of methane and methane decorated with charges in spherically confined water droplets. Free energy profiles for a single methane molecule in droplets, ranging in diameter D, from 1 to 4 nm, show that the droplet…