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We propose a fully ab initio theory to compute the electron density response under the perturbation in the local field. This method is based on our recently developed local dielectric response theory [Phys. Rev. B 92, 241107(R), 2015],…

Materials Science · Physics 2020-02-18 Xiaochuan Ge , Deyu Lu

The nonlocal dielectric properties of liquid water are studied in the context of {\it ab initio} molecular dynamics simulations based on density functional theory. We calculate the dielectric response from the charge structure factor of 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…

Materials Science · Physics 2015-07-10 Kevin Leung , Andrew Leenheer

We present an efficient implemention of a non-equilibrium Green function (NEGF) method for self-consistent calculations of electron transport and forces in nanostructured materials. The electronic structure is described at the level of…

Mesoscale and Nanoscale Physics · Physics 2015-06-04 Jingzhe Chen , Kristian S. Thygesen , Karsten W. Jacobsen

Manipulation of the charge of the dielectric interface between two bulk liquids not only enables the adjustment of the interfacial tension but also controls the storage capacity of ions in the ionic double layers adjacent to each side of…

Soft Condensed Matter · Physics 2018-03-14 Marise J. E. Westbroek , Niels Boon , René van Roij

We theoretically study the electronic transport in the monolayer of dithiolated phenylene vinylene oligomeres coupled to the (111) surfaces of gold electrodes. We use non-equilibrium Green functions (NEGF) and density functional theory(DFT)…

Materials Science · Physics 2009-11-10 Z. Crljen , A. Grigoriev , G. Wendin , K. Stokbro

Unraveling the atomistic and the electronic structure of solid-liquid interfaces is the key to the design of new materials for many important applications, from heterogeneous catalysis to battery technology. Density functional theory (DFT)…

Materials Science · Physics 2022-01-25 Marco Eckhoff , Jörg Behler

The accurate modeling of the dielectric properties of water is crucial for many applications in physics, computational chemistry and molecular biology. This becomes possible in the framework of nonlocal electrostatics, for which we propose…

Classical Physics · Physics 2009-11-10 A. Hildebrandt , R. Blossey , S. Rjasanow , O. Kohlbacher , H. -P. Lenhof

The discrete and charge-separated nature of matter - electrons and nuclei - results in local electrostatic fields that are ubiquitous in nanoscale structures and are determined by their shape, material, and environment. Such fields are…

We show that when a molecular junction is under an external bias, its properties can not be uniquely determined by the total electron density in the same manner as the density functional theory (DFT) for ground state (GS) properties. In…

Mesoscale and Nanoscale Physics · Physics 2013-11-26 Shuanglong Liu , Yuan Ping Feng , Chun Zhang

We study dynamic nonequilibrium electron charging phenomena in ballistic molecular devices at room temperature that compromise their response to bias and whose nature is evidently distinguishable from static Schottky-type potential…

Mesoscale and Nanoscale Physics · Physics 2008-05-13 Ioannis Deretzis , Antonino La Magna

The design of better heterogeneous catalysts for applications such as fuel cells and electrolyzers requires a mechanistic understanding of electrocatalytic reactions and the dependence of their activity on operating conditions such as pH. A…

Chemical Physics · Physics 2016-06-16 Kathleen Schwarz , Bingjun Xu , Yushan Yan , Ravishankar Sundararaman

A first-principles approach is demonstrated to calculate the relationship between aqueous semiconductor interface structure and energy level alignment. The physical interface structure is sampled using density functional theory based…

Materials Science · Physics 2015-06-22 Neerav Kharche , James T. Muckerman , Mark S. Hybertsen

Electronic properties of heterostructures in which a finite number of Mott-insulator layers are sandwiched by semi-infinite metallic leads are investigated by using the dynamical-mean-field method combined with the Keldysh Green's function…

Strongly Correlated Electrons · Physics 2009-11-13 Satoshi Okamoto

Transport properties of molecular junctions are notoriously expensive to calculate with ab initio methods, primarily due to the semi-infinite electrodes. This has led to the introduction of different approximation schemes for the…

Mesoscale and Nanoscale Physics · Physics 2014-03-18 C. J. O. Verzijl , J. S. Seldenthuis , J. M. Thijssen

In the last decade, computational studies of liquid water have mostly concentrated on ground state properties. However recent spectroscopic measurements have been used to infer the structure of water, and the interpretation of optical and…

Materials Science · Physics 2016-08-31 David Prendergast , Jeffrey C. Grossman , Giulia Galli

A variational theory is developed to study electrolyte solutions, composed of interacting point-like ions in a solvent, in the presence of dielectric discontinuities and charges at the boundaries. Three important and non-linear…

Soft Condensed Matter · Physics 2013-05-29 Sahin Buyukdagli , Manoel Manghi , John Palmeri

Dielectric interfaces are crucial to the behavior of charged membranes, from graphene to synthetic and biological lipid bilayers. Understanding electrolyte behavior near these interfaces remains a challenge, especially in the case of rough…

Soft Condensed Matter · Physics 2024-04-03 Nicholas Pogharian , Alexandre P. dos Santos , Ali Ehlen , Monica Olvera de la Cruz

Density functional theory (DFT) is used to rationalize magnetic parameters of hydrated electron trapped in alkaline glasses as observed using Electron Paramagnetic Resonance (EPR) and Electron Spin Echo Envelope Modulation (ESEEM)…

General Physics · Physics 2016-09-28 I. A. Shkrob

Long-range ion induced water-water correlations were recently observed in femtosecond elastic second harmonic scattering experiments of electrolyte solutions. To further the qualitative understanding of these correlations, we derive an…

Statistical Mechanics · Physics 2017-09-06 David M. Wilkins , David E. Manolopoulos , Sylvie Roke , Michele Ceriotti