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We show that generalized spherical harmonics are well suited for representing the space and orientation molecular density in the resolution of the molecular density functional theory. We consider the common system made of a rigid solute of…

Chemical Physics · Physics 2017-10-11 Lu Ding , Maximilien Levesque , Daniel Borgis , Luc Belloni

Accurately describing strong electron correlation in complex systems remains a prominent challenge in computational chemistry as near-term quantum algorithms treating total correlation often require prohibitively deep circuits. Here we…

Computational Engineering, Finance, and Science · Computer Science 2026-04-21 Zhanou Liu , Yuhao Chen , Yingjin Ma , Xiao He , Yuxin Deng

Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…

Quantum Physics · Physics 2023-07-17 Taehee Ko , Xiantao Li , Chunhao Wang

Classical density-functional theory provides an efficient alternative to molecular dynamics simulations for understanding the equilibrium properties of inhomogeneous fluids. However, application of density-functional theory to multi-site…

Computational Physics · Physics 2014-02-14 Ravishankar Sundararaman , T. A. Arias

The influence of a chemically or electrically heterogeneous distribution of interaction sites at a planar substrate on the number density of an adjacent fluid is studied by means of classical density functional theory (DFT). In the case of…

Soft Condensed Matter · Physics 2018-05-25 Maximilian Mußotter , Markus Bier , S. Dietrich

In this work we give a comprehensive derivation of an exact and numerically feasible method to perform ab-initio calculations of quantum particles interacting with a quantized electromagnetic field. We present a hierachy of…

We investigate the impact of electronic correlations and quantum delocalization onto the static structure factor and static density response function of the strongly coupled electron liquid. In contrast to a classical system, the density…

Chemical Physics · Physics 2024-05-21 Tobias Dornheim , Panagiotis Tolias , Jan Vorberger , Zhandos Moldabekov

Solvation is a notoriously difficult and nagging problem for the rigorous theoretical description of chemistry in the liquid phase. Successes and failures of various approaches ranging from implicit solvation modeling through dielectric…

Chemical Physics · Physics 2020-04-01 Gregor N. Simm , Paul L. Türtscher , Markus Reiher

New ways to treat electron correlation in electronic structure problems are discussed in the context of many-electron theory. The present work focuses primarily on static correlation. In related work, a method for including dynamical…

Chemical Physics · Physics 2018-09-05 Jerry L. Whitten

We present a reformulation of QM/MM as a fully quantum mechanical theory of interacting subsystems, all treated at the level of density functional theory (DFT). For the MM subsystem, which lacks orbitals, we assign an ad hoc electron…

Classical density-functional theory is the most direct approach to equilibrium structures and free energies of inhomogeneous liquids, but requires the construction of an approximate free-energy functional for each liquid of interest. We…

Soft Condensed Matter · Physics 2014-10-10 Ravishankar Sundararaman , Kendra Letchworth-Weaver , T A Arias

Density functional theory is the workhorse of modern electronic structure calculations, with wide-ranging applications in chemistry, physics, materials science, and machine learning. At its heart lies the exchange-correlation functional, a…

Chemical Physics · Physics 2026-02-20 Fabien Tran , Susi Lehtola , Stefano Pittalis , Miguel A. L. Marques

The influence of poor solvent quality on fluid demixing of a model mixture of colloids and nonadsorbing polymers is investigated using density functional theory. The colloidal particles are modelled as hard spheres and the polymer coils as…

Soft Condensed Matter · Physics 2009-11-07 Matthias Schmidt , Alan R. Denton

We present a continuum theory of electrolytes composed of a waterlike solvent and univalent ions. First, we start with a density functional $\cal F$ for the coarse-grained solvent, cation, and anion densities, including the Debye-H\"uckel…

Soft Condensed Matter · Physics 2020-08-20 Ryuichi Okamoto , Kenichiro Koga , Akira Onuki

Modelling electrolytes accurately on both a nanoscale and cell level can contribute to improving battery chemistries.[Armand and Tarascon, Nature, 2008, 451, 652-657] We previously presented a thermodynamic continuum model for…

Chemical Physics · Physics 2024-08-09 Constantin Schwetlick , Max Schammer , Arnulf Latz , Birger Horstmann

Stochastic density functional theory is applied to analyze the conductivity of strong two species electrolytes at arbitrary field strengths. The corresponding stochastic equations for the density of the electrolyte species are solved by…

Statistical Mechanics · Physics 2016-05-04 Vincent Démery , David S Dean

A crucial aspect in the simulation of electrochemical interfaces consists in treating the distribution of electronic charge of electrode materials that are put in contact with an electrolyte solution. Recently, it has been shown how a…

Materials Science · Physics 2024-07-16 Andrea Grisafi , Mathieu Salanne

One of the potential applications of a quantum computer is solving quantum chemical systems. It is known that one of the fastest ways to obtain somewhat accurate solutions classically is to use approximations of density functional theory.…

Quantum Physics · Physics 2020-11-18 Thomas E. Baker , David Poulin

The solvation model proposed by Fattebert and Gygi [Journal of Computational Chemistry 23, 662 (2002)] and Scherlis et al. [Journal of Chemical Physics 124, 074103 (2006)] is reformulated, overcoming some of the numerical limitations…

Chemical Physics · Physics 2012-08-09 Oliviero Andreussi , Ismaila Dabo , Nicola Marzari

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…

Soft Condensed Matter · Physics 2017-04-24 Andreas Reindl , Markus Bier , S. Dietrich