Related papers: Solvation Lies Within: Simulating Condensed-Phase …
By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…
We propose an approach that links density functional theory (DFT) and molecular dynamics (MD) simulation to study fluid behavior in nanopores in contact with bulk (macropores). It consists of two principal steps. First, the theoretical…
Despite the modern level of development of computational chemistry methods and techno-logical progress, fast and accurate determination of solvation free energy remains a huge problem for physical chemists. In this paper, we describe two…
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…
We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…
We present a family of alchemical perturbation potentials that enable the calculation of hydration free energies of small to medium-sized molecules in a concerted single alchemical coupling step instead of the commonly used sequence of two…
Energy decomposition analysis (EDA) based on absolutely localized molecular orbitals provides detailed insights into intermolecular bonding by decomposing the total molecular binding energy into physically meaningful components. Here, we…
Many important applications of electronic structure methods involve molecules or solid surfaces in a solvent medium. Since explicit treatment of the solvent in such methods is usually not practical, calculations often employ continuum…
We generate representative structural models of amorphous carbon (a-C) from constant-volume quenching from the liquid with subsequent relaxation of internal stresses in molecular dynamics simulations using empirical and machine-learning…
Spatially resolved electron energy-loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM) has been used to investigate as fluidic phase in nanoubbles embedded in a metallic Pd90Pt10 matrix. Using the 1s->2p…
The electronic charge density plays a central role in determining the behavior of matter at the atomic scale, but its computational evaluation requires demanding electronic-structure calculations. We introduce an atom-centered,…
We present a computational protocol, based on density matrix perturbation theory, to obtain non-adiabatic, frequency-dependent electron-phonon self-energies for molecules and solids. Our approach enables the evaluation of electron-phonon…
Second-Harmonic Scatteringh (SHS) experiments provide a unique approach to probe non-centrosymmetric environments in aqueous media, from bulk solutions to interfaces, living cells and tissue. A central assumption made in analyzing SHS…
Extensive molecular dynamics computer simulations have been conducted for ethanol-water liquid mixtures in the water-rich side of the composition range, with 10, 20 and 30 mol % of the alcohol, at temperatures between room temperature and…
Acid solutions exhibit a variety of complex structural and dynamical features arising from the presence of multiple interacting reactive proton defects and counterions. However, disentangling the transient structural motifs of proton…
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…
Methanol-water liquid mixtures have been investigated by high-energy synchrotron X-ray and neutron diffraction at low temperatures. We are thus able to report the first complete sets of both X-ray and neutron weighted total scattering…
Starting from the observation that one of the most successful methods for solving the Kohn-Sham equations for periodic systems -- the plane-wave method -- is a spectral method based on eigenfunction expansion, we formulate a spectral method…
We present results of theoretical description and numerical calculation of the dynamics of molecular liquids based on the Reference Interaction Site Model / Mode-Coupling Theory. They include the temperature-pressure(density) dependence of…
We apply a number of atomic decomposition schemes across the standard QM7 dataset -- a small model set of organic molecules at equilibrium geometry -- to inspect the possible emergence of trends among contributions to atomization energies…