Related papers: Water: one molecule, two surfaces, one mistake
An overview of computational methods to describe high-dimensional potential energy surfaces suitable for atomistic simulations is given. Particular emphasis is put on accuracy, computability, transferability and extensibility of the methods…
For a given many-electron molecule, it is possible to define a corresponding one-electron Schr\"odinger equation, using potentials derived from simple atomic densities, whose solution predicts fairly accurate molecular orbitals for single-…
Solid-On-Solid (SOS) computer simulations are employed to investigate the sublimation of surfaces. We distinguish three sublimation regimes: layer-by-layer sublimation, free step flow and hindered step flow. The sublimation regime is…
Accurate, yet computationally efficient energy functions are essential for state-of-the art molecular dynamics (MD) studies of condensed phase systems. Here, a generic workflow based on a combination of machine learning-based and empirical…
Transition state theory was introduced in the 1930s to account for chemical reactions. Central to this theory is the idea of a potential energy surface (PES). It was assumed that such a surface could be constructed using eigensolutions of…
We introduce a general framework for many-body force field models, the Completely Multipolar Model (CMM), that utilizes multipolar electrical moments modulated by exponential decay of electron density as a common functional form for all…
Calculations of transition intensities for small molecules like H$_2$O, CO, CO$_2$ based on s high-quality potential energy surface (PES) and dipole moment surface (DMS) can nowadays reach sub-percent accuracy. An extension of this…
Effective mass and energy are investigated using the Schwinger-Dyson equation (SDE) in the complex plane. As simple examples, we solve the SDE for the (1+1)-dimensional model and the strongly coupled quantum electrodynamics (QED). We also…
Water is a notoriously difficult substance to model both accurately and efficiently. Here, we focus on descriptions with a single coarse-grained particle per molecule using the so-called Approximate Non-Conformal (ANC) and generalized…
Understanding the local structure of water at the interfaces of metallic electrodes is a key problem in aqueous-based electrochemistry. Nevertheless, a realistic simulation of such setup is challenging, particularly when the electrodes are…
Multipole moments are the first order responses of the energy to spatial derivatives of the electric field strength. The quality of density functional theory (DFT) prediction of molecular multipole moments thus characterizes errors in…
As the most important solvent, water has been at the center of interest since the advent of computer simulations. While early molecular dynamics and Monte Carlo simulations had to make use of simple model potentials to describe the atomic…
The impact of targeted replacement of individual terms in empirical force fields is quantitatively assessed for pure water, dichloromethane (DCM), and solvated K$^+$ and Cl$^-$ ions. For the electrostatics, point charges (PCs) and machine…
The Standard Model (SM) is the best description of fundamental particles and their interactions we have to date. From this theory, all phenomena in the macroscopic world (except for gravity) can be explained, and it has successfully…
Treating water as a linearly responding dielectric continuum on molecular length scales allows very simple estimates of solvation structure and thermodynamics for charged and polar solutes. While this approach can successfully account for…
A dielectric model of electrostatic solvation is applied to describe potentials of mean force in water along reaction paths for: a) formation of a sodium chloride ion pair; b) the symmetric SN2 exchange of chloride in methylchloride; and c)…
Atomistic simulations are a powerful tool for studying the dynamics of molecules, proteins, and materials on wide time and length scales. Their reliability and predictiveness, however, depend directly on the accuracy of the underlying…
For a given many-electron molecule, it is possible to define a corresponding one-electron Schr\"odinger equation, using potentials derived from simple atomic densities, whose solution predicts fairly accurate molecular orbitals for single-…
The calculation time for the energy of atoms and molecules scales exponentially with system size on a classical computer but polynomially using quantum algorithms. We demonstrate that such algorithms can be applied to problems of chemical…
There has been a veritable explosion of methods and software to perform machine-learned regression on datasets of electronic energies and forces to develop high-dimensional machine learned potential energy surfaces (ML-PESs). A major, but…