Related papers: Using molecular similarity to construct accurate s…
An exponential interaction is constructed so that one-dimensional atoms and chains of atoms mimic the general behavior of their three-dimensional counterparts. Relative to the more commonly used soft-Coulomb interaction, the exponential…
The derivative discontinuity of the exchange-correlation functional of density-functional theory is cast as the difference of two types of electron affinities. We show that standard Kohn-Sham calculations can be used to calculate both…
Machine-learning of atomic-scale properties amounts to extracting correlations between structure, composition and the quantity that one wants to predict. Representing the input structure in a way that best reflects such correlations makes…
Maximum entropy models are increasingly being used to describe the collective activity of neural populations with measured mean neural activities and pairwise correlations, but the full space of probability distributions consistent with…
Reduced density-matrix functional theory (RDMFT) is a promising alternative approach to the problem of electron correlation. Like standard density functional theory, it contains an unknown exchange-correlation functional, for which several…
A parameterization strategy for molecular models on the basis of force fields is proposed, which allows a rapid development of models for small molecules by using results from quantum mechanical (QM) ab initio calculations and thermodynamic…
We show here that the Hamiltonian for an electronic system may be written exactly in terms of fluctuation operators that transition constituent fragments between internally correlated states, accounting rigorously for inter-fragment…
We develop a quantum mechanical theory to describe the optical response of semiconductor nanostructures with a particular emphasis on higher-order harmonic Generation. Based on a tight-binding approach we take all two-particle correlations…
First-principles calculations combining density-functional theory and continuum solvation models enable realistic theoretical modeling and design of electrochemical systems. When a reaction proceeds in such systems, the number of electrons…
Interacting electrons in a semiconductor quantum dot at strong magnetic fields exhibit a rich set of states, including correlated quantum fluids and crystallites of various symmetries. We develop in this paper a perturbative scheme based on…
In this perspective, the various measures of electron correlation used in wavefunction theory, density functional theory and quantum information theory are briefly reviewed. We then focus on a more traditional metric based on dominant…
We investigate the accuracy and efficiency of the semiclassical Frozen Gaussian method in describing electron dynamics in real time. Model systems of two soft-Coulomb-interacting electrons are used to study correlated dynamics under…
Using the optimized effective potential method in conjunction with the semi-analytical approximation due to Krieger, Li and Iafrate, we have performed fully self-consistent exact exchange-only density-functional calculations for diatomic…
A simple comparison between the exact and approximate correlation components U of the electron-electron repulsion energy of several states of few-electron harmonium atoms with varying confinement strengths provides a superior validation…
Because of the potentially large number of important applications of nonlinear optics, researchers have expended a great deal of effort to optimize the second-order molecular nonlinear-optical response, called the hyperpolarizability. The…
In this chapter we focus first on the theoretical methods and relevant computational approaches to calculate the electronic structure of atoms, molecules, and clusters containing heavy elements for which relativistic effects become…
Machine learning has emerged as a powerful tool for predicting molecular properties in chemical reaction networks with reduced computational cost. However, accurately predicting energies of transition state (TS) structures remains a…
Molecular electronics on silicon has distinct advantages over its metallic counterpart. We describe a theoretical formalism for transport through semiconductor-molecule heterostructures, combining a semi-empirical treatment of the bulk…
We combine density-functional theory with density-matrix functional theory to get the best of both worlds. This is achieved by range separation of the electronic interaction which permits to rigorously combine a short-range density…
Achieving long-range ferrimagnetic order in purely organic systems remains a major challenge in molecular magnetism. Here we report the synthesis and characterization of heterospin-coupling motifs, formed by covalently linking spin-1/2 and…