Related papers: An Open-Source Framework for Analyzing $N$-Electro…
In this contribution, we extend our framework for analyzing and visualizing correlated many-electron dynamics to non-variational, highly scalable electronic structure method. Specifically, an explicitly time-dependent electronic wave packet…
The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures and reaction mechanism of these many-body quantum objects are defined on the level of…
We develop a density matrix formalism to describe coupled electron-nuclear dynamics. To this end we introduce an effective Hamiltonian formalism that describes electronic transitions and small (quantum) nuclear fluctuations along a…
Due to a beneficial balance of computational cost and accuracy, real-time time-dependent density functional theory has emerged as a promising first-principles framework to describe electron real-time dynamics. Here we discuss recent…
The study of electronic transitions within a molecule connected to the absorption or emission of light is a common task in the process of the design of new materials. The transitions are complex quantum mechanical processes and a detailed…
This paper derives and demonstrates a new, purely density-based ab initio approach for calculation of the energies and properties of many-electron systems. It is based upon the discovery of relationships that govern the "mechanics" of the…
Time-dependent (current) density functional theory for many-electron systems strongly coupled to quantized electromagnetic modes of a microcavity is proposed. It is shown that the electron-photon wave function is a unique functional of the…
Various ways to analyze the dynamical response of clusters and molecules to electromagnetic perturbations exist. Particularly rich information can be obtained from measuring the properties of electrons emitted in the course of the…
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 propose a first-principles time-dependent density functional theoretical (TDDFT) approach in momentum (P) space for quantitative study of electron transport in molecular devices under arbitrary biases. In this approach, the basic…
We present two methods for computing the dynamic structure factor for warm dense hydrogen without invoking either the Born-Oppenheimer approximation or the Chihara decomposition, by employing a wave-packet description that resolves the…
Conceiving a molecule as composed of smaller molecular fragments, or subunits, is one of the pillars of the chemical and physical sciences, and leads to productive methods in quantum chemistry. Using a fragmentation scheme, efficient…
We present the fully general time-dependent multiconfiguration self-consistent-field method to describe the dynamics of a system consisting of arbitrary different kinds and numbers of interacting fermions and bosons. The total wave function…
Multi-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from electronic excitations, to open-shell…
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 method which computes many-electron energies and eigenfunctions by a full configuration interaction which uses a basis of atomistic tight-binding wave functions. This approach captures electron correlation as well as atomistic…
An electron density functional approach for the calculation of the nuclear multipole moments is presented. The electronic matrix elements entering the experimentally observed hyperfine electron-nucleus interaction constants in atoms are…
Many-electron wavepacket dynamics based on time-dependent configuration interaction (TDCI) is a numerically rigorous approach to quantitatively model electron-transfer across molecular junctions. TDCI simulations of cyanobenzene…
To leverage the redundancy between the electronic structure computed at each step of first-principles molecular dynamics, we present a data-driven modeling framework for Kohn-Sham Density Functional Theory that bypasses the explicit…
A first-principles approach to describe electron dynamics in open quantum systems driven far from equilibrium via external time-dependent stimuli is introduced. Within this approach, the driven Liouville von Neumann methodology is used to…