Related papers: Time-dependent restricted-active-space self-consis…

The present work explores quantitative limits to the Single-Active Electron (SAE) approximation, often used to deal with strong-field ionization and subsequent attosecond dynamics. Using a time-dependent multi\-configuration approach,…

High harmonic generation (HHG) provides a flexible framework for the development of coherent light sources in the extreme-ultraviolet and soft x-ray regimes. However it suffers from low conversion efficiencies as the control of the HHG…

We present a novel theoretical scheme for orbital relaxation in configuration interaction singles (CIS) based on a perturbative treatment of its electronic Hessian, whose analytical derivation is also established in this work. The proposed…

We present a grid-based implementation of the time-dependent configuration-interaction singles method suitable for computing the strong-field ionization of small gas-phase molecules. After outlining the general equations of motion used in…

Given the time-evolution of an electron charge density, the local potential in Kohn-Sham time-dependent density functional theory (KS-TDDFT) can be modeled as a sum of instantaneous and dynamic contributions by assuming a certain form of…

We propose a framework to learn the time-dependent Hartree-Fock (TDHF) inter-electronic potential of a molecule from its electron density dynamics. Though the entire TDHF Hamiltonian, including the inter-electronic potential, can be…

We introduce a framework for resolving electron-hole dynamics within wavefunction-based multiconfigurational time-dependent Hartree-Fock (MCTDHF) theory. Central to this framework is a time-domain generalization of the extended Koopmans'…

We present the extension of the time-dependent configuration interaction singles (TDCIS) method to the computation of the electron kinetic-energy spectrum in photoionization processes. Especially for strong and long ionizing light pulses…

Electron-positron interactions have been utilized in various fields of science. Here we develop time-dependent multi-component density functional theory to study the coupled electron-positron dynamics from first principles. We prove that…

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and…

We report the derivation and implementation of orbital optimization algorithms for the active space decomposition (ASD) model, which are extensions of complete active space self-consistent field (CASSCF) and its occupation-restricted…

A major challenge in using spin-flip time-dependent density functional theory (SF-TD-DFT) for spin-flip-down excitations is the presence of spin contamination. While several improved methods have been developed in the past, a simple and…

In this Colloquium, the wavefunction-based Multiconfigurational Time-Dependent Hartree approaches to the dynamics of indistinguishable particles (MCTDH-F for Fermions and MCTDH-B for Bosons) are reviewed. MCTDH-B and MCTDH-F or, together,…

We present the theory, implementation, and benchmarking of a real-time time-dependent density functional theory (RT-TDDFT) module within the RMG code, designed to simulate the electronic response of molecular systems to external…

The time-dependent surface flux method developed for the description of electronic spectra [L. Tao and A. Scrinzi, New J. Phys. 14, 013021 (2012); A. Scrinzi, New J. Phys. 14, 085008 (2012)] is extended to treat dissociation and…

The Direct Simulation Monte Carlo (DSMC) method is widely employed for simulating rarefied nonequilibrium gas flows. With advances in aerospace engineering and micro/nano-scale technologies, gas flows exhibit the coexistence of rarefied and…

The complete active space self-consistent field (CASSCF) method is the principal approach employed for studying strongly correlated systems. However, exact CASSCF can only be performed on small active spaces of ~20 electrons in ~20 orbitals…

We propose a self-consistent scheme for the determination of the ground-state (GS) properties of interacting electrons in a magnetic field, and of systems whose GS's time-reversal-symmetry (TRS) is spontaneously broken. It is based on a…

Accurately modeling chemical reactions at the atomistic level requires high-level electronic structure theory due to the presence of unpaired electrons and the need to properly describe bond breaking and making energetics. Commonly used…