Related papers: Time Dependent Adaptive Configuration Interaction …
The family of temporal difference (TD) methods span a spectrum from computationally frugal linear methods like TD({\lambda}) to data efficient least squares methods. Least square methods make the best use of available data directly…
Attosecond charge migration is a periodic evolution of the charge density of a molecule on a time scale defined by the energy intervals between the electronic states involved. Here, we report the observation of charge migration in neutral…
Recently, a new distributed implementation of the full configuration interaction (FCI) method has been reported [Gao et al. J. Chem Theory Comput. 2024, 20, 1185]. Thanks to a hybrid parallelization scheme, the authors were able to compute…
We present the concept, derivation, and implementation of dynamical configuration interaction, a quantum embedding theory that combines Green's function methodology with the many-body wave function. In a strongly-correlated active space, we…
We present a new method to accelerate real time-time dependent density functional theory (rt-TDDFT) calculations with hybrid exchange-correlation functionals. For large basis set, the computational bottleneck for large scale calculations is…
Inspired by our earlier semi-stochastic work aimed at converging high-level coupled-cluster (CC) energetics [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017); J. Chem. Phys. 154, 124103 (2021)], we propose a novel…
The calculation of time-dependent charge and energy currents in nanoscale systems is a challenging task. Nevertheless it is crucial for gaining a deep understanding of the relevant processes at the nanoscale. We extend the auxiliary-mode…
This paper revisits the temporal difference (TD) learning algorithm for the policy evaluation tasks in reinforcement learning. Typically, the performance of TD(0) and TD($\lambda$) is very sensitive to the choice of stepsizes. Oftentimes,…
While providing a highly accurate framework for simulating laser-induced many-electron dynamics in atom and molecules, including linear and nonlinear steady-state and transient absorption spectra, time-dependent coupled-cluster theory does…
We present a plane-wave basis set implementation of charge constrained density functional molecular dynamics (CDFT-MD) for simulation of electron transfer reactions in condensed phase systems. Following earlier work of Wu et al. Phys. Rev.…
An iterative configuration interaction (iCI)-based multiconfigurational self-consistent field (SCF) theory, iCISCF, is proposed to handle systems that require large complete active spaces (CAS). The success of iCISCF stems from three…
Transition charge density (TCD) for $ 0^+\to 2_1^+ $ excitation have been calculated for $\rm ^{70,72,74,76}Ge$ nuclei within microscopic variational framework employing $2p_{3/2}, 1f_{5/2}, 2p_{1/2}$ and $1g_{9/2}$ valence space. The…
Attosecond interferometry (AI) is an experimental technique based on ionizing a system with an attosecond pulse train in the presence of an assisting laser. This assisting laser provides multiple pathways for the photoelectron wave packet…
In this work, we develop a mathematical framework for a Selected Configuration Interaction (SCI) algorithm within a bi-orthogonal basis for transcorrelated (TC) calculations. The bi-orthogonal basis used here serves as the equivalent of the…
To avoid the combinatorial computational cost of configuration interaction (CI), we have previously introduced the symmetric tensor decomposition CI (STD-CI) method, where we take advantage of the antisymmetric nature of the electronic wave…
Many records in environmental sciences exhibit asymmetric trajectories and there is a need for simple and tractable models which can reproduce such features. In this paper we explore an approach based on applying both a time change and a…
Selected configuration interaction (SCI) methods, when complemented with a second-order perturbative correction, provide near full configuration interaction (FCI) quality energies with only a small fraction of the Slater determinants of the…
Many robotic systems are underactuated, meaning not all degrees of freedom can be directly controlled due to lack of actuators, input constraints, or state-dependent actuation. This property, compounded by modeling uncertainties and…
We present two improvements to the tight-binding approximation of time-dependent density functional theory (TD-DFTB): Firstly, we add an exact Hartree-Fock exchange term, which is switched on at large distances, to the ground state…
Charged excitations are electronic transitions that involve a change in the total charge of a molecule or material. Understanding the properties and reactivity of charged species requires insights from theoretical calculations that can…