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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…

Chemical Physics · Physics 2026-03-06 Takashi Tsuchimochi

Functionals that explicitly depend on occupied, unoccupied, or fractionally-occupied orbitals are rigorously formalized using Clifford algebras, and a variational principle is established that facilitates orbital (and occupation)…

Quantum Physics · Physics 2024-04-26 Neil Qiang Su

A time-dependent equation of motion coupled cluster singles and doubles (TD-EOM-CCSD) method is implemented, which uses a reduced basis calculated with the asymmetric band Lanczos algorithm. The approach is used to study weak-field…

The dissipative dynamics of many-electron systems interacting with a thermal environment has remained a long-standing challenge within time-dependent density functional theory (TDDFT). Recently, the formal foundations of open quantum…

Other Condensed Matter · Physics 2015-05-20 David G. Tempel , Alán Aspuru-Guzik

By using stochastic ensembles of walkers in physical and in one-body Hilbert spaces the recently proposed time-dependent quantum Monte Carlo (TDQMC) method offers the unique capability to calculate one-body density matrices at fully…

Quantum Physics · Physics 2025-02-07 Ivan P. Christov

Density matrix embedding theory (DMET) is a fully quantum-mechanical embedding method which shows great promise as a method of defeating the inherent exponential cost scaling of multiconfigurational wave function-based calculations by…

Chemical Physics · Physics 2019-02-07 Matthew R. Hermes , Laura Gagliardi

Thermospheric mass density is a major driver of satellite drag, the largest source of uncertainty in accurately predicting the orbit of satellites in low Earth orbit (LEO) pertinent to space situational awareness. Most existing models for…

Space Physics · Physics 2018-08-01 Piyush M. Mehta , Richard Linares , Eric K. Sutton

The computation of the nuclear quantum dynamics of molecules is challenging, requiring both accuracy and efficiency to be applicable to systems of interest. Recently, theories have been developed for employing time-dependent basis functions…

Kinetic transport equations are notoriously difficult to simulate because of their complex multiscale behaviors and the need to numerically resolve a high dimensional probability density function. Past literature has focused on building…

Numerical Analysis · Mathematics 2022-11-10 Zhichao Peng , Yanlai Chen , Yingda Cheng , Fengyan Li

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…

Computational Physics · Physics 2016-11-09 R. J. Magyar

The $4d \to 3p$ x-ray transitions in Cu- and Ni-like tungsten ions have been studied theoretically. The multiconfiguration Dirac-Hartree-Fock (MCDHF) method and the large-scale relativistic configuration-interaction (CI) method have been…

Atomic Physics · Physics 2024-05-16 Karol Kozioł , Jacek Rzadkiewicz

The route to reliable quantum nanoelectronic devices hinges on precise control of the electrostatic environment. For this reason, accurate methods for electrostatic simulations are essential in the design process. The most widespread…

Mesoscale and Nanoscale Physics · Physics 2023-02-28 Waldemar Svejstrup , Andrea Maiani , Kevin Van Hoogdalem , Karsten Flensberg

This paper presents the first application of the direct parametrisation method for invariant manifolds to a fully coupled multiphysics problem involving the nonlinear vibrations of deformable structures subjected to an electrostatic field.…

Numerical Analysis · Mathematics 2023-12-25 Attilio Frangi , Alessio Colombo , Alessandra Vizzaccaro , Cyril Touzé

Fragmentation methods applied to multireference wave functions constitute a road towards the application of highly accurate ab initio wave function calculations to large molecules and solids. However, it is important for reproducibility and…

Chemical Physics · Physics 2020-07-23 Matthew R. Hermes , Laura Gagliardi

The accurate resolution of the chemical properties of strongly correlated systems, such as biradicals, requires the use of electronic structure theories that account for both multi-reference as well as dynamic correlation effects. A variety…

Chemical Physics · Physics 2023-01-03 Jan-Niklas Boyn , David A. Mazziotti

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…

Computational Physics · Physics 2021-12-22 Daniel S. Levine , Diptarka Hait , Norm M. Tubman , Susi Lehtola , K. Birgitta Whaley , Martin Head-Gordon

As a universal quantum mechanical approach to the dynamical many-body problem, the time-dependent density functional theory (TDDFT) might be inadequate to describe crucial observables that rely on two-body evolution behavior, like the…

Computational Physics · Physics 2025-11-17 Jiong-Hang Liang , Yunfeng Xiong

We have verified a mechanism for Raman excitation of atoms through continuum levels previously obtained by quantum optimal control using the multi-configurational time-dependent Hartree-Fock (MCTDHF) method. For the optimal control, which…

Atomic Physics · Physics 2017-07-19 Loren Greenman , K. Birgitta Whaley , Daniel J. Haxton , C. William McCurdy

In dynamical mean-field theory, the correlations between electrons are assumed to be purely local. The dual fermion approach provides a systematic way of adding non-local corrections to the dynamical mean-field theory starting point.…

Strongly Correlated Electrons · Physics 2021-01-27 Erik G. C. P. van Loon

We present the first calculations of the inelastic part of the dynamical structure factor (DSF) for warm dense matter (WDM) using Time-Dependent Orbital-Free Density Functional Theory (TD-OF-DFT) and Mixed-Stochastic-Deterministic (mixed)…

Plasma Physics · Physics 2024-11-05 Alexander J. White