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Complete active space self-consistent field (CASSCF) computations can be realized at polynomial cost via the variational optimization of the active-space two-electron reduced-density matrix (2-RDM). Like conventional approaches to CASSCF,…

Chemical Physics · Physics 2018-12-10 Mohammad Mostafanejad , A. Eugene DePrince

We present the theory and implementation of a fully variational wave function -- density functional theory (DFT) hybrid model, which is applicable to many cases of strong correlation. We denote this model the multiconfigurational…

Due to their small size and unique properties, single-molecule electronics have long seen research interest from experimentalists and theoreticians alike. From a theoretical standpoint, modeling these systems using electronic structure…

Chemical Physics · Physics 2021-10-04 Andrew M. Sand , Justin T. Malme , Erik P. Hoy

We propose a multiconfigurational hybrid density-functional theory which rigorously combines a multiconfiguration self-consistent-field calculation with a density-functional approximation based on a linear decomposition of the…

Chemical Physics · Physics 2012-08-20 Kamal Sharkas , Andreas Savin , Hans Jørgen Aa. Jensen , Julien Toulouse

Multiconfiguration pair-density functional theory (MC-PFDT) has previously been applied successfully to carry out ground-state and excited-state calculations. However, because it includes no interaction between electronic states, MC-PDFT…

Multiconfiguration pair-density functional theory (MC-PDFT) is a post-MCSCF multireference electronic-structure method that explicitly models strong electron correlation, and linearized pair-density functional theory (L-PDFT) is a recently…

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

Nonadiabatic molecular dynamics is an effective method for modeling nonradiative decay in electronically excited molecules. Its accuracy depends strongly on the quality of the potential energy surfaces, and its affordability for long…

Chemical Physics · Physics 2024-10-11 Matthew R. Hennefarth , Donald G. Truhlar , Laura Gagliardi

A combined density and first-order reduced-density-matrix (1RDM) functional method is proposed for the calculation of potential energy curves (PECs) of molecular multibond dissociation. Its 1RDM functional part, a pair density functional,…

Chemical Physics · Physics 2020-09-23 Robert van Meer , Oleg Gritsenko , Jeng-Da Chai

Multi-configuration range-separated density-functional theory is extended to the time-dependent regime. An exact variational formulation is derived. The approximation, which consists in combining a long-range…

Chemical Physics · Physics 2013-02-27 Emmanuel Fromager , Stefan Knecht , Hans Jørgen Aa. Jensen

Multi-center transition metal complexes (MCTMs) with magnetically interacting ions have been proposed as components for information processing devices and storage units. For any practical application of MCTMs as magnetic units, it is…

Chemical Physics · Physics 2023-04-03 Henry C. Fitzhugh , James W. Furness , Mark R. Pederson , Juan E. Peralta , Jianwei Sun

The interaction between excited states of a closed-shell chromophore and a nearby free radical species gives rise to spin-coupled doublet states, namely singdoublet and tripdoublet, as well as a quartet state. This coupling facilitates…

Chemical Physics · Physics 2025-03-25 Chenyu Liu , Yang Xu , Peng Bao , Yangyi Lu , Jiali Gao

A range-separated double-hybrid (RSDH) scheme which generalizes the usual range-separated hybrids and double hybrids is developed. This scheme consistently uses a two-parameter Coulomb-attenuating-method (CAM)-like decomposition of the…

Chemical Physics · Physics 2018-05-23 Cairedine Kalai , Julien Toulouse

Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…

Chemical Physics · Physics 2020-04-16 Christopher J. Stein , Markus Reiher

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

The Ziegler-Rauk-Baerends multiplet sum method (MSM) assumes that density-functional theory (DFT) provides a good description of states dominated by a single determinant. It then uses symmetry to add static correlation to DFT. In our…

Chemical Physics · Physics 2025-04-15 Mark E. Casida , Abraham Ponra , Carolyne Bakasa , Anne Justine Etindele

We introduce a novel density-based multilevel approach in density functional theory. In this multilevel density functional theory (MLDFT), the system is partitioned in an active and an inactive fragment, and all interactions are retained…

Linear-response quantum electrodynamical density functional theory (QEDFT) enables the description of molecular spectra under strong coupling to quantized photonic modes, such as those in optical cavities. Recently, this approach was…

Chemical Physics · Physics 2025-07-11 Lukas Konecny , Valeriia P. Kosheleva , Michael Ruggenthaler , Michal Repisky , Angel Rubio

New density functional theory approach based on a complete active space self-consistent field (CASSCF) reference function in Extended Koopmans' approximation is discussed. Recently, the number of generalizations of density functional theory…

Chemical Physics · Physics 2018-02-15 Sergey Gusarov , Yurii Dmitriev

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…

Chemical Physics · Physics 2017-04-27 Gunter Hermann , Vincent Pohl , Jean Christophe Tremblay
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