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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…

Chemical Physics · Physics 2023-02-08 Souloke Sen , Bruno Senjean , Lucas Visscher

Accurate prediction of electron transport coefficients is crucial for understanding warm dense matter. Utilizing the density functional theory (DFT) with the Kubo-Greenwood formula is widely used to evaluate the electrical and thermal…

Materials Science · Physics 2024-02-27 Qianrui Liu , Mohan Chen

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

Orbital-free density functional theory (OF-DFT) for real-space systems has historically depended on Lagrange optimization techniques, primarily due to the inability of previously proposed electron density approaches to ensure the…

Chemical Physics · Physics 2024-11-08 Alexandre de Camargo , Ricky T. Q. Chen , Rodrigo A. Vargas-Hernández

This work presents a new class of hybrid density functional theory (DFT) approximations, incorporating nonlocal exact exchange in predefined states such as core atomic orbitals (AOs). These projected hybrid density functionals are a…

Chemical Physics · Physics 2023-05-16 Benjamin G. Janesko

While density functional theory (DFT) is widely applied for its combination of cost and accuracy, corrections (e.g., DFT+U) that improve it are often needed to tackle correlated transition-metal chemistry. In principle, the functional form…

Chemical Physics · Physics 2021-03-12 Akash Bajaj , Heather J. Kulik

We propose a local real-space formulation for orbital-free DFT with density dependent kinetic energy functionals and a unified variational framework for computing the configurational forces associated with geometry optimization of both…

Materials Science · Physics 2015-06-15 Sambit Das , Mrinal Iyer , Vikram Gavini

We introduce an efficient finite-element approach for large-scale real-space pseudopotential density functional theory (DFT) calculations incorporating noncollinear magnetism and spin-orbit coupling. The approach, implemented within the…

Materials Science · Physics 2025-06-11 Nikhil Kodali , Phani Motamarri

A recently proposed "DFT+dispersion" treatment (Rajchel et al., Phys. Rev. Lett., 2010, 104, 163001) is described in detail and illustrated by more examples. The formalism derives the dispersion-free density functional theory (DFT)…

Recently, an approximate theoretical framework was introduced, called local reduced density matrix functional theory (local-RDMFT), where functionals of the one-body reduced density matrix (1-RDM) are minimized under the additional…

Over many years, computational simulations based on Density Functional Theory (DFT) have been used extensively to study many different materials at the atomic scale. However, its application is restricted by system size, leaving a number of…

Mesoscale and Nanoscale Physics · Physics 2018-12-05 Carlos Romero-Muñiz , Ayako Nakata , Pablo Pou , David R. Bowler , Tsuyoshi Miyazaki , Rubén Pérez

Despite a large number of nonlocal kinetic energy density functionals (KEDFs) available for large-scale calculations, most of those nonlocal KEDFs designed for the extended systems cannot be directly applied to isolated systems. In this…

Materials Science · Physics 2020-05-29 Qiang Xu , Jian Lv , Yanchao Wang , Yanming Ma

We introduce natural atomic orbitals as the local projector to define the correlated subspace for DFT + DMFT (density functional theory plus dynamical mean-field theory) calculation. The natural atomic orbitals are found to be stably…

Strongly Correlated Electrons · Physics 2020-01-01 Jae-Hoon Sim , Myung Joon Han

Density Functional Theory (DFT) has become a cornerstone in the modeling of metals. However, accurately simulating metals, particularly under extreme conditions, presents two significant challenges. First, simulating complex metallic…

Chemical Physics · Physics 2024-03-08 Jake P. Vu , Ming Chen

Density functional theory (DFT) is an exact alternative formulation of quantum mechanics, in which it is possible to calculate the total energy, the spin and the charge density of many-electron systems in the ground state. In practice, it…

Atomic Physics · Physics 2014-03-25 Uri Argaman , Guy Makov , Eli Kraisler

Electrons in zero external magnetic field can be studied with density functional theory (DFT) or with spin-DFT (SDFT). The latter is normally used for open shell systems because its approximations appear to model better the exchange and…

Chemical Physics · Physics 2022-04-06 Timothy Callow , Benjamin Pearce , Nikitas Gidopoulos

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

By invoking a divide-and-conquer strategy, subsystem DFT dramatically reduces the computational cost of large-scale, \textit{ab-initio} electronic structure simulations of molecules and materials. The central ingredient setting subsystem…

Materials Science · Physics 2020-08-24 Wenhui Mi , Michele Pavanello

We present an Augmented Lagrangian formulation and its real-space implementation for non-periodic orbital-free Density Functional Theory (OF-DFT) calculations. In particular, we rewrite the constrained minimization problem of OF-DFT as a…

Computational Physics · Physics 2015-06-19 Phanish Suryanarayana , Deepa Phanish

By partitioning the electron density into subsystem contributions, the Frozen Density Embedding (FDE) formulation of subsystem DFT has recently emerged as a powerful tool for reducing the computational scaling of Kohn--Sham DFT. To date,…

Materials Science · Physics 2015-06-22 Alessandro Genova , Davide Ceresoli , Michele Pavanello
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