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While Born-Oppenheimer molecular dynamics (BOMD) has been widely studied by resorting to powerful methods in mathematical analysis, this paper presents a geometric formulation in terms of Hamilton's variational principle and…

Mathematical Physics · Physics 2023-07-20 Paul Bergold , Cesare Tronci

A general set of methods is presented for calculating chemical potentials in solid and liquid mixtures using {\em ab initio} techniques based on density functional theory (DFT). The methods are designed to give an {\em ab initio} approach…

Materials Science · Physics 2009-11-07 D. Alfe` , M. J. Gillan , G. D. Price

Experiments have demonstrated that vibrational strong coupling between molecular vibrations and light modes can significantly change molecular properties, such as ground-state reactivity. Theoretical studies towards the origin of this…

Chemical Physics · Physics 2024-01-09 Marit R. Fiechter , Jeremy O. Richardson

We present a numerical modeling workflow based on machine learning (ML) which reproduces the the total energies produced by Kohn-Sham density functional theory (DFT) at finite electronic temperature to within chemical accuracy at negligible…

Classical density functional theory (DFT) provides an exact variational framework for determining the equilibrium properties of inhomogeneous fluids. We report a generalization of DFT to treat the non-equilibrium dynamics of classical…

Soft Condensed Matter · Physics 2013-09-06 Matthias Schmidt , Joseph M. Brader

The Born-Oppenheimer (BO) approximation is less accurate in the presence of a strong magnetic field than in the absence of a field. This is due to the complicated and unpredictable response of electronic structure to the field, especially…

Chemical Physics · Physics 2023-03-29 Tanner Culpitt , Laurens D. M. Peters , Erik I. Tellgren , Trygve Helgaker

In this paper, we show how to calculate analytical atomic forces within self-consistent density functional theory + dynamical mean-field theory (DFT+DMFT) approach in the case when ultra-soft or norm-conserving pseudopotentials are used. We…

Strongly Correlated Electrons · Physics 2021-12-20 Evgeny Plekhanov , Nicola Bonini , Cedric Weber

Time-dependent density functional theory (TDDFT) is rapidly emerging as a premier method for solving dynamical many-body problems in physics and chemistry. The mathematical foundations of TDDFT are established through the formal existence…

Quantum Physics · Physics 2014-08-22 J. D. Whitfield , M. -H. Yung , D. G. Tempel , S. Boixo , A. Aspuru-Guzik

Graph-based linear scaling electronic structure theory for quantum-mechanical molecular dynamics simulations is adapted to the most recent shadow potential formulations of extended Lagrangian Born-Oppenheimer molecular dynamics, including…

Chemical Physics · Physics 2023-03-08 Christian F. A. Negre , Michael E. Wall , Anders M. N. Niklasson

This is a follow-up of our recently proposed work on pseudopotential calculation (Ref. [21]) of atoms and molecules within DFT framework, using cartesian coordinate grid. Detailed results are presented to demonstrate the usefulness,…

Chemical Physics · Physics 2015-05-18 Amlan K. Roy

Despite the variety of available computational approaches, state-of-the-art methods for calculating excitation energies such as time-dependent density functional theory (TDDFT), are computationally demanding and thus limited to moderate…

Chemical Physics · Physics 2022-03-10 Martina Stella , Kritam Thapa , Luigi Genovese , Laura E. Ratcliff

The construction of a better exchange-correlation potential in time-dependent density functional theory (TDDFT) can improve the accuracy of TDDFT calculations and provide more accurate predictions of the properties of many-electron systems.…

Quantum Physics · Physics 2023-08-23 Jun Yang , James D Whitfield

We develop a method in which the electronic densities of small fragments determined by Kohn-Sham density functional theory (DFT) are embedded using stochastic DFT to form the exact density of the full system. The new method preserves the…

Chemical Physics · Physics 2015-06-19 Daniel Neuhauser , Roi Baer , Eran Rabani

We have proposed a method for correcting the Kohn-Sham eigen energies in the density functional theory (DFT) based on the Koopmans theorem using Wannier functions. The method provides a general approach applicable for molecules and solids…

Computational Physics · Physics 2015-03-02 Jie Ma , Lin-Wang Wang

Stochastic and mixed stochastic-deterministic density functional theory (DFT) are promising new approaches for the calculation of the equation-of-state and transport properties in materials under extreme conditions. In the intermediate warm…

Computational Physics · Physics 2023-09-27 Vidushi Sharma , Lee A. Collins , Alexander J. White

Orbital-free density functional theory (OFDFT) is a quantum chemistry formulation that has a lower cost scaling than the prevailing Kohn-Sham DFT, which is increasingly desired for contemporary molecular research. However, its accuracy is…

Machine Learning · Statistics 2024-03-12 He Zhang , Siyuan Liu , Jiacheng You , Chang Liu , Shuxin Zheng , Ziheng Lu , Tong Wang , Nanning Zheng , Bin Shao

Extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) in its most recent shadow potential energy version has been implemented in the semiempirical PyTorch-based software PySeQM. The implementation includes finite electronic…

Nuclear Density Functional Theory (DFT) plays a prominent role in the understanding of nuclear structure, being the approach with the widest range of applications. Hohenberg and Kohn theorems warrant the existence of a nuclear Energy…

Nuclear Theory · Physics 2020-03-03 G. Accorto , P. Brandolini , F. Marino , A. Porro , A. Scalesi , G. Colò , X. Roca-Maza , E. Vigezzi

We introduce a shadow molecular dynamics (MD) approach based on the Atom-Condensed Kohn-Sham second-order (ACKS2) charge-potential equilibration model. In contrast to regular flexible charge models, the ACKS2 model includes both flexible…

Chemical Physics · Physics 2025-02-14 Robert Stanton , Cagri Mehmet Kaymak , Anders M. N. Niklasson

Density functional theory constitutes the workhorse of modern electronic structure calculations due to its favourable computational cost despite the fact that it usually fails to describe strongly correlated systems. A particularly…

Quantum Gases · Physics 2022-05-06 Julia Liebert