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We use density-matrix renormalization group, applied to a one-dimensional model of continuum Hamiltonians, to accurately solve chains of hydrogen atoms of various separations and numbers of atoms. We train and test a machine-learned…

Strongly Correlated Electrons · Physics 2016-12-28 Li Li , Thomas E. Baker , Steven R. White , Kieron Burke

Kohn-Sham Density Functional Theory (KS-DFT) provides the exact ground state energy and electron density of a molecule, contingent on the as-yet-unknown universal exchange-correlation (XC) functional. Recent research has demonstrated that…

Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…

We introduce a non-equilibrium density-functional theory of local temperature and associated local energy density that is suited for the study of thermoelectric phenomena. The theory rests on a local temperature field coupled to the…

Strongly Correlated Electrons · Physics 2014-05-16 F. G. Eich , M. Di Ventra , G. Vignale

As a proof of principle, self-consistent Kohn--Sham calculations are performed with the exact exchange-correlation functional. Finding the exact functional for even one trial density requires solving the interacting Schr\"odinger equation…

Chemical Physics · Physics 2014-07-14 Lucas O. Wagner , Thomas E. Baker , E. M. Stoudenmire , Kieron Burke , Steven R. White

The Kohn-Sham equations underlie many important applications such as the discovery of new catalysts. Recent machine learning work on catalyst modeling has focused on prediction of the energy, but has so far not yet demonstrated significant…

Machine Learning · Computer Science 2023-10-31 Phillip Pope , David Jacobs

We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Computational Physics · Physics 2020-01-08 Sebastian Dick , Marivi Fernandez-Serra

Over the past decade, machine learning has been successfully applied in various fields of science. In this study, we employ a deep learning method to analyze a Skyrme energy density functional (Skyrme-EDF), that is a Kohn-Sham type…

Nuclear Theory · Physics 2023-06-28 N. Hizawa , K. Hagino , K. Yoshida

We have developed and implemented a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation…

Plasma Physics · Physics 2015-06-22 Travis Sjostrom , Jerome Daligault

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

Numerical Analysis · Mathematics 2022-01-19 Xiaoying Dai , Stefano de Gironcoli , Bin Yang , Aihui Zhou

A sufficiently damped iteration of the Kohn-Sham equations with the exact functional is proven to always converge to the true ground-state density, regardless of the initial density or the strength of electron correlation, for finite…

Materials Science · Physics 2013-08-30 Lucas O. Wagner , E. M. Stoudenmire , Kieron Burke , Steven R. White

We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…

Mesoscale and Nanoscale Physics · Physics 2021-01-15 M. J. P. Hodgson , J. D. Ramsden , T. R. Durrant , R. W. Godby

Kohn-Sham density functional theory (KS-DFT) is a powerful method to obtain key materials' properties, but the iterative solution of the KS equations is a numerically intensive task, which limits its application to complex systems. To…

Materials Science · Physics 2023-05-29 Bruno Focassio , Michelangelo Domina , Urvesh Patil , Adalberto Fazzio , Stefano Sanvito

The recently developed Deep Potential [Phys. Rev. Lett. 120, 143001, 2018] is a powerful method to represent general inter-atomic potentials using deep neural networks. The success of Deep Potential rests on the proper treatment of locality…

Computational Physics · Physics 2019-12-05 Leonardo Zepeda-Núñez , Yixiao Chen , Jiefu Zhang , Weile Jia , Linfeng Zhang , Lin Lin

Orbital-free density functional theory (OF-DFT) holds the promise to compute ground state molecular properties at minimal cost. However, it has been held back by our inability to compute the kinetic energy as a functional of the electron…

Chemical Physics · Physics 2023-10-25 Roman Remme , Tobias Kaczun , Maximilian Scheurer , Andreas Dreuw , Fred A. Hamprecht

A density functional theory (DFT) framework is presented that links functional derivatives of free-energy functionals to non-linear static density response functions in quantum many-body systems. Within this framework, explicit expressions…

Ground-state Kohn-Sham density functional theory provides, in principle, the exact ground-state energy and electronic spin-densities of real interacting electrons in a static external potential. In practice, the exact density functional for…

Chemical Physics · Physics 2022-07-11 Aaron D. Kaplan , Mel Levy , John P. Perdew

A Kohn-Sham (KS) inversion determines a KS potential and orbitals corresponding to a given electron density, a procedure that has applications in developing and evaluating functionals used in density functional theory. Despite the utility…

Computational Physics · Physics 2021-04-07 Seungsoo Nam , Ryan J. McCarty , Hansol Park , Eunji Sim

According to density functional theory, any chemical property can be inferred from the electron density, making it the most informative attribute of an atomic structure. In this work, we demonstrate the use of established physical methods…

Materials Science · Physics 2023-09-12 Ethan M. Sunshine , Muhammed Shuaibi , Zachary W. Ulissi , John R. Kitchin

Time-dependent (current) density functional theory for many-electron systems strongly coupled to quantized electromagnetic modes of a microcavity is proposed. It is shown that the electron-photon wave function is a unique functional of the…

Mesoscale and Nanoscale Physics · Physics 2013-12-10 I. V. Tokatly