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We introduce a local machine-learning method for predicting the electron densities of periodic systems. The framework is based on a numerical, atom-centred auxiliary basis, which enables an accurate expansion of the all-electron density in…

Chemical Physics · Physics 2021-11-10 Alan M. Lewis , Andrea Grisafi , Michele Ceriotti , Mariana Rossi

We present an extension of reverse engineered Kohn-Sham potentials from a density matrix renormalization group calculation towards the construction of a density functional theory functional via deep learning. Instead of applying machine…

Disordered Systems and Neural Networks · Physics 2021-05-05 Peter Schmitteckert

We study the accuracy of Kohn-Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with…

Computational Physics · Physics 2024-11-21 Phanish Suryanarayana , Arpit Bhardwaj , Xin Jing , Shashikant Kumar , John E. Pask

The Hubbard model provides a test bed to investigate the complex behaviour arising from electron-electron interaction in strongly-correlated systems and naturally emerges as the foundation model for lattice density functional theory (DFT).…

Strongly Correlated Electrons · Physics 2025-01-29 Eoghan Cronin , Rajarshi Tiwari , Stefano Sanvito

Chemical accuracy serves as an important metric for assessing the effectiveness of the numerical method in Kohn--Sham density functional theory. It is found that to achieve chemical accuracy, not only the Kohn--Sham wavefunctions but also…

Computational Physics · Physics 2023-10-25 Yang Kuang , Yedan Shen , Guanghui Hu

A complete solution to the inverse problem of Kohn-Sham (KS) density functional theory is proposed. Our method consists of two steps. First, the effective KS potential is determined from the ground state density of a given system. Then, the…

Nuclear Theory · Physics 2022-03-14 A. Liardi , F. Marino , G. Colò , X. Roca-Maza , E. Vigezzi

A long-standing goal of science is to accurately solve the Schr\"odinger equation for large molecular systems. The poor scaling of current quantum chemistry algorithms on classical computers imposes an effective limit of about a few dozen…

Chemical Physics · Physics 2022-02-11 Joshua A. Rackers , Lucas Tecot , Mario Geiger , Tess E. Smidt

We use voxel deep neural networks to predict energy densities and functional derivatives of electron kinetic energies for the Thomas-Fermi model and Kohn-Sham density functional theory calculations. We show that the ground-state electron…

Mesoscale and Nanoscale Physics · Physics 2022-01-24 Kevin Ryczko , Sebastian J. Wetzel , Roger G. Melko , Isaac Tamblyn

Density-functional theory is a formally exact description of a many-body quantum system in terms of its density; in practice, however, approximations to the universal density functional are required. In this work, a model based on deep…

Computational Physics · Physics 2016-08-02 Jeffrey M. McMahon

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

The rectangular collocation approach makes it possible to solve the Schr\"odinger equation with basis functions that do not have amplitude in all regions in which wavefunctions have significant amplitude. Collocation points can be…

Computational Physics · Physics 2020-07-01 Jonas Ku , Aditya Kamath , Tucker Carrington , Sergei Manzhos

With the development of low order scaling methods for performing Kohn-Sham Density Functional Theory, it is now possible to perform fully quantum mechanical calculations of systems containing tens of thousands of atoms. However, with an…

Chemical Physics · Physics 2020-04-03 William Dawson , Stephan Mohr , Laura E. Ratcliff , Takahito Nakajima , Luigi Genovese

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

The Kohn-Sham equation is a powerful, widely used approach for computation of ground state electronic energies and densities in chemistry, materials science, biology, and nanosciences. In this paper, we study the adaptive finite element…

Numerical Analysis · Mathematics 2013-11-22 Huajie Chen , Xiaoying Dai , Xingao Gong , Lianhua He , Aihui Zhou

A generalization of the Kohn--Sham approach is derived where the correlation-energy functional depends on the one-particle density matrix of noninteracting states and on the external potential from the interacting target-state. The…

Chemical Physics · Physics 2007-05-23 James P. Finley

Electronic structure theory calculations offer an understanding of matter at the quantum level, complementing experimental studies in materials science and chemistry. One of the most widely used methods, density functional theory (DFT),…

Computational Physics · Physics 2024-04-11 Vincent Martinetto , Karan Shah , Attila Cangi , Aurora Pribram-Jones

We present a rigorous formulation of generalized Kohn-Sham density-functional theory. This provides a straightforward Kohn-Sham description of many-body systems based not only on particle-density but also on any other observable. We…

Strongly Correlated Electrons · Physics 2008-02-03 M. Valiev , G. W. Fernando

Drawing inspiration from the domain of image super-resolution, we view the electron density as a 3D grayscale image and use a convolutional residual network to transform a crude and trivially generated guess of the molecular density into an…

Chemical Physics · Physics 2025-07-30 Chenghan Li , Or Sharir , Shunyue Yuan , Garnet K. Chan

Predictivity of the Kohn-Sham approach to dynamical problems, when regarded as an initial value problem in a time-dependent density functional framework, is analysed for a class of models for which the argument devised in the work of Maitra…

Other Condensed Matter · Physics 2015-06-16 Walter Tarantino

With the growth of computational resources, the scope of electronic structure simulations has increased greatly. Artificial intelligence and robust data analysis hold the promise to accelerate large-scale simulations and their analysis to…

Materials Science · Physics 2023-07-27 Lenz Fiedler , Karan Shah , Michael Bussmann , Attila Cangi