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We revisit the problem of unphysical charge density delocalization/fractionalization induced by the self-interaction error of common approximate Kohn-Sham Density Functional Theory functionals on simulation of small to medium-size proteins…

Chemical Physics · Physics 2024-07-30 Samuel A. Slattery , Jaden C. Yon , Edward F. Valeev

We introduce new and robust decompositions of mean-field Hartree-Fock (HF) and Kohn-Sham density functional theory (KS-DFT) relying on the use of localized molecular orbitals and physically sound charge population protocols. The new…

Chemical Physics · Physics 2020-12-04 Janus J. Eriksen

In the distributed nucleus approximation we represent the singular nucleus as smeared over a smallportion of a Cartesian grid. Delocalizing the nucleus allows us to solve the Poisson equation for theoverall electrostatic potential using a…

chem-ph · Physics 2009-10-28 Karthik A. Iyer , Michael P. Merrick , Thomas L. Beck

Surface parameterizations are widely applied in computer graphics, medical imaging and transformation optics. In this paper, we rigorously derive the gradient vector and Hessian matrix of the discrete conformal energy for spherical…

Numerical Analysis · Mathematics 2023-12-01 Zhong-Heng Tan , Tiexiang Li , Wen-Wei Lin , Shing-Tung Yau

We present a new linear scaling method for the energy minimization step of semiempirical and first-principles Hartree-Fock and Kohn-Sham calculations. It is based on the self-consistent calculation of the optimum localized orbitals of any…

Materials Science · Physics 2009-11-10 Luis Seijo , Zoila Barandiaran

The capability of discretization of matrix elements in the problem of quadratic functional minimization with linear member built on matrix in N-dimensional configuration space with discrete coordinates is researched. It is shown, that…

Neural and Evolutionary Computing · Computer Science 2012-05-04 Boris Kryzhanovsky , Mikhail Kryzhanovsky , Magomed Malsagov

Two of the most widely used electronic structure theory methods, namely Hartree-Fock and Kohn-Sham density functional theory, both requires the iterative solution of a set of Schr\"odinger-like equations. The speed of convergence of such…

Chemical Physics · Physics 2024-06-06 S. Hazra , U. Patil , S. Sanvito

To leverage the redundancy between the electronic structure computed at each step of first-principles molecular dynamics, we present a data-driven modeling framework for Kohn-Sham Density Functional Theory that bypasses the explicit…

Numerical Analysis · Mathematics 2026-02-27 Siu Wun Cheung , Youngsoo Choi , Jean-Luc Fattebert , Jonas Kaufman , Daniel Osei-Kuffuor

In this work we propose an efficient and accurate multi-scale optical simulation algorithm by applying a numerical version of slowly varying envelope approximation in FEM. Specifically, we employ the fast iterative method to quickly compute…

Optics · Physics 2024-12-03 Fan Xiao , Jingwei Wang , Zhongfei Xiong , Yuntian Chen

Locality of compact one-electron orbitals expanded strictly in terms of local subsets of basis functions can be exploited in density functional theory (DFT) to achieve linear growth of computation time with systems size, crucial in…

Computational Physics · Physics 2021-10-01 Yifei Shi , Jessica Karaguesian , Rustam Z. Khaliullin

The simulation of charge transport in ultra-scaled electronic devices requires the knowledge of the atomic configuration and the associated potential. Such "atomistic" device simulation is most commonly handled using a tight-binding…

Mesoscale and Nanoscale Physics · Physics 2019-10-02 Maarten L. Van de Put , Massimo V. Fischetti , William G. Vandenberghe

We introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density…

Chemical Physics · Physics 2020-05-27 Guido Falk von Rudorff , O. Anatole von Lilienfeld

The universal functional of Hohenberg-Kohn is given as a coupling-constant integral over the density as a functional of the potential. Conditions are derived under which potential-functional approximations are variational. Construction via…

Other Condensed Matter · Physics 2011-06-13 Attila Cangi , Donghyung Lee , Peter Elliott , Kieron Burke , E. K. U. Gross

The Hohenberg-Kohn theorem of the density functional theory is extended by modifying the Levy constrained-search formulation. The new theorem allows us to choose arbitrary physical quantities as the basic variables which determine the…

Condensed Matter · Physics 2009-11-10 M. Higuchi , K. Higuchi

In this work, we introduce an original self-consistent scheme based on the one-body reduced density matrix ($\gamma$) formalism. A significant feature of this methodology is the utilization of an optimal unitary transformation of the…

Strongly Correlated Electrons · Physics 2023-11-10 Quentin Marécat , Benjamin Lasorne , Emmanuel Fromager , Matthieu Saubanère

While quantum computers have shown significant promise for electronic structure calculations, their potential to accelerate density functional theory (DFT) calculations remains unclear. In this work, we present a qubit-efficient encoding…

We present a basis-set-free approach to the variational quantum eigensolver using an adaptive representation of the spatial part of molecular wavefunctions. Our approach directly determines system-specific representations of qubit…

Quantum Physics · Physics 2021-01-05 Jakob S. Kottmann , Philipp Schleich , Teresa Tamayo-Mendoza , Alán Aspuru-Guzik

A new method is presented for performing first-principles molecular-dynamics simulations of systems with variable occupancies. We adopt a matrix representation for the one-particle statistical operator Gamma, to introduce a ``projected''…

Materials Science · Physics 2009-10-30 Nicola Marzari , David Vanderbilt , M. C. Payne

The self consistent version of the density functional theory is presented, which allows to calculate the ground state and dynamic properties of finite multi-electron systems. An exact functional equation for the effective interaction, from…

Materials Science · Physics 2017-08-23 M. Ya. Amusia , A. Z. Msezane , V. R. Shaginyan

We suggest an efficient algorithm for the selection of sparse subsets of a set of influence for the numerical discretization of differential operators on irregular nodes with polynomial consistency of a given order with the help of the QR…

Numerical Analysis · Mathematics 2019-08-06 Oleg Davydov
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