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In this paper, we study finite dimensional approximations of Kohn-Sham models, which are widely used in electronic structure calculations. We prove the convergence of the finite dimensional approximations and derive the a priori error…

Numerical Analysis · Mathematics 2011-08-10 Huajie Chen , Xingao Gong , Lianhua He , Zhang Yang , Aihui Zhou

We review our recently developed electronic structure calculation methods used for the dynamics of large-scale solids or liquids with an efficient algorithm for large scale simultaneous linear equations. The electronic structure calculation…

Materials Science · Physics 2011-02-02 T. Fujiwara , S. Yamamoto , T. Hoshi , S. Nishino , H. Teng , T. Sogabe , S. -L. Zhang , M. Ikeda , M. Nakashima , N. Watanabe

The paper develops a hybrid method for solving a system of advection--diffusion equations in a bulk domain coupled to advection--diffusion equations on an embedded surface. A monotone nonlinear finite volume method for equations posed in…

Computational Physics · Physics 2018-06-05 Alexey Y. Chernyshenko , Maxim A. Olshanskii , Yuri V. Vassilevski

Quantum embedding theories are playing an increasingly important role in bridging different levels of approximation to the many body Schr\"odinger equation in physics, chemistry and materials science. In this paper, we present a linear…

Computational Physics · Physics 2019-04-10 Lin Lin , Leonardo Zepeda-Núñez

Given a partition of a large system into an active quantum mechanical (QM) region and its environment, we present a simple way of embedding the QM region into an effective electrostatic potential representing the environment. This potential…

Chemical Physics · Physics 2017-07-20 Stephan Mohr , Michel Masella , Laura E. Ratcliff , Luigi Genovese

We review thermodynamic limits and scaling limits of electronic structure models for condensed matter. We discuss several mathematical ways to implement these limits in three models of increasing chemical complexity and mathematical…

Mathematical Physics · Physics 2023-09-12 David Gontier , Jianfeng Lu , Christoph Ortner

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

Quantum computers hold promise to enable efficient simulations of the properties of molecules and materials; however, at present they only permit ab initio calculations of a few atoms, due to a limited number of qubits. In order to harness…

Materials Science · Physics 2020-07-07 He Ma , Marco Govoni , Giulia Galli

Density functional theory is currently the most widely applied method in electronic structure theory. The Kohn-Sham method, based on a fictitious system of non-interacting particles, is the work horse of the theory. The particular form of…

Chemical Physics · Physics 2016-06-01 Hubertus J J van Dam

The Kohn-Sham method uses a single model system, and corrects it by a density functional the exact user friendly expression of which is not known and is replaced by an approximated, usable, model. We propose to use instead more than one…

Chemical Physics · Physics 2021-12-28 Étienne Polack , Yvon Maday , Andreas Savin

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

By introducing a set of auxiliary equations representing a many-body system, we have derived an extension of the Kohn-Sham scheme for the density functional theory. These equations consist of a Kohn-Sham-type equation determining…

Materials Science · Physics 2009-11-07 Koichi Kusakabe

Frozen Density Embedding (FDE) represents a versatile embedding scheme to describe the environmental effect on the electron dynamics in molecular systems. The extension of the general theory of FDE to the real-time time-dependent Kohn-Sham…

We integrate the all-electron electronic structure code FHI-aims into the general ChemShell package for solid-state embedding (QM/MM) calculations. A major undertaking in this integration is the implementation of pseudopotential…

We present a quantum electronic embedding method derived from the exact factorization approach to calculate static properties of a many-electron system. The method is exact in principle but the practical power lies in utilizing input from a…

Strongly Correlated Electrons · Physics 2020-05-27 Lionel Lacombe , Neepa T. Maitra

We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of freedom. We demonstrate its potential by…

Chemical Physics · Physics 2024-12-23 Stefano Battaglia , Max Rossmannek , Vladimir V. Rybkin , Ivano Tavernelli , Jürg Hutter

We present a new theory for partitioning simulations of periodic and solid-state systems into physically sound atomic contributions at the level of Kohn-Sham density functional theory. Our theory is based on spatially localized linear…

Chemical Physics · Physics 2024-10-01 Luna Zamok , Janus J. Eriksen

In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…

Hybrid quantum mechanics / molecular mechanics (QM/MM) models successfully describe the properties of biological macromolecules. However, most QM/MM methodologies are constrained to unrealistic gas phase models, thus limiting their…

Chemical Physics · Physics 2022-11-08 Simone Bonfrate , Nicolas Ferré , Miquel , Huix-Rotllant

A myriad of phenomena in materials science and chemistry rely on quantum-level simulations of the electronic structure in matter. While moving to larger length and time scales has been a pressing issue for decades, such large-scale…