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In this work, we present a computationally efficient methodology that utilizes a local real-space formulation of the projector augmented wave (PAW) method discretized with a finite-element (FE) basis to enable accurate and large-scale…

Computational Physics · Physics 2025-01-03 Kartick Ramakrishnan , Sambit Das , Phani Motamarri

Recent advances in X-ray free-electron laser diagnostics have enabled direct probing of the electronic structure under extreme pressures and temperatures, such as those encountered in stellar interiors and inertial confinement fusion…

Density Functional Resonance Theory (DFRT) is a complex-scaled version of ground-state Density Functional Theory (DFT) that allows one to calculate the resonance energies and lifetimes of metastable anions. In this formalism, the exact…

Quantum Physics · Physics 2011-11-09 Daniel L. Whitenack , Adam Wasserman

Despite of its huge successes in vast amount of applications, the Kohn-Sham scheme of density functional theory (DFT-Kohn-Sham) has not been able to get reliable ionization potentials (IP) for semiconductors, due to self-interaction error…

Materials Science · Physics 2016-04-07 Lin-Hui Ye

The reported new algorithm determines the exact exchange potential v_x in a iterative way using energy and orbital shifts (ES, OS) obtained - with finite-difference formulas - from the solutions (occupied orbitals and their energies) of the…

Atomic Physics · Physics 2015-05-20 M. Cinal , A. Holas

We present for the first time an efficient iterative method to directly solve the four-component Dirac-Kohn-Sham (DKS) density functional theory. Due to the existence of the negative energy continuum in the DKS operator, the existing…

Computational Physics · Physics 2013-05-03 Lin Lin , Sihong Shao , Weinan E

We derive and employ a local potential to represent the Fock exchange operator in electronic single-particle equations. This local Fock-exchange (LFX) potential is very similar to the exact exchange (EXX) potential in density functional…

Materials Science · Physics 2016-12-21 T. W. Hollins , S. J. Clark , K. Refson , N. I. Gidopoulos

Density functional theory (DFT) is a widespread and effective tool in electronic structure calculations for ground-state electron systems. Its success has prompted exploration into the use of DFT for non-collective excited states. The delta…

Chemical Physics · Physics 2025-08-12 Ethan Pollack , Rohan Maniar , John P. Perdew

The real-space density-functional perturbation theory (DFPT) for the computations of the response properties with respect to the atomic displacement and homogeneous electric field perturbation has been recently developed and implemented…

Computational Physics · Physics 2020-10-28 Honghui Shang , Wanzhen Liang , Yunquan Zhang , Jinlong Yang

We present a Gaussian-basis implementation of orbital-free density-functional theory (OF-DFT) in which the trust-region image method (TRIM) is used for optimization. This second-order optimization scheme has been constructed to provide…

Chemical Physics · Physics 2021-09-15 Matthew S. Ryley , Michael Withnall , Tom J. P. Irons , Trygve Helgaker , Andrew M. Teale

We use projector operators to correct the Kohn-Sham Hamiltonian of density functional theory (KS-DFT) so that the resulting mean-field scheme yields, in finite systems, virtual orbitals and energy gaps in better agreement with those…

Other Condensed Matter · Physics 2008-06-26 Hector Mera

Density functional theory (DFT) is routinely employed in material science and in quantum chemistry to simulate weakly correlated electronic systems. Recently, deep learning (DL) techniques have been adopted to develop promising functionals…

Strongly Correlated Electrons · Physics 2023-10-02 Emanuele Costa , Rosario Fazio , Sebastiano Pilati

We propose exchanging the energy functionals in ground-state DFT with physically equivalent exact force expressions as a new promising route towards approximations to the exchange-correlation potential and energy. In analogy to the usual…

The engineering of the optical response of materials is a paradigm that demands microscopic-level accuracy and reliable predictive theoretical tools. Here we compare and contrast the dispersive permittivity tensor, using both a low-energy…

Materials Science · Physics 2021-09-29 Mohammad Alidoust , Erlend E. Isachsen , Klaus Halterman , Jaakko Akola

The energy minimization involved in density functional calculations of electronic systems can be carried out using an exponential transformation that preserves the orthonormality of the orbitals. The energy of the system is then represented…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Elvar Ö. Jónsson , Tejs Vegge , Hannes Jónsson

Noncollinear (NC) magnetism and spin-orbit coupling (SOC) are indispensable for predictive ab initio materials simulations with pronounced relativistic effects and magnetic frustration, yet they significantly increase the cost of…

Frozen Density Embedding Theory (FDET) [Wesolowski {\it Phys. Rev. A} {\bf 77}, 012504 (2008)] provides the interpretation of the eigenvalue equations for an embedded $N'$-electron wavefunction, in which the embedding operator is…

Chemical Physics · Physics 2025-07-02 Tomasz Adam Wesolowski

Large biomolecular systems, whose function may involve thousands of atoms, cannot easily be addressed with parameter-free density functional theory (DFT) calculations. Until recently a central problem was that such systems possess an…

Materials Science · Physics 2026-01-29 Kristian Berland , Elisa Londero , Elsebeth Schroder , Per Hyldgaard

The single particle energies obtained in a Kohn--Sham density functional theory (DFT) calculation are generally known to be poor approximations to electron excitation energies that are measured in transport, tunneling and spectroscopic…

Numerical Analysis · Mathematics 2017-12-29 Meiyue Shao , Lin Lin , Chao Yang , Fang Liu , Felipe H. da Jornada , Jack Deslippe , Steven G. Louie

We present a substantial extension of our constraint-based approach for development of orbital-free (OF) kinetic-energy (KE) density functionals intended for the calculation of quantum-mechanical forces in multi-scale molecular dynamics…

Materials Science · Physics 2015-05-13 V. V. Karasiev , R. S. Jones , S. B. Trickey , Frank E. Harris