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We present a method to make highly accurate pseudopotentials for use with orbital-free density functional theory (OF-DFT) with given exchange-correlation and kinetic energy functionals, which avoids the compounding of errors of Kohn-Sham…

Materials Science · Physics 2015-02-04 Fleur Legrain , Sergei Manzhos

Performing high accuracy hybrid functional calculations for condensed matter systems containing a large number of atoms is at present computationally very demanding - when not out of reach - if high quality basis sets are used. We present a…

Materials Science · Physics 2017-12-22 Laura E. Ratcliff , A. Degomme , José A. Flores-Livas , Stefan Goedecker , Luigi Genovese

We present an orbital-resolved extension of the Hubbard $U$ correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly…

Materials Science · Physics 2024-09-18 Eric Macke , Iurii Timrov , Nicola Marzari , Lucio Colombi Ciacchi

Stochastic density functional theory (sDFT) is becoming a valuable tool for studying ground state properties of extended materials. The computational complexity of describing the Kohn-Sham orbitals is replaced by introducing a set of random…

Chemical Physics · Physics 2021-06-16 Ming Chen , Roi Baer , Daniel Neuhauser , Eran Rabani

The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

Chemical Physics · Physics 2017-03-16 Alain C. Vaucher , Markus Reiher

A new method for implementing the kinetic energy operator for real-space, grid-based electronic structure codes is developed. It is based on multi-order Adaptive Finite Differencing (AFD) and uses atomic pseudo orbitals produced by the…

Computational Physics · Physics 2023-05-23 E. L. Briggs , Wenchang Lu , J. Bernholc

We propose a local real-space formulation for orbital-free DFT with density dependent kinetic energy functionals and a unified variational framework for computing the configurational forces associated with geometry optimization of both…

Materials Science · Physics 2015-06-15 Sambit Das , Mrinal Iyer , Vikram Gavini

A previously proposed computational procedure for constructing a set of nonorthogonal strongly localised one-electron molecular orbitals (O. Danyliv, L. Kantorovich - physics/0401107) is applied to a perfect $\alpha$-quartz crystal…

Chemical Physics · Physics 2009-11-10 Oleh Danyliv , Lev Kantorovich

We investigate configuration-interaction (CI) calculations on a basis of molecular orbitals generated by preliminary density-functional theory (DFT) calculations. We use this CI/DFT framework to improve the modeling of core-excited states…

Chemical Physics · Physics 2025-09-11 Giorgio Visentin , Francois Mauger

The natural orbital functional theory (NOFT) has emerged as an alternative formalism to both density functional (DF) and wavefunction methods. In NOFT, the electronic structure is described in terms of the natural orbitals (NOs) and their…

Computational Physics · Physics 2020-10-28 Mario Piris , Ion Mitxelena

Quantum computers open up new avenues for modelling the physical properties of materials and molecules. Density Functional Theory (DFT) is the gold standard classical algorithm for predicting these properties, but relies on approximations…

Quantum Physics · Physics 2024-02-29 Evan Sheridan , Lana Mineh , Raul A. Santos , Toby Cubitt

We present a machine learning algorithm for the prediction of molecule properties inspired by ideas from density functional theory. Using Gaussian-type orbital functions, we create surrogate electronic densities of the molecule from which…

Chemical Physics · Physics 2019-11-27 Michael Eickenberg , Georgios Exarchakis , Matthew Hirn , Stéphane Mallat , Louis Thiry

We give a fairly comprehensive review of wavelets and of their application to density-functional theory (DFT) and to our recent application of a wavelet-based version of linear-response time-dependent DFT (LR-TD-DFT). Our intended audience…

Other Condensed Matter · Physics 2011-10-24 Bhaarathi Natarajan , Mark E. Casida , Luigi Genovese , Thierry Deutsch

Density functional theory offers accurate structure prediction at acceptable computational cost, but commonly used approximations suffer from delocalization error; this results in inaccurate predictions of quantities such as energy band…

Materials Science · Physics 2022-08-17 Aaron Mahler , Jacob Z. Williams , Neil Qiang Su , Weitao Yang

We present efficient implementations of the multilevel CC2 (MLCC2) and multilevel CCSD (MLCCSD) models. As the system size increases, MLCC2 and MLCCSD exhibit the scaling of the lower level coupled cluster model. In order to treat large…

Chemical Physics · Physics 2020-11-25 Sarai D. Folkestad , Eirik F. Kjønstad , Linda Goletto , Henrik Koch

Quantum computers will need effective error-correcting codes. Current quantum processors require precise control of each particle, so having fewer particles to control might be beneficial. Although traditionally quantum computers are…

Quantum Physics · Physics 2021-10-25 Arun J. Moorthy , Lane G. Gunderman

Quantum chemistry calculations of large, strongly correlated systems are typically limited by the computation cost that scales exponentially with the size of the system. Quantum algorithms, designed specifically for quantum computers, can…

We propose a state-specific orbital optimization scheme for improving the accuracy of excited states of the electronic structure Hamiltonian for the use on near-term quantum computers, which can be combined with any overlap-based…

Quantum Physics · Physics 2025-10-16 Guorui Zhu , Joel Bierman , Jianfeng Lu , Yingzhou Li

Hybrid functionals often improve considerably the accuracy of density-functional calculations, in particular of quantities resulting from the band structure. In plane-wave (PW) calculations this benefit comes at the cost of an increase in…

Materials Science · Physics 2019-02-04 J. D. Gouveia , J. Coutinho

A real-space formalism for density-functional perturbation theory (DFPT) is derived and applied for the computation of harmonic vibrational properties in molecules and solids. The practical implementation using numeric atom-centered…

Materials Science · Physics 2017-03-08 Honghui Shang , Christian Carbogno , Patrick Rinke , Matthias Scheffler