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We present a systematic study of the performance of numerical pseudo-atomic orbital basis sets in the calculation of dielectric matrices of extended systems using the self-consistent Sternheimer approach of [F. Giustino et al., Phys. Rev. B…

Materials Science · Physics 2015-06-04 Hannes Hübener , Miguel A. Pérez-Osorio , Pablo Ordejón , Feliciano Giustino

Density functional calculations on atoms are often used for determining accurate initial guesses as well as generating various types of pseudopotential approximations and efficient atomic-orbital basis sets for polyatomic calculations. To…

Computational Physics · Physics 2023-10-30 Susi Lehtola

Electronic structure calculation of atoms and molecules, in the past few decades has largely been dominated by density functional methods. This is primarily due to the fact that this can account for electron correlation effects in a…

Chemical Physics · Physics 2013-07-12 Amlan K. Roy

Standard flavors of density-functional theory (DFT) calculations are known to fail in describing anions, due to large self-interaction errors. The problem may be circumvented by using localized basis sets of reduced size, leaving no…

Chemical Physics · Physics 2019-12-23 Francesco Nattino , Céline Dupont , Nicola Marzari , Oliviero Andreussi

This chapter concerns with the recent development of a new DFT methodology for accurate, reliable prediction of many-electron systems. Background, need for such a scheme, major difficulties encountered, as well as their potential remedies…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

Localized orbital coupled cluster theory has recently emerged as an nonempirical alternative to DFT for large systems. Intuitively, one might expect such methods to perform less well for highly delocalized systems. In the present work, we…

Chemical Physics · Physics 2020-10-16 Nitai Sylvetsky , Ambar Banerjee , Mercedes Alonso , Jan M. L. Martin

A fundamental assumption of the dynamical density functional theory (DDFT) of colloidal systems is that a grand-canonical free energy functional may be employed to generate the thermodynamic driving forces. Using one-dimensional hard-rods…

Soft Condensed Matter · Physics 2013-06-04 Johannes Reinhardt , Joseph Michael Brader

In order to obtain a reasonably accurate and easily implemented approach to many-electron calculations, we will develop a new Density Functional Theory (DFT). Specifically, we derive an approximation to electron density, the first term of…

Materials Science · Physics 2010-04-23 Gregory C. Dente

To explore the applicability of orbital-free density functional theory (OF-DFT) in nuclear physics, we perform a systematic benchmark of 36 one-point kinetic energy density functionals, which are originally developed for electron systems in…

Nuclear Theory · Physics 2026-05-20 Tian Shuai Shang , Jian Li , Haozhao Liang , Xinhui Wu , Cheng Ma , Wenhui Mi , Xuecheng Shao , Yanchao Wang

We present, within Kohn-Sham Density Functional Theory calculations, a quantitative method to identify and assess the partitioning of a large quantum mechanical system into fragments. We then show how within this framework simple…

Chemical Physics · Physics 2017-09-28 Stephan Mohr , Michel Masella , Laura E. Ratcliff , Luigi Genovese

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…

The problem of construction of the Wannier functions (WFs) in a restricted Hilbert space of eigenstates of the one-electron Hamiltonian $\hat{H}$ (forming the so-called low-energy part of the spectrum) can be formulated in several different…

Strongly Correlated Electrons · Physics 2007-05-23 I. V. Solovyev , Z. V. Pchelkina , V. I. Anisimov

We develop a classical density functional theory (DFT) for two site associating fluids in spatially uniform external fields which exhibit orientational inhomogeneities. The Helmholtz free energy functional is obtain using Wertheim's…

Soft Condensed Matter · Physics 2015-06-17 B. D. Marshall , W. G. Chapman , M. M. Telo da Gama

Low-cost, non-empirical corrections to semi-local density functional theory are essential for accurately modeling transition metal chemistry. Here, we demonstrate the judiciously-modified density functional theory (jmDFT) approach with…

Materials Science · Physics 2022-05-25 Akash Bajaj , Chenru Duan , Aditya Nandy , Michael G. Taylor , Heather J. Kulik

The present work proposes to use density-functional theory (DFT) to correct for the basis-set error of wave-function theory (WFT). One of the key ideas developed here is to define a range-separation parameter which automatically adapts to a…

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

A new method for calculating optical absorption spectra within linear-scaling density-functional theory (LS-DFT) is presented, incorporating a scheme for optimizing a set of localized orbitals to accurately represent unoccupied Kohn-Sham…

Materials Science · Physics 2015-05-30 Laura E. Ratcliff , Nicholas D. M. Hine , Peter D. Haynes

Koopmans spectral functionals are a powerful extension of Kohn-Sham density-functional theory (DFT) that enable the prediction of spectral properties with state-of-the-art accuracy. The success of these functionals relies on capturing the…

Materials Science · Physics 2024-12-23 Yannick Schubert , Sandra Luber , Nicola Marzari , Edward Linscott

An open question in designing superconducting quantum circuits is how best to reduce the full circuit Hamiltonian which describes their dynamics to an effective two-level qubit Hamiltonian which is appropriate for manipulation of quantum…

Quantum Physics · Physics 2020-06-24 Gioele Consani , Paul A. Warburton

Approximate functionals used in practical density functional theory (DFT) deviate from the piecewise linear behavior of the exact functional for fractional charges. This deviation causes excess charge delocalization, which leads to…

Chemical Physics · Physics 2018-10-23 Diptarka Hait , Martin Head-Gordon