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To apply the Hubbard-corrected density-functional theory for predicting some known materials' properties, the Hubbard parameters are usually so tuned that the calculations give results in agreement with some experimental data and then one…

Materials Science · Physics 2023-06-13 Mahmoud Payami , Samira Sheykhi , Mohammad-Reza Basaadat

A generalization of the density-functional based tight-binding method (DFTB) for the use with range-separated exchange-correlation functionals is presented. It is based on the Generalized Kohn-Sham (GKS) formalism and employs the density…

Materials Science · Physics 2015-06-03 Thomas A. Niehaus , Fabio Della Sala

Phonons crucially impact a variety of properties of organic semiconductor materials. For instance, charge- and heat transport depend on low-frequency phonons, while for other properties, such as the free energy, especially high-frequency…

Screened range-separated hybrid (SRSH) functionals within generalized Kohn-Sham density functional theory (GKS-DFT) have been shown to restore a general $1/(r\varepsilon)$ asymptotic decay of the electrostatic interaction in dielectric…

Computational Physics · Physics 2023-06-26 Tammo van der Heide , Bálint Aradi , Ben Hourahine , Thomas Frauenheim , Thomas A. Niehaus

Elemental rare-earth metals provide a playground for studying novel electron correlation effects and complex magnetism. However, ab initio simulations of these systems remain challenging. Here, we employ fully charge self-consistent density…

Strongly Correlated Electrons · Physics 2024-12-23 Wenjun Ding , Yogesh K. Vohra , Cheng-Chien Chen

Semi-empirical quantum models such as Density Functional Tight Binding (DFTB) are attractive methods for obtaining quantum simulation data at longer time and length scales than possible with standard approaches. However, application of…

Materials Science · Physics 2023-04-26 Nir Goldman , Laurence E. Fried , Rebecca K. Lindsey , C. Huy Pham , R. Dettori

Semi-empirical quantum mechanical methods traditionally expand the electron density in a minimal, valence-only electron basis set. The minimal-basis approximation causes molecular polarization to be underestimated, and hence intermolecular…

Chemical Physics · Physics 2015-09-30 Anders S. Christensen , Marcus Elstner , Qiang Cui

In approximate density functional theory (DFT), the self-interaction error is an electron delocalization anomaly associated with underestimated insulating gaps. It exhibits a predominantly quadratic energy-density curve that is amenable to…

Chemical Physics · Physics 2016-12-21 Glenn Moynihan , Gilberto Teobaldi , David D. O'Regan

A derivation of non-adiabatic coupling vectors for the density functional based tight binding method (DFTB) between ground and excited states is presented. The analytical result is valid both for semi-local and long-range corrected DFTB and…

Chemical Physics · Physics 2020-10-29 Thomas A. Niehaus

The interaction within a hybrid system consisting of a spherical metal nanoparticle and a nearby organic dye molecule is formulated in a combined quantum-classical approach. Whereas the nanoparticle's polarization field is treated in…

Chemical Physics · Physics 2019-09-04 Xiaomeng Liu , Lennart Seiffert , Thomas Fennel , Oliver Kühn

The strong boundary normalized condition of wavefunction for fully occupied semicore 3d orbitals leads the linear response DFT+U on such metal oxide to have an insurmountable obstacle in Hubbard U determination. We treated the orbital…

Strongly Correlated Electrons · Physics 2015-11-17 Bolong Huang

Predicting the compositional phase stability of strongly correlated electron materials is an outstanding challenge in condensed matter physics, requiring precise computations of total energies. In this work, we employ the density functional…

Strongly Correlated Electrons · Physics 2020-07-28 Eric B. Isaacs , Chris A. Marianetti

We present optimized tight-binding models with atomic orbitals to improve \textit{ab initio} tight-binding models constructed by truncating full density functional theory (DFT) Hamiltonian based on localized orbitals. Retaining qualitative…

Mesoscale and Nanoscale Physics · Physics 2024-02-20 Sejoong Kim

We introduce a system-independent method to derive effective atomic C$_6$ coefficients and polarizabilities in molecules and materials purely from charge population analysis. This enables the use of dispersion-correction schemes in…

Materials Science · Physics 2016-09-05 Martin Stöhr , Georg S. Michelitsch , John C. Tully , Karsten Reuter , Reinhard J. Maurer

Using density functional theory, we determine parameters of tight-binding Hamiltonians for a variety of Fabre charge transfer salts, focusing in particular on the effects of temperature and pressure. Besides relying on previously published…

Strongly Correlated Electrons · Physics 2013-04-25 A. C. Jacko , H. Feldner , E. Rose , F. Lissner , M. Dressel , Roser Valentí , Harald O. Jeschke

Comparative molecular dynamics simulations of a hexamer cluster of the protic ionic liquid ethylammonium nitrate are performed using density functional theory (DFT) and density functional-based tight binding (DFTB) methods. The focus is on…

Chemical Physics · Physics 2017-03-24 Tobias Zentel , Oliver Kühn

The formalism of electronic density-functional-theory, with Hubbard-U corrections (DFT+U), is employed in a computational study of the energetics of U_{1-x} Ce_x O_2 mixtures. The computational approach makes use of a procedure which…

Materials Science · Physics 2012-03-08 B. E. Hanken , C. R. Stanek , N. Grønbech-Jensen , M. Asta

We propose a self-consistent site-dependent Hubbard $U$ approach for DFT+$U$ calculations of defects in complex transition-metal oxides, using Hubbard parameters computed via linear-response theory. The formation of a defect locally…

Materials Science · Physics 2019-04-04 Chiara Ricca , Iurii Timrov , Matteo Cococcioni , Nicola Marzari , Ulrich Aschauer

In this paper we use ab initio density functional theory (DFT) to calculate the electronic properties of C_50Cl_10. In comparison with the unstable C_50 which has a small t_lu(LUMO) - h_u(HOMO) energy gap and a high total free energy…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 Steven W. D. Bailey , Colin J. Lambert

Tight-binding (TB) molecular dynamics (MD) has emerged as a powerful method for investigating the atomic-scale structure of materials --- in particular the interplay between structural and electronic properties --- bridging the gap between…

Materials Science · Physics 2007-05-23 Laurent J Lewis , Normand Mousseau