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We present a framework for obtaining reliable solid-state charge and optical excitations and spectra from optimally-tuned range-separated hybrid density functional theory. The approach, which is fully couched within the formal framework of…

Materials Science · Physics 2015-09-30 Sivan Refaely-Abramson , Manish Jain , Sahar Sharifzadeh , Jeffrey B. Neaton , Leeor Kronik

The optical spectra of two-dimensional (2D) periodic systems provide a challenge for time-dependent density-functional theory (TDDFT) because of the large excitonic effects in these materials. In this work we explore how accurately these…

Materials Science · Physics 2021-01-27 Stefano Di Sabatino , J. A. Berger , Pina Romaniello

We present a fully parameter-free density-functional approach for the accurate description of optical absorption spectra of insulators, semiconductors and metals. We show that this can be achieved within time-dependent…

Materials Science · Physics 2015-10-28 J. A. Berger

We show that by nullifying the short-wave response to the long-wave excitation (local-field-effects), the adiabatic time-dependent density-functional theory (TDDFT) of optics of semiconductors and insulators can be brought into excellent…

Materials Science · Physics 2013-08-15 V. U. Nazarov , S. Kais

We formulate a time-dependent density functional theory (TDDFT) in terms of the density matrix to study ultrafast phenomena in semiconductor structures. A system of equations for the density matrix components, which is equivalent to the…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 V. Turkowski , C. A. Ullrich

We investigate optical absorption spectra obtained through time-dependent density functional theory (TD-DFT) based on nonempirical hybrid functionals that are designed to correctly reproduce the dielectric function. The comparison with…

Materials Science · Physics 2020-08-17 Alexey Tal , Peitao Liu , Georg Kresse , Alfredo Pasquarello

Within the framework of ab initio time-dependent density-functional theory (TD-DFT), we propose a static approximation to the exchange-correlation kernel based on the jellium-with-gap model. This kernel accounts for electron-hole…

We calculate the exact Kohn-Sham potential that describes, within time-dependent density-functional theory, the propagation of an electron quasiparticle wavepacket of non-zero crystal momentum added to a ground-state model semiconductor.…

Mesoscale and Nanoscale Physics · Physics 2015-06-05 J. D. Ramsden , R. W. Godby

Time-dependent density-functional theory (TDDFT) is a computationally efficient first-principles approach for calculating optical spectra in insulators and semiconductors, including excitonic effects. We show how exciton wave functions can…

Materials Science · Physics 2020-12-29 Jared R. Williams , Nicolas Tancogne-Dejean , Carsten A. Ullrich

Applying the novel exact-exchange (EXX) Kohn-Sham method within time-dependent density-functional theory, we obtained the optical absorption spectrum of bulk silicon in good agreement with experiments including excitonic features. Analysis…

Materials Science · Physics 2016-01-01 Yong-Hoon Kim , Andreas Goerling

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

Density functional approximations to the exchange-correlation energy of Kohn-Sham theory, such as the local density approximation and generalized gradient approximations, lack the well-known integer discontinuity, a feature that is critical…

Chemical Physics · Physics 2015-06-18 Martin A. Mosquera , Adam Wasserman

The self consistent version of the density functional theory is presented, which allows to calculate the ground state and dynamic properties of finite multi-electron systems. An exact functional equation for the effective interaction, from…

Materials Science · Physics 2017-08-23 M. Ya. Amusia , A. Z. Msezane , V. R. Shaginyan

We calculate the imaginary part of the frequency-dependent dielectric function of bulk silicon by applying time-dependent density-functional theory based on the exact-exchange (EXX) Kohn-Sham (KS) band structure and the adiabatic…

Materials Science · Physics 2016-01-01 Yong-Hoon Kim , Martin Staedele , Andreas Goerling

Molecular absorption and photo-electron spectra can be efficiently predicted with real-time time-dependent density-functional theory (TDDFT). We show here how these techniques can be easily extended to study time-resolved pump-probe…

Atomic and Molecular Clusters · Physics 2013-01-10 Umberto De Giovannini , Gustavo Brunetto , Alberto Castro , Jessica Walkenhorst , Angel Rubio

In the present work, we introduce a Self-Consistent Density-Functional Embedding technique, which leaves the realm of standard energy-functional approaches in Density Functional Theory and targets directly the density-to-potential mapping…

Computational Physics · Physics 2019-07-17 Uliana Mordovina , Teresa E. Reinhard , Iris Theophilou , Heiko Appel , Angel Rubio

We present calculations of the absorption spectrum of semiconductors and insulators comparing various approaches: (i) the two-particle Bethe-Salpeter equation of Many-Body Perturbation Theory; (ii) time-dependent density-functional theory…

Other Condensed Matter · Physics 2009-11-13 Francesco Sottile , Marherita Marsili , Valerio Olevano , Lucia Reining

We re-adapt a spectral renormalization method, introduced in nonlinear optics, to solve the Kohn-Sham (KS) equations of density functional theory (DFT), with a focus on functionals based on the strictly-correlated electrons (SCE) regime,…

Strongly Correlated Electrons · Physics 2020-04-23 Juri Grossi , Ziad H. Musslimani , Michael Seidl , Paola Gori-Giorgi

We calculate the optical spectra of silicon and germanium in the adiabatic time-dependent density functional formalism, making use of kinetic energy density-dependent (meta-GGA) exchange-correlation functionals. We find excellent agreement…

Strongly Correlated Electrons · Physics 2011-11-16 V. U. Nazarov , G. Vignale

By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…

Quantum Physics · Physics 2009-11-13 Xiao Zheng , Fan Wang , Chi Yung Yam , Yan Mo , GuanHua Chen
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