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We present a comprehensive theoretical description for an irradiation of an ultrashort light pulse normally on thin materials based on first-principles time-dependent density functional theory. As the most elaborate scheme, we develop a…

Optics · Physics 2018-12-31 Shunsuke Yamada , Masashi Noda , Katsuyuki Nobusada , Kazuhiro Yabana

We show that as an electron transfers between closed-shell molecular fragments at large separation, the exact correlation potential of time-dependent density functional theory gradually develops a step and peak structure in the bonding…

Chemical Physics · Physics 2014-02-11 Johanna I. Fuks , Peter Elliott , Angel Rubio , Neepa T. Maitra

The route to reliable quantum nanoelectronic devices hinges on precise control of the electrostatic environment. For this reason, accurate methods for electrostatic simulations are essential in the design process. The most widespread…

Mesoscale and Nanoscale Physics · Physics 2023-02-28 Waldemar Svejstrup , Andrea Maiani , Kevin Van Hoogdalem , Karsten Flensberg

The particle-hole interaction problem is longstanding within time-dependent density functional theory (TDDFT) and leads to extreme errors in the prediction of K-edge X-ray absorption spectra (XAS). We derive a linear-response formalism that…

Chemical Physics · Physics 2022-10-18 Kevin Carter-Fenk , Leonardo A. Cunha , Juan E. Arias-Martinez , Martin Head-Gordon

Chemical accuracy serves as an important metric for assessing the effectiveness of the numerical method in Kohn--Sham density functional theory. It is found that to achieve chemical accuracy, not only the Kohn--Sham wavefunctions but also…

Computational Physics · Physics 2023-10-25 Yang Kuang , Yedan Shen , Guanghui Hu

Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical…

Materials Science · Physics 2022-09-12 Marcus Annegarn , Juhan Matthias Kahk , Johannes Lischner

Two of the most widely used electronic structure theory methods, namely Hartree-Fock and Kohn-Sham density functional theory, both requires the iterative solution of a set of Schr\"odinger-like equations. The speed of convergence of such…

Chemical Physics · Physics 2024-06-06 S. Hazra , U. Patil , S. Sanvito

The density functional theory (DFT) is a remarkably successful theory of electronic structure of matter. At the foundation of this theory lies the Kohn-Sham (KS) equation. In this paper, we describe the long-time behaviour of the…

Analysis of PDEs · Mathematics 2021-05-11 Fabio Pusateri , Israel Michael Sigal

Long-range charge-transfer excitations pose a major challenge for time-dependent density functional approximations. We show that spin-symmetry-breaking offers a simple solution for molecules composed of open-shell fragments, yielding…

Chemical Physics · Physics 2015-03-17 Johanna I. Fuks , Angel Rubio , Neepa T. Maitra

Faithful representations of atomic environments and general models for regression can be harnessed to learn electron densities that are close to the ground state. One of the applications of data-derived electron densities is to orbital-free…

Materials Science · Physics 2019-03-01 Andrew T. Fowler , Chris J. Pickard , James A. Elliott

We present and test a new approximation for the exchange-correlation (xc) energy of Kohn-Sham density functional theory. It combines exact exchange with a compatible non-local correlation functional. The functional is by construction free…

Chemical Physics · Physics 2014-05-23 Tobias Schmidt , Eli Kraisler , Adi Makmal , Leeor Kronik , Stephan Kümmel

We present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe timescales from attoseconds…

Mesoscale and Nanoscale Physics · Physics 2016-01-28 Valerio Rizzi , Tchavdar N. Todorov , Jorge J. Kohanoff , Alfredo A. Correa

Methods based on propagation of the one-body reduced density-matrix hold much promise for the simulation of correlated many-electron dynamics far from equilibrium, but difficulties with finding good approximations for the interaction term…

Chemical Physics · Physics 2016-02-12 Peter Elliott , Neepa T. Maitra

We show that the energetics and lifetimes of resonances of finite systems under an external electric field can be captured by Kohn--Sham density functional theory (DFT) within the formalism of uniform complex scaling. Properties of…

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been…

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

Numerical Analysis · Mathematics 2022-01-19 Xiaoying Dai , Stefano de Gironcoli , Bin Yang , Aihui Zhou

We review the theoretical background for obtaining both quantum defects and scattering phase shifts from time-dependent density functional theory. The quantum defect on the negative energy side of the spectrum and the phase shift on the…

Other Condensed Matter · Physics 2019-03-27 Meta van Faassen , Kieron Burke

In this work, the existence, uniqueness and regularity of solutions to the time-dependent Kohn-Sham equations are investigated. The Kohn-Sham equations are a system of nonlinear coupled Schr\"odinger equations that describe multi-particle…

Analysis of PDEs · Mathematics 2018-03-14 Martin Sprengel , Gabriele Ciaramella , Alfio Borzì

We present a Lagrangian-based implementation of Ehrenfest dynamics with nuclear-electronic orbital (NEO) theory and real-time time-dependent density functional theory (RT-TDDFT) for extended periodic systems. In addition to a quantum…

Chemical Physics · Physics 2024-07-29 Jianhang Xu , Ruiyi Zhou , Tao E. Li , Sharon Hammes-Schiffer , Yosuke Kanai

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke