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We demonstrate the capabilities of time-dependent density functional theory (TDDFT) for strong-field, short wavelength (soft X-ray) physics, as compared to a formalism based on rate equations. We find that TDDFT provides a very good…

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…

量子物理 · 物理学 2024-02-29 Evan Sheridan , Lana Mineh , Raul A. Santos , Toby Cubitt

This paper studies the performance of time-dependent density-functional theory (TDDFT) for calculating the dielectric function of semiconductors and insulators at finite momentum transfer, comparing against the standard Bethe-Salpeter…

材料科学 · 物理学 2025-03-03 Didarul Alam , Jiuyu Sun , Carsten A. Ullrich

We present the extension of Frozen Density Embedding (FDE) theory to real-time Time Dependent Density Functional Theory (rt-TDDFT). FDE a is DFT-in-DFT embedding method that allows to partition a larger Kohn-Sham system into a set of…

化学物理 · 物理学 2015-06-23 Alisa Krishtal , Davide Ceresoli , Michele Pavanello

By including a fraction of exact exchange (EXX), hybrid functionals reduce the self-interaction error in semi-local density functional theory (DFT), and thereby furnish a more accurate and reliable description of the electronic structure in…

计算物理 · 物理学 2021-05-10 Hsin-Yu Ko , Junteng Jia , Biswajit Santra , Xifan Wu , Roberto Car , Robert A. DiStasio

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

化学物理 · 物理学 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state…

化学物理 · 物理学 2021-12-15 Kaili Jiang , Xuecheng Shao , Michele Pavanello

The purpose of the current work is to find numerical solutions of the steady state inhomogeneous Vlasov equation. This problem has a wide range of applications in the kinetic simulation of non-thermal plasmas. However, the direct…

计算物理 · 物理学 2018-08-14 Markus Gasteiger , Lukas Einkemmer , Alexander Ostermann , David Tskhakaya

Conical intersections are central to the description of photophysics and photochemistry. Nevertheless, in non-adiabatic molecular dynamics simulations, they are fundamentally challenging for single-reference electronic structure methods.…

化学物理 · 物理学 2026-04-23 Federico Rossi , Tommaso Giovannini , Henrik Koch

The adiabatic approximation in time-dependent density functional theory (TDDFT) is known to give an incorrect pole structure in the quadratic response function, leading to unphysical divergences in excited state-to-state transition…

化学物理 · 物理学 2023-05-01 Davood Dar , Saswata Roy , Neepa T. Maitra

Mixed-reference spin-flip time-dependent density functional theory (MRSF-TDDFT) has recently emerged as an attractive electronic-structure method for studying photochemical processes, given that it bridges the computational efficiency of…

化学物理 · 物理学 2026-04-13 Jiří Janoš , Andrew J. Orr-Ewing , Basile F. E. Curchod , Petr Slavíček

In this communication, we present a new approach towards RT-TDDFT through time-dependent KS equations based on an \emph{adiabatic eigenstate subspace} (AES) procedure. It introduces a second-order split operator technique in energy…

计算物理 · 物理学 2022-05-20 Abhisek Ghosal , Amlan K. Roy

Orbital-free density functional theory (OF-DFT) is a promising method for large-scale quantum mechanics simulation as it provides a good balance of accuracy and computational cost. Its applicability to large-scale simulations has been aided…

We prove the existence of the exact density-functional theory formalism for open electronic systems, and develop subsequently an exact time-dependent density-functional theory (TDDFT) formulation for the dynamic response. The TDDFT…

化学物理 · 物理学 2007-05-23 Xiao Zheng , GuanHua Chen

In this thesis we study the preconditioning of square, non-symmetric and real Toeplitz systems. We prove theoretical results, which constitute sufficient conditions for the efficiency of the proposed preconditioners and the fast convergence…

数值分析 · 数学 2023-03-07 Grigorios Tachyridis

Cavity quantum electrodynamics (QED) generalizations of time-dependent (TD) density functional theory (DFT) and equation-of-motion (EOM) coupled-cluster (CC) theory are used to model small molecules strongly coupled to optical cavity modes.…

化学物理 · 物理学 2023-07-19 Marcus D. Liebenthal , Nam Vu , A. Eugene DePrince

Given the time-evolution of an electron charge density, the local potential in Kohn-Sham time-dependent density functional theory (KS-TDDFT) can be modeled as a sum of instantaneous and dynamic contributions by assuming a certain form of…

计算物理 · 物理学 2016-11-09 R. J. Magyar

Time-Dependent Density Functional Theory (TDDFT) has recently been extended to describe many-body open quantum systems (OQS) evolving under non-unitary dynamics according to a quantum master equation. In the master equation approach,…

化学物理 · 物理学 2015-05-18 David G. Tempel , Mark A. Watson , Roberto Olivares-Amaya , Alán Aspuru-Guzik

An efficient Krylov subspace algorithm for computing actions of the $\varphi$ matrix function for large matrices is proposed. This matrix function is widely used in exponential time integration, Markov chains and network analysis and many…

数值分析 · 数学 2020-10-20 Mike A. Botchev , Leonid A. Knizhnerman , Eugene E. Tyrtyshnikov

The time-dependent density functional based tight-binding (TD-DFTB) approach is generalized to account for fractional occupations. In addition, an on-site correction leads to marked qualitative and quantitative improvements over the…

材料科学 · 物理学 2013-02-15 A. Domínguez , B. Aradi , T. Frauenheim , V. Lutsker , T. A. Niehaus