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Rabi oscillations have long been thought to be out of reach in simulations using time-dependent density functional theory (TDDFT), a prominent symptom of the failure of the adiabatic approximation for non-perturbative dynamics. We present a…

Chemical Physics · Physics 2024-06-21 Davood B. Dar , Anna Baranova , Neepa T. Maitra

A real-space representation of the current response of many-electron systems with possible applications to x-ray nonlinear spectroscopy and magnetic susceptibilities is developed. Closed expressions for the linear, quadratic and third-order…

Strongly Correlated Electrons · Physics 2009-11-10 Oleg Berman , Shaul Mukamel

Charge transfer plays a crucial role in many processes of interest in physics, chemistry, and bio-chemistry. In many applications the size of the systems involved calls for time-dependent density functional theory (TDDFT) to be used in…

Chemical Physics · Physics 2017-10-11 Neepa T. Maitra

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…

Chemical Physics · Physics 2023-05-01 Davood Dar , Saswata Roy , Neepa T. Maitra

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

Imaginary-time time-dependent Density functional theory (it-TDDFT) has been proposed as an alternative method for obtaining the ground state within density functional theory (DFT) which avoids some of the difficulties with convergence…

Computational Physics · Physics 2021-11-09 John McFarland , Efstratios Manousakis

Density functional theory (DFT) and linear-response time-dependent density functional theory (LR-TDDFT) rely on an exchange-correlation (xc) approximation that provides not only energy but also its functional derivatives that enter the…

Chemical Physics · Physics 2026-04-08 Xiaoyu Zhang

Various ways to analyze the dynamical response of clusters and molecules to electromagnetic perturbations exist. Particularly rich information can be obtained from measuring the properties of electrons emitted in the course of the…

Atomic and Molecular Clusters · Physics 2015-06-11 P. Wopperer , P. M. Dinh , P. -G. Reinhard , E. Suraud

Time-dependent density-functional theory (TDDFT) is a central tool for studying the dynamical electronic structure of molecules and solids, yet aspects of its mathematical foundations remain insufficiently understood. In this work, we…

The density linear response function for an inhomogeneous system of electrons in equilibrium with an array of fixed ions is considered. Two routes to its evaluation for extreme conditions (e.g., warm dense matter) are considered. The first…

Statistical Mechanics · Physics 2018-09-12 James Dufty , Kai Luo , S. B. Trickey

A time-dependent density functional theory (TDDFT) for a quantum many-body system on a lattice is formulated rigorously. We prove the uniqueness of the density-to-potential mapping and demonstrate that a given density is $v$-representable…

Strongly Correlated Electrons · Physics 2015-06-05 Mehdi Farzanehpour , I. V. Tokatly

Time-dependent density-functional theory (TDDFT) treats dynamical exchange and correlation (xc) via a single-particle potential, Vxc(r,t), defined as a nonlocal functional of the density n(r',t'). The popular adiabatic local-density…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 C. A. Ullrich , I. V. Tokatly

A decomposition of the exact exchange-correlation potential of time-dependent density functional theory into an interaction component and a kinetic component offers a new starting point for non- adiabatic approximations. The components are…

Chemical Physics · Physics 2018-11-14 Johanna I. Fuks , Lionel Lacombe , Soeren E. B. Nielsen , Neepa T. Maitra

Ultrafast electronic dynamics in solids lies at the core of modern condensed matter and materials physics. To build up a practical ab initio method for studying solids under photoexcitation, we develop a momentum-resolved real-time time…

Materials Science · Physics 2018-10-17 Chao Lian , Shi-Qi Hu , Meng-Xue Guan , Sheng Meng

Many application models in quantum physics and chemistry require to control multi-electron systems to achieve a desired target configuration. This challenging task appears possible in the framework of time-dependent density functional…

Optimization and Control · Mathematics 2018-03-14 Martin Sprengel , Gabriele Ciaramella , Alfio Borzì

Using the Runge-Gross theorem that establishes the foundation of Time-dependent Density Functional Theory (TDDFT) we prove that for a given electronic Hamiltonian, choice of initial state, and choice of fragmentation, there is a unique…

Chemical Physics · Physics 2015-06-15 Martin A. Mosquera , Daniel Jensen , Adam Wasserman

The nonequilibrium thermodynamics of interacting quantum many-body systems is investigated within the framework of thermal time-dependent density functional theory using a generalized linear-response formulation for the full quantum work…

Quantum Physics · Physics 2025-12-23 Antonio Palamara , Francesco Plastina , Antonello Sindona , Irene D'Amico

We formulate equations of time-dependent density functional theory (TDDFT) in the co-moving Lagrangian reference frame. The main advantage of the Lagrangian description of many-body dynamics is that in the co-moving frame the current…

Strongly Correlated Electrons · Physics 2009-11-10 I. V. Tokatly

In this work, the dynamics of dephasing (without relaxation) in the presence of a chaotic oscillator is theoretically investigated. The time-dependent density functional theory (TDDFT) framework was employed in tandem with the Lindblad…

Quantum Physics · Physics 2016-09-28 T. Ganesan

Real-time time-dependent density functional theory (RT-TDDFT) can in principle access the whole absorption spectrum of a many-electron system exposed to a narrow pulse. However, this requires an accurate and efficient propagator for the…

Chemical Physics · Physics 2024-06-19 Linfeng Ye , Hao Wang , Yong Zhang , Wenjian Liu
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