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We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

Real-time, time-dependent density functional theory (RT-TDDFT) has gained popularity as a first-principles approach to study a variety of excited-state phenomena such as optical excitations and electronic stopping. Within RT-TDDFT…

Materials Science · Physics 2019-07-23 Dillon C. Yost , Yi Yao , Yosuke Kanai

A top-level designed forecasting system for predicting computational times of density-functional theory (DFT)/time-dependent density-functional theory (TDDFT) calculations is presented. The computational time is assumed as the intrinsic…

Computational Physics · Physics 2020-12-18 Shuo Ma , Yingjin Ma , Baohua Zhang , Yingqi Tian , Zhong Jin

Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…

Quantum Physics · Physics 2023-07-17 Taehee Ko , Xiantao Li , Chunhao Wang

The inverse problem of Kohn-Sham density functional theory (DFT) is often solved in an effort to benchmark and design approximate exchange-correlation potentials. The forward and inverse problems of DFT rely on the same equations but the…

Chemical Physics · Physics 2017-08-02 Daniel Jensen , Adam Wasserman

In this study, we address the challenge of controlling quantum systems under environmental influences using the theory of dynamical invariants. We employ a reverse engineering approach to develop control protocols designed to be robust…

Quantum Physics · Physics 2024-08-20 Loris Maria Cangemi , Hilario Espinós , Ricardo Puebla , Erik Torrontegui , Amikam Levy

We revisit Kohn-Sham time-dependent density-functional theory (TDDFT) equations and show that they derive from a canonical Hamiltonian formalism. We use this geometric description of the TDDFT dynamics to define families of symplectic…

Computational Physics · Physics 2023-11-20 Francois Mauger , Cristel Chandre , Mette B. Gaarde , Kenneth Lopata , Kenneth J. Schafer

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…

Chemical Physics · Physics 2023-06-28 Justin J. Talbot , Martin Head-Gordon , Stephen J. Cotton

Time-dependent density functional theory (TDDFT) is a widely used method to investigate electron dynamics under various external perturbations such as laser fields. In this work, we present a novel approach to accelerate real time TDDFT…

Materials Science · Physics 2024-07-29 Karan Shah , Attila Cangi

Quantum effects of plasmonic phenomena have been explored through ab-initio studies, but only for exceedingly small metallic nanostructures, leaving most experimentally relevant structures too large to handle. We propose instead an…

Mesoscale and Nanoscale Physics · Physics 2015-09-24 Wei Yan , Martijn Wubs , N. Asger Mortensen

Direct simulation of the von Neumann dynamics for a general (pure or mixed) quantum state can often be expensive. One prominent example is the real-time time-dependent density functional theory (rt-TDDFT), a widely used framework for the…

Numerical Analysis · Mathematics 2022-10-19 Dong An , Di Fang , Lin Lin

In this work we focus on a recently introduced method [1] to construct the external potential $v$ that, for a given initial state, produces a prescribed time-dependent density in an interacting quantum many-body system. We show how this…

Quantum Physics · Physics 2014-12-12 S. E. B. Nielsen , M. Ruggenthaler , R. van Leeuwen

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

We show that the analytic structure of the dynamical xc kernels of semiconductors and insulators can be sensed in terms of its poles which mark physically relevant frequencies of the system where the counter-phase motion of discrete…

Materials Science · Physics 2023-04-19 D. R. Gulevich , Ya. V. Zhumagulov , V. Kozin , I. V. Tokatly

A formulation for the efficient calculation of the electromagnetic retarded potential generated by time-dependent electron density in the context of real-time time dependent density functional theory (RT-TDDFT) is presented. The electron…

Chemical Physics · Physics 2025-11-19 Matan Shapira , Vitaliy Lomakin , Amir Boag , Amir Natan

Real-time time-dependent density functional theory (RT-TDDFT) is known to be hindered by the very small time step (attosecond or smaller) needed in the numerical simulation due to the fast oscillation of electron wavefunctions, which…

Computational Physics · Physics 2018-10-25 Weile Jia , Dong An , Lin-Wang Wang , Lin Lin

In their famous paper Kohn and Sham formulated a formally exact density-functional theory (DFT) for the ground-state energy and density of a system of $N$ interacting electrons, albeit limited at the time by certain troubling…

Mesoscale and Nanoscale Physics · Physics 2015-06-16 Miquel Huix-Rotllant , Mark E. Casida

Adiabatic approximations in time-dependent density functional theory (TDDFT) will in general yield unphysical time-dependent shifts in the resonance positions of a system driven far from its ground-state. This spurious time-dependence is…

Chemical Physics · Physics 2016-08-24 Kai Luo , Johanna I. Fuks , Neepa T. Maitra

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

An atomic-orbital basis set framework is presented for carrying out velocity- gauge real-time time-dependent density functional theory (TDDFT) simulations in periodic systems employing range-separated hybrid functionals. Linear optical…

Materials Science · Physics 2018-10-02 C. D. Pemmaraju
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