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We discuss two problems which are particularly challenging for approximations in time-dependent density functional theory (TDDFT) to capture: momentum-distributions in ionization processes, and memory-dependence in real-time dynamics. We…

Materials Science · Physics 2010-03-22 Arun K. Rajam , Paul Hessler , Christian Gaun , Neepa T. Maitra

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…

Materials Science · Physics 2013-12-09 Dirk Hofmann , Heiko Appel , Massimiliano Di Ventra , Stephan Kümmel

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

Modulating ion transport through nanoporous membranes is critical to many important chemical and biological separation processes. The corresponding transport timescales, however, are often too long to capture accurately using conventional…

Statistical Mechanics · Physics 2022-12-23 Brian A Shoemaker , Tiago S Domingues , Amir Haji-Akbari

We formulate and implement Cyclic Density Functional Theory (Cyclic DFT) -- a self-consistent first principles simulation method for nanostructures with cyclic symmetries. Using arguments based on Group Representation Theory, we rigorously…

Materials Science · Physics 2017-03-16 Amartya S. Banerjee , Phanish Suryanarayana

The theoretical understanding of plasmon behavior is crucial for an accurate interpretation of inelastic scattering diagnostics in many experiments. We highlight the utility of linear-response time-dependent density functional theory…

Materials Science · Physics 2021-03-17 Kushal Ramakrishna , Attila Cangi , Tobias Dornheim , Andrew Baczewski , Jan Vorberger

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

Chemical Physics · Physics 2023-01-02 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

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

Materials Science · Physics 2025-12-02 Karan Shah , Attila Cangi

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein

Following a previous paper [Y. Shi, Phys. Rev. C 98, 014329(2018)], we present an extension of the density-functional theory to allow for dynamic calculations based on the obtained static Hartree-Fock results. We perform extensive benchmark…

Nuclear Theory · Physics 2020-11-04 Yue Shi , Nobuo Hinohara , Bastian Schuetrumpf

Real-time time-dependent density functional theory (RT-TDDFT) is a powerful approach for investigating various ultrafast phenomena in materials. However, most existing RT-TDDFT studies rely on adiabatic local or semi-local approximations,…

Materials Science · Physics 2025-12-23 Yuyang Ji , Haotian Zhao , Peize Lin , Xinguo Ren , Lixin He

We compare the predictions of the dynamic structure factor (DSF) of ambient polycrystalline aluminium from time-dependent density functional theory (TDDFT) in the pair continuum regime to recent ultrahigh resolution x-ray Thomson scattering…

Time-dependent current-density-functional theory (TDCDFT) provides an in principle exact scheme to calculate efficiently response functions for a very broad range of applications. However, the lack of approximations valid for a range of…

Strongly Correlated Electrons · Physics 2015-05-20 Matteo Gatti

The real-time-propagation formulation of time-dependent density-functional theory (RT-TDDFT) is an efficient method for modeling the optical response of molecules and nanoparticles. Compared to the widely adopted linear-response TDDFT…

Materials Science · Physics 2019-01-15 Tuomas P. Rossi , Mikael Kuisma , Martti J. Puska , Risto M. Nieminen , Paul Erhart

We present a real-space formulation and higher-order finite-difference implementation of periodic Orbital-free Density Functional Theory (OF-DFT). Specifically, utilizing a local reformulation of the electrostatic and kernel terms, we…

Computational Physics · Physics 2015-12-23 Swarnava Ghosh , Phanish Suryanarayana

We present a formulation of spin-conserving and spin-flip, hybrid time-dependent density functional theory (TDDFT), including the calculation of analytical forces, which allows for efficient calculations of excited state properties of…

Materials Science · Physics 2023-12-05 Yu Jin , Victor Wen-zhe Yu , Marco Govoni , Andrew C Xu , Giulia Galli

We consider offline reinforcement learning (RL) in $H$-horizon Markov decision processes (MDPs) under the linear $q^\pi$-realizability assumption, where the action-value function of every policy is linear with respect to a given…

Machine Learning · Computer Science 2024-05-28 Volodymyr Tkachuk , Gellért Weisz , Csaba Szepesvári

To examine the applicability of the time-dependent density-functional theory (TDDFT) for treating the electron-nucleus coupling in excited states, we calculate the strength distribution associated with the pi-pi* transition in ethylene. The…

Chemical Physics · Physics 2007-05-23 G. F. Bertsch , J. Giansiracusa , K. Yabana

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…

We present the theory, implementation, and benchmarking of a real-time time-dependent density functional theory (RT-TDDFT) module within the RMG code, designed to simulate the electronic response of molecular systems to external…