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We present an efficient method for propagating the time-dependent Kohn-Sham equations in free space, based on the recently introduced Fourier contour deformation (FCD) approach. For potentials which are constant outside a bounded domain,…

Chemical Physics · Physics 2023-07-10 Jason Kaye , Alex Barnett , Leslie Greengard , Umberto De Giovannini , Angel Rubio

Solving the time-dependent Schr\"odinger equation (TDSE) is pivotal for modeling non-adiabatic electron dynamics, a key process in ultrafast spectroscopy and laser-matter interactions. However, exact solutions to the TDSE remain…

Chemical Physics · Physics 2025-12-29 Bizi Huang , Weizhong Fu , Ji Chen

Density Functional Theory (DFT) is widely used for atomistic simulations. However, its reach stays limited due to several limitations such as lack of accurate exchange-correlation functional, requirement of costly O(N 3) diagonalization…

Quantum Physics · Physics 2026-05-18 Namrata Manglani , Samrit Kumar Maity , Shashank Sharma , Soham Phulare , Sanjay Wandhekar

Real-time time-dependent density functional theory (rt-TDDFT) with hybrid exchange-correlation functional has wide-ranging applications in chemistry and material science simulations. However, it can be thousands of times more expensive than…

Computational Physics · Physics 2019-05-07 Weile Jia , Lin-Wang Wang , Lin Lin

Spin-current density functional theory (SCDFT) is a formally exact framework designed to handle the treatment of interacting many-electron systems including spin-orbit coupling at the level of the Pauli equation. In practice, robust and…

In the exact Kohn-Sham density-functional theory (DFT), the total energy versus the number of electrons is a series of linear segments between integer points. However, commonly used approximate density functionals produce total energies…

Materials Science · Physics 2013-04-03 Eli Kraisler , Leeor Kronik

Linear-response time-dependent density functional theory (LR-TDDFT) simulations of disordered extended systems require averaging over different snapshots of ion configurations to minimize finite size effects due to the snapshot--dependence…

Computational Physics · Physics 2023-07-19 Zhandos A. Moldabekov , Jan Vorberger , Mani Lokamani , Tobias Dornheim

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

In this work we give a comprehensive derivation of an exact and numerically feasible method to perform ab-initio calculations of quantum particles interacting with a quantized electromagnetic field. We present a hierachy of…

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

We derive an exact expression for the photo-current of photo-emission spectroscopy using time-dependent current density functional theory (TDCDFT). This expression is given as an integral over the Kohn-Sham spectral function renormalized by…

Mesoscale and Nanoscale Physics · Physics 2015-06-18 A. -M. Uimonen , G. Stefanucci , R. van Leeuwen

The development of analytic-gradient methodology for excited states within conventional time-dependent density-functional theory (TDDFT) would seem to offer a relatively inexpensive alternative to better established quantum-chemical…

Other Condensed Matter · Physics 2010-08-11 Felipe Cordova , L. Joubert Doriol , Andrei Ipatov , Mark E. Casida , Claudia Filippi , Alberto Vela

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

We present the basic concepts and recent developments in the time-dependent density functional theory (TDDFT) for describing nuclear dynamics at low energy. The symmetry breaking is inherent in nuclear energy density functionals (EDFs),…

Nuclear Theory · Physics 2016-12-21 Takashi Nakatsukasa , Kenichi Matsuyanagi , Masayuki Matsuo , Kazuhiro Yabana

We apply the time-dependent current-density functional theory to the study of the relaxation of a closed many-electron system evolving from an non-equilibrium initial state. We show that the self-consistent unitary time evolution generated…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 Roberto D'Agosta , Giovanni Vignale

The Tamm-Dancoff Approximation (TDA) offers a computationally efficient alternative to full linear-response Time-Dependent Density Functional Theory (TDDFT) for calculating electronic excited states, particularly in large molecular systems.…

Chemical Physics · Physics 2025-07-02 Muhammed A. Dada , Sarah Pak , Matthew N. Ward , Megan Simons , Daniel R. Nascimento

Recent progress has been made in capturing spectral features of electronic states of double-excitation character in time-dependent density functional theory (TDDFT) through a frequency-dependent kernel. While it might appear that this…

Chemical Physics · Physics 2026-05-04 Dhyey Ray , Anna Baranova , Davood B. Dar , Neepa T. Maitra

We present a local control scheme 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. The numerical method is efficient and stable…

Strongly Correlated Electrons · Physics 2013-02-14 S. E. B. Nielsen , M. Ruggenthaler , R. van Leeuwen

Theoretical studies of photochemical processes require a description of the energy surfaces of excited electronic states, especially near degeneracies, where transitions between states are most likely. Systems relevant to photochemical…

Density functional theory (DFT) has emerged as one of the most versatile and lucrative approaches in electronic structure calculations of many-electron systems in past four decades. Here we give an account of the development of a…

Chemical Physics · Physics 2019-04-19 Abhisek Ghosal , Amlan K. Roy
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