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Orbital-free density functional theory (OF-DFT) holds the promise to compute ground state molecular properties at minimal cost. However, it has been held back by our inability to compute the kinetic energy as a functional of the electron…

Chemical Physics · Physics 2023-10-25 Roman Remme , Tobias Kaczun , Maximilian Scheurer , Andreas Dreuw , Fred A. Hamprecht

Density Functional Theory (DFT) underpins much of modern computational chemistry and materials science. Yet, the reliability of DFT-derived predictions of experimentally measurable properties remains fundamentally limited by the need to…

Ground-state electronic structure calculations using Kohn-Sham density functional theory (KS-DFT) offer an unprecedented balance between efficiency and accuracy, now paradigmatic to the fields of quantum chemistry and condensed matter…

Chemical Physics · Physics 2026-04-14 Lucien Dupuy , Toni Chiti , Jérémy Morere , Emmanuel Fromager

Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…

The treatment of degenerate states within Kohn-Sham density functional theory (KS-DFT) is a problem of longstanding interest. We propose a solution to this mapping from the interacting degenerate system to that of the noninteracting fermion…

Materials Science · Physics 2009-11-07 Viraht Sahni , Xiao-Yin Pan

Kohn-Sham density functional theory (KS-DFT) is a powerful method to obtain key materials' properties, but the iterative solution of the KS equations is a numerically intensive task, which limits its application to complex systems. To…

Materials Science · Physics 2023-05-29 Bruno Focassio , Michelangelo Domina , Urvesh Patil , Adalberto Fazzio , Stefano Sanvito

A density functional theory (DFT) framework is presented that links functional derivatives of free-energy functionals to non-linear static density response functions in quantum many-body systems. Within this framework, explicit expressions…

The accuracy of density-functional theory (DFT) is determined by the quality of the approximate functionals, such as exchange-correlation in electronic DFT and the excess functional in the classical DFT formalism of fluids. The exact…

Development of the electronic kinetic-energy density functional is a subject of major interest in theoretical physics and chemistry. In this work, the nonlocal kinetic-energy functional is developed in terms of the response function for the…

Chemical Physics · Physics 2022-06-17 Hideaki Takahashi

The predominance of Kohn-Sham density functional theory (KS-DFT) for the theoretical treatment of large experimentally relevant systems in molecular chemistry and materials science relies primarily on the existence of efficient software…

Computational Physics · Physics 2020-07-08 David B. Williams-Young , Wibe A. de Jong , Hubertus J. J. van Dam , Chao Yang

Orbital-free Density Functional Theory (OF-DFT) has been used when studying atoms, molecules and solids. In nuclear physics, there has been basically no application of OF-DFT so far, as the Density Functional Theory (DFT) has been widely…

Nuclear Theory · Physics 2023-08-03 Gianluca Colo' , Kouichi Hagino

The design of better exchange-correlation functionals for Density Functional Theory (DFT) is a central challenge of modern electronic structure theory. However, current developments are limited by the mathematical form of the functional,…

Chemical Physics · Physics 2024-08-19 Kyle Bystrom , Boris Kozinsky

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

This chapter presents the development of a density functional theory (DFT)-based method for accurate, reliable treatment of various resonances in atoms. Many of these are known to be notorious for their strong correlation, proximity to more…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

Accurate first-principles calculations for the energies, charge distributions, and spin symmetries of many-electron systems are essential to understand and predict the electronic and structural properties of molecules and materials.…

Chemical Physics · Physics 2024-01-24 Yuming Shi , Yi Shi , Adam Wasserman

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

The recently developed Deep Potential [Phys. Rev. Lett. 120, 143001, 2018] is a powerful method to represent general inter-atomic potentials using deep neural networks. The success of Deep Potential rests on the proper treatment of locality…

Computational Physics · Physics 2019-12-05 Leonardo Zepeda-Núñez , Yixiao Chen , Jiefu Zhang , Weile Jia , Linfeng Zhang , Lin Lin

Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham…

Computational Physics · Physics 2024-02-16 I-Te Lu , Michael Ruggenthaler , Nicolas Tancogne-Dejean , Simone Latini , Markus Penz , Angel Rubio

Orbital-free density functional theory (OFDFT) is a quantum chemistry formulation that has a lower cost scaling than the prevailing Kohn-Sham DFT, which is increasingly desired for contemporary molecular research. However, its accuracy is…

Machine Learning · Statistics 2024-03-12 He Zhang , Siyuan Liu , Jiacheng You , Chang Liu , Shuxin Zheng , Ziheng Lu , Tong Wang , Nanning Zheng , Bin Shao

Understanding many processes, e.g. fusion experiments, planetary interiors and dwarf stars, depends strongly on microscopic physics modeling of warm dense matter (WDM) and hot dense plasma. This complex state of matter consists of a…

Computational Physics · Physics 2020-08-05 Alexander J. White , Lee A. Collins