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We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

Chemical Physics · Physics 2015-06-23 Ralph Gebauer , Morrel H. Cohen , Roberto Car

Orbital-free density functional theory (OF-DFT) is a promising method for large-scale quantum mechanics simulation as it provides a good balance of accuracy and computational cost. Its applicability to large-scale simulations has been aided…

In [Phys. Rev. Lett. 127, 023001 (2021)] a reduced density matrix functional theory (RDMFT) has been proposed for calculating energies of selected eigenstates of interacting many-fermion systems. Here, we develop a solid foundation for this…

Quantum Physics · Physics 2022-05-06 Julia Liebert , Federico Castillo , Jean-Philippe Labbé , Christian Schilling

The real-time electronic dynamics on material surfaces is critically important to a variety of applications. However, their simulations have remained challenging for conventional methods such as the time-dependent density-functional theory…

Chemical Physics · Physics 2015-06-16 Rulin Wang , Dong Hou , Xiao Zheng

We prove that the electron density function of a real physical system can be uniquely determined by its values on any finite subsystem. This establishes the existence of a rigorous density-functional theory for any open electronic system.…

Quantum Physics · Physics 2007-05-23 Xiao Zheng , Fan Wang , GuanHua Chen

Orbital-free (OF) methods promise significant speed-up of computations based on density functional theory (DFT). In this field, the development of accurate kinetic-energy density functionals remains an open question. In this chapter we…

Materials Science · Physics 2013-05-03 Constantine Yannouleas , Uzi Landman

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

The fundamental gap of an interacting many-electron system is given by the sum of the single-particle Kohn-Sham gap and the derivative discontinuity. The latter can be generated by advanced approximations to the exchange-correlation (XC)…

Strongly Correlated Electrons · Physics 2018-07-16 Maria Hellgren

A density functional theory (DFT) of lattice fermion models is presented, which uses the single-particle density matrix gamma_{ij} as basic variable. A simple, explicit approximation to the interaction-energy functional W[gamma] of the…

Strongly Correlated Electrons · Physics 2009-11-07 R. Lopez-Sandoval , G. M. Pastor

Nuclear density functional theory (DFT) is the only microscopic, global approach to the structure of atomic nuclei. It is used in numerous applications, from determining the limits of stability to gaining a deep understanding of the…

Nuclear Theory · Physics 2015-02-06 Nicolas Schunck , Jordan D. McDonnell , Jason Sarich , Stefan M. Wild , Dave Higdon

Currently, there is a growing interest in the development of a new hierarchy of methods based on the concept of seniority, which has been introduced quite recently in quantum chemistry. Despite the enormous potential of these methods, the…

Chemical Physics · Physics 2022-12-07 Bruno Senjean , Saad Yalouz , Naoki Nakatani , Emmanuel Fromager

We provide a new formulation of Time-Dependent Density Functional Theory (TDDFT) based on the geometric structure of the set of states constrained to have a fixed density. Orbital-free TDDFT is formulated using a hydrodynamics equation…

We compute the ground-state properties of finite systems of neutrons in an external harmonic trap, interacting via the Minnesota potential, using the "exact-exchange" form of orbital-dependent density functional theory. We compare our…

Nuclear Theory · Physics 2011-07-28 Joaquín E. Drut , Lucas Platter

The density functional theory (DFT) is the most versatile electronic structure method used in quantum chemical calculations, and is increasingly applied in astrochemical research. This mini-review provides an overview of the applications of…

Astrophysics of Galaxies · Physics 2023-10-24 Qingli Liao , Junzhi Wang , Peng Xie , Enwei Liang , Zhao Wang

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been…

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

Over many years, computational simulations based on Density Functional Theory (DFT) have been used extensively to study many different materials at the atomic scale. However, its application is restricted by system size, leaving a number of…

Mesoscale and Nanoscale Physics · Physics 2018-12-05 Carlos Romero-Muñiz , Ayako Nakata , Pablo Pou , David R. Bowler , Tsuyoshi Miyazaki , Rubén Pérez

By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…

Quantum Physics · Physics 2009-11-13 Xiao Zheng , Fan Wang , Chi Yung Yam , Yan Mo , GuanHua Chen

Perdew et al. [Phys. Rev. Lett 49, 1691 (1982)] discovered and proved two different properties of exact Kohn-Sham density functional theory (DFT): (i) The exact total energy versus particle number is a series of linear segments between…

Other Condensed Matter · Physics 2015-03-13 Tamar Stein , Jochen Autschbach , Niranjan Govind , Leeor Kronik , Roi Baer

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…