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Orbital-free density functional theory (OF-DFT) for real-space systems has historically depended on Lagrange optimization techniques, primarily due to the inability of previously proposed electron density approaches to ensure the…

Chemical Physics · Physics 2024-11-08 Alexandre de Camargo , Ricky T. Q. Chen , Rodrigo A. Vargas-Hernández

A new algorithm for efficient and fully time-reversible integration of first-principles molecular dynamics based on orbital-free density functional theory (OFDFT) is presented. The algorithm adapts to this nontrivial case the recently…

Statistical Mechanics · Physics 2022-12-21 Alessandro Coretti , Taylor J. Baird , Rodolphe Vuilleumier , Sara Bonella

Determining ground state energies of quantum systems by hybrid classical/quantum methods has emerged as a promising candidate application for near-term quantum computational resources. Short of large-scale fault-tolerant quantum computers,…

Quantum Physics · Physics 2016-10-25 Nicholas C. Rubin

Quantum mechanical methods based on the density functional theory (DFT) offer a realistic possibility of first-principles design of organic donor-acceptor systems and engineered band-gap materials. This promise is contingent upon the…

Chemical Physics · Physics 2013-12-03 Marcin Modrzejewski , Grzegorz Chałasiński , Małgorzata M. Szczęśniak

Here, we report orbital-free density-functional theory (OF DFT) molecular dynamics simulations of the displacement cascade in aluminum. The electronic effect is our main concern. The displacement threshold energies are calculated using OF…

Materials Science · Physics 2017-09-26 Ruizhi Qiu

Density functional theory (DFT) based modeling of electronic excited states is of importance for investigation of the photophysical/photochemical properties and spectroscopic characterization of large systems. The widely used linear…

Chemical Physics · Physics 2021-05-11 Diptarka Hait , Martin Head-Gordon

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…

We present a method to make highly accurate pseudopotentials for use with orbital-free density functional theory (OF-DFT) with given exchange-correlation and kinetic energy functionals, which avoids the compounding of errors of Kohn-Sham…

Materials Science · Physics 2015-02-04 Fleur Legrain , Sergei Manzhos

Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state…

Chemical Physics · Physics 2021-12-15 Kaili Jiang , Xuecheng Shao , Michele Pavanello

In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…

Strongly Correlated Electrons · Physics 2009-11-13 Jeng-Da Chai , John D Weeks

Simulating differential equations on classical computers becomes an intractable problem if the grid size is extremely large. Quantum computers are believed to achieve a possibly exponential speedup in the matrix operation. In this paper, we…

Quantum Physics · Physics 2025-03-18 Xinchi Huang , Hirofumi Nishi , Taichi Kosugi , Yoshifumi Kawada , Yu-ichiro Matsushita

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 propose a nonvariational scheme for geometry optimization of molecules for the first-quantized eigensolver, a recently proposed framework for quantum chemistry using the probabilistic imaginary-time evolution (PITE) on a quantum…

Quantum Physics · Physics 2023-11-06 Taichi Kosugi , Hirofumi Nishi , Yuichiro Matsushita

To date, all proposed quantum algorithms for simulating quantum field theory (QFT) simulate (continuous-time) Hamiltonian lattice QFT as a stepping stone. Two overlooked issues are how large we can take the timestep in these simulations…

Quantum Physics · Physics 2020-07-27 Terry Farrelly , Julien Streich

Orbital-free density functional theory (OF-DFT) constitutes a computationally highly effective tool for modeling electronic structures of systems ranging from room-temperature materials to warm dense matter. Its accuracy critically depends…

Developing reliable pseudopotentials for orbital-free density functional theory (OF-DFT), especially for transition metals, remains a significant challenge. In this study, we provide a theoretical framework for analyzing pseudization…

Finite-temperature orbital-free density functional theory (FT-OFDFT) holds significant promise for simulating warm dense matter due to its favorable scaling with both system size and temperature. However, the lack of the numerically…

Computational Physics · Physics 2024-12-04 Cheng Ma , Min Chen , Yu Xie , Qiang Xu , Wenhui Mi , Yanchao Wang , Yanming Ma

This work presents a new class of hybrid density functional theory (DFT) approximations, incorporating nonlocal exact exchange in predefined states such as core atomic orbitals (AOs). These projected hybrid density functionals are a…

Chemical Physics · Physics 2023-05-16 Benjamin G. Janesko

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

Locality of compact one-electron orbitals expanded strictly in terms of local subsets of basis functions can be exploited in density functional theory (DFT) to achieve linear growth of computation time with systems size, crucial in…

Computational Physics · Physics 2021-10-01 Yifei Shi , Jessica Karaguesian , Rustam Z. Khaliullin