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Recent advances in X-ray free-electron laser diagnostics have enabled direct probing of the electronic structure under extreme pressures and temperatures, such as those encountered in stellar interiors and inertial confinement fusion…

Density-functional theory (DFT) has revolutionized computational prediction of atomic-scale properties from first principles in physics, chemistry and materials science. Continuing development of new methods is necessary for accurate…

We implement and benchmark the frozen core approximation, a technique commonly adopted in electronic structure theory to reduce the computational cost by means of mathematically fixing the chemically inactive core electron states. The…

Materials Science · Physics 2021-06-14 Victor Wen-zhe Yu , Jonathan Moussa , Volker Blum

Density functional theory (DFT) is an incredible success story. The low computational cost, combined with useful (but not yet chemical) accuracy, has made DFT a standard technique in most branches of chemistry and materials science.…

Chemical Physics · Physics 2015-06-03 Kieron Burke

Time-dependent (TD) density functional theory (TDDFT) promises a numerically tractable account of many-body electron dynamics provided good simple approximations are developed for the exchange-correlation (XC) potential functional (XCPF).…

Other Condensed Matter · Physics 2008-08-29 Roi Baer

The general expectation that, in principle, time-dependent density functional theory (TDDFT) be an exact formulation of the time-evolution of an interacting N-electron system is critically reexamined. It is demonstrated that the previous…

Other Condensed Matter · Physics 2007-08-13 J. Schirmer , A. Dreuw

We have formulated and implemented a fully charge-self-consistent density functional theory plus dynamical mean field theory methodology which enables an efficient calculation of the total energy of realistic correlated electron systems.…

Strongly Correlated Electrons · Physics 2015-06-22 Hyowon Park , Andrew J. Millis , Chris A. Marianetti

Despite the variety of available computational approaches, state-of-the-art methods for calculating excitation energies such as time-dependent density functional theory (TDDFT), are computationally demanding and thus limited to moderate…

Chemical Physics · Physics 2022-03-10 Martina Stella , Kritam Thapa , Luigi Genovese , Laura E. Ratcliff

Ensemble density functional theory (EDFT) is a promising alternative to time-dependent density functional theory for computing electronic excitation energies. Using coordinate scaling, we prove several fundamental exact conditions in EDFT…

Strongly Correlated Electrons · Physics 2023-07-04 Thais R. Scott , John Kozlowski , Steven Crisostomo , Aurora Pribram-Jones , Kieron Burke

We introduce a new implementation of time-dependent density-functional theory which allows the \emph{entire} spectrum of a molecule or extended system to be computed with a numerical effort comparable to that of a \emph{single} standard…

Materials Science · Physics 2009-11-13 Dario Rocca , Ralph Gebauer , Yousef Saad , Stefano Baroni

Conceiving a molecule as composed of smaller molecular fragments, or subunits, is one of the pillars of the chemical and physical sciences, and leads to productive methods in quantum chemistry. Using a fragmentation scheme, efficient…

Chemical Physics · Physics 2015-04-14 Martín A. Mosquera , Adam Wasserman

With tens of petaflops supercomputers already in operation and exaflops machines expected to appear within the next 10 years, efficient parallel computational methods are required to take advantage of such extreme-scale machines. In this…

Materials Science · Physics 2012-11-13 Truong Vinh Truong Duy , Taisuke Ozaki

Imaginary-time time-dependent Density functional theory (it-TDDFT) has been proposed as an alternative method for obtaining the ground state within density functional theory (DFT) which avoids some of the difficulties with convergence…

Computational Physics · Physics 2021-11-09 John McFarland , Efstratios Manousakis

Performing high accuracy hybrid functional calculations for condensed matter systems containing a large number of atoms is at present computationally very demanding - when not out of reach - if high quality basis sets are used. We present a…

Materials Science · Physics 2017-12-22 Laura E. Ratcliff , A. Degomme , José A. Flores-Livas , Stefan Goedecker , Luigi Genovese

In this paper, we are interested in the acceleration of numerical simulations. We focus on a hypersonic planetary reentry problem whose simulation involves coupling fluid dynamics and chemical reactions. Simulating chemical reactions takes…

Machine Learning · Statistics 2022-10-03 Paul Novello , Gaël Poëtte , David Lugato , Simon Peluchon , Pietro Marco Congedo

A myriad of phenomena in materials science and chemistry rely on quantum-level simulations of the electronic structure in matter. While moving to larger length and time scales has been a pressing issue for decades, such large-scale…

Motivated by high-accuracy scanning tunneling spectroscopy measurements on disordered two-dimensional electron gases in strong magnetic field, we present an exact solution for the local density of states (LDoS) of electrons moving in an…

Mesoscale and Nanoscale Physics · Physics 2009-10-29 Thierry Champel , Serge Florens

The high cost associated with the evaluation of Hartree-Fock exchange (HFX) makes hybrid functionals computationally challenging for large systems. In this work, we present an efficient way to accelerate HFX calculations with numerical…

Computational Physics · Physics 2020-09-09 Xinming Qin , Jie Liu , Wei Hu , Jinlong Yang

Differentiable programming has facilitated numerous methodological advances in scientific computing. Physics engines supporting automatic differentiation have simpler code, accelerating the development process and reducing the maintenance…

Computational Physics · Physics 2023-04-04 Chuin Wei Tan , Chris J. Pickard , William C. Witt

The exciton binding energy, the energy required to dissociate an excited electron-hole pair into free charge carriers, is one of the key factors to the optoelectronic performance of organic materials. However, it remains unclear whether…

Chemical Physics · Physics 2015-12-08 Jui-Che Lee , Jeng-Da Chai , Shiang-Tai Lin