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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…

Machine-learned potentials (MLPs) trained on ab initio data combine the computational efficiency of classical interatomic potentials with the accuracy and generality of the first-principles method used in the creation of the respective…

Chemical Physics · Physics 2024-08-07 Leonid Kahle , Benoit Minisini , Tai Bui , Jeremy T. First , Corneliu Buda , Thomas Goldman , Erich Wimmer

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

Molecules can form myriad crystalline polymorphs, each with distinct properties affecting their performance across diverse applications, from pharmaceuticals to functional materials and more. Predicting the thermodynamically most stable…

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

The nuclear time-dependent density functional theory (TDDFT) is a tool of choice for describing various dynamical phenomena in atomic nuclei. In a recent study, we reported an extension of the framework - the multiconfigurational TDDFT…

Nuclear Theory · Physics 2024-01-24 Petar Marević , David Regnier , Denis Lacroix

Electronic circular dichroism (ECD) is a powerful spectroscopical method for investigating chiral properties at the molecular level. ECD calculations with the commonly used linear-response time-dependent density functional theory (LR-TDDFT)…

State-specific orbital optimized approaches are more accurate at predicting core-level spectra than traditional linear-response protocols, but their utility had been restricted on account of the risk of `variational collapse' down to the…

Thomson scattering (TS) diagnostics provide reliable, minimally perturbative measurements of fundamental plasma parameters, such as electron density ($n_e$) and electron temperature ($T_e$). Deep neural networks can provide accurate…

Understanding the properties of warm dense hydrogen is of key importance for the modeling of compact astrophysical objects and to understand and further optimize inertial confinement fusion (ICF) applications. The work horse of warm dense…

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

We present an automated procedure for computing stacking fault energies in random alloys from large-scale simulations using moment tensor potentials (MTPs) with the accuracy of density functional theory (DFT). To that end, we develop an…

Materials Science · Physics 2021-11-23 Max Hodapp , Alexander Shapeev

Developing fast and accurate methods to discover intermetallic compounds is relevant for alloy design. While density-functional-theory (DFT)-based methods have accelerated design of binary and ternary alloys by providing rapid access to the…

Materials Science · Physics 2020-09-09 Zhaohan Zhang , Mu Li , Katharine Flores , Rohan Mishra

Density functional theory (DFT) serves as the basis for computational discovery in materials science and chemistry, yet each calculation demands extensive human effort: adjusting algorithms when convergence stalls, revising plans when…

Materials Science · Physics 2026-05-27 Penghui Yang , Zhonghan Zhang , Yue Li , Xinrun Wag , Yanchen Deng , Yuhao Lu , Bijun Tang , Zheng Liu , Bo An

We present a solution of the full TDDFT eigenvalue equation in the linear response formalism exhibiting a linear-scaling computational complexity with system size, without relying on the simplifying Tamm-Dancoff approximation (TDA). The…

Computational Physics · Physics 2016-01-20 Tim J. Zuehlsdorff , Nicholas D. M. Hine , Mike C. Payne , Peter D. Haynes

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

We show that a lattice formulation of density-functional theory (DFT), guided by renormalization-group concepts, can be used to obtain numerical predictions of energy gaps, spin-density profiles, critical exponents, sound velocities,…

Strongly Correlated Electrons · Physics 2009-11-13 Francisco C. Alcaraz , Klaus Capelle

The adiabatic approximation in time-dependent density functional theory (TDDFT) yields reliable excitation spectra with great efficiency in many cases, but fundamentally fails for states of double excitation character. We discuss how…

Chemical Physics · Physics 2015-05-27 Peter Elliott , Sharma Goldson , Chris Canahui , Neepa T. Maitra

A method for the calculation of the damping rate due to electron-hole pair excitation for atomic and molecular motion at metal surfaces is presented. The theoretical basis is provided by Time Dependent Density Functional Theory (TDDFT) in…

Computational Physics · Physics 2015-05-14 J. R. Trail , M. C. Graham , D. M. Bird

To further develop accurate and large-scale simulations of electrochemical interfaces, we propose a unified explicit electric potential framework to simultaneously predict atomic forces and electron density distributions. The framework…

Chemical Physics · Physics 2026-04-14 Jingwen Zhou , Yawen Yu , Xuwei Liu , Chungen Liu