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Polarons are widespread in functional materials and are key to device performance in several technological applications. However, their effective impact on material behavior remains elusive, as condensed matter studies struggle to capture…

We present a differentiation framework for plane-wave density-functional theory (DFT) that combines the strengths of forward-mode algorithmic differentiation (AD) and density-functional perturbation theory (DFPT). In the resulting AD-DFPT…

Materials Science · Physics 2025-12-23 Niklas Frederik Schmitz , Bruno Ploumhans , Michael F. Herbst

Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…

Chemical Physics · Physics 2020-04-16 Christopher J. Stein , Markus Reiher

We derive and validate a quantitative analytical model of the near-field electrostatic effects in the vicinity (>=3\AA) of two-dimensional (2D) materials. In solving the Poisson equation of a near-planar point charge ansatz for the…

Materials Science · Physics 2022-05-11 Qunfei Zhou , Michele Kotiuga , Pierre Darancet

We present a first-principles framework to extract deformation potentials in Silicon based on density-functional theory (DFT) and density-functional perturbation theory (DFPT). We compute the electronic band structures, phonon dispersion…

Materials Science · Physics 2021-11-05 Zhen Li , Patrizio Graziosi , Neophytos Neophytou

Understanding strongly correlated systems is essential for advancing quantum chemistry and materials science, yet conventional methods like Density Functional Theory (DFT) often fail to capture their complex electronic behavior. To address…

Chemical Physics · Physics 2025-09-01 Archith Rayabharam , N. R. Aluru

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein

We describe a scheme for efficient large-scale electronic-structure calculations based on the combination of the pole expansion and selected inversion (PEXSI) technique with the SIESTA method, which uses numerical atomic orbitals within the…

Computational Physics · Physics 2015-06-19 Lin Lin , Alberto García , Georg Huhs , Chao Yang

Site density functional theory (SDFT) provides a rigorous framework for statistical mechanics analysis of inhomogeneous molecular liquids. The key defining feature of these systems is the presence of two very distinct interactions scales…

Statistical Mechanics · Physics 2020-11-24 Gennady N. Chuev , Marina V. Fedotova , Marat Valiev

Time-dependent density-functional theory (TDDFT) is deemed to be a formally rigorous way of dealing with the time-evolution of a many-electron system at the level of electron densities rather than the underlying wavefunctions, which in turn…

Chemical Physics · Physics 2024-11-26 Jochen Schirmer

The systematic underestimation of band gaps is one of the most fundamental challenges in semilocal density functional theory (DFT). In addition to hindering the application of DFT to predicting electronic properties, the band gap problem is…

Chemical Physics · Physics 2024-08-27 Kyle Bystrom , Stefano Falletta , Boris Kozinsky

A framework for developing new approximate electronic structure methods is presented, in which the correlation energy of a many-electron system in the ground state is computed as in the single-reference second-order many-body perturbation…

Chemical Physics · Physics 2011-06-15 Dimitri Laikov

One of the most important open challenges in modern Kohn-Sham (KS) density-functional theory (DFT) is the correct treatment of fractional electron charges and spins. Approximate exchange-correlation (XC) functionals struggle to do this in a…

Chemical Physics · Physics 2015-12-24 Jonathan Nafziger , Adam Wasserman

Over this past decade, we combined the idea of stochastic resolution of identity with a variety of electronic structure methods. In our stochastic Kohn-Sham DFT method, the density is an average over multiple stochastic samples, with…

Chemical Physics · Physics 2020-01-08 Wenfei Li , Ming Chen , Eran Rabani , Roi Baer , Daniel Neuhauser

The electronic energy structures and magnetic properties of iron-based compounds with group VI elements (FeTe, BiFeO$_3$, SrFe$_{12}$O$_{19}$ and SrCoTiFe$_{10}$O$_{19}$) are studied using the density functional theory (DFT) methods.…

Materials Science · Physics 2015-10-05 G. E. Grechnev , A. A. Lyogenkaya , O. V. Kotlyar , A. S. Panfilov , V. P. Gnezdilov

Self-consistent phonon (SCP) theory and its application in computing thermodynamic properties of materials are reviewed from a historical perspective. Various more recent implementations based on first-principles electronic structure…

Materials Science · Physics 2019-11-05 Keivan Esfarjani , Yuan Liang

Density-functional perturbation theory (DFPT) is nowadays the method of choice for the accurate computation of linear and non-linear response properties of materials from first principles. A notable advantage of DFPT over alternative…

Materials Science · Physics 2019-06-19 Miquel Royo , Massimiliano Stengel

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

Accurate treatment of the electronic correlation in inhomogeneous electronic systems, combined with the ability to capture the correlation energy of the homogeneous electron gas, allows to reach high predictive power in the application of…

Strongly Correlated Electrons · Physics 2010-06-22 E. Rasanen , S. Pittalis , C. R. Proetto

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…

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