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Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in…

Materials Science · Physics 2026-03-23 Benjamin X. Shi , Timothy C. Berkelbach

Density Functional Theory (DFT) is widely used for atomistic simulations. However, its reach stays limited due to several limitations such as lack of accurate exchange-correlation functional, requirement of costly O(N 3) diagonalization…

Quantum Physics · Physics 2026-05-18 Namrata Manglani , Samrit Kumar Maity , Shashank Sharma , Soham Phulare , Sanjay Wandhekar

Density functional theory (DFT) can run into serious difficulties with localized states in elements such as transition metals with occupied-d states and oxygen. In contrast, Hartree-Fock (HF) method can be a better approach for such…

Materials Science · Physics 2018-08-01 Hengxin Tan , Yuanchang Li , S. B. Zhang , Wenhui Duan

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

Chemical Physics · Physics 2023-01-02 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

Kohn-Sham density functional theory (DFT) has long struggled with the accurate description of strongly correlated and open shell systems and improvements have been minor even in the newest hybrid functionals. In this Letter we treat the…

Chemical Physics · Physics 2021-04-01 Danny Gibney , Jan-Niklas Boyn , David A. Mazziotti

We decompose the energy error of any variational DFT calculation into a contribution due to the approximate functional and that due to the approximate density. Typically, the functional error dominates, but in many interesting situations,…

Chemical Physics · Physics 2015-06-12 Min-Cheol Kim , Eunji Sim , Kieron Burke

Density-functional Theory (DFT) approaches have recently been used to judge the topological order of various materials despite its well-known band gap underestimation. Use of the more accurate quasi-particle GW approach reveals here few…

Materials Science · Physics 2015-05-27 Julien Vidal , Xiuwen Zhang , Liping Yu , Jun-Wei Luo , Alex Zunger

Approximate density functional theory (DFT) suffers from many-electron self- interaction error, otherwise known as delocalization error, that may be diagnosed and then corrected through elimination of the deviation from exact piecewise…

Materials Science · Physics 2016-11-08 Terry Z. H. Gani , Heather J. Kulik

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

Accurately modeling compounds with partially filled $d$ and $f$ shells remains a hard challenge for density-functional theory, due to large self-interaction errors stemming from local or semi-local exchange-correlation functionals. Hubbard…

Materials Science · Physics 2026-01-19 Kinga Warda , Eric Macke , Iurii Timrov , Lucio Colombi Ciacchi , Piotr M. Kowalski

Detailed physisorption data from experiment for the H_2 molecule on low-index Cu surfaces challenge theory. Recently, density-functional theory (DFT) has been developed to account for nonlocal correlation effects, including van der Waals…

Common density-matrix functionals, the M\"uller and the power functional, have been benchmarked for the half-filled Hubbard dimer, which allows to model the bond dissociation problem and the transition from the weakly to the strongly…

Strongly Correlated Electrons · Physics 2016-03-09 Ebad Kamil , Robert Schade , Thomas Pruschke , Peter E. Blöchl

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

Linear response time dependent density functional theory (TDDFT), which builds upon configuration interaction singles (CIS) and TD-Hartree-Fock (TDHF), is the most widely used class of excited state quantum chemistry methods and is often…

Chemical Physics · Physics 2019-10-14 Diptarka Hait , Adam Rettig , Martin Head-Gordon

We present a Density Functional Theory (DFT) study of the structural and electronic properties of bare rutile VO$_{2}$(110) surfaces and its oxygen-rich terminations. We discuss the performance of various DFT functionals, including PBE,…

Materials Science · Physics 2021-08-31 Jakub Planer , Florian Mittendorfer , Josef Redinger

Self-consistent-field (SCF) approximations formulated using Hartree-Fock (HF) or Kohn-Sham Density Functional Theory (KS-DFT) both have the potential to yield multiple solutions. However, the formal relationship between multiple solutions…

Chemical Physics · Physics 2021-01-06 Rhiannon A. Zarotiadis , Hugh G. A. Burton , Alex J. W. Thom

Unlike covalent two-dimensional (2D) materials like graphene, 2D metals have non-layered structures due to their non-directional, metallic bonding. While experiments on 2D metals are still scarce and challenging, density-functional theory…

Materials Science · Physics 2023-01-06 Kameyab Raza Abidi , Pekka Koskinen

To apply the Hubbard-corrected density-functional theory for predicting some known materials' properties, the Hubbard parameters are usually so tuned that the calculations give results in agreement with some experimental data and then one…

Materials Science · Physics 2023-06-13 Mahmoud Payami , Samira Sheykhi , Mohammad-Reza Basaadat

Double hybrid (DH) density functionals are amongst the most accurate density functional approximations developed so far, largely due to incorporation of correlation effects from unoccupied orbitals via second order perturbation theory…

Chemical Physics · Physics 2018-05-07 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…