Long-Range Corrected Hybrid Density Functionals with Improved Dispersion Corrections

Lin, Yousheng; Li, Guan-De; Mao, Shan-Ping; Chai, Jeng-Da

doi:10.1021/ct300715s

Cited by 617 publications

(516 citation statements)

References 96 publications

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“…Nonetheless, as SCAN and PBE are both semilocal functionals, they cannot adequately describe the van der Waals (vdW) asymptote [10,15], which requires an accurate treatment of long-range dynamical correlation effects. Incorporating SCAN and PBE with the double-hybrid schemes [38][39][40][41][42][43][44][45][46][47][48][49][50][51][52][53][54][55], the DFT-D (KS-DFT with empirical dispersion corrections) schemes [44,[82][83][84][85][86][87][88], or fully nonlocal density functionals [89][90][91] may greatly improve the accuracy of SCAN and PBE for vdW interactions. Among the functionals examined on the S22 and S66 sets, SCAN0-2 ranks first, while SCAN-QIDH and PBE0-2 rank second and third, respectively.…”

Section: Resultsmentioning

confidence: 99%

SCAN-based hybrid and double-hybrid density functionals from models without fitted parameters

Hui

Chai

2016

The Journal of Chemical Physics

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By incorporating the nonempirical SCAN semilocal density functional [Sun, Ruzsinszky, and Perdew, Phys. Rev. Lett. 115, 036402 (2015)] in the underlying expression of four existing hybrid and double-hybrid models, we propose one hybrid (SCAN0) and three double-hybrid (SCAN0-DH, SCAN-QIDH, and SCAN0-2) density functionals, which are free from any fitted parameters. The SCAN-based double-hybrid functionals consistently outperform their parent SCAN semilocal functional for self-interaction problems and noncovalent interactions. In particular, SCAN0-2, which includes about 79% of Hartree-Fock exchange and 50% of second-order Møller-Plesset correlation, is shown to be reliably accurate for a very diverse range of applications, such as thermochemistry, kinetics, noncovalent interactions, and self-interaction problems.

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Section: Resultsmentioning

confidence: 99%

SCAN-based hybrid and double-hybrid density functionals from models without fitted parameters

Hui

Chai

2016

The Journal of Chemical Physics

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147

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“…Hybrid functionals, however, do not account for the long range part of the correlation hole energy and thus cannot reproduce dispersion forces. Effective ways to correct for these drawbacks have been proposed by several authors (Chai and Head-Gordon, 2008;Lin et al, 2013;Mardirossian and Head-Gordon, 2014). …”

Section: Density Functional Theorymentioning

confidence: 99%

Simulation and understanding of atomic and molecular quantum crystals

2017

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Quantum crystals abound in the whole range of solid-state species. Below a certain threshold temperature the physical behavior of rare gases ( 4 He and Ne), molecular solids (H 2 and CH 4 ), and some ionic (LiH), covalent (graphite), and metallic (Li) crystals can be only explained in terms of quantum nuclear effects (QNE). A detailed comprehension of the nature of quantum solids is critical for achieving progress in a number of fundamental and applied scientific fields like, for instance, planetary sciences, hydrogen storage, nuclear energy, quantum computing, and nanoelectronics. This review describes the current physical understanding of quantum crystals formed by atoms and small molecules, as well as the wide palette of simulation techniques that are used to investigate them. Relevant aspects in these materials such as phase transformations, structural properties, elasticity, crystalline defects and the effects of reduced dimensionality, are discussed thoroughly. An introduction to quantum Monte Carlo techniques, which in the present context are the simulation methods of choice, and other quantum simulation approaches (e. g., path-integral molecular dynamics and quantum thermal baths) is provided. The overarching objective of this article is twofold. First, to clarify in which crystals and physical situations the disregard of QNE may incur in important bias and erroneous interpretations. And second, to promote the study and appreciation of QNE, a topic that traditionally has been treated in the context of condensed matter physics, within the broad and interdisciplinary areas of materials science.

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“…As a result, it is not surprising that at least 15 B97-based density functionals have been parameterized since 1997. These include local functionals [5][6][7][8] (HCTH/93, HCTH/120, HCTH/147, HCTH/407, B97-D), global hybrid functionals 1,5,9,10 (B97, B97-1, B97-2, B97-3), range-separated hybrid functionals [11][12][13][14] (ωB97, ωB97X, ωB97X-D, ωB97X-D3, ωB97X-V), and even double hybrid functionals 15 (ωB97X-2).…”

Section: Introductionmentioning

confidence: 99%

Exploring the limit of accuracy for density functionals based on the generalized gradient approximation: Local, global hybrid, and range-separated hybrid functionals with and without dispersion corrections

Mardirossian

Head‐Gordon

2014

The Journal of Chemical Physics

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The limit of accuracy for semi-empirical generalized gradient approximation (GGA) density functionals is explored by parameterizing a variety of local, global hybrid (GH), and range-separated hybrid (RSH) functionals. The training methodology employed differs from conventional approaches in 2 main ways: 1). Instead of uniformly truncating the exchange, same-spin correlation, and opposite-spin correlation functional inhomogeneity correction factors, all possible fits up to fourth order are considered, and 2). Instead of selecting the optimal functionals based solely on their training set performance, the fits are validated on an independent test set and ranked based on their overall performance on the training and test sets. The 3 different methods of accounting for exchange are trained both with and without dispersion corrections (DFT-D2 and VV10), resulting in a total of 491508 candidate functionals. For each of the 9 functional classes considered, the results illustrate the trade-off between improved training set performance and diminished transferability. Since all 491508 functionals are uniformly trained and tested, this methodology allows the relative strengths of each type of functional to be consistently compared and contrasted. The range- * To whom correspondence should be addressed separated hybrid GGA functional paired with the VV10 nonlocal correlation functional emerges as the most accurate form for the present training and test sets, which span thermochemical energy differences, reaction barriers, and intermolecular interactions involving lighter main group elements.

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Long-Range Corrected Hybrid Density Functionals with Improved Dispersion Corrections

Cited by 617 publications

References 96 publications

SCAN-based hybrid and double-hybrid density functionals from models without fitted parameters

SCAN-based hybrid and double-hybrid density functionals from models without fitted parameters

Simulation and understanding of atomic and molecular quantum crystals

Exploring the limit of accuracy for density functionals based on the generalized gradient approximation: Local, global hybrid, and range-separated hybrid functionals with and without dispersion corrections

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