In Pursuit of the "Divine" Functional

Mattsson, Ann E.

doi:10.1126/science.1077710

Cited by 141 publications

(137 citation statements)

References 11 publications

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“…11,12 In situ electrochemical probes, operating under reaction or near reaction conditions, reveal the energetics, kinetics, and intermediates of the reaction pathway and their relation to the surface structure and composition of the reactants and catalysts. These powerful new experimental probes, combined with equally powerful and impressive computational quantum chemistry using density functional theory, 13 …”

Section: Realizing the Promisementioning

confidence: 99%

The Hydrogen Economy

2004

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Section: Realizing the Promisementioning

confidence: 99%

The Hydrogen Economy

2004

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“…The performance of the SVWN functional suggests that, for the singlet excited states within the benchmark set of the current study, climbing up Jacob's ladder in the ground state may not necessarily correspond to an improved performance in the excited state. 28 For triplet excited states, the B3LYP (MAE = 0.31 eV), X3LYP (MAE = 0.31 eV), and PBE0 (MAE = 0.32 eV) functionals offer the best performance among LDA, GGAs, and GH-GGAs. Among mGGAs and GH-mGGAs, the M06-2X functional (MAE = 0.24 eV) demonstrates the best performance for triplet excited states while the PKZB (MAE = 0.57 eV) functional is the worst.…”

Section: A Performance For Singlet and Triplet Excited Statesmentioning

confidence: 99%

“…26 Furthermore, with the aid of automatic code generators, 27 these sophisticated density functionals can be integrated into excited-state TDDFT codes. However, it is unclear if the progression towards more sophisticated density functionals (climbing up Jacob's ladder 28 ) in the ground state necessarily correlates with an improved description in the excited state.…”

Section: Introductionmentioning

confidence: 99%

Benchmarking the performance of time-dependent density functional methods

Leang

Zahariev

Gordon

2012

The Journal of Chemical Physics

310

319

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The performance of 24 density functionals, including 14 meta-generalized gradient approximation (mGGA) functionals, is assessed for the calculation of vertical excitation energies against an experimental benchmark set comprising 14 small-to medium-sized compounds with 101 total excited states. The experimental benchmark set consists of singlet, triplet, valence, and Rydbergexcited states. The global-hybrid (GH) version of the Perdew-Burke-Ernzerhoff GGA density functional (PBE0) is found to offer the best overall performance with a mean absolute error (MAE) of 0. The performance of 24 density functionals, including 14 meta-generalized gradient approximation (mGGA) functionals, is assessed for the calculation of vertical excitation energies against an experimental benchmark set comprising 14 small-to medium-sized compounds with 101 total excited states. The experimental benchmark set consists of singlet, triplet, valence, and Rydberg excited states. The global-hybrid (GH) version of the Perdew-Burke-Ernzerhoff GGA density functional (PBE0) is found to offer the best overall performance with a mean absolute error (MAE) of 0.28 eV. The GH-mGGA Minnesota 2006 density functional with 54% Hartree-Fock exchange (M06-2X) gives a lower MAE of 0.26 eV, but this functional encounters some convergence problems in the ground state. The local density approximation functional consisting of the Slater exchange and Volk-Wilk-Nusair correlation functional (SVWN) outperformed all non-GH GGAs tested. The best pure density functional performance is obtained with the local version of the Minnesota 2006 mGGA density functional (M06-L) with an MAE of 0.41 eV.

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“…More accurate modeling the non-local aspects of the exchange operator, through the inclusion of higher order Taylor expansions of the electron density, also known as Jacob's Ladder [87] [131], has lead to the development of modern density functionals . Local density functionals involve only the electron density, while a GGA functional uses both the electron density and the gradient of the electron density.…”

Section: The Kohn-sham Approach To Dftmentioning

confidence: 99%

Spectroscopy and Kinetics of U02 Fuel Oxidation Hydrolysis and Radiolysis: Applications to Radioactive Waste Management

Burggraf¹,

Beck²

2007

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An accurate and efficient hybrid Density Functional Theory (DFT) and Multireference Configuration Interaction (MRCI) model for computing electronic excitation energies in atoms and molecules was developed. The utility of a hybrid method becomes apparent when ground and excited states of large molecules, clusters of molecules, or even moderately sized molecules containing heavy element atoms are desired. In the case of large systems of lighter elements, the hybrid method brings to bear the numerical efficiency of the DFT method in computing the electron-electron dynamic correlation, while including non-dynamical electronic correlation via the Con- v After the scaling parameters were determined using the training suite of atoms and molecules, the method was applied to carbon monoxide, boron fluoride, the bromine atom, the uranium 5+ and 4+ ions, and the uranyl (UO 2+ 2 ) ion. In all cases, the correct ordering of ground and excited states was obtained using the DFT/MRCI model. In CO, a reduction in overall error of 26% with respect to Time Dependent Density Functional Theory (TDDFT) was observed over 6 ground and excited states.A reduction in overall error of 42% with respect to TDDFT was observed in 5 ground and excited states of BF, while an accuracy with respect to experiment of 11-22% for electronic excitation energies for the first excited states of the bromine atom and uranium 5+ and 4+ ions was observed.

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In Pursuit of the "Divine" Functional

Cited by 141 publications

References 11 publications

The Hydrogen Economy

The Hydrogen Economy

Benchmarking the performance of time-dependent density functional methods

Spectroscopy and Kinetics of U02 Fuel Oxidation Hydrolysis and Radiolysis: Applications to Radioactive Waste Management

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