Analytic atomic gradients in the fermi‐löwdin orbital self‐interaction correction

Trepte, Kai; Schwalbe, Sebastian; Hahn, Torsten; Kortus, Jens; Kao, Der-you; Yamamoto, Yoh; Baruah, Tunna; Zope, Rajendra R.; Withanage, Kushantha; Peralta, Juan E.; Jackson, Koblar Alan

doi:10.1002/jcc.25767

Cited by 21 publications

(13 citation statements)

References 33 publications

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“…This decrease in thermochemical error when applying SIC to LDA is in good agreement with previous reports on the subject. [16,47,49,50,127,128,130,131] The fact that SCAN performs better than LDA-FLO-SIC for atomization energies has also been noted before. [49]…”

Section: Gas Phasesupporting

confidence: 70%

“…[123] Furthermore, FLO-SIC and RSIC overbind and deliver very similar Δ f ,g H M ð298.15 KÞ, with a difference of only 3 kcal mol À1 . Both the overbinding tendency of FLO-SIC [47,49,128] and RSIC [47,127] as well as the close agreement between the two SIC approaches for standard enthalpies of formation [47] have been detailed in previous studies. The MAEs of both SIC methods are smaller than the MAE of LDA by about 50 kcal mol À1 .…”

Section: Gas Phasementioning

confidence: 70%

“…This LDA result is in agreement with the literature because the atomization energy D 0 enters the calculation of the standard enthalpy of formation with a negative sign in Equation ( 14), and LDA is known for its overestimation of D 0 , i.e., it is known to overbind. [49,[124][125][126][127][128] In contrast to the HF and LDA results, both SCAN and CCSD(T), whose MAEs are equal to 3 kcal mol À1 , hardly deviate from experiment at all and therefore come close to the chemical accuracy of 1 kcal mol À1 . The SCAN results are supported by earlier studies that demonstrated its improved prediction of atomization energies when compared with LDA [49,50,127,129] .…”

Section: Gas Phasementioning

confidence: 79%

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Testing Self‐Interaction Correction for Molecules in Solution

et al. 2021

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Two measures of reactivity, the ionization potential and the standard enthalpy of formation, are evaluated for the AQUA20 molecular test set in this theoretical study, comparing results from density functional theory, wavefunction approaches, and methods from the field of self-interaction correction. All calculations are carried out for the gas phase and for an aqueous solution as simulated with the conductor-like screening model. For the gas phase, previously reported tendencies are confirmed. With the presented computational approach for the aqueous solution, the application of self-interaction correction improves the standard enthalpies of formation, but not the ionization potentials.

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Section: Gas Phasesupporting

confidence: 70%

Section: Gas Phasementioning

confidence: 70%

Section: Gas Phasementioning

confidence: 79%

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Testing Self‐Interaction Correction for Molecules in Solution

et al. 2021

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“…More recently, Pederson et al . showed that unitarily invariant Fermi‐Löwdin orbitals proposed by Luken can be used to perform self‐consistent SIC calculations within the Fermi‐Löwdin orbital self‐interaction correction (FLO‐SIC) method.…”

Section: Introductionmentioning

confidence: 99%

Interpretation and Automatic Generation of Fermi‐Orbital Descriptors

et al. 2019

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We present an interpretation of Fermi‐orbital descriptors (FODs) and argue that these descriptors carry chemical bonding information. We show that a bond order derived from these FODs agrees well with reference values, and highlight that optimized FOD positions used within the Fermi‐Löwdin orbital self‐interaction correction (FLO‐SIC) method correspond to expectations from Linnett's double‐quartet theory, which is an extension of Lewis theory. This observation is independent of the underlying exchange‐correlation functional, which is shown using the local spin density approximation, the Perdew–Burke–Ernzerhof generalized gradient approximation (GGA), and the strongly constrained and appropriately normed meta‐GGA. To make FOD positions generally accessible, we propose and discuss four independent methods for the generation of Fermi‐orbital descriptors, their implementation as well as their advantages and drawbacks. In particular, we introduce a re‐implementation of the electron force field, an approach based on the centers of mass of orbital densities, a Monte Carlo‐based algorithm, and a method based on Lewis‐like bonding information. All results are summarized with respect to future developments of FLO‐SIC and related methods. © 2019 The Authors. Journal of Computational Chemistry published by Wiley Periodicals, Inc.

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“…The Fermi-Löwdin Orbital Self-Interaction Corrected DFT (FLOSIC-DFT) is viewed as a further step in developing methods for more universal treatment of unphysical SIE in DFT [43]. The main difference with respect to former SIE-corrected versions relies on how energy-minimizing orbitals are variably obtained, towards SIE-free properties, with the present variant offering computational advantages and with analytical gradients also available [44].…”

Section: Summary Of Some Emerging Dft Methodsmentioning

confidence: 99%

Emerging DFT Methods and Their Importance for Challenging Molecular Systems with Orbital Degeneracy

Maroto

Sancho‐García

2019

Computation

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We briefly present some of the most modern and outstanding non-conventional density-functional theory (DFT) methods, which have largely broadened the field of applications with respect to more traditional calculations. The results of these ongoing efforts reveal that a DFT-inspired solution always exists even for pathological cases. Among the set of emerging methods, we specifically mention FT-DFT, OO-DFT, RSX-DFT, MC-PDFT, and FLOSIC-DFT, complementing the last generation of existing density functionals, such as local hybrid and double-hybrid expressions.

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Analytic atomic gradients in the fermi‐löwdin orbital self‐interaction correction

Cited by 21 publications

References 33 publications

Testing Self‐Interaction Correction for Molecules in Solution

Testing Self‐Interaction Correction for Molecules in Solution

Interpretation and Automatic Generation of Fermi‐Orbital Descriptors

Emerging DFT Methods and Their Importance for Challenging Molecular Systems with Orbital Degeneracy

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