Automated generation of highly accurate, efficient and transferable pseudopotentials

Hansel, Rachael A.; Brock, Casey N.; Paikoff, Brandon C.; Tackett, Alan; Walker, D. G.

doi:10.1016/j.cpc.2015.06.014

Cited by 12 publications

(6 citation statements)

References 23 publications

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“…In this paper, electronic cross-correlation was described with a GGA-PBE , functional theory in the CASTEP program . Using ultrasoft pseudopotential (USPP) to illustrate the interaction between ion real and valence electrons, Broyden–Fletcher–Goldfarb–Shanno (BFGS) served as the geometric optimization . Cutoff energy was set as 450 eV.…”

Section: Methodsmentioning

confidence: 99%

Adsorption Mechanism of PbO/PbCl₂ on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory

Jiefei

Zhong

et al. 2020

Energy Fuels

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In the field of heavy-metal emission control during coal combustion, kaolinite can be used as an additive in furnaces to effectively capture semivolatile heavy-metal elements. To investigate the microscopic mechanism of the interaction between PbO/PbCl2 and kaolinite/metakaolin, quantum chemistry computations were utilized to examine the interaction among the frontier orbitals during the adsorption process and the active variation occurring during the thermal conversion of kaolinite. The calculations indicate that metakaolin possesses a stronger adsorption activity than that of kaolinite. The lowest unoccupied molecular orbital (LUMO) of kaolinite (DeOH 001) and the highest occupied molecular orbital (HOMO) of PbO/PbCl2 effortlessly interact in the adsorption process. PbO is more conveniently adsorbed on the surface of kaolinite (DeOH 001) than PbCl2. During the dehydroxylation of kaolinite, the active sites of adsorption move to the vicinity of V/IV-coordinated Al, which is favorable for the adsorption of PbO/PbCl2. Nevertheless, III-coordinated Al in metakaolin and the thermal decomposition products (mullite and cristobalite) lowers the adsorption activity. During the adsorption process, PbO/PbCl2 and the surface of kaolinite (DeOH 001) form stable bonding orbitals and unstable antibonding orbitals, respectively. In addition, charge transfer mainly takes place in the p orbitals. We expect that the results can provide effective guidance and theoretical support for the emission control of the heavy metals PbO/PbCl2 by kaolinite during coal combustion and the modification of kaolinite additives in high-temperature furnaces.

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Section: Methodsmentioning

confidence: 99%

Adsorption Mechanism of PbO/PbCl₂ on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory

Jiefei

Zhong

et al. 2020

Energy Fuels

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“…As DAKOTA was intended to be used together with a separate application, it considers the simulation code as a ''black box''. There exist many cases in literature where DAKOTA has been coupled with different simulation software for this purpose [37][38][39]. OptiSMOKE++ was written in C++ which allows for a direct and fast communication between DAKOTA and OpenSMOKE++.…”

Section: Dakota (Design Analysis Kit For Optimization and Terascalementioning

confidence: 99%

OptiSMOKE++: A toolbox for optimization of chemical kinetic mechanisms

Fürst

Bertolino

Cuoci

et al. 2021

Computer Physics Communications

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As detailed chemical mechanisms are becoming viable for large scale simulations, knowledge and control of the uncertainty correlated to the kinetic parameters are becoming crucial to ensure accurate numerical predictions. A flexible toolbox for the optimization of chemical kinetics has therefore been developed in this work. The toolbox is able to use different optimization methodologies, as well as it can handle a large amount of uncertain parameters simultaneously. It can also handle experimental targets from different sources: Batch reactors, Plug Flow Reactors, Perfectly Stirred Reactors, Rapid Compression Machines and Laminar Flame Speeds. This work presents the different features of this toolbox together with five different test cases which exemplifies these features.

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“…The design of transferable NCPPs is essential for accurate DFT calculations. Traditionally, pseudopotential design has involved hand-picking parameters; however, optimization algorithms have recently been used to automate the selection of parameters for nonlocal pseudopotentials [9][10][11][12] . In this paper we revisit the designed-nonlocal (DNL) pseudopotential approach, in which the local potential of a separable norm-conserving pseudopotential is modified by adding an augmentation function in order to improve transferability 13 .…”

Section: Introductionmentioning

confidence: 99%

“…We consider augmentation functions in the form of a sum of cosine functions, and use a conjugate gradient algorithm to select the coefficients in the sum that minimize transferability errors for the isolated atom. Some recent work on the use of optimization algorithms to design pseudopotentials has involved selecting parameters (such as core radii and kinetic energy truncation cutoff) that optimize the accuracy of solid-state properties [9][10][11][12] . Here, we take the different approach of optimizing transferability in the isolated atom only, and we show that this leads to dramatic improvements in the accuracy of solid-state properties.…”

Section: Introductionmentioning

confidence: 99%

Automated selection of the local potential for transferable pseudopotentials

Barkan,

Rappe

2018

Preprint

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We develop an automated procedure to select the local potential of a separable pseudopotential that minimizes transferability errors for the isolated atom, and we show that this optimization leads to significant improvements in the accuracy of predicted solid-state properties. We present pseudopotentials for Y, In, and Sn. For these pseudopotentials, our method reduces solid-state errors by 88% on average, as measured by the ∆-factor test. These pseudopotentials are constructed in the Kleinman-Bylander form; however, our method is applicable to all separable pseudopotentials, such as ONCV pseudopotentials. We perform plane-wave convergence tests according to SSSP standards and show that the modifications to the local potential leave plane-wave convergence unchanged.

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Automated generation of highly accurate, efficient and transferable pseudopotentials

Cited by 12 publications

References 23 publications

Adsorption Mechanism of PbO/PbCl₂ on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory

Adsorption Mechanism of PbO/PbCl₂ on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory

OptiSMOKE++: A toolbox for optimization of chemical kinetic mechanisms

Automated selection of the local potential for transferable pseudopotentials

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Automated generation of highly accurate, efficient and transferable pseudopotentials

Cited by 12 publications

References 23 publications

Adsorption Mechanism of PbO/PbCl2 on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory

Adsorption Mechanism of PbO/PbCl2 on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory

OptiSMOKE++: A toolbox for optimization of chemical kinetic mechanisms

Automated selection of the local potential for transferable pseudopotentials

Contact Info

Product

Resources

About

Adsorption Mechanism of PbO/PbCl₂ on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory

Adsorption Mechanism of PbO/PbCl₂ on Kaolinite Surfaces during Coal Combustion Based on Frontier Orbital Theory