Second-generation charge-optimized many-body potential for<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:mtext>Si</mml:mtext><mml:mo>/</mml:mo><mml:msub><mml:mrow><mml:mtext>SiO</mml:mtext></mml:mrow><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:math>and amorphous silica

Shan, Tzu Ray; Devine, Bryce D.; Hawkins, Jeffery M.; Asthagiri, Aravind; Phillpot, Simon R.; Sinnott, Susan B.

doi:10.1103/physrevb.82.235302

Cited by 96 publications

(39 citation statements)

References 29 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In this paper, therefore, we develop a COMB potential that, by design, gives the correct phase order and reasonably well reproduces key properties of both elemental hafnium and hafnia polymorphs. Moreover, the potential is compatible with the previously developed potentials for the Si/ SiO 2 system and amorphous silica, 19 allowing the simulation of HfO 2 / Si interfaces.…”

Section: Introductionmentioning

confidence: 88%

“…A charge-optimized many-body ͑COMB͒ potential, which allows dynamic charge equilibration, has previously been developed for Si/ SiO 2 systems. 18 It has recently been improved and extended to include amorphous silica 19 and well describes the properties and phase order among silicon and silica polymorphs. In this paper, therefore, we develop a COMB potential that, by design, gives the correct phase order and reasonably well reproduces key properties of both elemental hafnium and hafnia polymorphs.…”

Section: Introductionmentioning

confidence: 99%

“…tem, described more fully elsewhere. 19,20 Briefly, the COMB potential formalism is based on the empirical Tersoff potential for silicon. 21,22 The Tersoff potential describes manybody interactions, allows the breaking of existing bonds and the formation of new bonds, and has been successfully applied to study various properties of silicon and diamond.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Charge-optimized many-body potential for the hafnium/hafnium oxide system

et al. 2010

Self Cite

View full text Add to dashboard Cite

A dynamic-charge, many-body potential function is proposed for the hafnium/hafnium oxide system. It is based on an extended Tersoff potential for semiconductors and the charge-optimized many-body potential for silicon oxide. The materials fidelity of the proposed formalism is demonstrated for both hafnium metal and various hafnia polymorphs. In particular, the correct orders of the experimentally observed polymorphs of both the metal and the oxide are obtained. Satisfactory agreement is found for the structural and mechanical properties, defect energetics, and phase stability as compared to first-principles calculations and/or experimental values. The potential can be used in conjunction with the previously determined potentials for the Si and SiO 2 system. This transferability is demonstrated by comparing the structure of a hafnia/silicon interface to that previously determined from electronic-structure calculations.

show abstract

Section: Introductionmentioning

confidence: 88%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Charge-optimized many-body potential for the hafnium/hafnium oxide system

et al. 2010

Self Cite

View full text Add to dashboard Cite

show abstract

“…On the purely empirical side, restricting our discussion to the more transferable methods, Baskes and co-workers have developed the embedded atom method (EAM 65,66 ), which-opposite to ReaxFF-was mainly formulated for metals, yet has since been modified (MEAM 67 ) to treat oxides, hydrides and hydrocarbons. Furthermore, the bondorder concept, as initiated by Abell, 68 Tersoff, 69,70 and Brenner, 71 was further developed into the AIREBO method 72 by Stuart, Tutein and Harrison, as well as into the highly transferable COMB method [73][74][75][76][77] by Sinnott, Philpott, and co-workers. We refer readers to recent reviews for more in-depth comparisons of empirical reactive methods, 73,74 and of simulation methods for large-scale molecular dynamics on reactive systems.…”

Section: Current Reaxff Methodologymentioning

confidence: 99%

The ReaxFF reactive force-field: development, applications and future directions

et al. 2016

View full text Add to dashboard Cite

The reactive force-field (ReaxFF) interatomic potential is a powerful computational tool for exploring, developing and optimizing material properties. Methods based on the principles of quantum mechanics (QM), while offering valuable theoretical guidance at the electronic level, are often too computationally intense for simulations that consider the full dynamic evolution of a system. Alternatively, empirical interatomic potentials that are based on classical principles require significantly fewer computational resources, which enables simulations to better describe dynamic processes over longer timeframes and on larger scales. Such methods, however, typically require a predefined connectivity between atoms, precluding simulations that involve reactive events. The ReaxFF method was developed to help bridge this gap. Approaching the gap from the classical side, ReaxFF casts the empirical interatomic potential within a bond-order formalism, thus implicitly describing chemical bonding without expensive QM calculations. This article provides an overview of the development, application, and future directions of the ReaxFF method. INTRODUCTIONAtomistic-scale computational techniques provide a powerful means for exploring, developing and optimizing promising properties of novel materials. Simulation methods based on quantum mechanics (QM) have grown in popularity over recent decades due to the development of user-friendly software packages making QM level calculations widely accessible. Such availability has proved particularly relevant to material design, where QM frequently serves as a theoretical guide and screening tool. Unfortunately, the computational cost inherent to QM level calculations severely limits simulation scales. This limitation often excludes QM methods from considering the dynamic evolution of a system, thus hampering our theoretical understanding of key factors affecting the overall behaviour of a material. To alleviate this issue, QM structure and energy data are used to train empirical force fields that require significantly fewer computational resources, thereby enabling simulations to better describe dynamic processes. Such empirical methods, including reactive force-field (ReaxFF), 1 trade accuracy for lower computational expense, making it possible to reach simulation scales that are orders of magnitude beyond what is tractable for QM.Atomistic force-field methods utilise empirically determined interatomic potentials to calculate system energy as a function of atomic positions. Classical approximations are well suited for nonreactive interactions, such as angle-strain represented by harmonic potentials, dispersion represented by van der Waals potentials and Coulombic interactions represented by various polarisation schemes. However, such descriptions are inadequate for modelling changes in atom connectivity (i.e., for modelling chemical reactions as bonds break and form). This motivates the

show abstract

“…Reactive force fields are available for barium titanate [30], aluminum oxide [31], and silica [32]. Similarly, charge-optimized many-body potentials have been developed to model Si/SiO 2 and Hf/HfO 2 interfaces [33,34]. However, there remains the need to extend this methodology to the heavy-element compounds that are being considered as candidate ceramic waste forms.…”

Section: Modeling Schemesmentioning

confidence: 99%

Challenges in Modeling the Degradation of Ceramic Waste Forms

Devanathan¹,

Gao²,

X³

2011

View full text Add to dashboard Cite

We identify the state of the art, gaps in current understanding, and key research needs in the area of modeling the long-term degradation of ceramic waste forms for nuclear waste disposition. The directed purpose of this report is to define a roadmap for Waste IPSC needs to extend capabilities of waste degradation to ceramic waste forms, which overlaps with the needs of the subcontinuum scale of FMM (fundamental methods and method) interests. The key knowledge gaps are in the areas of i) methodology for developing reliable interatomic potentials to model the complex atomic-level interactions in waste forms; ii) characterization of water interactions at ceramic surfaces and interfaces; and iii) extension of atomic-level insights to the long time and distance scales relevant to the problem of actinide and fission product immobilization.

show abstract

Second-generation charge-optimized many-body potential forSi/SiO2and amorphous silica

Cited by 96 publications

References 29 publications

Charge-optimized many-body potential for the hafnium/hafnium oxide system

Charge-optimized many-body potential for the hafnium/hafnium oxide system

The ReaxFF reactive force-field: development, applications and future directions

Challenges in Modeling the Degradation of Ceramic Waste Forms

Contact Info

Product

Resources

About