Bayesian automated weighting of aggregated DFT, MD, and experimental data for candidate thermodynamic models of aluminum with uncertainty quantification

Gabriel, Joshua J.; Paulson, Noah H.; Duong, Thien; Becker, Chandler A.; Tavazza, Francesca; Kattner, Ursula R.; Stan, Marius

doi:10.1016/j.mtla.2021.101216

Cited by 5 publications

(3 citation statements)

References 56 publications

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“…43 Relaxation was carried out on the unit cell until the forces acting on the atoms were less than 0.01 eV/Å. 44,45 The low-index surfaces were obtained from optimized bulk unit cells of β-C 2 S and M3-C 3 S, and in-plane crystal periodicity was preserved in the process. Stoichiometry and neutrality were maintained on all surfaces, effectively avoiding polarized electric fields.…”

Section: Methodsmentioning

confidence: 99%

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Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

et al. 2022

J Am Ceram Soc

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The differences in hydration between β-C 2 S and M3-C 3 S, the main phases of silicate cement, have not been fully investigated. In this study, density functional theory calculations were used to investigate the structure and bond order of β-C 2 S and M3-C 3 S before and after the molecular and dissociative adsorption of single water atoms. The unit cell of M3-C 3 S was found to have some O atoms with lower bond orders than those in β-C 2 S, implying higher chemical reactivity of O atoms in M3-C 3 S. The total bond orders of water atoms generally decreased after molecular adsorption, but reductions were minimal, and there were even increases, when the hydrogen bonding among H and surface O atoms was very weak in several M3-C 3 S surfaces. In the case of dissociative adsorption, the bond orders of water O-H hydroxyl tended to increase, and the other bond orders among water atoms decreased sharply, even to zero in some cases. Moreover, the bond order variations of water atoms of β-C 2 S and M3-C 3 S in molecular adsorption were highly correlated with the adsorption energy, with correlation coefficients of 0.9070 and 0.8330, respectively. In both molecular and dissociative adsorption of β-C 2 S and M3-C 3 S, the total bond order among Ca atoms with other surface atoms decreased after the Ca atoms adsorbed water atoms. This phenomenon also appeared in the dissociative adsorption of surface O atoms. In M3-C 3 S, the total strength of the surface O atom bonded to other surface atoms after dissociative adsorption was similar to the strength of the surface O-H hydroxyl bond. The special O atoms in M3-C 3 S showed a clear layered arrangement on the surfaces.

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Section: Methodsmentioning

confidence: 99%

“…After the full convergence test, the energy cutoff chosen for the calculation was 600 eV, and the energy tolerance was 1.0 × 10 −5 eV per atom 43 . Relaxation was carried out on the unit cell until the forces acting on the atoms were less than 0.01 eV/Å 44,45 …”

Section: Methodsmentioning

confidence: 99%

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

et al. 2022

J Am Ceram Soc

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“…Frequently, the correlation of the fit parameters is missing too. However, uncertainty estimation is now the focus of recently published papers, e.g., in [14], where experimental data and atomistic experiments are included in the model development. In general, thermodynamic modeling relies on the significance of the experimental data, their availability and on the adequacy of the model functions.…”

Section: Introductionmentioning

confidence: 99%

Extended Regression Analysis for Debye–Einstein Models Describing Low Temperature Heat Capacity Data of Solids

Gamsjäger,

Wiessner

2024

Entropy

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Heat capacity data of many crystalline solids can be described in a physically sound manner by Debye–Einstein integrals in the temperature range from 0K to 300K. The parameters of the Debye–Einstein approach are either obtained by a Markov chain Monte Carlo (MCMC) global optimization method or by a Levenberg–Marquardt (LM) local optimization routine. In the case of the MCMC approach the model parameters and the coefficients of a function describing the residuals of the measurement points are simultaneously optimized. Thereby, the Bayesian credible interval for the heat capacity function is obtained. Although both regression tools (LM and MCMC) are completely different approaches, not only the values of the Debye–Einstein parameters, but also their standard errors appear to be similar. The calculated model parameters and their associated standard errors are then used to derive the enthalpy, entropy and Gibbs energy as functions of temperature. By direct insertion of the MCMC parameters of all 4·105 computer runs the distributions of the integral quantities enthalpy, entropy and Gibbs energy are determined.

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Uncertainty reduction and quantification in computational thermodynamics

Otis

2022

Computational Materials Science

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Bayesian automated weighting of aggregated DFT, MD, and experimental data for candidate thermodynamic models of aluminum with uncertainty quantification

Cited by 5 publications

References 56 publications

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

Effect of single water adsorption on the bond order of calcium silicates and its implication for hydration variation

Extended Regression Analysis for Debye–Einstein Models Describing Low Temperature Heat Capacity Data of Solids

Uncertainty reduction and quantification in computational thermodynamics

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