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MARCO BERTANI
Dottorando
Dipartimento di Scienze Chimiche e Geologiche
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Pubblicazioni
2024
- Accurate and Transferable Machine Learning Potential for Molecular Dynamics Simulation of Sodium Silicate Glasses
[Articolo su rivista]
Bertani, Marco; Charpentier, Thibault; Faglioni, Francesco; Pedone, Alfonso
abstract
2024
- Decoding crystallization behavior of aluminoborosilicate glasses: From structural descriptors to Quantitative Structure – Property Relationship (QSPR) based predictive models
[Articolo su rivista]
Zhang, Yingcheng; Bertani, Marco; Pedone, Alfonso; Youngman, Randall E.; Tricot, Gregory; Kumar, Aditya; Goel, Ashutosh
abstract
2023
- Comparison of five empirical potential models for aluminosilicate systems: Albite and anorthite as test cases
[Articolo su rivista]
Pallini, Annalisa; Bertani, Marco; Rustichelli, Daniel; Ziebarth, Benedikt; Mannstadt, Wolfgang; Pedone, Alfonso
abstract
2023
- Effects of magnesium on the structure of aluminoborosilicate glasses: NMR assessment of interatomic potentials models for molecular dynamics
[Articolo su rivista]
Bertani, Marco; Bisbrouck, Nicolas; Delaye, Jean‐marc; Angeli, Frédéric; Pedone, Alfonso; Charpentier, Thibault
abstract
Classical molecular dynamics simulations have been used to investigate the structural role of Mg and its effect when it is incorporated in sodium aluminoborosilicate glasses. The simulations have been performed using three interatomic potentials; one is based on the rigid ionic model parameterized by Wang et al. (2018) and two slightly different parameterization of the core-shell model provided by Stevensson et al. (2018) and Pedone et al. (2020) The accuracies of these models have been assessed by detailed structural analysis and comparing the simulated nuclear magnetic resonance (NMR) spectra for spin active nuclei (Si-29, Al-27, B-11, O-17, Mg-25, and Na-23) with the experimental counterparts collected in a previous work. Our simulations reveal that the core-shell parameterizations provide better structural models. In fact, they better reproduce the NMR spectra of all the investigated nuclei and give better agreement with known experimental data. Magnesium is found to be five coordinated on average with distances with oxygen in between a network modifier (like Na) and an intermediate network formed (like Al). It prefers to lay closer to three-coordinated B atoms, forming B-NBO bonds, with respect to Si and especially Al. This can explain the formation of AlO5 and AlO6 units in the investigated Na-free glass, together with a Si clusterization.
2023
- Erratum for a new self‐consistent empirical potential model for multicomponent borate and borosilicate glasses (Journal of the American Ceramic Society, (2022), 105, 12, (7254-7271), 10.1111/jace.18681)
[Articolo su rivista]
Bertani, M.; Pallini, A.; Lodesani, F.; Cocchi, M.; Menziani, M. C.; Pedone, A.
abstract
The manuscript contains a mistake in Equation (6) and an erroneous value of the B-ij term of B-O interaction in Table 2. An additional sentence is needed in paragraph 2.2. These errata acknowledge and correct the mistakes and add the needed information. The corrections do not lead to any changes in the results, discussion, and conclusion.
2022
- A new self-consistent empirical potential model for multicomponent borate and borosilicate glasses
[Articolo su rivista]
Bertani, M.; Pallini, A.; Cocchi, M.; Menziani, M. C.; Pedone, A.
abstract
A new self-consistent empirical potential model based on the BMP potential [Bertani et al., Phys. Rev. Mat. 5 (2021) 045602] has been developed for the simulation of multicomponent borate and borosilicate glasses. We exploited the Bayesian optimization approach to create a set of parameters for the B–O interaction, which depends on the glass composition, and in particular on the R = ([A2O]+[AEO])/[B2O3] (A = alkaline and AE alkaline-earth ions) and K = [SiO2]/[B2O3] ratios. The obtained force field (FF) has been applied to several borate and borosilicate glass series containing, as modifier oxide, Na2O, Li2O, CaO, and MgO and tested on experimental data, such as the fraction of BO4 (N4), density, non-bridging oxygen speciation, neutron diffraction spectra, 11B, 29Si, and 17O magic angle spinning nuclear magnetic resonance. A comparison with other interatomic potentials available in literature has also been performed. The results show that the FF reproduces well almost all the abovementioned properties, showing excellent agreement with experimental data in a wide range of compositions.
2022
- Interatomic potentials for oxide glasses: Past, present, and future
[Articolo su rivista]
Pedone, A.; Bertani, M.; Brugnoli, L.; Pallini, A.
abstract
The continuous development and improvement of interatomic potential models for oxide glasses have made classical molecular dynamics a powerful computational technique routinely used for studying the structure and properties of such materials on a par with the more advanced experimental techniques. In this brief review, we retrace the development of the most used interatomic potential models from the earliest MD simulations up to now with a look at the possible future developments in this field due to the advent of the machine learning era and data-driven methods.
2021
- Impact of magnesium on the structure of aluminoborosilicate glasses: A solid‐state NMR and Raman spectroscopy study
[Articolo su rivista]
Bisbrouck, Nicolas; Bertani, Marco; Angeli, Frédéric; Charpentier, Thibault; Ligny, Dominique; Delaye, Jean‐marc; Gin, Stéphane; Micoulaut, Matthieu
abstract
Seven magnesium- containing aluminoborosilicate glasses, with three to five oxides,
have been studied through comprehensive multinuclear solid- state NMR (
11
B,
27
Al,
29
Si,
23
Na,
17
O, and
25
Mg) and Raman spectroscopy. The progressive addition of cati-
ons and the substitution of sodium and calcium by magnesium illuminate the impact of
magnesium on the glass structure. The proportion of tri- coordinated boron drastically
increased with magnesium addition, demonstrating the poor charge- compensating
capabilities of magnesium in tetrahedral boron units. Oxygen- 17 NMR showed the
formation of mixing sites containing both Na and Mg near nonbridging oxygen sites.
Furthermore, a high magnesium content appears to result in the formation of two
subnetworks (boron and silicon rich) with different polymerization degrees as well
as to promote the formation of high- coordination aluminum sites (Al[V] and Al[VI]).
Finally, magnesium coordination ranging from 4 to 6, with a mean value shifting from
5 to 6 along the series, suggests that magnesium might endorse an intermediate role
in these glasses.
2021
- Improved empirical force field for multicomponent oxide glasses and crystals
[Articolo su rivista]
Bertani, M.; Menziani, M. C.; Pedone, A.
abstract
In this paper, the self-consistent PMMCS force fields (FFs) [Pedone et al., J. Phys. Chem. B 110, 11780 (2006)10.1021/jp0611018] widely used for the simulation of a large variety of silicates, aluminosilicate and phosphate crystals, and multicomponent oxide glasses have been revised and improved by the inclusion of two types of three-body interactions acting between T-O-T bridges (T=Si and P) and network former-network former repulsive interactions. The FFs named Bertani-Menziani-Pedone (BMP)-harm and BMP-shrm better reproduce the T-O-T bond angle distributions (BADs) and network former-oxygen distances. Consequently, the prediction of Qn distributions (Q stands for quaternary species, and n is the number of bridging oxygens around it), neutron total distribution functions, solid-state nuclear magnetic resonance spectra of spin active nuclei (Si29, O17, P31, Al27), and the density have also been hugely improved with respect to the previous version of our FF. These results also highlight the strong correlation between the T-O-T BADs and the other short and intermediate structural properties in oxide glasses, which have been largely neglected in the past. In addition to the improvement of the structure, the FF has been revealed to reproduce well the ionic conductivity in mixed alkali aluminosilicate glasses and the elastic properties. The systematic comparison with other interatomic potential models, including the polarizable core-shell model, carried out in this paper showed that our potential model is more balanced and effective for simulating a vast family of crystalline and amorphous oxide-based systems.
2021
- Influence of Magnesium on the Structure of Complex Multicomponent Silicates: Insights from Molecular Simulations and Neutron Scattering Experiments
[Articolo su rivista]
Bisbrouck, N.; Micoulaut, M.; Delaye, J. -M.; Bertani, M.; Charpentier, T.; Gin, S.; Angeli, F.
abstract
2020
- Combined Experimental and Computational Approach toward the Structural Design of Borosilicate-Based Bioactive Glasses
[Articolo su rivista]
Stone-Weiss, N.; Bradtmuller, H.; Fortino, M.; Bertani, M.; Youngman, R. E.; Pedone, A.; Eckert, H.; Goel, A.
abstract
Transitioning beyond a trial-and-error based approach for the compositional design of next-generation borosilicate-based bioactive glasses requires a fundamental understanding of the underlying compositional and structural drivers controlling their degradation and ion release in vitro and in vivo. Accordingly, the present work combines magic-angle spinning (MAS) NMR techniques, MD simulations, and DFT calculations based on GIPAW and PAW algorithms, to build a comprehensive model describing the short-to-medium-range structure of potentially bioactive glasses in the Na2O-P2O5-B2O3-SiO2 system over a broad compositional space. P2O5 preferentially tends to attract network modifier species, thus resulting in a repolymerization of the silicate network and a restructuring of the borate component. 11B{31P} and 31P{11B} dipolar recoupling experiments suggest that the ability of glasses to incorporate P2O5 without phase separation is related to the formation of P-O-B(IV) linkages integrated into the borosilicate glass network. An analogous approach is used for elucidating the local environments of the Na+ network modifiers. This work, along with future studies aimed at elucidating composition-structure-solubility/bioactivity relationships, will lay the foundation for the development of quantitative structure-property relationship (QSPR) models, thus representing a leap forward in the design of functional borosilicate bioactive glasses with controlled ionic release behavior.