2026
ACL
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Yufan Zhao, Jinglin You, Shixiang Wang, Jiawen Lu, Feiyan Xu, Longxing Zhang, Bilal Ghafoor, Aurélien Canizarès, Kai Tang, Liming Lu, Qingli Zhang, Songming Wan, 'Quantitative analysis of binary CaO-Al2O3 glasses structure integrating experiments and simulations', J. Non-Cryst. Solids 675 (2026) doi:10.1016/j.jnoncrysol.2025.123932
This study systematically investigates the local structure of binary (100-x)CaO-xAl2O3 (x = 25, 31, 37, 43, 50 %mol) glasses through an integrated approach combining classical molecular dynamics (CMD) simulations, 27Al magic-angle spinning nuclear magnetic resonance (27Al MAS NMR), and Raman spectroscopy. Both experimental characterization and CMD simulations reveal that, with the increasing Al2O3 content, the glass network predominantly comprises [AlO4] tetrahedra, accompanied by minor but the increasing contributions from [AlO5] and [AlO6] species. CMD-derived angular distribution function analysis identifies clear peak separations between corner-sharing and edge-sharing species, closely matching the deconvolution of Raman spectra in mid-wavenumber range and correlating with the emergence of high-coordination Aluminum species equally observed by 27Al MAS NMR. This multi-method agreement confirmed that the structure transition from primarily corner-sharing to the increased edge-sharing connectivity. Furthermore, Gaussian deconvolution of Raman spectra in high-wavenumber range, combined with a refined Q4 calculation model, enables precise quantitative analysis of Qi species (where i = 0∼4, denotes the number of bridging oxygen in each [AlO4] tetrahedron) by effectively compensating the influence of Raman scattering cross-sections. These integrated findings offer crucial insights into the structure evolution and topological transformations in binary CaO-Al2O3 glasses, laying a theoretical foundation for the rational design and optimization of network connectivity.
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