Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental Raman
The vibrational spectroscopic properties of crystalline anhydrous calcium carbonate polymorphs, i.e. calcite, aragonite and vaterite, are computed with state-of-the-art computational techniques. We present a refined protocol that significantly enhances the quality of spectra obtained via the autocor...
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| Format: | Article |
| Language: | English |
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Elsevier
2025-08-01
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| Series: | Materials & Design |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S0264127525005854 |
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| author | Fileto Rodríguez Robin Francotte Beata Taudul Jianing Wang Ionut Tranca Diane Sorgeloos Enrique Lozano Diz Monica Calatayud Frederik Tielens |
| author_facet | Fileto Rodríguez Robin Francotte Beata Taudul Jianing Wang Ionut Tranca Diane Sorgeloos Enrique Lozano Diz Monica Calatayud Frederik Tielens |
| author_sort | Fileto Rodríguez |
| collection | DOAJ |
| description | The vibrational spectroscopic properties of crystalline anhydrous calcium carbonate polymorphs, i.e. calcite, aragonite and vaterite, are computed with state-of-the-art computational techniques. We present a refined protocol that significantly enhances the quality of spectra obtained via the autocorrelation function formalism, particularly for ionic materials. For the first time, Voronoi Radical Tessellation (VRT) is applied for the computation of electromagnetic properties of ionic systems in combination with Bader’s Quantum Theory of Atoms In Molecules (QTAIM). The use of the later allows for the determination of accurate Voronoi radii, making VRT completely ab initio. Our findings lead the way for the accurate computation of vibrational spectra in materials where anharmonicity, temperature or conformational variety have a considerable impact in the resulting spectrum. This work represents a step forward in accurately modeling and interpreting the spectroscopic behavior of ionic materials, pushing the boundaries of computational materials science. |
| format | Article |
| id | doaj-art-6936b469f63f4ce88d5e4ddbcf33f381 |
| institution | DOAJ |
| issn | 0264-1275 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Materials & Design |
| spelling | doaj-art-6936b469f63f4ce88d5e4ddbcf33f3812025-08-20T03:22:04ZengElsevierMaterials & Design0264-12752025-08-0125611416510.1016/j.matdes.2025.114165Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental RamanFileto Rodríguez0Robin Francotte1Beata Taudul2Jianing Wang3Ionut Tranca4Diane Sorgeloos5Enrique Lozano Diz6Monica Calatayud7Frederik Tielens8General Chemistry ALGC – Materials Modelling Group, Vrije Universiteit Brussel, Pleinlaan 2 Brussel, BelgiumGeneral Chemistry ALGC – Materials Modelling Group, Vrije Universiteit Brussel, Pleinlaan 2 Brussel, BelgiumSorbonne Université, MONARIS, CNRS-UMR 8233, 4 Place Jussieu, F-75005 Paris, FranceGeneral Chemistry ALGC – Materials Modelling Group, Vrije Universiteit Brussel, Pleinlaan 2 Brussel, BelgiumGeneral Chemistry ALGC – Materials Modelling Group, Vrije Universiteit Brussel, Pleinlaan 2 Brussel, BelgiumGeneral Chemistry ALGC – Materials Modelling Group, Vrije Universiteit Brussel, Pleinlaan 2 Brussel, BelgiumELODIZ Ltd. High Wycombe, UKSorbonne Université, MONARIS, CNRS-UMR 8233, 4 Place Jussieu, F-75005 Paris, France; Corresponding authors.General Chemistry ALGC – Materials Modelling Group, Vrije Universiteit Brussel, Pleinlaan 2 Brussel, Belgium; Corresponding authors.The vibrational spectroscopic properties of crystalline anhydrous calcium carbonate polymorphs, i.e. calcite, aragonite and vaterite, are computed with state-of-the-art computational techniques. We present a refined protocol that significantly enhances the quality of spectra obtained via the autocorrelation function formalism, particularly for ionic materials. For the first time, Voronoi Radical Tessellation (VRT) is applied for the computation of electromagnetic properties of ionic systems in combination with Bader’s Quantum Theory of Atoms In Molecules (QTAIM). The use of the later allows for the determination of accurate Voronoi radii, making VRT completely ab initio. Our findings lead the way for the accurate computation of vibrational spectra in materials where anharmonicity, temperature or conformational variety have a considerable impact in the resulting spectrum. This work represents a step forward in accurately modeling and interpreting the spectroscopic behavior of ionic materials, pushing the boundaries of computational materials science.http://www.sciencedirect.com/science/article/pii/S0264127525005854IRRamanAIMDCaCO3PolymorphismDFT |
| spellingShingle | Fileto Rodríguez Robin Francotte Beata Taudul Jianing Wang Ionut Tranca Diane Sorgeloos Enrique Lozano Diz Monica Calatayud Frederik Tielens Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental Raman Materials & Design IR Raman AIMD CaCO3 Polymorphism DFT |
| title | Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental Raman |
| title_full | Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental Raman |
| title_fullStr | Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental Raman |
| title_full_unstemmed | Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental Raman |
| title_short | Advanced spectroscopic characterization of calcium carbonate polymorphs: Ab initio dynamic approaches and experimental Raman |
| title_sort | advanced spectroscopic characterization of calcium carbonate polymorphs ab initio dynamic approaches and experimental raman |
| topic | IR Raman AIMD CaCO3 Polymorphism DFT |
| url | http://www.sciencedirect.com/science/article/pii/S0264127525005854 |
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