Geometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonate
Amorphous calcium carbonate is an important precursor for biomineralization in marine organisms. Key outstanding problems include understanding the structure of amorphous calcium carbonate and rationalizing its metastability as an amorphous phase. Here we report high-quality atomistic models of amor...
| Main Authors: | , , , , , , , |
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| Format: | Journal article |
| Language: | English |
| Published: |
Springer Nature
2023
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| _version_ | 1826311855885254656 |
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| author | Nicholas, TC Stones, AE Patel, A Michel, FM Reeder, RJ Aarts, DGAL Deringer, V Goodwin, A |
| author_facet | Nicholas, TC Stones, AE Patel, A Michel, FM Reeder, RJ Aarts, DGAL Deringer, V Goodwin, A |
| author_sort | Nicholas, TC |
| collection | OXFORD |
| description | Amorphous calcium carbonate is an important precursor for biomineralization in marine organisms. Key outstanding problems include understanding the structure of amorphous calcium carbonate and rationalizing its metastability as an amorphous phase. Here we report high-quality atomistic models of amorphous calcium carbonate generated using state-of-the-art interatomic potentials to help guide fits to X-ray total scattering data. Exploiting a recently developed inversion approach, we extract from these models the effective Ca⋯Ca interaction potential governing the structure. This potential contains minima at two competing distances, corresponding to the two different ways that carbonate ions bridge Ca2+-ion pairs. We reveal an unexpected mapping to the Lennard-Jones–Gauss model normally studied in the context of computational soft matter. The empirical model parameters for amorphous calcium carbonate take values known to promote structural complexity. We thus show that both the complex structure and its resilience to crystallization are actually encoded in the geometrically frustrated effective interactions between Ca2+ ions. |
| first_indexed | 2024-03-07T08:17:28Z |
| format | Journal article |
| id | oxford-uuid:9f63afaa-609d-4d4e-9886-ec2f16d99ad0 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T08:17:28Z |
| publishDate | 2023 |
| publisher | Springer Nature |
| record_format | dspace |
| spelling | oxford-uuid:9f63afaa-609d-4d4e-9886-ec2f16d99ad02024-01-09T09:43:32ZGeometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonateJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:9f63afaa-609d-4d4e-9886-ec2f16d99ad0EnglishSymplectic ElementsSpringer Nature2023Nicholas, TCStones, AEPatel, AMichel, FMReeder, RJAarts, DGALDeringer, VGoodwin, AAmorphous calcium carbonate is an important precursor for biomineralization in marine organisms. Key outstanding problems include understanding the structure of amorphous calcium carbonate and rationalizing its metastability as an amorphous phase. Here we report high-quality atomistic models of amorphous calcium carbonate generated using state-of-the-art interatomic potentials to help guide fits to X-ray total scattering data. Exploiting a recently developed inversion approach, we extract from these models the effective Ca⋯Ca interaction potential governing the structure. This potential contains minima at two competing distances, corresponding to the two different ways that carbonate ions bridge Ca2+-ion pairs. We reveal an unexpected mapping to the Lennard-Jones–Gauss model normally studied in the context of computational soft matter. The empirical model parameters for amorphous calcium carbonate take values known to promote structural complexity. We thus show that both the complex structure and its resilience to crystallization are actually encoded in the geometrically frustrated effective interactions between Ca2+ ions. |
| spellingShingle | Nicholas, TC Stones, AE Patel, A Michel, FM Reeder, RJ Aarts, DGAL Deringer, V Goodwin, A Geometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonate |
| title | Geometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonate |
| title_full | Geometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonate |
| title_fullStr | Geometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonate |
| title_full_unstemmed | Geometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonate |
| title_short | Geometrically-frustrated interactions drive structural complexity in amorphous cal- cium carbonate |
| title_sort | geometrically frustrated interactions drive structural complexity in amorphous cal cium carbonate |
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