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Seeds of imperfection rule the mesocrystalline disorder in natural anhydrite single crystals

  • In recent years, we have come to appreciate the astounding intricacies associated with the formation of minerals from ions in aqueous solutions. In this context, a number of studies have revealed that the nucleation of calcium sulfate systems occurs nonclassically, involving the aggregation and reorganization of nanosized prenucleation species. In recent work, we have shown that this particle-mediated nucleation pathway is actually imprinted in the resultant micrometer-sized CaSO4 crystals. This property of CaSO4 minerals provides us with the unique opportunity to search for evidence of nonclassical nucleation pathways in geological environments. In particular, we focused on large anhydrite Crystals extracted from the Naica Mine in Mexico. We were able to shed light on this mineral's growth history by mapping defects at different length scales. Based on this, we argue that the nanoscale misalignment of the structural subunits, observed in the initial calcium sulfate crystal seeds,In recent years, we have come to appreciate the astounding intricacies associated with the formation of minerals from ions in aqueous solutions. In this context, a number of studies have revealed that the nucleation of calcium sulfate systems occurs nonclassically, involving the aggregation and reorganization of nanosized prenucleation species. In recent work, we have shown that this particle-mediated nucleation pathway is actually imprinted in the resultant micrometer-sized CaSO4 crystals. This property of CaSO4 minerals provides us with the unique opportunity to search for evidence of nonclassical nucleation pathways in geological environments. In particular, we focused on large anhydrite Crystals extracted from the Naica Mine in Mexico. We were able to shed light on this mineral's growth history by mapping defects at different length scales. Based on this, we argue that the nanoscale misalignment of the structural subunits, observed in the initial calcium sulfate crystal seeds, propagates through different length scales both in morphological, as well as in strictly crystallographic aspects, eventually causing the formation of large mesostructured single crystals of anhydrite. Hence, the nonclassical nucleation mechanism introduces a “seed of imperfection,” which leads to a macroscopic “single” crystal whose fragments do not fit together at different length scales in a self-similar manner. Consequently, anisotropic voids of various sizes are formed with very welldefined walls/edges. However, at the same time, the material retains in part its single crystal nature.zeige mehrzeige weniger

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  • Seeds of imperfection rule the mesocrystalline disorder in natural anhydrite single crystals.pdf
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    Article.

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    Supporting information 1.

  • Download_Dataset_S01.txt
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    Supporting information 2.

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    Supporting information 3: 3D projection of a reconstructed crystal derived from the X-ray microtomography (μCT) measurements. 360° rotation of the crystal around the Z-axis in the XY-plane.

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    Supporting information 4: 3D projection of a reconstructed crystal derived from the X-ray microtomography (μCT) measurements. 360° rotation of the crystal around the Y-axis in the XZ-plane.

  • Download_03.wmv
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    Supporting information 5: 3D projection of a reconstructed crystal derived from the X-ray microtomography (μCT) measurements with a segmentation highlighting the voids. 360° rotation of the crystal around the Z-axis in the XY-plane.

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Metadaten
Autor*innen:Tomasz StawskiORCiD, Glen Jacob SmalesORCiD, E. ScoppolaORCiD, D. Jha, L. F. G. MoralesORCiD, A. MoyaORCiD, R. Wirth, Brian Richard PauwORCiD, Franziska EmmerlingORCiD, A. E. S. Van DriesscheORCiD
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):Proceedings of the National Academy of Sciences of the United States of America (PNAS)
Jahr der Erstveröffentlichung:2021
Organisationseinheit der BAM:6 Materialchemie
6 Materialchemie / 6.3 Strukturanalytik
6 Materialchemie / 6.5 Synthese und Streuverfahren nanostrukturierter Materialien
Verlag:National Academy of Sciences (USA)
Verlagsort:Washington
Jahrgang/Band:118
Ausgabe/Heft:48
Aufsatznummer:e2111213118
Erste Seite:1
Letzte Seite:11
DDC-Klassifikation:Naturwissenschaften und Mathematik / Chemie / Analytische Chemie
Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Ingenieurwissenschaften und zugeordnete Tätigkeiten
Freie Schlagwörter:Anhydrite; Calcium sulfate; Mesocrystal; Naica; Nucleation
Themenfelder/Aktivitätsfelder der BAM:Chemie und Prozesstechnik
Material
Material / Materialdesign
Material / Nano
DOI:10.1073/pnas.2111213118
ISSN:0027-8424
Zugehöriger Identifikator:https://opus4.kobv.de/opus4-bam/frontdoor/index/index/docId/53630
Zugehöriger Identifikator:https://opus4.kobv.de/opus4-bam/frontdoor/index/index/docId/53765
Verfügbarkeit des Dokuments:Datei im Netzwerk der BAM verfügbar ("Closed Access")
Datum der Freischaltung:25.11.2021
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:29.11.2021
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