Author
Listed:
- Guomin Zhu
(Pacific Northwest National Laboratory
University of Washington)
- Maria L. Sushko
(Pacific Northwest National Laboratory)
- John S. Loring
(Pacific Northwest National Laboratory)
- Benjamin A. Legg
(Pacific Northwest National Laboratory
University of Washington)
- Miao Song
(Pacific Northwest National Laboratory)
- Jennifer A. Soltis
(Pacific Northwest National Laboratory)
- Xiaopeng Huang
(Pacific Northwest National Laboratory)
- Kevin M. Rosso
(Pacific Northwest National Laboratory)
- James J. De Yoreo
(Pacific Northwest National Laboratory
University of Washington)
Abstract
Crystallization by particle attachment (CPA) is a frequently occurring mechanism of colloidal crystallization that results in hierarchical morphologies1–4. CPA has been exploited to create nanomaterials with unusual properties4–6 and is implicated in the development of complex mineral textures1,7. Oriented attachment7,8—a form of CPA in which particles align along specific crystallographic directions—produces mesocrystals that diffract as single crystals do, although the constituent particles are still discernible2,9. The conventional view of CPA is that nucleation provides a supply of particles that aggregate via Brownian motion biased by attractive interparticle potentials1,9–12. However, mesocrystals often exhibit regular morphologies and uniform sizes. Although many crystal systems form mesocrystals1–9 and individual attachment events have been directly visualized10, how random attachment events lead to well defined, self-similar morphologies remains unknown, as does the role of surface-bound ligands, which are ubiquitous in nanoparticle systems3,9,11. Attempts to understand mesocrystal formation are further complicated in many systems by the presence of precursor nanoparticles with a phase distinct from that of the bulk1,13,14. Some studies propose that such particles convert before attachment15, whereas others attribute conversion to the attachment process itself16 and yet others conclude that transformation occurs after the mesocrystals exceed a characteristic size14,17. Here we investigate mesocrystal formation by iron oxides, which are important colloidal phases in natural environments18,19 and classic examples of systems forming ubiquitous precursor phases and undergoing CPA accompanied by phase transformations15,19–21. Combining in situ transmission electron microscopy (TEM) at 80 degrees Celsius with ‘freeze-and-look’ TEM, we tracked the formation of haematite (Hm) mesocrystals in the presence of oxalate (Ox), which is abundant in soils, where iron oxides are common. We find that isolated Hm particles rarely appear, but once formed, interfacial gradients at the Ox-covered surfaces drive Hm particles to nucleate repeatedly about two nanometres from the surfaces, to which they then attach, thereby generating mesocrystals. Comparison to natural and synthetic systems suggests that interface-driven pathways are widespread.
Suggested Citation
Guomin Zhu & Maria L. Sushko & John S. Loring & Benjamin A. Legg & Miao Song & Jennifer A. Soltis & Xiaopeng Huang & Kevin M. Rosso & James J. De Yoreo, 2021.
"Self-similar mesocrystals form via interface-driven nucleation and assembly,"
Nature, Nature, vol. 590(7846), pages 416-422, February.
Handle:
RePEc:nat:nature:v:590:y:2021:i:7846:d:10.1038_s41586-021-03300-0
DOI: 10.1038/s41586-021-03300-0
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Citations
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Cited by:
- Bum Chul Park & Min Jun Ko & Young Kwang Kim & Gyu Won Kim & Myeong Soo Kim & Thomas Myeongseok Koo & Hong En Fu & Young Keun Kim, 2022.
"Surface-ligand-induced crystallographic disorder–order transition in oriented attachment for the tuneable assembly of mesocrystals,"
Nature Communications, Nature, vol. 13(1), pages 1-11, December.
- Miao Song & Dingri Zhang & Dan Leng & Jaewon Lee & Ziang Yang & Jiaxuan Chen & Dan Li & Lei Wang & Gang Zhou & Rui Yang & Kechao Zhou, 2024.
"In situ atomic observations of aggregation growth and evolution of penta-twinned gold nanocrystals,"
Nature Communications, Nature, vol. 15(1), pages 1-10, December.
- Fatima A. Davila-Hernandez & Biao Jin & Harley Pyles & Shuai Zhang & Zheming Wang & Timothy F. Huddy & Asim K. Bera & Alex Kang & Chun-Long Chen & James J. Yoreo & David Baker, 2023.
"Directing polymorph specific calcium carbonate formation with de novo protein templates,"
Nature Communications, Nature, vol. 14(1), pages 1-11, December.
- Guomin Zhu & Benjamin A. Legg & Michel Sassi & Xinran Liang & Meirong Zong & Kevin M. Rosso & James J. Yoreo, 2023.
"Crystal dissolution by particle detachment,"
Nature Communications, Nature, vol. 14(1), pages 1-11, December.
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