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Cited by 212nanoparticles nucleation surface interactionsCrystallization and Solubility StudiesSolidification and crystal growth phenomena

How crystals form: A theory of nucleation pathways

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Lutsko, James F.·2019·Science Advances
DOI 10.1126/sciadv.aav7399PMC PMC6450691
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Abstract

A theory of nucleation that is able to predict nonclassical pathways and intermediates for crystallization is formulated.

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Crossref · 10.1126/sciadv.aav7399

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  • A variety of precursor phases exist in the early stages of carbonate crystallization, including prenucleation clusters, metastable liquid-like precursors, mesocrystals and amorphous and nanophase precursors.

    “Recent studies have shown that a variety of precursor phases exist in the early stages of carbonate crystallization, including prenucleation clusters, metastable liquid-like precursors, mesocrystals and amorphous and nanophase precursors [114-123].”

    From Thermodynamic and Kinetic Studies of Dolomite Formation: A Review (2023) · cites this paper as [123]

    The Introduction says complex nucleation pathways have been reported for calcium carbonate, and the References identify a study of stable prenucleation calcium carbonate clusters. But this paper does not establish that metastable liquid-like precursors, mesocrystals, or amorphous and nanophase precursors all occur in early carbonate crystallization; its discussion of other precursor types concerns crystallization more generally. Page numbers were not available in our copy. (LLM, conf=0.85)

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  1. [2]Ablasser A., Phase separation focuses DNA sensing. Science 361, 646– 647 (2018). 30115795
  2. [3]Olafson K. N., Nguyen T. Q., Rimer J. D., Vekilov P. G., Antimalarials inhibit hematin crystallization by unique drug–surface site interactions. Proc. Natl. Acad. Sci. U.S.A. 114, 7531– 7536 (2017). 28559329 PMC5530657
  3. [4]Harper J. D., Lieber C. M., Lansbury P. T. Jr., Atomic force microscopic imaging of seeded fibril formation and fibril branching by the Alzheimer’s disease amyloid-β protein. Chem. Biol. 4, 951– 959 (1997). 9427660
  4. [5]Walsh D. M., Lomakin A., Benedek G. B., Condron M. M., Teplow D. B., Amyloid β-protein fibrillogenesis. Detection of a protofibrillar intermediate. J. Biol. Chem. 272, 22364– 22372 (1997). 9268388
  5. [6]Erdemir D., Lee A. Y., Myerson A. S., Polymorph selection: The role of nucleation, crystal growth and molecular modeling. Curr. Opin. Drug Discov. Dev. 10, 746– 755 (2007). 17987526
  6. [8]Lam J., Lutsko J. F., Lattice induced crystallization of nanodroplets: The role of finite-size effects and substrate properties in controlling polymorphism. Nanoscale 10, 4921– 4926 (2018). 29480297
  7. [9]Driessche A. E. S. V., Van Gerven N., Bomans P. H. H., Joosten R. R. M., Friedrich H., Gil-Carton D., Sommerdijk N. A. J. M., Sleutel M., Molecular nucleation mechanisms and control strategies for crystal polymorph selection. Nature 556, 89– 94 (2018). 29620730
  8. [10]Schreiber R. E., Houben L., Wolf S. G., Leitus G., Lang Z.-L., Carbó J. J., Poblet J. M., Neumann R., Real-time molecular scale observation of crystal formation. Nat. Chem. 9, 369– 373 (2017). 28338680
  9. [11]J. Zhou, Y. Yang, Y. Yang, D. S. Kim, A. Yuan, X. Tian, C. Ophus, F. Sun, A. K. Schmid, M. Nathanson, H. Heinz, Q. An, H. Zeng, P. Ercius, J. Miao, Capturing nucleation at 4D atomic resolution. arXiv: 1807.10709 [cond-mat.mtrl-sci] (27 July 2018). · arXiv
  10. [12]Sosso G. C., Chen J., Cox S. J., Fitzner M., Pedevilla P., Zen A., Michaelides A., Crystal nucleation in liquids: Open questions and future challenges in molecular dynamics simulations. Chem. Rev. 116, 7078– 7116 (2016). 27228560 PMC4919765
  11. [13]Tanaka H., Bond orientational order in liquids: Towards a unified description of waterlike anomalies, liquid-liquid transition, glass transition, and crystallization. Eur. Phys. J. E 35, 113 (2012). 23104614
  12. [14]ten Wolde P. R., Frenkel D., Enhancement of protein crystal nucleation by critical density fluctuations. Science 77, 1975– 1978 (1997). 9302288
  13. [15]Galkin O., Vekilov P. G., Control of protein crystal nucleation around the metastable liquid–liquid phase boundary. Proc. Natl. Acad. Sci. U.S.A. 97, 6277– 6281 (2000). 10823898 PMC18593
  14. [16]Gebauer D., Volkel A., Cölfen H., Stable prenucleation calcium carbonate clusters. Science 322, 1819– 1822 (2008). 19095936
  15. [18]Lee S., Wi H. S., Jo W., Cho Y. C., Lee H. H., Jeong S.-Y., Kim Y.-I., Lee G. W., Multiple pathways of crystal nucleation in an extremely supersaturated aqueous potassium dihydrogen phosphate (KDP) solution droplet. Proc. Natl. Acad. Sci. U.S.A. 113, 13618– 13623 (2016). 27791068 PMC5137746
  16. [19]Ma X., Zhang S., Jiao F., Newcomb C. J., Zhang Y., Prakash A., Liao Z., Baer M. D., Mundy C. J., Pfaendtner J., Noy A., Chen C.-L., De Yoreo J. J., Tuning crystallization pathways through sequence engineering of biomimetic polymers. Nat. Mater. 16, 767– 774 (2017). 28414316
  17. [20]Hedges L. O., Whitelam S., Limit of validity of Ostwald’s rule of stages in a statistical mechanical model of crystallization. J. Chem. Phys. 135, 164902 (2011). 22047264
  18. [22]Lutsko J. F., Recent developments in classical density functional theory. Adv. Chem. Phys. 144, 1 (2010).
  19. [24]Lutsko J. F., Density functional theory of inhomogeneous liquids. III. Liquid-vapor nucleation. J. Chem. Phys. 129, 244501 (2008). 19123511
  20. [26]Lutsko J. F., A dynamical theory of nucleation for colloids and macromolecules. J. Chem. Phys. 136, 034509 (2012). 22280769
  21. [27]Durán-Olivencia M. A., Yatsyshin P., Goddard B., Kalliadasis S., General framework for fluctuating dynamic density functional theory. New J. Phys. 19, 123022 (2017).
  22. [28]Goddard B. D., Nold A., Savva N., Pavliotis G., Kalliadasis S., General dynamical density functional theory for classical fluids. Phys. Rev. Lett. 109, 120603 (2012). 23005931
  23. [31]Gallo M., Magaletti F., Casciola C. M., Thermally activated vapor bubble nucleation: The Landau-Lifshitz–Van der Waals approach. Phys. Rev. Fluids 3, 053604 (2018).
  24. [32]Lutsko J. F., Systematically extending classical nucleation theory. New J. Phys. 20, 103015 (2018).
  25. [35]M. I. Freidlin, A. D. Wentzell, Random Perturbations of Dynamical Systems (Springer, 1998).
  26. [36]Weinan E., Ren W., Vanden-Eijnden E., Simplified and improved string method for computing the minimum energy paths in barrier-crossing events. J. Chem. Phys. 126, 164103 (2007). 17477585
  27. [37]Qiu C., Qian T., Nucleation of wetting films on cylindrical and spherical substrates: A numerical study by the string method. J. Chem. Phys. 131, 124708 (2009). 19791913
  28. [38]Backofen R., Voigt A., A phase-field-crystal approach to critical nuclei. J. Phys. Cond. Matter 22, 364104 (2010). 21386520
  29. [40]Roth R., Fundamental measure theory for hard-sphere mixtures: A review. J. Phys. Condens. Matter 22, 063102 (2010). 21389360
  30. [41]Elder K. R., Katakowski M., Haataja M., Grant M., Modeling elasticity in crystal growth. Phys. Rev. Lett. 88, 245701 (2002). 12059316
  31. [42]Elder K. R., Grant M., Modeling elastic and plastic deformations in nonequilibrium processing using phase field crystals. Phys. Rev. E 70, 051605 (2004). 15600626
  32. [43]van Teeffelen S., Backofen R., Voigt A., Löwen H., Derivation of the phase-field-crystal model for colloidal solidification. Phys. Rev. E 79, 051404 (2009). 19518453
  33. [44]Tóth G. I., Pusztai T., Tegze G., Tóth G., Gránásy L., Amorphous nucleation precursor in highly nonequilibrium fluids. Phys. Rev. Lett. 107, 175702 (2011). 22107540
  34. [45]Tóth G. I., Tegze G., Pusztai T., Tóth G., Gránásy L., Polymorphism, crystal nucleation and growth in the phase-field crystal model in 2D and 3D. J. Phys. Condens. Matter 22, 364101 (2010). 21386517
  35. [47]Lutsko J. F., Nucleation of colloids and macromolecules in a finite volume. J. Chem. Phys. 137, 154903 (2012). 23083187
  36. [48]Lutsko J. F., Durán-Olivencia M. A., A two-parameter extension of classical nucleation theory. J. Phys. Condens. Matter 27, 235101 (2015). 25993497
  37. [49]Merikanto J., Zapadinsky E., Lauri A., Vehkamäki H., Origin of the failure of classical nucleation theory: Incorrect description of the smallest clusters. Phys. Rev. Lett. 98, 145702 (2007). 17501289
  38. [50]Lutsko J. F., Lam J., Classical density functional theory, unconstrained crystallization, and polymorphic behavior. Phys. Rev. E 98, 012604 (2018). 30110790
  39. [51]Girshick S. L., Agarwal P., Truhlar D. G., Homogeneous nucleation with magic numbers: Aluminum. J. Chem. Phys. 131, 134305 (2009). 19814551
  40. [53]Sleutel M., Van Driessche A. E. S., Role of clusters in nonclassical nucleation and growth of protein crystals. Proc. Natl. Acad. Sci. U.S.A. 111, E546– E553 (2014). 24449867 PMC3918807
  41. [54]Savage J. R., Dinsmore A. D., Experimental evidence for two-step nucleation in colloidal crystallization. Phys. Rev. Lett. 102, 198302 (2009). 19519003
  42. [56]Barros K., Klein W., Liquid to solid nucleation via onion structure droplets. J. Chem. Phys. 139, 174505 (2013). 24206314
  43. [58]Langer J. S., Turski L. A., Hydrodynamic model of the condensation of a vapor near its critical point. Phys. Rev. A 8, 3230 (1973).
  44. [61]Lutsko J. F., A dynamical theory of homogeneous nucleation for colloids and macromolecules. J. Chem. Phys. 135, 161101 (2011). 22047221
  45. [62]D. J. Wales, J. P. K. Doye, A. Dullweber, M. P. Hodges, F. Y. Naumkin, F. Calvo, J. Hernández-Rojas, T. F. Middleton, The Cambridge Cluster Database.
  46. [63]Xiang Y., Jiang H., Cai W., Shao X., An efficient method based on lattice construction and the genetic algorithm for optimization of large Lennard-Jones clusters. J. Phys. Chem. A 108, 3586– 3592 (2004). 28413878

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Authors
Lutsko, J. F.
Affiliations
Université Libre de Bruxelles (BE)
Corresponding author
Lutsko, James F.
ORCID
Lutsko, James F.
Venue
Science Advances
Publisher
American Association for the Advancement of Science (AAAS)
Published
2019-04-05
Volume
5
Issue
4
Pages
eaav7399-eaav7399
ISSN
2375-2548 (ISSN-L)
DOI
10.1126/sciadv.aav7399
PMC
PMC6450691
OpenAlex
W2935294972
Cited by
212
References
1
Citations by year
2026: 25 · 2025: 30 · 2024: 26 · 2023: 27 · 2022: 43 · 2021: 30 · 2020: 24 · 2019: 7
FWCI
10.31
Type
journal article
Language
en
Open access
Locations
  • Science Advances (publishedVersion)
  • Europe PMC (PubMed Central) (publishedVersion, cc-by-nc)
  • PubMed Central (publishedVersion, cc-by-nc)
  • PubMed (publishedVersion)
  • arXiv (Cornell University) (submittedVersion)
  • Dépôt institutionnel de l'Université libre de Bruxelles (Université Libre de Bruxelles) (submittedVersion, other-oa)
  • Dépôt institutionnel de l'Université libre de Bruxelles (Université Libre de Bruxelles) (submittedVersion)
  • arXiv (Cornell University)
Funders
European Space Agency (ESA AO-2004-070)
Topics
  • Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › nanoparticles nucleation surface interactions
  • Physical Sciences › Materials Science › Materials Chemistry › Crystallization and Solubility Studies
  • Physical Sciences › Materials Science › Materials Chemistry › Solidification and crystal growth phenomena
Keywords
nucleation pathways, crystallization, non-classical nucleation, classical density functional theory, stochastic process theory, rare event sampling, macromolecular solutions, liquid-liquid separation, free energy landscape

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