Real-time molecular scale observation of crystal formation

Roy E. Schreiber, Lothar Houben, Sharon G. Wolf, Gregory Leitus, Zhong Ling Lang, Jorge J. Carbó, Josep M. Poblet, Ronny Neumann

Research output: Contribution to journalArticle

19 Citations (Scopus)

Abstract

How molecules in solution form crystal nuclei, which then grow into large crystals, is a poorly understood phenomenon. The classical mechanism of homogeneous crystal nucleation proceeds via the spontaneous random aggregation of species from liquid or solution. However, a non-classical mechanism suggests the formation of an amorphous dense phase that reorders to form stable crystal nuclei. So far it has remained an experimental challenge to observe the formation of crystal nuclei from five to thirty molecules. Here, using polyoxometallates, we show that the formation of small crystal nuclei is observable by cryogenic transmission electron microscopy. We observe both classical and non-classical nucleation processes, depending on the identity of the cation present. The experiments verify theoretical studies that suggest non-classical nucleation is the lower of the two energy pathways. The arrangement in just a seven-molecule proto-crystal matches the order found by X-ray diffraction of a single bulk crystal, which demonstrates that the same structure was formed in each case.

Original languageEnglish
Pages (from-to)369-373
Number of pages5
JournalNature Chemistry
Volume9
Issue number4
DOIs
Publication statusPublished - Apr 1 2017

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Crystals
Nucleation
Molecules
Cryogenics
Cations
Agglomeration
Positive ions
Transmission electron microscopy
X ray diffraction
Liquids
Experiments

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Cite this

Schreiber, R. E., Houben, L., Wolf, S. G., Leitus, G., Lang, Z. L., Carbó, J. J., ... Neumann, R. (2017). Real-time molecular scale observation of crystal formation. Nature Chemistry, 9(4), 369-373. https://doi.org/10.1038/nchem.2675

Real-time molecular scale observation of crystal formation. / Schreiber, Roy E.; Houben, Lothar; Wolf, Sharon G.; Leitus, Gregory; Lang, Zhong Ling; Carbó, Jorge J.; Poblet, Josep M.; Neumann, Ronny.

In: Nature Chemistry, Vol. 9, No. 4, 01.04.2017, p. 369-373.

Research output: Contribution to journalArticle

Schreiber, RE, Houben, L, Wolf, SG, Leitus, G, Lang, ZL, Carbó, JJ, Poblet, JM & Neumann, R 2017, 'Real-time molecular scale observation of crystal formation', Nature Chemistry, vol. 9, no. 4, pp. 369-373. https://doi.org/10.1038/nchem.2675
Schreiber RE, Houben L, Wolf SG, Leitus G, Lang ZL, Carbó JJ et al. Real-time molecular scale observation of crystal formation. Nature Chemistry. 2017 Apr 1;9(4):369-373. https://doi.org/10.1038/nchem.2675
Schreiber, Roy E. ; Houben, Lothar ; Wolf, Sharon G. ; Leitus, Gregory ; Lang, Zhong Ling ; Carbó, Jorge J. ; Poblet, Josep M. ; Neumann, Ronny. / Real-time molecular scale observation of crystal formation. In: Nature Chemistry. 2017 ; Vol. 9, No. 4. pp. 369-373.
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