Microscopic Evidence for Liquid-Liquid Separation in Supersaturated CaCO 3 Solutions

Author:

Wallace Adam F.123,Hedges Lester O.12,Fernandez-Martinez Alejandro14,Raiteri Paolo5,Gale Julian D.5,Waychunas Glenn A.1,Whitelam Stephen2,Banfield Jillian F.16,De Yoreo James J.278

Affiliation:

1. Earth Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

2. The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

3. Department of Geological Sciences, University of Delaware, Newark, DE 19716, USA.

4. Institut des Sciences de la Terre (ISTerre), Université de Grenoble 1, CNRS, 38041 Grenoble, France.

5. Nanochemistry Research Institute, Department of Chemistry, Curtin University, Post Office Box U1987, Perth, WA 6845, Australia.

6. Department of Earth and Planetary Science, University of California, Berkeley, Berkeley, CA 94720, USA.

7. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, Berkeley, CA 94720, USA.

8. Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, USA.

Abstract

Making Crystals The initial transition from a disordered solution to the formation of nuclei that grow into crystals continues to be a puzzle. Recent experiments suggested the formation of stable ordered clusters that appear prior to the formation of the first nuclei. Wallace et al. (p. 885 ; see the Perspective by Myerson and Trout ) used molecular dynamics to look at the potential structure and dynamics of these clusters and lattice gas simulations to explore the population dynamics of the cluster populations prior to nucleation. A liquid-liquid phase separation process was observed whereby one phase becomes more concentrated in ions and becomes the precursor for nuclei to form.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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