3D visualization of additive occlusion and tunable full-spectrum fluorescence in calcite

David C. Green, Johannes Ihli, Paul D. Thornton, Mark A. Holden, Bartosz Marzec, Yi-Yeoun Kim, Alex N. Kulak, Mark A. Levenstein, Chiu Tang, Christophe Lynch, Stephen E. D. Webb, Christopher J. Tynan and Fiona C. Meldrum ()
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David C. Green: School of Chemistry, University of Leeds
Johannes Ihli: School of Chemistry, University of Leeds
Paul D. Thornton: School of Chemistry, University of Leeds
Mark A. Holden: School of Chemistry, University of Leeds
Bartosz Marzec: School of Chemistry, University of Leeds
Yi-Yeoun Kim: School of Chemistry, University of Leeds
Alex N. Kulak: School of Chemistry, University of Leeds
Mark A. Levenstein: School of Chemistry, University of Leeds
Chiu Tang: Diamond Light Source, Harwell Science and Innovation Campus
Christophe Lynch: Central Laser Facility, Science and Technology Facilities Council, Research Complex at Harwell, Rutherford Appleton Laboratory
Stephen E. D. Webb: Central Laser Facility, Science and Technology Facilities Council, Research Complex at Harwell, Rutherford Appleton Laboratory
Christopher J. Tynan: Central Laser Facility, Science and Technology Facilities Council, Research Complex at Harwell, Rutherford Appleton Laboratory
Fiona C. Meldrum: School of Chemistry, University of Leeds

Nature Communications, 2016, vol. 7, issue 1, 1-13

Abstract: Abstract From biomineralization to synthesis, organic additives provide an effective means of controlling crystallization processes. There is growing evidence that these additives are often occluded within the crystal lattice. This promises an elegant means of creating nanocomposites and tuning physical properties. Here we use the incorporation of sulfonated fluorescent dyes to gain new understanding of additive occlusion in calcite (CaCO3), and to link morphological changes to occlusion mechanisms. We demonstrate that these additives are incorporated within specific zones, as defined by the growth conditions, and show how occlusion can govern changes in crystal shape. Fluorescence spectroscopy and lifetime imaging microscopy also show that the dyes experience unique local environments within different zones. Our strategy is then extended to simultaneously incorporate mixtures of dyes, whose fluorescence cascade creates calcite nanoparticles that fluoresce white. This offers a simple strategy for generating biocompatible and stable fluorescent nanoparticles whose output can be tuned as required.

Date: 2016
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DOI: 10.1038/ncomms13524

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