4.7 Article

Critical Step Length as an Indicator of Surface Supersaturation during Crystal Growth from Solution

Journal

CRYSTAL GROWTH & DESIGN
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.cgd.1c01249

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Funding

  1. EPSRC [EP/R018820/1] Funding Source: UKRI

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This study demonstrates a method to determine local supersaturation by utilizing the thermodynamic feature of crystal surfaces, allowing for quantitative measurement of surface-controlled kinetics. By applying this method to calcite measurements, the discrepancies between growth rates measured under different mass transport conditions are resolved, and the departure of the Gibbs-Thomson effect in calcite from classical theory is revealed.
The surface processes that control crystal growth from solution can be probed in real-time by in situ microscopy. However, when mass transport (partly) limits growth, the interfacial solution conditions are difficult to determine, precluding quantitative measurement. Here, we demonstrate the use of a thermodynamic feature of crystal surfaces -the critical step length -to convey the local supersaturation, allowing the surface-controlled kinetics to be obtained. Applying this method to atomic force microscopy measurements of calcite, which are shown to fall within the regime of mixed surface/transport control, unites calcite step velocities with the Kossel-Stranski model, resolves disparities between growth rates measured under different mass transport conditions, and reveals why the Gibbs-Thomson effect in calcite departs from classical theory. Our approach expands the scope of in situ microscopy by decoupling quantitative measurement from the influence of mass transport.

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