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Phys Rev Lett. 2018 Mar 16;120(11):116101. doi: 10.1103/PhysRevLett.120.116101.

Resolving Point Defects in the Hydration Structure of Calcite (10.4) with Three-Dimensional Atomic Force Microscopy.

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Institute of Physical Chemistry, Johannes Gutenberg University Mainz, Duesbergweg 10-14, 55099 Mainz, Germany.
Graduate School Materials Science in Mainz, Staudinger Weg 9, 55128 Mainz, Germany.
Curtin Institute for Computation and Department of Chemistry, Curtin University, P.O. Box U1987, Perth, Western Australia 6845, Australia.
Division of Electrical Engineering and Computer Science, Kanazawa University, Kanazawa 920-1192, Japan.
The Institute for Geoscience Research (TIGeR), Curtin University, P.O. Box U1987, Perth, Western Australia 6845, Australia.
WPI Nano Life Science Institute (WPI-NanoLSI), Kanazawa University, Kanazawa 920-1192, Japan.
Physical Chemistry I, Bielefeld University, Universitätsstraße 25, 33615 Bielefeld, Germany.


It seems natural to assume that defects at mineral surfaces critically influence interfacial processes such as the dissolution and growth of minerals in water. The experimental verification of this claim, however, is challenging and requires real-space methods with utmost spatial resolution, such as atomic force microscopy (AFM). While defects at mineral-water interfaces have been resolved in 2D AFM images before, the perturbation of the surrounding hydration structure has not yet been analyzed experimentally. In this Letter, we demonstrate that point defects on the most stable and naturally abundant calcite (10.4) surface can be resolved using high-resolution 3D AFM-even within the fifth hydration layer. Our analysis of the hydration structure surrounding the point defect shows a perturbation of the hydration with a lateral extent of approximately one unit cell. These experimental results are corroborated by molecular dynamics simulations.

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