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Calcite occurs widely as a mineral component in the exoskeletons and tissues of marine and freshwater invertebrates. Matrix macromolecules involved in regulating the biological growth of calcite in these organisms are known to share a carboxylic-rich character that arises from an abundance of the acidic amino acids aspartate (Asp) and glutamate (Glu). This study determines the interactions of Asp with calcite {101̄4} faces during dissolution using in situ fluid-cell atomic force microscopy (AFM) and macroscopic ex situ optical methods. In control experiments, etch-pit morphologies produced_by dissolution in simple undersaturated solutions reflect the inherent symmetry of the {101̄4} faces with a rhombus form. With the introduction of Asp. surface site reactivities are modified to yield isosceles triangular etch pits and hillocks. With continued exposure to Asp-bearing solutions, these triangular pits coalesce and the surface evolves into a network of interconnected tetrahedral etch hillocks. The component tetrahedral “sides”have Miller-Bravais indices of (0001), (1̄101), and (01̄11). These faces intersect the (101̄4) face in the [01̄0], [451̄], and [4̅11] directions to compose the tlnee edges of the triangular etch pits. Structural and stereo­chemical contraints suggest that the (1̄101) and (01̄11) faces in the hillock are a combi­nation of corresponding faces from the {1102} and {1̄100} crystallographic forms.

Surface site-specific interactions of aspartate with calcite during dissolution: Implications for biomineralization