We show that single atomic layer growth can be induced, controlled, and characterized using atomic force microscopy (AFM). The controlling parameters include contact force, solution chemistry, and scanning direction relative to the crystal axes. We present new evidence for the role of AFM tip motion across terraces in inducing localized deposition in pre-existing pits on otherwise atomically smooth surfaces. Low contact force scanning also hinders major roughening mechanisms, including 3D nucleation and growth, by tribochemically dissolving these deposits. Consequently, atomically flat surfaces can be generated. Finally, we show a new method of “scribing” <40 nm wide lines a single atomic layer deep on inorganic substrates. The materials under study are model biominerals: calcite (CaCO3) and brushite (CaHPO42H2O). Thus this work relates to the production of smooth surfaces on bone-like materials..

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