Dissolution of the barite (001) surface in aqueous solutions of 0.18 M CDTA (trans-1,2-cyclohexylene-diaminetetraacetic acid) and 0.18 M EDTA (ethylenediaminetetraacetic acid) at pH 12 was investigated using ex situ scanning force microscopy. In both solutions, triangular and trapezoidal etch pits developed on the (001) surface and became deeper and longer with increasing dissolution time. The orientation of the etch pits in CDTA and EDTA solutions was elongated along the crystallographie b axis. Furthermore, dissolution of the (001) surface in a layer-by-layer fashion was observed. This resulted in the formation of "alternating" etch pits with heights of one half-unit cell (about 3.6 Angstrom), with the orientations of any two consecutive etch pits pointing oppositely to each other. In CDTA, etch pits within the half-unit cell were frequently bounded along the (120) and (010) directions. However, in EDTA, etch pits within the half-unit cell were bounded along the (110) and (010) directions. The dissolution behavior of barite in these two solutions is different based on the observed differences in the etch pits geometries as an assay for specific interactions between the crystal surface and organic molecules, Thus, we suggest that CDTA molecules bind to one Ba2+ cation along the (120) and/or (010) directions and EDTA molecules bind along the (110) directions to two Ba2+ cations exposed on the (001) surface.