On the basis of the framework of the terrace-ledge-kink model of disso
lution, the site-specific dissolution kinetics at the CaCO3(10(1) over
bar 4)-water interface have been investigated using atomic force micr
oscopy. The experiment was carried out in a solution cell where the ''
real-time'' dissolution kinetics were examined under different flow an
d temperature conditions. Results show that dissolution proceeds via t
he creation of pits and the retreat of steps on the surface. In the su
rface-reaction controlled regime, retreat of steps was found to be ani
sotropic with two different velocities. From the temperature dependenc
e of the two step velocities, the effective activation energies of dis
solution associated with different kink sites were obtained. The study
not only provides valuable information on the relationship between th
e atomic and the site-specific reactivity of the surfaces, but also qu
antitatively demonstrates the morphological variation of the CaCO3(10(
1) over bar 4) surface resulting from dissolution.