We investigated the J-aggregation process of pseudoisocyanine chloride at a mica/solution interface by using
tapping mode atomic force microscopy (TM-AFM) and polarization absorption measurements. At a mica/solution interface, pseudoisocyanine chlorides form J aggregates that have three-dimensional leaf-like island
structures. The islands are anisotropically oriented with respect to the lattice of a mica substrate. This anisotropic
alignment may result from the epitaxial interaction between the positively charged N atoms of the molecules
and the regularly aligned negative holes left by the dissociating K+ ions. On the basis of both the orientation
of islands to the lattice of a mica and the epitaxial interaction, we proposed that in the internal structure of
the J aggregate, the long axis of the dye molecules is parallel to the long axis of the islands.