The inherently surface-specific technique of second-harmonic generation was employed to probe the adsorption of an organic molecule, a hemicyanine dye, on b-oriented silicalite-1 films in situ. Measurements were performed in a purpose-built cell for solution experiments. By measuring at two different polarization combinations of the fundamental and second-harmonic light, the orientation of the adsorbed molecules was measured continuously. It has been observed that the adsorbed molecules gradually align themselves with the straight pores of the zeolite crystallites, thus adsorbing into the pores.