With a linearly polarized laser beam of wavelength λ= 1.06μm acting on the monolayer of the laser dye 2-(p-Dimethylaminostryry L)-Pyridyethyl iodide (DASPI) and the organic molecules N, N -diethyl-pseudoisocynanine chloride (PIC) on a smooth surface made of fused quarz or glass, the SHG by DASPI or PIG can be detected easily. By changing the direction of the linear polarization of the fundamental wave and ratating the substrate, we have found that axes (electrio-dipole) of both kinds of molecules are perpen.