Laser beam at λ=1.06 μm was used as fundamental wave to irradiate on the adsorbed layers of the photosynthetic pigment molecules (baoteriochlorophyll and phycocyanin) on the optical surface. The harmonic generation is observed. It is discussed that the adsorbed layer of phyoooyanin can generate only third harmonic (THG) not second harmonic (SHG).