A monolayer of a 1:4 mixture of ( N,N'-dioctadecyl-4,4′-dicarboxamide-2,2′-bipyridine)-bis (2,2′-bipyridine)ruthenium(II) perchlorate (RuC18B) and dioctadecyldimethylammonium bromide (2C18NB) was deposited alternately with a monolayer of 2C18NB alone. A second harmonic signal from alternate Langmuir-Blodgett (LB) films was observed upon irradiation with an Nd:YAG laser at 1064 nm. When alternate LB films were excited with the third harmonic (355 nm, 0.1–10 mJ cm −2) of an Nd:YAG laser before irradiation of a 1064 nm pulse, the intensity of second harmonic light (SHL) from the LB films decreased depending on the intensity of the 355 nm pulse. The intensity of SHL was varied reversibly many times. Such photochemical modulation of SHL was most probably attributed to the difference of second order nonlinear coefficients between the ground and the excited state of the Ru-complex.
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