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25 February 1993 Dispersion of the molecular second-order nonlinear optical susceptibilities of nitropyridine derivatives
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Molecular second-order nonlinear optical properties of a series of interesting nitropyridine derivatives, namely 2-cyclooctylamino-5-nitropyridine (COANP), 2-docosylamino-5- nitropyridine (DCANP), and 2-(N-prolinol)-5-nitropyridine (PNP) were investigated with two different methods: electric field-induced second-harmonic generation (EFISH) and a solvatochromic method. Both techniques yield the same values within the experimental errors, showing that the main contribution of the microscopic nonlinearity arises from a single intramolecular charge transfer transition. The measured values were shown to follow the theoretical two-level dispersion. A comparison of the hyperpolarizabilities and the macroscopic nonlinear optical coefficients shows a good quantitative agreement. This illustrates that intramolecular contributions are the main source for the large nonlinear optical responses observed in these crystals.
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Christian Bosshard, Guenter Knoepfle, Philippe Pretre, and Peter Guenter "Dispersion of the molecular second-order nonlinear optical susceptibilities of nitropyridine derivatives", Proc. SPIE 1775, Nonlinear Optical Properties of Organic Materials V, (25 February 1993);

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