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首页> 美国政府科技报告 >Probing Structure-Property Relationships in Third-Order Nonlinear Optical Polymers: Third Harmonic Generation Spectroscopy and Theoretical Modeling of Systematically Derivatized Conjugated Aromatic Polyimines
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Probing Structure-Property Relationships in Third-Order Nonlinear Optical Polymers: Third Harmonic Generation Spectroscopy and Theoretical Modeling of Systematically Derivatized Conjugated Aromatic Polyimines

机译：探讨三阶非线性光学聚合物的结构 - 性质关系：三次谐波产生光谱和系统衍生的共轭芳香多胺的理论模型

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Picosecond third harmonic generation (THG) spectroscopy in the range 0.9-2.4 microns (0.52-1.38 eV) combined with sum-over-states (SOS) theoretical modeling have been used to investigate the third-order nonlinear optical properties of a series of 9 conjugated aromatic polyimines designed to elucidate structure-Chi(3) relationships in conjugated polymers. The THG-measured frequency dispersed third-order susceptibility Chi(3) of the series of polymers has off-resonant and three-photon resonance-enhanced values in the range of 1.1 x 10 to the -12th power to 2.0 x 10 to the -11 power esu and 6.4 x 10 to the -12 power to 7.2 x 10 to the -11th power esu, respectively, demonstrating a large modulation of nonlinear optical response by simple structural variations. A random copolymer was found to have enhanced Chi(3) compared to either of its parent homopolymers. Asymmetric donor side- group substitutions was found to result in 7-10-fold enhancement of off-resonant Chi(3) compared to either symmetric substitutions or no substitutions. Theoretical three and four-level SOS models, justified by site-selective fluorescence spectroscopy, were found to describe the Chi(3) dispersion data and the observed multiphoton resonances very well. The zero- frequency Chi(3) was predicted from the SOS models to be negative for eight of the nine polymers and to be in the range of -0.43 to 8.12 x 10 to the -12 power esu, The magnitudes of which are very close to observed off-resonance values at 2.4 microns (0.52 eV).

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