Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 128, Issue 18, Pages 6194-6205Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja060185v
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A novel type of X-shaped two-dimensional electro-optic (EO) chromophore with extended conjugation has been synthesized and characterized. This chromophore is found to exhibit a remarkably blue-shifted optical maximum (357 nm in CH2Cl2) while maintaining a very large first hyperpolarizability (beta). Hyper-Rayleigh Scattering (HRS) measurements at 800 nm provide a beta(zzz) value of 1840 x 10(-30) esu. Self-assembled thin films of this chromophore were fabricated via a layer-by-layer chemisorptive siloxane-based approach. The chromophoric multilayers have been characterized by transmission optical spectroscopy, advancing contact angle measurements, synchrotron X-ray reflectivity, atomic force microscopy, and angle-dependent polarized second harmonic generation spectroscopy. The self-assembled chromophoric films exhibit a dramatically blue-shifted optical maximum ( 325 nm) while maintaining a large EO response (chi((2))(333) similar to 232 pm/V at 1064 nm; r(33) similar to 45 pm/V at 1310 nm). This work demonstrates an attractive approach to developing EO materials offering improved nonlinearity-transparency trade-offs.
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