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매우 높은 오프-다이아고날 비선형 광학 특성을 가진 플루오르화 벤조사이아졸리움 기반의 유기 결정

new fluorinated benzothiazolium-based organic crystals with extremely large off-diagonal optical nonlinearity

초록/요약

For various application of nonlinear optics, π-conjugated organic materials have to exhibit large macroscopic diagonal and off-diagonal nonlinear optical response in crystalline state. We designed new organic ionic crystals consisting of fluorinated benzothiazolium based PM5FB (5-fluoro-2-(4-(4-(hydroxymethyl)piperidin-1-yl)styryl-3-methylbenzo[d]thiazol-3-ium) cation and various counter anions. We observed that PM5FB based chromophores have high thermal stability and microscopic optical nonlinearity. All of PM5FB based organic crystals have isomorphic series-type crystal structure formed by hydrogen bonding between cation and anion which is similar to previously reported PMB-T (2-(4-(4-(hydroxymethyl)piperidin-1-yl)styryl-3-methylbenzo[d]thiazol-3-ium 4-methylsulfonate) crystal. Surprisingly, it was investigated that PM5FB-CBS (5-fluoro-2-(4-(4-(hydroxymethyl)piperidin-1-yl)styryl-3-methylbenzo[d]thiazol-3-ium 4-chlorobenzenesulfonate) has molecular ordering of 56.7° which is very close to optimal angle for maximizing off-diagonal component. In THz generation experiment, off-diagonal term of PM5FB-CBS crystal shows a 3 times more efficient peak-to-peak THz electric field than diagonal term of standard inorganic ZnTe crystal and reduced dimples in the THz wave spectra which indicate that phonon mode was suppressed.

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목차

1. Introduction 1
2. Experiments 5
3. Results and Discussion 18
4. Conclusions 41
5. References 42

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