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Linear and third-order nonlinear optical properties for the heptamethine cyanine chromophore H-aggregates thin film

ISSN号：1674-1056
期刊名称：《中国物理B：英文版》
时间：0
分类：O6[理学—化学]
作者机构：[1]State Key Laboratory of Precision Spectroscopy, and Department of Physics, East China Normal University, Shanghai 200062, China, [2]School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China
相关基金：Supported by the National Natural Science Foundation of China （Grant No. 10574046）, National Key Project for Basic Research of China （Grant Nos. 2006CB806006 and 2006CB921105）, Program for Changjiang Scholars and Innovative Research Team in University （PCSIRT）, Program for New Century Excellent Talents in University （NCET-04-0420）, the Doctoral Program of High Education （Grant No. 20050269011 ）, Phosphor Program Sponsored by Shanghai Science and Technology Committee （Grant No. 06QH 14003）

作者： YUAN YiZhong[1,2], KANG HaiFeng[1], SUN ZhenRong[1], WANG ZuGeng[1]

关键词：铬, 密度泛函理论, 非线性光学, 三水平模式, 混合物, chromium tricarbonyl complexes, third-order nonlinear optics, three-level model, density functional theory

中文摘要：

退化四波浪的混合大小用在 532 nm 的 35 ps 脉搏，被采用了在 NH ₂-substituted 芳基戒指( 1 )或 unsubstituted 戒指( 2 )和他们的先锋 3-amino-9-ethylcarbazole ( AECz )调查二铬 tricarbonyl 建筑群η ⁶-bonded 的第三顺序的非线性的光参数到 3-amino-9-ethylcarbazole 。1 和 2 被发现是 42.9 × 1 的混合物的秒顺序 hyperpolarizability Y 0 ⁻³¹ 和 35.9 × 1 0 ⁻³¹ esu，分别地比 AECz 大约一个数量级。在分子结构和混合物的秒顺序 hyperpolarizability 之间的关系 1 和 2 基于三水平的模型和密度详细被探索功能的理论(DFT ) 计算。理论结果显示电子密度的空间分发在第三顺序的非线性的光性质有深刻角色。

英文摘要：

Degenerate four-wave mixing measurements, using the 35 ps pulses at 532 nm, have been employed to investigate the third-order nonlinear optical parameters of two chromium tricarbonyl complexes η6-bonded to 3-amino-9-ethylcarbazole at either the NH2-substituted aryl ring （1） or the unsubstituted ring （2） and their precursor 3-amino-9-ethylcarbazole （AECz）. The second-order hyperpolarizability y of the compounds 1 and 2 were found to be 42.9×10^-31 and 35.9×10^-31 esu, respectively, approximately one order of magnitude greater than AECz. The relation between the molecular structure and second-order hyperpolarizability of the compounds I and 2 was explored in detail based on the three-level model and the density functional theory （DFT） calculation. The theoretical results indicate that the spatial distribution of electron density has the profound role in the third-order nonlinear optical properties.

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