Large Femtosecond Two-Photon Absorption Cross-Sections of Fullerosome Vesicle Nanostructures Derived from Highly Photoresponsive Amphiphilic C(60)-Light-Harvesting Fluorene Dyad.
Large Femtosecond Two-Photon Absorption Cross-Sections of Fullerosome Vesicle Nanostructures Derived from Highly Photoresponsive Amphiphilic C(60)-Light-Harvesting Fluorene Dyad.
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由高光响应性两亲性 C(60)-光捕获芴二元组衍生的富勒体囊泡纳米结构的大飞秒双光子吸收横截面。
DOI：
10.1021/jp207047k
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发表时间：
2011
期刊：
影响因子：
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通讯作者：
Chiang,LongY
中科院分区：
文献类型：
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作者：
Wang,Min;Nalla,Venkatram;Jeon,Seaho;Mamidala,Venkatesh;Ji,Wei;Tan,Loon-Seng;Cooper,Thomas;Chiang,LongY
我们展示了双层富勒体囊泡纳米结构的超快飞秒非线性光学（NLO）吸收特性，该纳米结构源自两亲寡聚（乙二醇）C60-（光捕获二苯氨基芴天线）的分子自组装。富勒烯缀合物旨在通过在 C60 笼和二苯氨基芴天线亚基之间应用可异构化的共轭连接体，以仅 <3.0 Å 的分子内接触距离增强飞秒时间尺度的光响应。基于 C60(>DPAF-EG12C1) 的富勒体纳米囊泡在水中的形态特征为由双层壳组成，球体直径为 20-70 nm，发色团壳宽度为 9.0-10 nm，与分子长度的头对头堆积结构很好地吻合。当水中的估计有效纳米囊泡浓度低至 5.5 × 10–8MV（分子摩尔浓度为 5.0 × 10–4M）时，发现双光子吸收 (2PA) 现象是主要的光物理事件，显示出大摩尔浓度不敏感的 2PA 横截面值，平均相当于纳米囊泡形式的 8500 GM。观察到的 NLO 特性导致输入激光强度高于 100 GW/cm2 时，光透射强度出现有效降低的急剧趋势。
We demonstrated ultrafast femtosecond nonlinear optical (NLO) absorption characteristics of bilayered fullerosome vesicle nanostructures derived from molecular self-assembly of amphiphilic oligo(ethylene glycolated) C60-(light-harvesting diphenylaminofluorene antenna). Fullerene conjugates were designed to enhance photoresponse in a femtosecond time scale by applying an isomerizable periconjugation linker between the C60cage and a diphenylaminofluorene antenna subunit in an intramolecular contact distance of only <3.0 Å. Morphology of C60(>DPAF-EG12C1)-based fullerosome nanovesicles in H2O was characterized to consist of a bilayered shell with a sphere diameter of 20–70 nm and a chromophore shell width of 9.0–10 nm, fitting well with a head-to-head packing configuration of the molecular length. At the estimated effective nanovesicle concentration as low as 5.5 × 10–8MV (molecular molar concentration of 5.0 × 10–4M) in H2O, two-photon absorption (2PA) phenomena were found to be the dominating photophysical events showing a large molar concentration-insensitive 2PA cross-section value equivalent to 8500 GM in a form of nanovesicles, on average. The observed NLO characteristics led to a sharp trend of efficient light-transmittance intensity reduction at the input laser intensity above 100 GW/cm2.