Linear and Nonlinear Optical Properties of Photoresponsive [60]Fullerene Hybrid Triads and Tetrads with Dual NIR Two-Photon Absorption Characteristics.

Linear and Nonlinear Optical Properties of Photoresponsive [60]Fullerene Hybrid Triads and Tetrads with Dual NIR Two-Photon Absorption Characteristics.
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DOI:
10.1021/jp405424q
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发表时间:
2013-08-20
期刊:
The journal of physical chemistry. C, Nanomaterials and interfaces
影响因子:
--
通讯作者:
Chiang LY
Chiang LY
中科院分区:
其他
文献类型:
--
作者:
Jeon S;Haley J;Flikkema J;Nalla V;Wang M;Sfeir M;Tan LS;Cooper T;Ji W;Hamblin MR;Chiang LY

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合成并表征了两种具有三联体C60(>DPAF-C18)(>CPAF-C2M)和四联体C60(>DPAF-C18)(>CPAF-C2M)2纳米结构的C60-(天线)x类似物。这种结构设计的目的是为了促进光激发的C60[>1(DPAF)*-C18](>CPAF-C2M)1或2或C60(>DPAF-C18)[>1(CPAF)*-C2M]1或2分别在780 nm或980 nm的双光子泵浦下从分子内超快fS转移到C60>笼状部分。后一种纳米结构在400-550 nm范围内表现出大致相等的光吸收消光系数,相当于宽带非线性光学(NLO)应用的近红外双光子激发波长780-1100 nm。除了它们在780 nm处增强的双光子吸收(2PA)活性外,我们还展示了在980 nm处的超快光响应,杂化四分体的2PA截面(σ2)值为995-1100GM。这些σ-2值与在110GW/cm~2的光强下观察到的将飞秒透光率降低到35%的良好效果相关联。因此,这些纳米结构在多个近红外波长下的2PA特性为它们在600-1100 nm处用作宽带NLO纳米材料提供了支持,这包括两个天线的2PA能力,DPAF(700-850 nm)和CPAF(850-1100 nm),以及在较短波长(600-700 nm)的富勒烯笼子。
Two C60-(antenna)x analogous compounds having branched hybrid triad C60(>DPAF-C18)(>CPAF-C2M) and tetrad C60(>DPAF-C18)(>CPAF-C2M)2 nanostructures were synthesized and characterized. The structural design was intended to facilitate the ultrafast fs intramolecular energy-transfer from photoexcited C60[>1(DPAF)*-C18](>CPAF-C2M)1or2 or C60(>DPAF-C18)[>1(CPAF)*-C2M]1or2 to the C60> cage moiety upon two-photon pumping at either 780 or 980 nm, respectively. The latter nanostructure showed approximately equal extinction coefficients of optical absorption over 400–550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780–1100 nm for broadband nonlinear optical (NLO) applications. Aside from their enhanced two-photon absorption (2PA) activity at 780 nm, we also demonstrated ultrafast photo-responses at 980 nm showing 2PA cross-section (σ2) values of 995–1100 GM for the hybrid tetrad. These σ2 values were correlated to the observed good efficiency in reducing fs light-transmittance down to 35% at the light intensity of 110 GW/cm2. Accordingly, 2PA characteristics of these nanostructures at multiple NIR wavelengths provided support for their suitability in uses as broadband NLO nanomaterials at 600–1100 nm that includes the 2PA ability of two antenna, DPAF (700–850 nm) and CPAF (850–1100 nm), and the fullerene cage at shorter wavelengths (600–700 nm).
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