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Order-Disorder Transition of Carboxyl Terminated Chains in Polydiacetylenes Vesicles Probed by Second Harmonic Generation and Two-Photon Fluorescence
Shun-li Chen,Xue-feng Zhu,Fang-yuan Yang,Xue-cong Pan,Wei Gan*,Qun-hui Yuan*
Author NameAffiliationE-mail
Shun-li Chen Laboratory of Environmental Science and Technology, Xinjiang Technical Institute of Physics and Chemistry, Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, China  
Xue-feng Zhu Laboratory of Environmental Science and Technology, Xinjiang Technical Institute of Physics and Chemistry, Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, China  
Fang-yuan Yang Laboratory of Environmental Science and Technology, Xinjiang Technical Institute of Physics and Chemistry, Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, China  
Xue-cong Pan Laboratory of Environmental Science and Technology, Xinjiang Technical Institute of Physics and Chemistry, Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, China  
Wei Gan* Laboratory of Environmental Science and Technology, Xinjiang Technical Institute of Physics and Chemistry, Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, China;School of Sciences, Harbin Institute of Technology(Shenzhen), Shenzhen 518055, China ganwei@hit.edu.cn 
Qun-hui Yuan* School of Materials Science and Engineering, Harbin Institute of Technology(Shenzhen), Shenzhen 518055, China yuanqunhui@hit.edu.cn 
Abstract:
To understand and control the interfacial properties of polydiacetylenes (PDAs) vesicles with π-conjugated backbone is very important for their colorimetric sensing of chemical and biological targets. In this work, we adopted 10, 12-pentacosadiynoic acid (PCDA) as the model molecule to prepare PDAs vesicles in aqueous solution with different forms (from monomer to blue-to-purple-to-red phase) by controlling the UV irradiation dose. The variations of the interfacial conformation of PDAs vesicles during chromatic transitions were inspected by the adsorption behaviors of probe molecules (4-(4-diethylaminostyry)-1-methylpyridinium iodide, D289) on vesicle surface with surface-specific second harmonic generation (SHG) and zeta potential measurements. Resonant SHG signal from D289 adsorbed on vesicle surface attenuated sharply, and the adsorption free energy as well as the corresponding two-photon fluorescence signal decreased slightly in chromatic transitions. While, the change in the surface density of the adsorbed D289 molecules for PDAs vesicles with different forms was relatively small as estimated from zeta potential measurements. The attenuation of the SHG intensity was thus attributed to the overall order-disorder transition and the changed orientation of D289 molecules caused by the gradual distortion of carboxyl head group driven by backbone perturbation.
Key words:  Polydiacetylenes vesicle  Polymerization  interfacial adsorption  Second harmonic generation  Order-disorder transition
FundProject:This work was supported by the National Natural Science Foundation of China (No.21403292, No.21403293, No.21473249, and No.21673285), and the funding from the Shenzhen city (No.JCYJ20170307150520453).
聚联乙炔囊泡羧基端链有序-无序转变的二次谐波与双光子荧光研究
陈顺利,朱雪锋,杨方源,潘学聪,干为*,袁群惠*
摘要:
理解和调控具有π共轭骨架的聚联乙炔(PDAs)囊泡的界面特性对其变色传感化学及生物靶标分子的能力极其重要.本文采用联乙炔作为模型分子,通过调节紫外光辐照剂量制备了具有不同相态的PDAs水溶液样品(包括单体、蓝色相、紫色相和红色相).基于具有表面选择性的二次谐波(SHG)技术和zeta电位测量,通过探测探针分子D289在囊泡表面的吸附行为来研究PDAs囊泡变色过渡转变中界面构型的变化.SHG探测结果表明:在PDAs囊泡变色转变过程中,D289分子吸附贡献的共振SHG信号强度急剧衰减,对应的吸附自由能和双光子荧光信号强度均略有减小.依据zeta电位测量结果估算,具有不同相态的PDAs囊泡表面吸附D289分子的表面密度之间的差别相对较小.因此,SHG信号强度的衰减可归因于囊泡骨架结构发生扰动而驱动囊泡的羧基端链逐渐扭曲,进一步诱导D289分子取向变化及其整体结构的有序-无序转变.
关键词:  聚联乙炔囊泡  聚合  界面吸附  二次谐波  有序-无序转变
DOI:10.1063/1674-0068/31/cjcp1712238
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