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利用单分子光学探针测量幂律分布的聚合物动力学

李斌 张国峰 景明勇 陈瑞云 秦成兵 高岩 肖连团 贾锁堂

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Citation:

利用单分子光学探针测量幂律分布的聚合物动力学

李斌, 张国峰, 景明勇, 陈瑞云, 秦成兵, 高岩, 肖连团, 贾锁堂

Single molecule optical-probes measured power law distribution of polymer dynamics

Li Bin, Zhang Guo-Feng, Jing Ming-Yong, Chen Rui-Yun, Qin Cheng-Bing, Gao Yan, Xiao Lian-Tuan, Jia Suo-Tang
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  • 研究聚合物薄膜纳米尺度的动力学特性对于高性能材料的制备具有重要的意义.本文利用尼罗红单分子作为光学探针吸附在聚丙烯酸甲酯(PMA)聚合物链上,研究该聚合物薄膜的动力学特性.通过单分子散焦宽场荧光成像显微镜技术测量了单分子随PMA聚合物链转动弛豫的三维再取向特性,当环境温度高于PMA的玻璃点温度19 K时,发现处于PMA聚合物薄膜中的单分子光学探针的转动态和非转动态的持续时间概率密度服从指数截止的幂律分布.研究结果表明该温度下PMA聚合物薄膜的纳米环境动力学仍存在空间和时间异构性.
    The optical signals of single molecules provide information about structures and dynamic behaviors of their nanoscale environments, and eliminations of space and time averaging effect. These are particularly useful whenever complex structures or dynamic behaviors are present, especially in polymers. The single molecules absorbed onto polymer chains rotate with rotational relaxation of polymer chains. Thus, we can measure the dynamic properties of polymer thin films by measuring the rotational properties of single molecules. Here, we use single Nile Red(NR) dye molecules as nano-probes to measure polymer dynamic behaviors of poly(methyl acrylate)(PMA) polymer film. The polymer films are prepared on cleaned glass coverslips by spin-coating 1.0 wt.%solution of PMA containing ~10-9 mol/L NR molecules in toluene. Defocused wide-field fluorescence microscopy is used to measure the three-dimensional molecular rotational diffusion of single NR molecules in PMA polymer thin film. The local environmental change driven by heterogeneous dynamics of the polymer can be probed by parallel imaging of several molecules. It is found that at Tg+19 K, rotations of NR single molecules in different nano-areas are in two different ways, i.e., rotational way(rotational molecules account for ~83%) and non-rotaional way(non-rotational molecules occupy~17%). The rotational molecules include the single molecules of intermittent rotation with a short time and a long time. The different rotational patterns indicate that there is still a spatial and temporal heterogeneity of dynamics in PMA polymer film at a temperature of Tg+19 K. The autocorrelation function C(t) of angular change of dipole orientation of NR single molecules is calculated to reveal the property of polymer dynamics. The decay of C(t) can be fitted by Kohlrausch-Williams-Watt stretched exponential function. The averaged timescale of rotational diffusion c for 183 rotational NR single molecules indicates that the timescale of polymer dynamics at 300 K is~3 s. In order to investigate the temporal heterogeneity of PMA polymer dynamics, we define a threshold to separate the single molecular rotation into two parts:rotational state and non-rotational state. According to the statistics of duration time of rotational state and non-rotational state, we can obtain the probability densities of duration time of rotational states and non-rotational states of the single molecules. The probability densities obey a truncated power law, which indicates that there are still the behaviors of trapping and self-trapping in PMA polymer chains at Tg+19 K. The researches of spatial and temporal heterogeneity of dynamics of PMA polymers in nano-environment have great significance for preparing the high performance materials.
      通信作者: 肖连团, guofeng.zhang@sxu.edu.cn;xlt@sxu.edu.cn
    • 基金项目: 国家重点基础研究发展计划(批准号:2012CB921603)、国家自然科学基金(批准号:61527824,11434007,11374196,11404200,11504216,U1510133)、教育部长江学者和创新团队发展计划(批准号:IRT13076)、中国博士后科学基金(批准号:2014M550151)和山西省留学回国人员科技活动择优项目资助的课题.
      Corresponding author: Xiao Lian-Tuan, guofeng.zhang@sxu.edu.cn;xlt@sxu.edu.cn
    • Funds: Project supported by the National Basic Research Program of China(Grant No. 2012CB921603), the National Natural Science Foundation of China(Grant Nos. 61527824, 11434007, 11374196, 11404200, 11504216, U1510133), the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(Grant No. IRT13076), the China Postdoctoral Science Foundation(Grant No. 2014M550151), and the Fund Program for the Scientific Activities of Selected Returned Overseas Professionals in Shanxi Province, China.
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    Zhang G F, Zhang F, Cheng F Y, Sun J H, Xiao L T, Jia S T 2009 Acta Phys. Sin. 58 2364(in Chinese)[张国峰, 张芳, 程峰钰, 孙建虎, 肖连团, 贾锁堂2009物理学报58 2364]

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    Vogelsang J, Brazard J, Adachi T, Bolinger J C, Barbara P F 2011 Angew. Chem. Int. Edit. 50 2257

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    Vallee R A L, Cotlett M, van der Auweraer M, Hofkens J, Mullen K, de Schryver F C 2004 J. Am. Chem. Soc. 126 2296

    [32]

    Uji-i H, Melnikov S M, Deres A, Bergamini G, de Schryver F, Herrmann A, Mllen K, Enderlein J, Hofkens J 2006 Polymer 47 2511

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    Cser A, Nagy K, Biczok L 2002 Chem. Phys. Lett. 360 473

    [34]

    Yoo H, Furumaki S, Yang J, Lee J E, Chung H, Oba T, Kobayashi H, Rybtchinski B, Wilson T M, Wasielewski M R, Vacha M, Kim D 2012 J. Phys. Chem. B 116 12878

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    Wang Z, Zhang G F, Li B, Chen R Y, Qin C B, Xiao L T, Jia S T 2015 Acta Phys. Sin. 64 247803(in Chinese)[王早, 张国峰, 李斌, 陈瑞云, 秦成兵, 肖连团, 贾锁堂2015物理学报64 247803]

  • [1]

    Orrit M, Ha T, Sandoghdar V 2014 Chem. Soc. Rev. 43 973

    [2]

    Janssen K P F, de Cremer G, Neely R K, Kubarev A V, van Loon J, Martens J A, de Vos D E, Roeffaers M B J, Hofkens J 2014 Chem. Soc. Rev. 43 990

    [3]

    Kern A M, Zhang D, Brecht M, Chizhik A I, Failla A V, Wackenhut F, Meixner A J 2014 Chem. Soc. Rev. 43 1263

    [4]

    Kozankiewicz B, Orrit M 2014 Chem. Soc. Rev. 43 1029

    [5]

    Stennett E M S, Ciuba M A, Levitus M 2014 Chem. Soc. Rev. 43 1057

    [6]

    van de Linde S, Sauer M 2014 Chem. Soc. Rev. 43 1076

    [7]

    Zheng Y J, Zhang Z Y, Zhang X Z 2009 Acta Phys. Sin. 58 8194(in Chinese)[郑雨军, 张兆玉, 张西忠2009物理学报58 8194]

    [8]

    Han B P, Zheng Y J, Hu F, Fan Q B 2015 Chin. Phys. Lett. 32 063303

    [9]

    Orrit M 2014 Nat. Photon. 8 887

    [10]

    Oh H, Green P F 2009 Nat. Mater. 8 139

    [11]

    Wöll D, Braeken E, Deres A, de Schryver F C, Uji-i H, Hofkens J 2009 Chem. Soc. Rev. 38 313

    [12]

    Gaiduk A, Yorulmaz M, Ruijgrok P V, Orrit M 2010 Science 330 353

    [13]

    Hutchison J A, Uji-i H, Deres A, Vosch T, Rocha S, Muller S, Bastian A A, Enderlein J, Nourouzi H, Li C, Herrmann A, Mullen K, de Schryver F, Hofkens J 2014 Nat. Nanotech. 9 131

    [14]

    Stigler J, Ziegler F, Gieseke A, Gebhardt J C M, Rief M 2011 Science 334 512

    [15]

    Rezus Y L, Walt S G, Lettow R, Renn A, Zumofen G, Gotzinger S, Sandoghdar V 2012 Phys. Rev. Lett. 108 093601

    [16]

    Puller V, Lounis B, Pistolesi F 2013 Phys. Rev. Lett. 110 125501

    [17]

    Graves E T, Duboc C, Fan J, Stransky F, Leroux-Coyau M, Strick T R 2015 Nat. Struct. Mol. Biol. 22 452

    [18]

    Sugo N, Morimatsu M, Arai Y, Kousoku Y, Ohkuni A, Nomura T, Yanagida T, Yamamoto N 2015 Sci. Rep. 5 10662

    [19]

    Kulzer F, Xia T, Orrit M 2010 Angew Chem. Int. Ed. Engl. 49 854

    [20]

    Paeng K, Kaufman L J 2014 Chem. Soc. Rev. 43 977

    [21]

    Piwonski H, Sokolowski A, Waluk J 2015 J. Phys. Chem. Lett. 6 2477

    [22]

    Krause S, Neumann M, Frobe M, Magerle R, von Borczyskowski C 2016 ACS Nano 10 1908

    [23]

    Bolinger J C, Traub M C, Adachi T, Barbara P F 2016 Science 331 565

    [24]

    Zhang G F, Zhang F, Cheng F Y, Sun J H, Xiao L T, Jia S T 2009 Acta Phys. Sin. 58 2364(in Chinese)[张国峰, 张芳, 程峰钰, 孙建虎, 肖连团, 贾锁堂2009物理学报58 2364]

    [25]

    Deres A, Floudas G A, Mllen K, van der Auweraer M, de Schryver F, Enderlein J, Uji-i H, Hofkens J 2011 Macromolecules 44 9703

    [26]

    Vogelsang J, Brazard J, Adachi T, Bolinger J C, Barbara P F 2011 Angew. Chem. Int. Edit. 50 2257

    [27]

    Abadi M, Serag M F, Habuchi S 2015 Macromolecules 48 6263

    [28]

    Zhang G, Xiao L, Zhang F, Wang X, Jia S 2010 Phys. Chem. Chem. Phys. 12 2308

    [29]

    Habuchi S, Fujiwara S, Yamamoto T, Vacha M, Tezuka Y 2013 Anal. Chem. 85 7369

    [30]

    Schob A, Cichos F, Schuster J, von Borczyskowski C 2004 Eur. Polym. J. 40 1019

    [31]

    Vallee R A L, Cotlett M, van der Auweraer M, Hofkens J, Mullen K, de Schryver F C 2004 J. Am. Chem. Soc. 126 2296

    [32]

    Uji-i H, Melnikov S M, Deres A, Bergamini G, de Schryver F, Herrmann A, Mllen K, Enderlein J, Hofkens J 2006 Polymer 47 2511

    [33]

    Cser A, Nagy K, Biczok L 2002 Chem. Phys. Lett. 360 473

    [34]

    Yoo H, Furumaki S, Yang J, Lee J E, Chung H, Oba T, Kobayashi H, Rybtchinski B, Wilson T M, Wasielewski M R, Vacha M, Kim D 2012 J. Phys. Chem. B 116 12878

    [35]

    Wang Z, Zhang G F, Li B, Chen R Y, Qin C B, Xiao L T, Jia S T 2015 Acta Phys. Sin. 64 247803(in Chinese)[王早, 张国峰, 李斌, 陈瑞云, 秦成兵, 肖连团, 贾锁堂2015物理学报64 247803]

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出版历程
  • 收稿日期:  2016-06-14
  • 修回日期:  2016-07-31
  • 刊出日期:  2016-11-05

利用单分子光学探针测量幂律分布的聚合物动力学

  • 1. 山西大学激光光谱研究所, 量子光学与光量子器件国家重点实验室, 太原 030006;
  • 2. 山西大学极端光学协同创新中心, 太原 030006
  • 通信作者: 肖连团, guofeng.zhang@sxu.edu.cn;xlt@sxu.edu.cn
    基金项目: 国家重点基础研究发展计划(批准号:2012CB921603)、国家自然科学基金(批准号:61527824,11434007,11374196,11404200,11504216,U1510133)、教育部长江学者和创新团队发展计划(批准号:IRT13076)、中国博士后科学基金(批准号:2014M550151)和山西省留学回国人员科技活动择优项目资助的课题.

摘要: 研究聚合物薄膜纳米尺度的动力学特性对于高性能材料的制备具有重要的意义.本文利用尼罗红单分子作为光学探针吸附在聚丙烯酸甲酯(PMA)聚合物链上,研究该聚合物薄膜的动力学特性.通过单分子散焦宽场荧光成像显微镜技术测量了单分子随PMA聚合物链转动弛豫的三维再取向特性,当环境温度高于PMA的玻璃点温度19 K时,发现处于PMA聚合物薄膜中的单分子光学探针的转动态和非转动态的持续时间概率密度服从指数截止的幂律分布.研究结果表明该温度下PMA聚合物薄膜的纳米环境动力学仍存在空间和时间异构性.

English Abstract

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