单分子动力学特性的测量及操控
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摘要
经过二十多年的发展,单分子光谱学已经逐渐从低温光谱方法演化为一个通用的工具,被广泛用于研究物理、化学、生物和材料科学中的各类相关问题。单分子消除了系综平均,可以作为一个纳米光学探针探测它们所处局部环境的结构和动力学信息,这些信息对研究复杂的聚合物材料或其他种类的复杂物质具有重要的意义,单分子光谱可以提供纳米尺度环境的精细图像,展示了局部环境的异构和异于系综平均的信息。染料荧光单分子已经被用作纳米尺度的量子元件或部件,如触发的单光子源和单分子开关,同时这种有机染料分子材料能够用于下一代的半导体器件,如有机发光二极管、有机场效应管和有机太阳能电池等。研究有机单分子与金属、半导体等材料之间的相互作用以及对电场、电流的响应特性可以为制备分子量子器件与分子器件奠定理论基础与技术储备。
本文主要工作是探测了在室温条件下单分子在液体环境和聚合物薄膜表面及内部的动力学特性,并分别利用电场和电流来操控分子的动力学特性。通过宽场照明成像和共焦扫描系统两种手段跟踪测量了单分子在液体环境下的随机扩散运动的性质；基于共焦扫描光学实验系统和荧光偏振探测相结合的方法测量了聚合物PMMA薄膜上单分子的偶极再取向动力学特性；通过散焦成像和环形照明的技术手段测量了单分子在聚合物薄膜中的转动动力学。研究了电场作用下单分子的荧光偏振度和荧光发射强度的变化,并通过建立相关的理论模型解释了观察到的实验现象。研究了有机染料分子/半导体纳米粒子系统中系综分子和单分子的界面电子转移动力学特性；测量了电流作用下的单分子荧光强度和荧光寿命的变化,并对实验结果进行了数值模拟。
本论文工作的创新点：
1.测量了聚合物PMMA薄膜表面单分子的动力学特性,首次发现单分子的偶极再取向具有三种典型的跳跃模式,利用转动关联时间表征聚合物薄膜表面的动力学特征,测量获得PMMA薄膜表面单分子的平均转动关联时间约为0.1s。
2.基于宽场荧光显微镜对单分子实现散焦光学成像,利用其成像的特征强度分布获得单分子荧光发射的角分布特性,测量了单分子在聚合物薄膜中的平动与转动动力学,同时实现了多个分子的取向跟踪测量。
3.利用50V/μm的电场强度操控PMMA聚合物薄膜中的染料单分子的荧光强度,通过测量单分子荧光强度对电场响应特性,发现分子荧光对电场响应的滞后效应以及分子荧光对电场操控存在的记忆效应。
4.首次将电流引入染料单分子／半导体纳米粒子(IT0)系统中,观察到了电流操控下的单分子荧光强度和寿命的变化,在10-50mA/mm2的电流强度作用下有效地熄灭或增强单分子的荧光辐射,数值计算模拟结果与实验结果相吻合。研究发现平衡费米能级和最高占据分子轨道(HOMO)能级之差△Eg决定着两种不同类型的分子动力学变化特性,当△Eg<0时,分子荧光会发生熄灭；当△Eg>0时,分子荧光会出现增强。
Over the past twenty years, single-molecule spectroscopy has evolved from a specialized variety of optical spectroscopy at low temperatures into a versatile tool used to address a broad range of questions in physics, chemistry, biology, and materials science. The optical detection of single molecules provides information about structures and dynamics of their nanoscale environment, free from space and time averaging. These data are particularly useful whenever complex structures or dynamics are present, as in polymers or in porous oxides, but also in many other classes of materials, where heterogeneity is less obvious. Single molecules provide a detailed picture of condensed matter, often revealing surprisingly large inhomogeneity and deviations from the average. Recent work aims at using single molecules as nanoparts or nanoelements in a variety of molecular-scale devices, from triggered sources of single photons to single-molecular switches. This organic dye molecular material also can be used for the next generation of semiconductor devices. Effectively directed material development, however, requires microscopic information on the relationship between chemical structure and physical properties, which is accessible through measurements on single molecules. To understand the intrinsic properties of a molecular semiconductor in a device configuration, such as a light-emitting diode or a field-effect transistor and solar cells, it is imperative to study the behaviour of single molecules under the influence of an external electric field and electric current.
The main work in the PHD thesis is that the measurement of dynamics of single molecules in glycerin, polymer, and on the surface of polymer, and manipulation of molecular fluorescence by using of electric voltage and current. The diffusion dynamics of single-molecule in glycerin was tracked by the method of image of wide-field microscopy and the track of confocal fluorescence microscopy, respectively. The reorientation dynamics of single molecules adsorbed onto the polymer films surface was measured by scanning confocal microscopy combined with fluorescence polarization analysis. The methods of defocused wide-field imaging and annular illumination were used to measure single molecules rotational diffusion in the glassy polymer also. The polarization and intensity of molecular fluorescence were manipulated by the electric voltage and the theory models proposed were used to explain the observed phenomenon. An external electric current was applied to dyes/ITO system, we find that the fluorescence emission of single-molecule can be enhanced or quenched. A concise model based on semi-empirical charge transport description is proposed and discussed to interpret the observed change of intensity under EEC.
The innovations of this paper:
1. We probe dynamics with reorientation of single dye molecules spin-coated onto polymer films Rotation jumps in transition dipole orientation are observed for approximately 30% of all single molecules. It is found for the first time that there are mainly three typical jumping patterns of orientation:dithering jump, alternate jump and stepping jump patterns. The distributon of rotational correlation time are used to characterize the dynamics of polymer glasses surface. It is found that～0.1 s is a reasonable mean time scale for the dynamics of the polymer glasses surface.
2. Defocused wide-field fluorescence microscopy was used to trace the 3D rotational diffusion of a fluorescence molecule in a polymer thin film. Orientation dynamics of single molecules can be obtained from the features of intensity distribution of single-molecule fluorescence. The diffusion and rotational dynamics of single molecules are measured simultaneously.
2. The fluorescence intensity of single dye molecules embedded in PMMA is modulated by electric field, we observed that a large delaying hysteresis response and the voltage dependence of fluorescence. The phenomenon never been reported previously.
3. We study the dyes/ITO nanoparticle system under external electric current for the first time. The fluorescence emission of single-molecule can be quenched or enhanced by adjusting electric current of 10-50mA/mm2 which is applied to the DiD/ITO nanoparticle system. The calculated results agree with the experimental data and in particular, both the experiment and the simulation have found two kinds of molecules. This is a consequence of different relative positions of the molecular HOMO energy E1 with respect to the material equilibrium Fermi energy EF0. The molecule would show quenching of fluorescence emission under voltage when AEg< 0, and enhancement (firstly enhancing and then quenching) when AEg> 0.
本文主要工作是探测了在室温条件下单分子在液体环境和聚合物薄膜表面及内部的动力学特性,并分别利用电场和电流来操控分子的动力学特性。通过宽场照明成像和共焦扫描系统两种手段跟踪测量了单分子在液体环境下的随机扩散运动的性质；基于共焦扫描光学实验系统和荧光偏振探测相结合的方法测量了聚合物PMMA薄膜上单分子的偶极再取向动力学特性；通过散焦成像和环形照明的技术手段测量了单分子在聚合物薄膜中的转动动力学。研究了电场作用下单分子的荧光偏振度和荧光发射强度的变化,并通过建立相关的理论模型解释了观察到的实验现象。研究了有机染料分子/半导体纳米粒子系统中系综分子和单分子的界面电子转移动力学特性；测量了电流作用下的单分子荧光强度和荧光寿命的变化,并对实验结果进行了数值模拟。
本论文工作的创新点：
1.测量了聚合物PMMA薄膜表面单分子的动力学特性,首次发现单分子的偶极再取向具有三种典型的跳跃模式,利用转动关联时间表征聚合物薄膜表面的动力学特征,测量获得PMMA薄膜表面单分子的平均转动关联时间约为0.1s。
2.基于宽场荧光显微镜对单分子实现散焦光学成像,利用其成像的特征强度分布获得单分子荧光发射的角分布特性,测量了单分子在聚合物薄膜中的平动与转动动力学,同时实现了多个分子的取向跟踪测量。
3.利用50V/μm的电场强度操控PMMA聚合物薄膜中的染料单分子的荧光强度,通过测量单分子荧光强度对电场响应特性,发现分子荧光对电场响应的滞后效应以及分子荧光对电场操控存在的记忆效应。
4.首次将电流引入染料单分子／半导体纳米粒子(IT0)系统中,观察到了电流操控下的单分子荧光强度和寿命的变化,在10-50mA/mm2的电流强度作用下有效地熄灭或增强单分子的荧光辐射,数值计算模拟结果与实验结果相吻合。研究发现平衡费米能级和最高占据分子轨道(HOMO)能级之差△Eg决定着两种不同类型的分子动力学变化特性,当△Eg<0时,分子荧光会发生熄灭；当△Eg>0时,分子荧光会出现增强。
Over the past twenty years, single-molecule spectroscopy has evolved from a specialized variety of optical spectroscopy at low temperatures into a versatile tool used to address a broad range of questions in physics, chemistry, biology, and materials science. The optical detection of single molecules provides information about structures and dynamics of their nanoscale environment, free from space and time averaging. These data are particularly useful whenever complex structures or dynamics are present, as in polymers or in porous oxides, but also in many other classes of materials, where heterogeneity is less obvious. Single molecules provide a detailed picture of condensed matter, often revealing surprisingly large inhomogeneity and deviations from the average. Recent work aims at using single molecules as nanoparts or nanoelements in a variety of molecular-scale devices, from triggered sources of single photons to single-molecular switches. This organic dye molecular material also can be used for the next generation of semiconductor devices. Effectively directed material development, however, requires microscopic information on the relationship between chemical structure and physical properties, which is accessible through measurements on single molecules. To understand the intrinsic properties of a molecular semiconductor in a device configuration, such as a light-emitting diode or a field-effect transistor and solar cells, it is imperative to study the behaviour of single molecules under the influence of an external electric field and electric current.
The main work in the PHD thesis is that the measurement of dynamics of single molecules in glycerin, polymer, and on the surface of polymer, and manipulation of molecular fluorescence by using of electric voltage and current. The diffusion dynamics of single-molecule in glycerin was tracked by the method of image of wide-field microscopy and the track of confocal fluorescence microscopy, respectively. The reorientation dynamics of single molecules adsorbed onto the polymer films surface was measured by scanning confocal microscopy combined with fluorescence polarization analysis. The methods of defocused wide-field imaging and annular illumination were used to measure single molecules rotational diffusion in the glassy polymer also. The polarization and intensity of molecular fluorescence were manipulated by the electric voltage and the theory models proposed were used to explain the observed phenomenon. An external electric current was applied to dyes/ITO system, we find that the fluorescence emission of single-molecule can be enhanced or quenched. A concise model based on semi-empirical charge transport description is proposed and discussed to interpret the observed change of intensity under EEC.
The innovations of this paper:
1. We probe dynamics with reorientation of single dye molecules spin-coated onto polymer films Rotation jumps in transition dipole orientation are observed for approximately 30% of all single molecules. It is found for the first time that there are mainly three typical jumping patterns of orientation:dithering jump, alternate jump and stepping jump patterns. The distributon of rotational correlation time are used to characterize the dynamics of polymer glasses surface. It is found that～0.1 s is a reasonable mean time scale for the dynamics of the polymer glasses surface.
2. Defocused wide-field fluorescence microscopy was used to trace the 3D rotational diffusion of a fluorescence molecule in a polymer thin film. Orientation dynamics of single molecules can be obtained from the features of intensity distribution of single-molecule fluorescence. The diffusion and rotational dynamics of single molecules are measured simultaneously.
2. The fluorescence intensity of single dye molecules embedded in PMMA is modulated by electric field, we observed that a large delaying hysteresis response and the voltage dependence of fluorescence. The phenomenon never been reported previously.
3. We study the dyes/ITO nanoparticle system under external electric current for the first time. The fluorescence emission of single-molecule can be quenched or enhanced by adjusting electric current of 10-50mA/mm2 which is applied to the DiD/ITO nanoparticle system. The calculated results agree with the experimental data and in particular, both the experiment and the simulation have found two kinds of molecules. This is a consequence of different relative positions of the molecular HOMO energy E1 with respect to the material equilibrium Fermi energy EF0. The molecule would show quenching of fluorescence emission under voltage when AEg< 0, and enhancement (firstly enhancing and then quenching) when AEg> 0.
引文
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