核壳纳米晶ZnSe@CdS（e）和碳纳米管/ZnSe@CdSe纳米晶异质结的制备及其光学性质研究
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摘要
纳米材料和纳米结构以其特异的物理化学性质引起研究者的广泛关注。纳米组装体系的结构与性质研究成为现在研究的热点。由于纳米结构材料是获取并发展纳米器件的基础,低维纳米结构材料又具有独特的物理和化学性质,近年来,该方面研究受到了高度的重视,多种一维纳米结构材料被制备出来,其物化性能被广泛研究。尤为值得注意的是,一维纳米管的出现,利用其作为载体在其上固定具有捕获光能的纳米晶更是具有很大的挑战。依赖于一维纳米材料为平台(载体),将不同的具有优异性能的纳米颗粒(团簇)与之组装:既可以发挥颗粒的独特性能,也利用一维材料的优势。两者优势的结合必然引起新的纳米革命。为此,我们进行了以下两部分的工作。
第一部分采用非络合剂作为溶剂,在高温下采用快速注入的方法,低温生长反I和II型纳米晶,并对其光学和结构性质进行了表征。反I和II型纳米晶,由于其在形成核壳结构的异质结结构时,其核材料和壳材料中导带和价带的错位,而形成的特殊的“能带”结构,使得其展现出了不同于I型纳米晶的新奇的性质。例如,其荧光发射峰位的宽范围的连续调节等。反I型纳米晶我们选择ZnSe@CdSe作为研究对象。II型纳米晶我们选择ZnSe@CdS作为研究体系。我们发现采用不同尺寸的核和不同厚度的壳的包覆,所得的异质结结构的纳米晶的发射峰位是连续可调的。其中反TYPE-I型ZnSe@CdSe异质结中,颗粒尺寸分布均匀,分散性好。电镜图片表明其尺寸随着壳层的增加,核壳结构纳米晶的尺寸从3.5nm逐渐增大为8nm左右;且荧光谱图表明其发射峰位可以从400nm连续可调至650nm;而对TYPE-II型的ZnSe@CdS异质结纳米晶发射峰位则可以从400nm发射调节到580nm发射。
第二部分选择碳纳米管作为研究平台,采用有机物(PAH)包覆的方法来功能化碳纳米管。这种方法对碳纳米管是非破坏性的、且没有引入杂质。随后采用室温自组装的方法,将纳米晶量子点组装到功能化的碳纳米管的表面上去。实验结果表明:通过单一改变反应纳米晶的含量,可以改变纳米晶在碳纳米管上的覆盖率;且具有优异发光性能的ZnSe@CdSe纳米晶在结合到功能化的碳纳米管上之后,荧光发生了显著的淬灭;我们推测其原因是:处于激发态的纳米晶量子点将能量(电子)以非辐射的方式转移到了功能化的碳纳米管上去。这种淬灭效应所致的电荷的分离能导致光电流的产生,势必将提高碳纳米管的电学性能。
The studies of unique properties of nano-materials and nano-structures have great importance in both basic theory studies and practical applications. One particularly intriguing case is the study of the structures and properties of nanoscale assembled systems, One-dimensional nanostructured materials is the base to get and develop nanodevice, low dimensional nanostructured materials have special physical and chemical properties. So, this aspect was highly strengthened in recent years. All kinds of one-dimensional nanotructured materials were gradually prepared and their physical and chemical properties were widely investigated. Specially, with the recent advance in the design of nanotube architecture, the obvious challenge is to use carbon nanotube as support to anchor light-harvesting semiconductor nanocrystals. Based on upper background, we had done some special work on core@shell nanocrystals and nanocrystals-carbon nanotubes heterostructures in this paper, the main contents are as follows:
The synthesis nanocrystals were conducted in noncoordinating solvents. We choose High injection, low growth temperatures. In the reverse type-I and type-II core/shell nanocrystals, because of their special structure of the“band gap”, emission spectra can be continuously tunable (from violet to NIR) compared to the so-called type-I nanocrystals. We synthesized inverse type-I ZnSe@CdSe and type-II ZnSe@CdS core@shell nanocrystals (NCs) in noncoordinating solvents. The results showed that in the inversed type-I nanocrystals the photoluminescence (PL) is continuously tunable between 400 and 650 nm with the different thickness of shell, the size of the core/shell nanocrystals ranged from 3.5nm to 8nm; in the type-II nanocrystals system, photoluminescence (PL) is continuously tunable between 400 and 580 nm with the different thickness of shell。
We choose carbon nanotubes as Scaffolds. We report on carbon nanotubes nanocrystals (CNs/NCs) heterostructures. Colloidal semiconductor nanocrystals were covalently attached to CNTs, which were pre-functionalized by a polymer wrapping technique that is not invasive and does not introduce defects to the structure of CNTs, via the self-assembly approach developed very recently. The pre-functionalized CNTs have high stability in a range of organic solvents. The results showed that the number of bound quantum dots per nanotube can relatively be controlled by varying the quantum dot/nanotube mole ratio, Upon light excitation at 350 nm, the emission of ZnSe@CdSe nanocrystals is totally quenched when it is bound to the CNTs, A possible pathway for the deactivation of excited ZnSe@CdSe nanocrystals is electron transfer to the CNTs. this quenching effect improved charge separation which is very prone to photo-current occurrence。It enhanced the electrical properties of CNTs.
第一部分采用非络合剂作为溶剂,在高温下采用快速注入的方法,低温生长反I和II型纳米晶,并对其光学和结构性质进行了表征。反I和II型纳米晶,由于其在形成核壳结构的异质结结构时,其核材料和壳材料中导带和价带的错位,而形成的特殊的“能带”结构,使得其展现出了不同于I型纳米晶的新奇的性质。例如,其荧光发射峰位的宽范围的连续调节等。反I型纳米晶我们选择ZnSe@CdSe作为研究对象。II型纳米晶我们选择ZnSe@CdS作为研究体系。我们发现采用不同尺寸的核和不同厚度的壳的包覆,所得的异质结结构的纳米晶的发射峰位是连续可调的。其中反TYPE-I型ZnSe@CdSe异质结中,颗粒尺寸分布均匀,分散性好。电镜图片表明其尺寸随着壳层的增加,核壳结构纳米晶的尺寸从3.5nm逐渐增大为8nm左右;且荧光谱图表明其发射峰位可以从400nm连续可调至650nm;而对TYPE-II型的ZnSe@CdS异质结纳米晶发射峰位则可以从400nm发射调节到580nm发射。
第二部分选择碳纳米管作为研究平台,采用有机物(PAH)包覆的方法来功能化碳纳米管。这种方法对碳纳米管是非破坏性的、且没有引入杂质。随后采用室温自组装的方法,将纳米晶量子点组装到功能化的碳纳米管的表面上去。实验结果表明:通过单一改变反应纳米晶的含量,可以改变纳米晶在碳纳米管上的覆盖率;且具有优异发光性能的ZnSe@CdSe纳米晶在结合到功能化的碳纳米管上之后,荧光发生了显著的淬灭;我们推测其原因是:处于激发态的纳米晶量子点将能量(电子)以非辐射的方式转移到了功能化的碳纳米管上去。这种淬灭效应所致的电荷的分离能导致光电流的产生,势必将提高碳纳米管的电学性能。
The studies of unique properties of nano-materials and nano-structures have great importance in both basic theory studies and practical applications. One particularly intriguing case is the study of the structures and properties of nanoscale assembled systems, One-dimensional nanostructured materials is the base to get and develop nanodevice, low dimensional nanostructured materials have special physical and chemical properties. So, this aspect was highly strengthened in recent years. All kinds of one-dimensional nanotructured materials were gradually prepared and their physical and chemical properties were widely investigated. Specially, with the recent advance in the design of nanotube architecture, the obvious challenge is to use carbon nanotube as support to anchor light-harvesting semiconductor nanocrystals. Based on upper background, we had done some special work on core@shell nanocrystals and nanocrystals-carbon nanotubes heterostructures in this paper, the main contents are as follows:
The synthesis nanocrystals were conducted in noncoordinating solvents. We choose High injection, low growth temperatures. In the reverse type-I and type-II core/shell nanocrystals, because of their special structure of the“band gap”, emission spectra can be continuously tunable (from violet to NIR) compared to the so-called type-I nanocrystals. We synthesized inverse type-I ZnSe@CdSe and type-II ZnSe@CdS core@shell nanocrystals (NCs) in noncoordinating solvents. The results showed that in the inversed type-I nanocrystals the photoluminescence (PL) is continuously tunable between 400 and 650 nm with the different thickness of shell, the size of the core/shell nanocrystals ranged from 3.5nm to 8nm; in the type-II nanocrystals system, photoluminescence (PL) is continuously tunable between 400 and 580 nm with the different thickness of shell。
We choose carbon nanotubes as Scaffolds. We report on carbon nanotubes nanocrystals (CNs/NCs) heterostructures. Colloidal semiconductor nanocrystals were covalently attached to CNTs, which were pre-functionalized by a polymer wrapping technique that is not invasive and does not introduce defects to the structure of CNTs, via the self-assembly approach developed very recently. The pre-functionalized CNTs have high stability in a range of organic solvents. The results showed that the number of bound quantum dots per nanotube can relatively be controlled by varying the quantum dot/nanotube mole ratio, Upon light excitation at 350 nm, the emission of ZnSe@CdSe nanocrystals is totally quenched when it is bound to the CNTs, A possible pathway for the deactivation of excited ZnSe@CdSe nanocrystals is electron transfer to the CNTs. this quenching effect improved charge separation which is very prone to photo-current occurrence。It enhanced the electrical properties of CNTs.
引文
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