利用N型半导体纳米材料抑制单量子点的荧光闪烁特性

利用N型半导体纳米材料氧化铟锡(ITO)作为单CdSe/ZnS量子点的基质来抑制单量子点的荧光闪烁特性. 实验采用激光扫描共聚焦显微成像系统测量了单量子点荧光的亮、暗态持续时间的概率密度分布的指数截止的幂律特性, 并与直接吸附在SiO₂玻片上的单CdSe/ZnS量子点的荧光特性进行比较. 研究发现处于ITO中的单量子点比SiO₂玻片上的单量子点荧光亮态持续时间提高两个数量级, 掺杂于ITO中的单量子点的荧光寿命约减小为SiO₂玻片上的单量子点的荧光寿命的41%, 并且寿命分布宽度变小50%.     

电场调谐InAs量子点荷电激子光学跃迁

在低温5 K下, 采用光致发光光谱及外加偏压调谐量子点电荷组态研究了InAs单量子点的精细结构和对应发光光谱的偏振性、不同带电荷激子的圆偏振特性. 得出如下结果: 1) 指认InAs单量子点中不同荷电激子的发光光谱和对应的激子本征态的偏振特性; 2) 外加偏压可以调谐量子点的荷电激子的发光光谱; 3) 伴随着电子、空穴的能量弛豫, 电子的自旋弛豫时间远大于空穴的自旋弛豫时间. 关键词： InAs量子点 激子 荧光光谱 电场调谐     

低强度飞秒激光激发下CdTe和CdTe/CdS核壳量子点的荧光上转换研究

利用400 nm和800 nm不同波长的低强度飞秒激光,对CdTe和CdTe/CdS核壳量子点溶胶进行激发,研究其稳态和时间分辨荧光性质.800 nm飞秒激光激发下,CdTe和CdTe/CdS核壳量子点产生上转换发光现象,上转换荧光峰与400 nm激发下的荧光峰相比蓝移最多达15 nm,而且蓝移值与荧光量子产率有关.变功率激发确认激发光功率与上转换荧光强度间满足二次方关系,时间分辨荧光的研究表明荧光动力学曲线服从双e指数衰减.提出表面态辅助的双光子吸收模型是低激发强度上转换发光的主要机理.CdTe和CdT 关键词： CdTe量子点 CdTe/CdS核壳量子点 时间分辨荧光 上转换荧光     

SiO/SiO_2超晶格结构界面发光的研究

利用热蒸发技术在硅衬底上制备了层厚不同的SiO/SiO2超晶格样品.对其光致发光谱进行研究发现,随着SiO/SiO2超晶格中SiO层厚度的增加,发光峰在400～600 nm之间移动.研究表明,样品的发光中心来自于SiO/SiO2界面处的缺陷发光(界面态发光).即在样品沉积的过程中,在SiO/SiO2的界面处由于晶格的不连续性,会形成大量的Si-O悬挂键,这些悬挂键本身相互结合可以形成一定数量的缺陷,同时由于O原子容易脱离Si原子的束缚而产生扩散,因此,这些悬挂键可以与扩散的O原子结合,随着SiO层厚度的增加,在SiO/SiO2的界面处先后出现WOB(O3<≡Si-O-O·),NOV(O3≡Si-Si≡O3),E'中心(O≡Si·),NBOHC(O3≡Si-O·)等缺陷,这些缺陷在SiO层厚度增大的过程中对发光先后起到主导作用,从而使得发光峰产生红移.     

ITO负载单原子钇吸附NO和CO的第一性原理研究

基于密度泛函理论,对氧化铟锡(Indium Tin Oxide,ITO)表面负载单原子Y模型的表面性能进行了第一性原理计算.根据表面能计算结果可知,单原子Y最稳定负载位置为空位(H),即确定了ITO负载单原子钇(Single-atom Y supported on ITO,Y/ITO)稳定模型.对ITO和Y/ITO表面吸附气体分子(NO和CO)模型的吸附性能进行了第一性原理计算.根据对比ITO和Y/ITO表面的吸附能和态密度计算结果可知,单原子钇负载提高了ITO表面的稳定性和吸附性能.根据对比Y/ITO表面吸附NO和CO气体分子的吸附能和态密度计算结果可知,NO和CO气体分子吸附均为自发行为,过程放热.且NO气体分子更容易吸附在Y/ITO表面,即Y/ITO对NO气体分子更敏感.     

本体聚合法制备PbSe/PMMA量子点光纤材料

通过本体聚合法,制备出以聚甲基丙烯酸甲酯(PMMA)为基底的PbSe量子点光纤材料PbSe/PMMA.用透射电镜(TEM)观测了PMMA中PbSe量子点的形貌特征,用紫外可见近红外分光光度仪和荧光光谱仪分析了吸收谱和荧光发射(PL)谱.结果表明,PbSe/PMMA材料中生成的PbSe量子点为近似球形、边界明晰、分布均匀...     

ZnS薄膜参数对有机/无机复合发光器件特性的影响

半导体量子点(QDs)具有发光效率高和发光波长可调等特点。采用胶体CdSe QDs作电致发光器件的有源材料,TPD(N,N′-biphenyl-N,N′-bis-(3-methylphenyl)-1,1′-biphenyl-4,4′-diamine)作空穴传输层,ZnS作电子传输层,研究了有机/无机复合发光器件ITO/TPD/CdSe QDs/ZnS/Ag的电致发光特性。TPD和CdSe QDs薄膜采用旋涂方法、ZnS薄膜采用磁控溅射方法沉积,器件表面平整。CdSe QDs的光致发光和电致发光谱峰位波长均位于～580 nm,属于量子点的带边激子发光。我们与以前的ITO/ZnS/CdSe QDs/ZnS/Ag发光器件结构进行了对比,发现新的器件结构的电致发光谱没有观察到QDs表面态的发光,而且新器件的发光强度是ITO/ZnS/CdSe QDs/ZnS/Ag结构的～10倍。发光效率的提高归因于碰撞激发与载流子注入两种发光机制并存的结果：一方面电子经过ZnS 层加速后,碰撞激发CdSe QDs发光;另一方面,空穴从TPD层注入CdSe QDs 与QDs中激发的电子复合发光。我们进一步研究了ZnS电子加速层厚度对发光特性的影响,选择ZnS薄膜的厚度分别是80,120 和160 nm,发现随着ZnS层厚度增大,器件启亮电压升高,EL强度增大,但是击穿电压降低。EL峰位随着ZnS厚度的减小发生明显蓝移,对上述实验现象进行了机理解释。     

硅量子点的形状及其弯曲表面效应

硅量子点的弯曲表面引起系统的对称性破缺, 致使某些表面键合在能带的带隙中形成局域电子态.计算结果表明:硅量子点的表面曲率不同形成的表面键合结合能和电子态分布明显不同. 例如, Si–O–Si桥键在曲率较大的表面键合能够在带隙中形成局域能级, 而在硅量子点曲率较小的近平台表面上键合不会形成任何局域态, 但此时的键合结合能较低. 用弯曲表面效应(CS)可以解释较小硅量子点的光致荧光光谱的红移现象. CS效应揭示了纳米物理中又一奇妙的特性. 实验证实, CS效应在带隙中形成的局域能级可以激活硅量子点发光. 关键词： 硅量子点 弯曲表面效应 表面键合 局域能级     

InAs 单量子点中级联辐射光子的关联测量

利用分子束外延生长InAs单量子点样品,温度为5 K时,测量了单量子点中单、双激子自发辐射的荧光(PL)光谱.研究了单、双激子发光强度随激发功率的变化及对应发光峰的偏振特性和精细结构劈裂.基于Hanbury-Brown Twiss(HBT) 实验,测量了单、双激子间发光光谱的关联函数,证实了其发光过程为级联发射过程. 关键词： InAs 单量子点 单、双激子 荧光光谱 级联辐射     

金纳米颗粒光散射提高InAs单量子点荧光提取效率

采用光学方法确定InAs/GaAs单量子点在样品外延面上的位置坐标, 利用AlAs牺牲层把含有量子点的GaAs层剥离并放置在含有金纳米颗粒或平整金膜上, 研究量子点周围环境不同对量子点自发辐射寿命及发光提取效率的影响. 实验结果显示, 剥离前后量子点发光寿命的变化小于13%, 含有金纳米颗粒的量子点发光强度是剥离前的7倍, 含有金属薄膜的量子点发光强度是剥离前的2倍. 分析表明在金纳米颗粒膜上的量子点荧光强度的增加主要来自于金纳米颗粒对量子点荧光的散射效应, 从而提高量子点发光的提取效率.     

Linear dipole behavior of single quantum dots encased in metal oxide semiconductor nanoparticles films

Understanding of charge/energy exchange processes and interfacial interactions that occur between quantum dots (QDs) and the metal oxides is of critical importance to these QD-based optoelectronic devices. This work reports on linear dipole behavior of single near-infrared emitting CdSeTe/ZnS core/shell QDs which are encased in indium tin oxide (ITO) semiconductor nanoparticles films. A strong polarization anisotropy in photoluminescence emission is observed by defocused wide-field imaging and polarization measurement techniques, and the average polarization degree is up to 0.45. A possible mechanism for the observation is presented in which the electrons, locating at single QD surface from ITO by electron transfer due to the equilibration of the Fermi levels, result in a significant Stark distortion of the QD electron/hole wavefunctions. The Stark distortion results in the linear polarization property of the single QDs. The investigation of linear dipole behavior for single QDs encased in ITO films would be helpful for further improving QD-based device performance.     

Influence of surface charges on the emission polarization properties of single CdSe/CdS dot-in-rods

We report an experimental investigation of the influence of surface charges on the emission polarization properties of single CdSe/CdS dot-in-rods (DRs), which is important for their polarization-based practical applications. By covering the single DRs with N-type semiconductor indium tin oxide (ITO) nanoparticles, the surface of single DRs is charged by ITO through interfacial electron transfer. This is confirmed by the experimental observations of the reduced photoluminescence intensities and lifetimes as well as the suppressing blinking. It is found that the full width at half maximum of histogram of polarization degrees of the single DRs is broadened from 0.24 (on glass) to 0.41 (in ITO). In order to explain the exprimental results, the band-edge exciton fine structure of single DRs is calculated by taking into account the sample parameters, the emission polarization, and the surface charges. The calculation results show that the level ordering of the emitting states determines the polarization degrees tending to increase or decrease under the influence of surface electrons. The surface electrons can induce an increase in the spacing between the emitting levels to change the populations and thus change the polarization degrees. In addition, different numbers of surface electrons may randomly distribute on the long CdSe/CdS rods, leading to the heterogeneous influences on the single DRs causing the broadening of polarization degrees also.     

倒置器件结构及局域等离子体效应对CdSe量子点LED发光性能的改进

研究了倒置器件结构以及CdSe量子点发光材料与金属纳米粒子之间的相互作用对量子点的电致发光性能的影响。利用TiO₂作为电子传输/注入层,成功地制备了倒置结构的量子点电致发光器件。通过对单载流子器件电压-电流特性的分析,证明了ITO作为阴极到TiO₂的电子注入特性与Al作为阴极时的效果几乎相同。观察到金属纳米粒子产生的局域等离子体效应提高了器件的效率,使得效率随电流增大而降低的速度明显减小。在电流密度为200 mA/cm²时,电致发光器件的效率大约提高了42%。     

Analyzing Increased Fluorescence of Single Quantum Dots on Dehydrated Agarose by Single-Molecular Imaging

A single-molecule imaging technique was used to study emission behaviors of quantum dots (QDs) on the surface of glass and dehydrated agarose. The luminescence intensity of single QDs on the dehydrated agarose film was 2 or 3 times that on the glass. Our results revealed that the roughness and the hydrophobic nature of dehydrated agarose gel can suppress the blinking of single QDs. A clear decrease in the power law exponent for “on” time but an increase for “off” time was observed when the glass was replaced with 4% and 8% dehydrated agarose. The enhanced luminescence of QDs on dehydrated agarose will make their applications on microarrays more attractive.     

Enhanced fluorescence intermittency of CdSe-ZnS quantum-dot clusters

Fluorescence intermittency, or blinking, of individual close-packed clusters containing two or more CdSe-ZnS quantum dots (QDs) was investigated. The QD clusters exhibited rapid, intense blinking that was distinct from that of isolated QDs blinking independently. This enhanced blinking is suggested to occur when the QDs in the cluster become electronically coupled. The nature of this coupling is not known, though electrons trapped from QDs when they blink off may play a role by altering the electronic environment of neighboring QDs and enhancing their fluorescence properties.     

Redox-mediated reversible modulation of the photoluminescence of single quantum dots

Precise control over the photoluminescence(PL) of single quantum dots(QDs) is important for their practical applications. We show that the PL of individual Cd Se/Zn S core/shell QDs can be effectively enhanced and continuously modulated by electrochemically manipulating the electron transfer(ET) between the QDs and the attached redox-active ligands such as 2-mercaptoethanol(BME). We found that i) the ET from BME to the QDs' surface trap states suppresses the blinking of the QDs, ii) the ET from the QDs' conduction band to the oxidization product results in dimmed PL when BME is oxidized,and iii) further oxidization of BME results in a significant PL brightening. The single particle measurements help us unveil the important features hidden in ensemble measurements and understand the underlying mechanism of the PL modulation.The results also suggest a simple yet efficient method to produce bright and non-blinking QDs and offer opportunities for further development of high resolution fluorescent bioimaging and nanodevices.     

Work function changes and surface chemistry of oxygen, hydrogen, and carbon on indium tin oxide

The surface chemistry of indium tin oxide (ITO) has been investigated with Auger electron spectroscopy (AES) and high resolution electron energy loss spectroscopy (HREELS). A vibrating Kelvin probe (KP) with a graphite reference was used to monitor the absolute work function (Φ) of ITO as a function of chemical modification. The ITO was exposed in situ to molecular hydrogen (H₂), hot-filament-activated oxygen (O₂^*), and hot-filament-activated deuterium (D₂^*). The initial Φ of ITO was determined to be 5.2 eV, and surface chemical changes had strong effects on this value, as seen by KP. Exposure of clean ITO to O₂^* increased Φ to 5.6 eV, but the increase was short-lived. The changes in Φ over time were correlated with the uptake of carbon impurities in ultra high vacuum (UHV), as monitored by AES.

The HREELS of ITO revealed significant hydrocarbon impurities. Chemical reduction of ITO produced a metallic surface and dehydrogenated the adsorbed hydrocarbons. Both re-oxidation of metallic ITO and oxidation of clean ITO temporarily removed adventitious carbon from the surface, but oxidized ITO adsorbed an even larger quantity of carbon over time.     

自组织量子点的量子态光学探测

半导体量子点主要包括在真空中外延生长的自组织量子点和在溶液中采用化学方法合成的胶体量子点,由于量子限制效应所导致的分立能级结构使得它们通常被称为“人工原子”。和自然原子不同,半导体量子点的能级结构强烈依赖于其尺寸和形状,这样就提供了更为灵活的方法来控制固体材料中的光与材料的相互作用。近年来,许多类原子的量子光学现象(包括量子干涉、Rabi振荡和Mollow荧光)都已经在单个的自组织量子点中揭示出来。与此形成对比的是,上述所有的类原子量子光学特性目前还没有在单个的胶体量子点中观察得到。在本文中,我们将侧重于介绍我们科研组以及我们和别的科研组合作对单个自组织量子点的单量子态在光学探测和相干控制方面完成的一系列工作。对单个的胶体量子点,我们认为量子相干特性的测量和控制将在新近合成的非荧光闪烁或荧光闪烁得到抑制的材料体系中得以实现.     

自组织量子点的量子态光学探测(英文)

半导体量子点主要包括在真空中外延生长的自组织量子点和在溶液中采用化学方法合成的胶体量子点,由于量子限制效应所导致的分立能级结构使得它们通常被称为"人工原子"。和自然原子不同,半导体量子点的能级结构强烈依赖于其尺寸和形状,这样就提供了更为灵活的方法来控制固体材料中的光与材料的相互作用。近年来,许多类原子的量子光学现象(包括量子干涉、Rabi振荡和Mollow荧光)都已经在单个的自组织量子点中揭示出来。与此形成对比的是,上述所有的类原子量子光学特性目前还没有在单个的胶体量子点中观察得到。在本文中,我们将侧重于介绍我们科研组以及我们和别的科研组合作对单个自组织量子点的单量子态在光学探测和相干控制方面完成的一系列工作。对单个的胶体量子点,我们认为量子相干特性的测量和控制将在新近合成的非荧光闪烁或荧光闪烁得到抑制的材料体系中得以实现。