纳秒激光加工生成硅量子点的发光性质研究

该文报道氧气、氮气或空气等不同氛围中用纳秒脉冲激光在硅基上加工生成量子点结构,发现这些样品在700 nm波长附近均有增强的光致发光(Photoluminescence,PL),且各样品的PL峰很相似;经适当退火处理后,在某些样品上观察到随机受激发光.通过第一性原理计算,发现各种量子点结构表面的成键类型与密度是形成PL发光增强的关键,并由此提出相应的物理模型.     

Hybridization of electronic states in quantum dots through photon emission

The self-assembly of semiconductor quantum dots has opened up new opportunities in photonics. Quantum dots are usually described as 'artificial atoms', because electron and hole confinement gives rise to discrete energy levels. This picture can be justified from the shell structure observed as a quantum dot is filled either with excitons (bound electron-hole pairs) or with electrons. The discrete energy levels have been most spectacularly exploited in single photon sources that use a single quantum dot as emitter. At low temperatures, the artificial atom picture is strengthened by the long coherence times of excitons in quantum dots, motivating the application of quantum dots in quantum optics and quantum information processing. In this context, excitons in quantum dots have already been manipulated coherently. We show here that quantum dots can also possess electronic states that go far beyond the artificial atom model. These states are a coherent hybridization of localized quantum dot states and extended continuum states: they have no analogue in atomic physics. The states are generated by the emission of a photon from a quantum dot. We show how a new version of the Anderson model that describes interactions between localized and extended states can account for the observed hybridization.     

一维光子晶体的光子带隙研究

通过改变一维光子晶体的周期排列常数、两种介质的折射率比观察了电磁波在光子晶体中的光子带隙(PBG)行为.当两种介质的排列周期常数a:b=1:1和1:2时,发现光子晶体在可见光区存在一个很宽的频率截止带,即光子带隙区.另外,当两种介质的介电常数比εα:εb小于1:5,在可见光区无光子带隙存在;而当该比率大于1:5时则出现一个很宽的光子带隙.说明两种介质的介电常数比对光子带隙的影响很大,该比例越大,越容易获得光子带隙.     

Fabrication of photonic crystals for the visible spectrum by holographic lithography

The term 'photonics' describes a technology whereby data transmission and processing occurs largely or entirely by means of photons. Photonic crystals are microstructured materials in which the dielectric constant is periodically modulated on a length scale comparable to the desired wavelength of operation. Multiple interference between waves scattered from each unit cell of the structure may open a 'photonic bandgap'--a range of frequencies, analogous to the electronic bandgap of a semiconductor, within which no propagating electromagnetic modes exist. Numerous device principles that exploit this property have been identified. Considerable progress has now been made in constructing two-dimensional structures using conventional lithography, but the fabrication of three-dimensional photonic crystal structures for the visible spectrum remains a considerable challenge. Here we describe a technique--three-dimensional holographic lithography--that is well suited to the production of three-dimensional structures with sub-micrometre periodicity. With this technique we have made microperiodic polymeric structures, and we have used these as templates to create complementary structures with higher refractive-index contrast.     

Synthesis of CdSe quantum dots

Water-soluble CdSe quantum dots（QDs） were synthesized in aqueous solution with thioglycollic acid as stabilizer.CdSe QDswere characterized using Transmission electron microscopy（TEM）,UV-Vis absorption spectrum（UV-Vis） and fluorescence spectra（FL）.The characterization results indicate that as-synthesized CdSe QD was uniform at about 3.5 nm.     

Molecular dynamics studied by analysis of the X-ray diffuse scattering from lysozyme crystals

It is now well established that the biological activity of proteins is related not only to their mean molecular structure, but also to their intramolecular mobility. Nearly all techniques sensitive to dynamics have given evidence for intramolecular mobility in proteins: NMR, ESR, Raman spectroscopy, fluorescence quenching, M?ssbauer spectroscopy, neutron scattering, measurements of elastic constants and hydrogen-deuterium exchange. The dynamics of proteins has also been approached by theoretical calculations. We report here investigations of the atomic and molecular displacements in hen egg-white lysozyme crystals using a new technique. This technique, based on the X-ray diffuse scattering analysis (scattering out of the Bragg reflections), can yield information on the atomic displacements, provided that they are correlated. Rigid-body molecular displacements, correlated along short rows of aligned molecules in two perpendicular directions, have been detected and analysed (mean square amplitude of the order of 5 X 10(-4) nm2). This technique can be also applied to the detection and analysis of intramolecular displacements.     

二维芯壳异质结构光子晶体禁带特性分析

研究了一种新的二维芯壳型异质结构光子晶体,即介质纳米柱外被覆盖一薄层材料.针对正方排列及三角排列两种方式,利用平面波方法,比较了在折射率为2的介质纳米柱外表面涂覆折射率为3.5的薄层后,其能带曲线的变化,发现光子晶体的禁带明显变宽,且三角排列比正方排列更易形成较宽的光子禁带.     

Optical emission from a charge-tunable quantum ring

Quantum dots or rings are artificial nanometre-sized clusters that confine electrons in all three directions. They can be fabricated in a semiconductor system by embedding an island of low-bandgap material in a sea of material with a higher bandgap. Quantum dots are often referred to as artificial atoms because, when filled sequentially with electrons, the charging energies are pronounced for particular electron numbers; this is analogous to Hund's rules in atomic physics. But semiconductors also have a valence band with strong optical transitions to the conduction band. These transitions are the basis for the application of quantum dots as laser emitters, storage devices and fluorescence markers. Here we report how the optical emission (photoluminescence) of a single quantum ring changes as electrons are added one-by-one. We find that the emission energy changes abruptly whenever an electron is added to the artificial atom, and that the sizes of the jumps reveal a shell structure.     

L-半胱氨酸配位合成CdTe量子点的理论研究

本文利用密度泛函理论,研究了L-半胱氨酸及L-胱氨酸在CdTe上的吸附特征. 优化之后分别得到了四种稳定的吸附构型,计算了它们的吸附能、电荷密度、前沿分子轨道以及紫外可见吸收光谱等. 研究发现:L-半胱氨酸在CdTe上的吸附能较大、紫外可见光吸收较强,说明L-半胱氨酸在CdTe上的吸附较稳定,容易产生分子荧光,而L-半胱氨酸转化为L-胱氨酸之后,吸附稳定性降低、紫外可见光吸收强度减弱. 该研究为L-半胱氨酸配体合成的CdTe QDs荧光材料用于生物体内H2O2和葡萄糖的检测提供了理论支撑.     

自组织生长Ge量子点材料研究

利用超高真空化学气相淀积设备在Si衬底上生长Ge量子点.通过3因素3水平的正交实验,研究不同的生长参数(衬底温度、GeH4气体流量、生长时间)对Ge量子点生长的影响,从而得到优化的Ge量子点生长参数.透射电镜、X射线双晶衍射测试结果表明,利用优化的生长参数得到的多层Ge量子点材料,具有较好的晶体质量.     

用AAO模板及脉冲激光溅射制备量子点阵

 利用多孔阳极氧化铝(anodic aluminum oxide,AAO)作为模板,采用准分子脉冲激光溅射方法(pulsed laser deposition,PLD)成功制备了光荧光材料La_0.95Eu_0.05BaB₉O₁₆的量子点阵,用扫描电镜表征了AAO模板和制备的量子点阵,测量了靶材和量子点阵的光荧光谱.讨论了用此方法制备的量子点阵的结构和发光特性.证明此方法可为未来制备其它材料的量子点阵开辟了一条途径.     

水溶性硅包CdTe量子点的合成方法研究

本研究成功地合成了水溶性CdTe量子点(QDs).考察温度对回流时间、荧光强度及粒径大小等因素的影响,实验优化合成条件之后确定最佳反应温度为105 ℃.接着,本研究运用改进后的Stober法更为简易地合成了硅包CdTe量子点复合微球,该微球的粒径可通过改变正硅酸乙酯及水的含量控制在160~260 nm之间,同时根据复合微粒的电镜拍摄图初步探讨了SiO₂在CdTe表面的生长模式.为了将来能运用到生物检测中,此实验加入3-氨基丙基三乙氧基硅烷（APTS）,引入氨基团,并优化了 APTS 加入时间,得到的粒子表面氨基含量最高.这种复合微粒具有与原来量子点相当的量子产率,同时具有良好的水溶性、胶体稳定性、化学反应性,为量子点作为荧光标记物的应用打下了基础.     

量子点半导体光放大器的自发辐射特性研究

从导带、价带和浸润层的能级跃迁出发,采用分段模型对量子点半导体光放大器的增益和自发辐射进行了数值研究．物理模型包括自发辐射行波方程和各能级栽流子与光子数速率方程．经过大量数值计算,得到基态电子占用概率随注入光脉冲的变化,以及增益动态过程（饱和与恢复）和输出光脉冲的时域波形畸变．进一步研究了量子点光放大器自发辐射谱和增益平坦性,结果表明自发辐射功率随输入信号功率增大而减小,引入合适的钳制光,可在20nm带宽内获得小于0．3dB的增益平坦度,或者40nm带宽内小于1．0dB．     

非圆形空气孔型二维光子晶体带隙率模拟

采用平面波展开法对两类晶格(三角晶格和正方晶格)及圆形空气孔或两种非圆形空气孔(正方形和六边形)构成的二维光子晶体带隙率进行了数值研究,分析了填充比f对带隙率ωR的影响.结果表明,晶格对称结构和空气孔形状对带隙大小有影响.给定晶格对称结构,选择具有相同对称形状的空气孔能得到较大的绝对光子带隙.在这3种空气孔当中,三角晶格对应六边形空气孔有最大带隙率,当填充比f=0.8时,带隙率ωR=23.3%;正方晶格对应正方形空气孔有最大带隙率,当填充比f=0.67时,带隙率ωR=14.7%.     

Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots

Photoluminescence blinking--random switching between states of high (ON) and low (OFF) emissivities--is a universal property of molecular emitters found in dyes, polymers, biological molecules and artificial nanostructures such as nanocrystal quantum dots, carbon nanotubes and nanowires. For the past 15 years, colloidal nanocrystals have been used as a model system to study this phenomenon. The occurrence of OFF periods in nanocrystal emission has been commonly attributed to the presence of an additional charge, which leads to photoluminescence quenching by non-radiative recombination (the Auger mechanism). However, this 'charging' model was recently challenged in several reports. Here we report time-resolved photoluminescence studies of individual nanocrystal quantum dots performed while electrochemically controlling the degree of their charging, with the goal of clarifying the role of charging in blinking. We find that two distinct types of blinking are possible: conventional (A-type) blinking due to charging and discharging of the nanocrystal core, in which lower photoluminescence intensities correlate with shorter photoluminescence lifetimes; and a second sort (B-type), in which large changes in the emission intensity are not accompanied by significant changes in emission dynamics. We attribute B-type blinking to charge fluctuations in the electron-accepting surface sites. When unoccupied, these sites intercept 'hot' electrons before they relax into emitting core states. Both blinking mechanisms can be electrochemically controlled and completely suppressed by application of an appropriate potential.     

二维光子晶体中导模的优化

提出了方形二维光子晶体的结构,并引入缺陷形成耦合腔波导和线缺陷波导。应用时域有限差分(FDTD)法研究其传输特性,结果表明对于耦合腔波导,当缺陷周围介质柱直径变化时,第一光子禁带中会出现宽频缺陷模。并且当介质柱直径减小时,缺陷模会向高频移动,而导模宽度则会有规律地扩展或者缩小。在线缺陷波导中,逐渐减小缺陷两侧介质柱的直径或介电常数,发现导带向高频移动,并且带宽逐渐减小     

Crossover from 'mesoscopic' to 'universal' phase for electron transmission in quantum dots

The measurement of phase in coherent electron systems--that is, 'mesoscopic' systems such as quantum dots--can yield information about fundamental transport properties that is not readily apparent from conductance measurements. Phase measurements on relatively large quantum dots recently revealed that the phase evolution for electrons traversing the dots exhibits a 'universal' behaviour, independent of dot size, shape, and electron occupancy. Specifically, for quantum dots in the Coulomb blockade regime, the transmission phase increases monotonically by pi throughout each conductance peak; in the conductance valleys, the phase returns sharply to its starting value. The expected mesoscopic features in the phase evolution--related to the dot's shape, spin degeneracy or to exchange effects--have not been observed, and there is at present no satisfactory explanation for the observed universality in phase behaviour. Here we report the results of phase measurements on a series of small quantum dots, having occupancies of between only 1-20 electrons, where the phase behaviour for electron transmission should in principle be easier to interpret. In contrast to the universal behaviour observed thus far only in the larger dots, we see clear mesoscopic features in the phase measurements when the dot occupancy is less than approximately 10 electrons. As the occupancy increases, the manner of phase evolution changes and universal behaviour is recovered for some 14 electrons or more. The identification of a transition from the expected mesoscopic behaviour to universal phase evolution should help to direct and constrain theoretical models for the latter.     

氮掺杂碳量子点荧光探针快速检测山梨酸钾

山梨酸钾属于酸性食品防腐剂,能有效地抑制霉菌、酵母菌和好氧性细菌的活性,延长食品的保存时间,并保持食品原有的风味.本研究通过一步水热法合成了水溶性良好的荧光氮掺杂碳量子点（NCQDs）,基于山梨酸钾能有效地猝灭NCQDs而构建了快速检测山梨酸钾的荧光探针.在最佳实验条件下,山梨酸钾浓度在3.0×10^-5～1.0×10^-4mol/L和1.0×10^-7～3.0×10^-5mol/L范围内与NCQDs荧光猝灭强度呈现良好的线性关系,检出限为9.5×10^-8mol/L.我们已将其用于苏打水及白醋中山梨酸钾含量的测定,回收率分别为98.25%～102.7%和98.33%～101.8%.