Aqueous phase synthesis and fluorescence properties of inverted core/shell ZnSe/CdSe nanocrystals

We report a facile aqueous phase synthesis for prepar-ing water-soluble inverted core/shell ZnSe/CdSe semiconductor nanocrystals. The samples were characterized by X-ray diffraction (XRD),transmission electron microscopy (TEM),and their optical properties were investigated by using UV-vis-NIR spectropho-tometer and fluorescence spectrophotometer. The results indicate that the synthesized ZnSe/CdSe nanocrystals are inverted core/shell structure with diameter of about 5 nm. Furthermore,their absorption band-edge is red-shifted with the growth of CdSe shell; correspondingly,their emission wavelength can be tuned from 460 nm to 604 nm.     

纳米氧化锌颗粒的荧光光谱特性及测试条件的影响

分别用沉淀法和有机物单源的热分解方法从溶液中生长了不同尺寸的氧化锌纳米晶体,研究了纳米晶体的荧光特性及其对测量样品状态的依赖关系.尺寸比较大的ZnO纳米晶体在固态下其荧光光谱为宽阔的发光带,并在宽阔发光带上出现一系列明显的精细结构,而分散于有机溶剂中时其荧光由激子复合发射和通过氧空位的复合发射组成.分散于有机溶剂中的中等尺寸的表面包裹的纳米ZnO晶体的荧光由激子荧光、通过浅杂质的发射和通过本征缺陷复合的荧光组成,其强度随着测量浓度的升高而增强,并且激子的荧光发生红移;尺寸比较小的表面包裹的纳米晶体的荧光为激子复合和通过氧空位复合的荧光组成,激子荧光强度、通过氧空位的发光强度及其相对强度随着纳米晶体浓度的变化而变化,测量浓度的升高,激子发光峰没有位移,但与缺陷态相关的激发光荧光发生红移.     

Controlling the dynamics of spontaneous emission from quantum dots by photonic crystals

Control of spontaneously emitted light lies at the heart of quantum optics. It is essential for diverse applications ranging from miniature lasers and light-emitting diodes, to single-photon sources for quantum information, and to solar energy harvesting. To explore such new quantum optics applications, a suitably tailored dielectric environment is required in which the vacuum fluctuations that control spontaneous emission can be manipulated. Photonic crystals provide such an environment: they strongly modify the vacuum fluctuations, causing the decay of emitted light to be accelerated or slowed down, to reveal unusual statistics, or to be completely inhibited in the ideal case of a photonic bandgap. Here we study spontaneous emission from semiconductor quantum dots embedded in inverse opal photonic crystals. We show that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal. Modified emission is observed over large frequency bandwidths of 10%, orders of magnitude larger than reported for resonant optical microcavities. Both inhibited and enhanced decay rates are observed depending on the optical emission frequency, and they are controlled by the crystals' lattice parameter. Our experimental results provide a basis for all-solid-state dynamic control of optical quantum systems.     

High-temperature ultrafast polariton parametric amplification in semiconductor microcavities.

Cavity polaritons, the elementary optical excitations of semiconductor microcavities, may be understood as a superposition of excitons and cavity photons. Owing to their composite nature, these bosonic particles have a distinct optical response, at the same time very fast and highly nonlinear. Very efficient light amplification due to polariton-polariton parametric scattering has recently been reported in semiconductor microcavities at liquid-helium temperatures. Here we demonstrate polariton parametric amplification up to 120 K in GaAlAs-based microcavities and up to 220 K in CdTe-based microcavities. We show that the cut-off temperature for the amplification is ultimately determined by the binding energy of the exciton. A 5-micrometer-thick planar microcavity can amplify a weak light pulse more than 5,000 times. The effective gain coefficient of an equivalent homogeneous medium would be 107 cm-1. The subpicosecond duration and high efficiency of the amplification could be exploited for high-repetition all-optical microscopic switches and amplifiers. 105 polaritons occupy the same quantum state during the amplification, realizing a dynamical condensate of strongly interacting bosons which can be studied at high temperature.     

CuCl团簇组装薄膜的荧光红移现象

利用气相蒸发技术成功的制备了两个ＣｕＣｌ团簇薄膜样品．ＣｕＣｌ团簇被沉积到单晶Ｓｉ和石英衬底上,然后覆盖一层ＮａＣｌ以防氧化．通过透射电镜和选区衍射观察得知,两个样品主要由ＣｕＣｌ纳米晶和少量的Ｃｕ聚集体构成,其中ＣｕＣｌ纳米晶的直径分别约为３ｎｍ和６ｎｍ;通过室温下测得的光吸收和荧光光谱,发现ＣｕＣｌ激子吸收峰并未出现,而荧光峰向低能方向移动,这可能是激子声子强相互作用引起的结果．在７７Ｋ温度观察到由激子声子耦合而展宽的荧光峰,其峰值近似与量子限制模型的计算结果一致,同时观察到来自陷阱态的宽峰．通过比较３００Ｋ温度下激子荧光峰的展宽和红移量,发现团簇尺寸小的薄膜样品（３ｎｍ）中激子声子相互作用更强,这与理论预测定性一致     

Energy-transfer pumping of semiconductor nanocrystals using an epitaxial quantum well

As a result of quantum-confinement effects, the emission colour of semiconductor nanocrystals can be modified dramatically by simply changing their size. Such spectral tunability, together with large photoluminescence quantum yields and high photostability, make nanocrystals attractive for use in a variety of light-emitting technologies--for example, displays, fluorescence tagging, solid-state lighting and lasers. An important limitation for such applications, however, is the difficulty of achieving electrical pumping, largely due to the presence of an insulating organic capping layer on the nanocrystals. Here, we describe an approach for indirect injection of electron-hole pairs (the electron-hole radiative recombination gives rise to light emission) into nanocrystals by non-contact, non-radiative energy transfer from a proximal quantum well that can in principle be pumped either electrically or optically. Our theoretical and experimental results indicate that this transfer is fast enough to compete with electron-hole recombination in the quantum well, and results in greater than 50 per cent energy-transfer efficiencies in the tested structures. Furthermore, the measured energy-transfer rates are sufficiently large to provide pumping in the stimulated emission regime, indicating the feasibility of nanocrystal-based optical amplifiers and lasers based on this approach.     

ZnS：Tb／SiO2核壳结构纳米晶的光学性质

用微乳液法合成了ZnS：Tb／SiO2核壳结构纳米晶,并通过X射线粉末衍射（XRD）、透射电子显微镜（TEM）、荧光光谱等手段对产物的结构、尺寸、形貌、荧光特性进行了表征。结果表明,ZnS：Tb纳米晶的粒径为3nm,ZnS：Tb／SiO2核壳结构纳米晶的粒径为5nm左右,这样就得出壳的厚度约为1nm。在ZnS：Tb／SiO2核壳结构纳米晶的发射光谱上可以观察到有5个发射峰为460、489、544、584和620nm,分别对应ZnS基质的发光和Tb^3＋离子的^5D4→^7F6、^5D4→^7F5、^5D4→^7F4、^5D4→^7F3跃迁。     

An all-silicon Raman laser

The possibility of light generation and/or amplification in silicon has attracted a great deal of attention for silicon-based optoelectronic applications owing to the potential for forming inexpensive, monolithic integrated optical components. Because of its indirect bandgap, bulk silicon shows very inefficient band-to-band radiative electron-hole recombination. Light emission in silicon has thus focused on the use of silicon engineered materials such as nanocrystals, Si/SiO2 superlattices, erbium-doped silicon-rich oxides, surface-textured bulk silicon and Si/SiGe quantum cascade structures. Stimulated Raman scattering (SRS) has recently been demonstrated as a mechanism to generate optical gain in planar silicon waveguide structures. In fact, net optical gain in the range 2-11 dB due to SRS has been reported in centimetre-sized silicon waveguides using pulsed pumping. Recently, a lasing experiment involving silicon as the gain medium by way of SRS was reported, where the ring laser cavity was formed by an 8-m-long optical fibre. Here we report the experimental demonstration of Raman lasing in a compact, all-silicon, waveguide cavity on a single silicon chip. This demonstration represents an important step towards producing practical continuous-wave optical amplifiers and lasers that could be integrated with other optoelectronic components onto CMOS-compatible silicon chips.     

Generation of single optical plasmons in metallic nanowires coupled to quantum dots

Control over the interaction between single photons and individual optical emitters is an outstanding problem in quantum science and engineering. It is of interest for ultimate control over light quanta, as well as for potential applications such as efficient photon collection, single-photon switching and transistors, and long-range optical coupling of quantum bits. Recently, substantial advances have been made towards these goals, based on modifying photon fields around an emitter using high-finesse optical cavities. Here we demonstrate a cavity-free, broadband approach for engineering photon-emitter interactions via subwavelength confinement of optical fields near metallic nanostructures. When a single CdSe quantum dot is optically excited in close proximity to a silver nanowire, emission from the quantum dot couples directly to guided surface plasmons in the nanowire, causing the wire's ends to light up. Non-classical photon correlations between the emission from the quantum dot and the ends of the nanowire demonstrate that the latter stems from the generation of single, quantized plasmons. Results from a large number of devices show that efficient coupling is accompanied by more than 2.5-fold enhancement of the quantum dot spontaneous emission, in good agreement with theoretical predictions.     

A continuous-wave Raman silicon laser

Achieving optical gain and/or lasing in silicon has been one of the most challenging goals in silicon-based photonics because bulk silicon is an indirect bandgap semiconductor and therefore has a very low light emission efficiency. Recently, stimulated Raman scattering has been used to demonstrate light amplification and lasing in silicon. However, because of the nonlinear optical loss associated with two-photon absorption (TPA)-induced free carrier absorption (FCA), until now lasing has been limited to pulsed operation. Here we demonstrate a continuous-wave silicon Raman laser. Specifically, we show that TPA-induced FCA in silicon can be significantly reduced by introducing a reverse-biased p-i-n diode embedded in a silicon waveguide. The laser cavity is formed by coating the facets of the silicon waveguide with multilayer dielectric films. We have demonstrated stable single mode laser output with side-mode suppression of over 55 dB and linewidth of less than 80 MHz. The lasing threshold depends on the p-i-n reverse bias voltage and the laser wavelength can be tuned by adjusting the wavelength of the pump laser. The demonstration of a continuous-wave silicon laser represents a significant milestone for silicon-based optoelectronic devices.     

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.     

Experimental observation of electron-hole recollisions

An intense laser field can remove an electron from an atom or molecule and pull the electron into a large-amplitude oscillation in which it repeatedly collides with the charged core it left behind. Such recollisions result in the emission of very energetic photons by means of high-order-harmonic generation, which has been observed in atomic and molecular gases as well as in a bulk crystal. An exciton is an atom-like excitation of a solid in which an electron that is excited from the valence band is bound by the Coulomb interaction to the hole it left behind. It has been predicted that recollisions between electrons and holes in excitons will result in a new phenomenon: high-order-sideband generation. In this process, excitons are created by a weak near-infrared laser of frequency f(NIR). An intense laser field at a much lower frequency, f(THz), then removes the electron from the exciton and causes it to recollide with the resulting hole. New emission is predicted to occur as sidebands of frequency f(NIR)?+?2nf(THz), where n is an integer that can be much greater than one. Here we report the observation of high-order-sideband generation in semiconductor quantum wells. Sidebands are observed up to eighteenth order (+18f(THz), or n = 9). The intensity of the high-order sidebands decays only weakly with increasing sideband order, confirming the non-perturbative nature of the effect. Sidebands are strongest for linearly polarized terahertz radiation and vanish when the terahertz radiation is circularly polarized. Beyond their fundamental scientific significance, our results suggest a new mechanism for the ultrafast modulation of light, which has potential applications in terabit-rate optical communications.     

太赫兹场作用下的GaAs双量子阱的光吸收分析

用密度矩阵理论分析了在超快脉冲及太赫兹场作用下GaAs量子阱和双量子阱的光吸收谱.分析表明：在直流和太赫兹场作用下,由于量子约束斯塔克效应,光吸收谱呈现出多个激子吸收峰.改变太赫兹的强度和频率,吸收谱出现恶歇分裂,并产生边带,这些分裂主要来源于太赫兹作用下激子的非线性效应.     

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.     

Electromagnetically induced transparency with resonant nuclei in a cavity

The manipulation of light-matter interactions by quantum control of atomic levels has had a profound impact on optical sciences. Such manipulation has many applications, including nonlinear optics at the few-photon level, slow light, lasing without inversion and optical quantum information processing. The critical underlying technique is electromagnetically induced transparency, in which quantum interference between transitions in multilevel atoms renders an opaque medium transparent near an atomic resonance. With the advent of high-brilliance, accelerator-driven light sources such as storage rings or X-ray lasers, it has become attractive to extend the techniques of optical quantum control to the X-ray regime. Here we demonstrate electromagnetically induced transparency in the regime of hard X-rays, using the 14.4-kiloelectronvolt nuclear resonance of the M?ssbauer isotope iron-57 (a two-level system). We exploit cooperative emission from ensembles of the nuclei, which are embedded in a low-finesse cavity and excited by synchrotron radiation. The spatial modulation of the photonic density of states in a cavity mode leads to the coexistence of superradiant and subradiant states of nuclei, respectively located at an antinode and a node of the cavity field. This scheme causes the nuclei to behave as effective three-level systems, with two degenerate levels in the excited state (one of which can be considered metastable). The radiative coupling of the nuclear ensembles by the cavity field establishes the atomic coherence necessary for the cancellation of resonant absorption. Because this technique does not require atomic systems with a metastable level, electromagnetically induced transparency and its applications can be transferred to the regime of nuclear resonances, establishing the field of nuclear quantum optics.     

基于BaLuF5 颐Yb3+ ,Er3+ 纳米晶掺杂的聚合物光波导放大器

为提高聚合物光波导放大器的增益性能, 利用高温法合成了BaLuF5 颐Yb3+ ,Er3+纳米晶, 并分别对纳米晶的形貌、晶体结构和近红外发射特性进行了表征。测试结果表明, 纳米晶平均粒径为13 nm, 并在1 530 nm 处具有较强的发射, 荧光半高宽为50 nm。将合成的纳米晶掺杂入SU-8 聚合物作为光波导放大器的芯层材料, 使
用光刻显影等工艺, 在表面长有二氧化硅的硅衬底上制备出了聚合物光波导放大器。当980 nm 波长泵浦光功率为280 mW、信号光波长为1 530 nm 且功率为0. 1 mW 时, 在长度为1. 1 cm 的光波导放大器中, 获得了3. 95 dB的相对增益。     

Formation cross-sections of singlet and triplet excitons in pi-conjugated polymers

Electroluminescence in organic light-emitting diodes arises from a charge-transfer reaction between the injected positive and negative charges by which they combine to form singlet excitons that subsequently decay radiatively. The quantum yield of this process (the number of photons generated per electron or hole injected) is often thought to have a statistical upper limit of 25 per cent. This is based on the assumption that the formation cross-section of singlet excitons, sigmaS, is approximately the same as that of any one of the three equivalent non-radiative triplet exciton states, sigmaT; that is, sigmaS/sigmaT approximately 1. However, recent experimental and theoretical work suggests that sigmaS/sigmaT may be greater than 1. Here we report direct measurements of sigmaS/sigmaT for a large number of pi-conjugated polymers and oligomers. We have found that there exists a strong systematic, but not monotonic, dependence of sigmaS/sigmaT on the optical gap of the organic materials. We present a detailed physical picture of the charge-transfer reaction for correlated pi-electrons, and quantify this process using exact valence bond calculations. The calculated sigmaS/sigmaT reproduces the experimentally observed trend. The calculations also show that the strong dependence of sigmaS/sigmaT on the optical gap is a signature of the discrete excitonic energy spectrum, in which higher energy excitonic levels participate in the charge recombination process.     

一种可用于压缩态光场弱信号探测的放大电路

根据基于基尔霍夫电流定律的平衡零拍探测原理,设计了一种新的测试方法,在测试过程中脱离以往复杂光路的搭建以及实验环境的高要求,直接对平衡零拍探测中所需的量子噪声光电流信号进行放大测试,并且可以判断出对微弱的量子噪声电流信号的放大效果.另外,在测试过程中,该放大电路具有高灵敏度性和高增益性,能够对微弱的量子噪声很好地进行放大.测试结果表明,该种测试方法能够很简捷地测试出放大后的量子噪声.     

Stimulated emission of polarization-entangled photons

Entangled photon pairs-discrete light quanta that exhibit non-classical correlations-play a crucial role in quantum information science (for example, in demonstrations of quantum non-locality, quantum teleportation and quantum cryptography). At the macroscopic optical-field level non-classical correlations can also be important, as in the case of squeezed light, entangled light beams and teleportation of continuous quantum variables. Here we use stimulated parametric down-conversion to study entangled states of light that bridge the gap between discrete and macroscopic optical quantum correlations. We demonstrate experimentally the onset of laser-like action for entangled photons, through the creation and amplification of the spin-1/2 and spin-1 singlet states consisting of two and four photons, respectively. This entanglement structure holds great promise in quantum information science where there is a strong demand for entangled states of increasing complexity.     

Optical gain in silicon nanocrystals

Adding optical functionality to a silicon microelectronic chip is one of the most challenging problems of materials research. Silicon is an indirect-bandgap semiconductor and so is an inefficient emitter of light. For this reason, integration of optically functional elements with silicon microelectronic circuitry has largely been achieved through the use of direct-bandgap compound semiconductors. For optoelectronic applications, the key device is the light source--a laser. Compound semiconductor lasers exploit low-dimensional electronic systems, such as quantum wells and quantum dots, as the active optical amplifying medium. Here we demonstrate that light amplification is possible using silicon itself, in the form of quantum dots dispersed in a silicon dioxide matrix. Net optical gain is seen in both waveguide and transmission configurations, with the material gain being of the same order as that of direct-bandgap quantum dots. We explain the observations using a model based on population inversion of radiative states associated with the Si/SiO2 interface. These findings open a route to the fabrication of a silicon laser.