Nanotwinning in CdS quantum dots

High resolution transmission electron microscopy, X-ray diffraction and photoluminescence measurements are carried out in order to study the defects in CdS quantum dots (QDs), synthesized in cubic phase by chemical co-precipitation method. The nanotwinning structures in CdS quantum dots (∼2.7 nm) are reported for the first time. Mostly CdS QDs are characterized by existence of nanotwin structures. The twinning structures are present together with stacking faults in some QDs while others exist with grain boundaries. Raman spectroscopy analysis shows intense and broad peaks corresponding to fundamental optical phonon mode (LO) and the first over tone mode (2LO) of CdS at 302 cm⁻¹ and 605 cm⁻¹ respectively. A noticeable shift is observed in Raman lines indicating the effect of phonon confinement. Fourier transform infrared spectroscopy analysis confirms the presence of Cd–S stretching bands at 661 cm⁻¹ and 706 cm⁻¹. The photoluminescence spectrum shows emission in yellow and red regions of visible spectrum. The presence of stacking faults and other defects are explained on the basis of X-rays diffraction patterns and are correlated with photoluminescence spectrum. These nanotwinning and microstructural defects are responsible for different emissions from CdS QDs.     

Photoluminescence quenching of CdTe/CdS core-shell quantum dots in aqueous solution by ZnO nanocrystals

Photoluminescence (PL) properties of 3-mercaptopropionic acid (MPA) coated CdTe/CdS core-shell quantum dots (QDs) in aqueous solution in the presence of ZnO colloidal nanocrystals were studied by steady-state and time-resolved PL spectroscopy. The PL quenching of CdTe/CdS core-shell QDs with addition of purified ZnO nanocrystals resulted in a decrease in PL lifetime and a small red shift of the PL band. It was found that CdTe(1.5 nm)/CdS type II core-shell QDs exhibited higher efficiency of PL quenching than the CdTe(3.0 nm)/CdS type I core-shell QDs, indicating an electron transfer process from CdTe/CdS core-shell QDs to ZnO nanocrystals. The experimental results indicated that the efficient electron transfer process from CdTe/CdS core-shell QDs to ZnO nanocrystals could be controlled by changing the CdTe core size on the basis of the quantum confinement effect.     

Entropies associated with electron emission from InAs/GaAs quantum dots

Entropies associated with the transition of electrons into and out of InAs/GaAs quantum dots (QDs) are calculated by considering the temperature dependence of energy eigenvalues due to strain and energy band offset variations. It is found that, for InAs/GaAs quantum dots with base/height dimensions of 20/10 nm, the contribution from the surrounding lattice to entropy is smaller than for the temperature region below 100 K, where most measurements of thermal emission rates are performed. Including the electron degeneracy, the total entropy change has an upper limit of when releasing the first electron from the s-shell, while the second released s-electron is connected with an entropy change not larger than the absolute value of .     

CdS量子点的酿酒酵母仿生合成及光谱表征

以酿酒酵母为载体,常温下利用仿生法成功合成了CdS量子点。荧光发射光谱、紫外吸收光谱以及荧光显微镜照片证明,该方法合成的CdS量子点的荧光发射峰位置在443nm,在紫外灯下能发蓝绿色荧光。透射电子显微镜(TEM)表征结果表明,该仿生法合成的CdS量子点为六方纤锌矿结构。以荧光发射和紫外吸收光谱为性能指标,考察了酿酒酵母生长时期、Cd2+的反应浓度以及反应时间等条件对合成CdS量子点的影响。当酿酒酵母处于生长稳定期初期时,与浓度为0.5mmol.L-1的Cd2+共培养24h后所合成的CdS量子点荧光最强。实验中观察到,换液培养可有效提高酿酒酵母合成CdS量子点的产量。     

Investigation of the relation between photoluminescence intensity and decay time reduction with plasmon effect in InGaAs quantum dots

Plasmonic effects on photoluminescence are investigated via time-integrated and resolved photoluminescence (PL) in epitaxially grown InGaAs quantum dots (QDs). The decay time and PL intensities are compared as a function of the density of Ag nanoplates. Optimal conditions for both reduction lifetime and enhanced PL intensity were found to be a 1:15 ratio of Ag nanoplates to water. Both less and greater than that ratio 1:15, the lifetime increased and the enhancement factor of PL intensity decreased. In addition, the plasmon effect was investigated via resonance wavelength and temperature-dependent PL measurements. At 150K near the resonance conditions between PL from InGaAs QDs and Ag nanoplates, both the lifetime reduction and enhancement factor are maximized. Intensity enhancement is correlated to lifetime reduction for various conditions to identify a condition for maximized enhancement of radiative recombination for designing future ultrafast plasmonic nanolasers.     

Luminescence study of Si/Ge quantum dots

We present a photoluminescence (PL) study of Ge quantum dots embedded in Si. Two different types of recombination processes related to the Ge quantum dots are observed in temperature-dependent PL measurements. The Ge dot-related luminescence peak near 0.80 eV is ascribed to the spatially indirect recombination in the type-II band lineup, while a high-energy peak near 0.85 eV has its origin in the spatially direct recombination. A transition from the spatially indirect to the spatially direct recombination is observed as the temperature is increased. The PL dependence of the excitation power shows an upshift of the Ge quantum dot emission energy with increasing excitation power density. The blueshift is ascribed to band bending at the type-II Si/Ge interface at high carrier densities. Comparison is made with results derived from measurements on uncapped samples. For these uncapped samples, no energy shifts due to excitation power or temperatures are observed in contrast to the capped samples.     

各向异性量子点单光子发射的高偏振度特性

研究了线偏振脉冲光场激发下,单个各向异性InGaAs量子点的高偏振光发射. 给出其偏振因子与两个正交本征态之间的交叉弛豫之间的关系式. 分析表明，交叉弛豫随激发场强度增大，并导致偏振因子随激发场入射脉冲面积减小. 关键词： 量子点 单光子发射 偏振度     

Correlated photon emission from semiconductor quantum dots grown in inverted pyramids

We demonstrate photon antibunching and deterministic single-photon operation using single InGaAs/AlGaAs semiconductor quantum dots grown on pre-patterned substrates. Additionally, we observe several types of single-photon cascades involving biexcitonic and other excitonic complexes and have modeled this behavior using numerical Monte-Carlo simulations. This method allows us to determine different non-radiative mechanisms otherwise not directly accessible via conventional spectroscopic methods.     

Activation of silicon quantum dots for emission

The emission of silicon quantum dots is weak when their surface is passivated well. Oxygen or nitrogen on the surface of silicon quantum dots can break the passivation to form localized electronic states in the band gap to generate active centers where stronger emission occurs. From this point of view, we can build up radiative matter for emission. Emissions of various wavelengths can be obtained by controlling the surface bonds of silicon quantum dots. Our experimental results demonstrate that annealing is important in the treatment of the activation, and stimulated emissions at about 600 and 700 nm take place on active silicon quantum dots.     

Stimulated emission from PbS‐quantum dots in glass matrix

The luminescence behavior of PbS‐quantum dots in glass matrix (PbS:Glass) is investigated. Steady‐state and time‐resolved photoluminescence are applied in a wide range of excitation densities up to pulse energies exceeding 50 µJ/cm². While perfect linear recombination is observed across four orders of magnitude, an additional radiative recombination mechanism emerges at an excitation density of 1 µ J/cm² per pulse at 390 nm excitation and increases the external quantum efficiency. The time constant of this process is ∼20–40 ps. It is ascribed to stimulated emission. No hint to any non‐linear non‐radiative processes such as Auger recombination is observed. Thermal effects, however, still set limits. This is encouraging news for PbS:Glass as potential laser material.     

Luminescence of CsPbBr3-like quantum dots in CsBr single crystals

Luminescence and decay kinetics of the Pb²⁺ aggregates in CsBr host crystals were measured in the 4–300 K temperature interval and in 10⁻¹⁰–10⁻³ time scale. Their emission properties are similar to those of CsPbBr₃ bulk crystal showing a subnanosecond free exciton emission in the 520–540 nm spectral region and slower trapped exciton emission in the 530–580 nm spectral region. An efficient energy exchange between the free and trapped exciton states is shown by the temperature dependencies of emission spectra. The quantum size effect is demonstrated in the high energy shift and broadening of the absorption and emission spectra and an estimate of the size of the CsPbBr₃-like aggregates is provided. Independent evidence of the presence of the CsPbBr₃ and Cs₄PbBr₆ aggregated phases in the CsBr host was obtained by X-ray structural studies.     

硅量子点发光的激活及其物理模型研究

在真空或惰性气体中制备的硅量子点发光很弱,硅量子点表面被氢较好钝化后的发光也不强.硅量子点表面的硅氧键或硅氮键能破坏这种钝化并在带隙中形成局域电子态,在局域电子态对应的激活中心有很强的发光.可以用这种方式构建发光物质,控制硅量子点表面的键合可获得不同波长的发光.在硅量子点的发光激活处理过程中,退火是很重要的环节.对于硅量子点发光激活的机理,本文给出了相应的物理模型.实验证明,在600和700 nm波长附近观察到了激活硅量子点的受激发光,在1500 nm到1600 nm波长范围观察到了激活硅量子点的较强发光.     

Facile and highly effective synthesis of nitrogen-doped graphene quantum dots as a fluorescent sensing probe for Cu2+ detection

Nitrogen-doped graphene quantum dots (N-GQDs) with high blue fluorescence efficiency were synthesized by the hydrothermal method from p-Phenylenediamine and p-Coumaric acid. The N-GQDs possess several superiorities, most significantly in excellent solubility and superior photostability. Besides, the as-prepared N-GQDs exhibit a uniform size distribution with a diameter of about 3.8 ± 0.5 nm. After dispersing the N-GQDs in water, the formed aqueous solution still presents a stable and homogeneous phase even after 2 months at room temperature. The N-GQD dispersion was further utilized as sensing probes for the selective detection of copper ions (Cu²⁺), which is realized by the photoluminescence (PL) quenching of N-GQDs after adding Cu²⁺. The detection limit for Cu²⁺ was found to be 57 nM L⁻¹, with superior selectivity in the presence of other commonly interfering metal ions. The presented results in this study provide a facile and high-efficiency method for synthesizing N-GQDs, with ultra-high detectivity and selectivity for Cu²⁺ detection, offering numerous opportunities for the development of biosensing, bioimaging, environment monitoring, and others.     

Lifetime determination of materials that exhibit a stretched exponential luminescent decay

We report frequency- and time-domain luminescent lifetime measurements for materials that exhibit a broad spectrum of lifetimes, specifically, those for which the observed decay dynamics can be described by a stretched exponential function. The spectrum of lifetimes of such materials can be characterized by an average lifetime, and in principle this average can be extracted from either time- or frequency-domain measurements. In practice, this requires some care, because the extent to which the various states are excited depends on how long their lifetime is relative to the excitation pulse width or period. For the complex luminescent materials ZnS:Cu,Al and CdS quantum dots we compare the average lifetime obtained from frequency-domain data and from time-domain data under both pulsed laser excitation and steady-state, dc excitation. The agreement between the average measured lifetimes is good, but not perfect, showing that quoted average lifetimes for complex materials can be dependent on the measurement technique. Finally, a spectrum of lifetimes is given that gives rise to stretched exponential relaxation and this spectrum is used to compute frequency-domain data for a stretched exponential material.     

Preparation of water-soluble CdTe/CdS core/shell quantum dots with enhanced photostability

CdTe/CdS core/shell quantum dots (QDs) have been synthesized in an aqueous phase using thioacetamide as a sulfur source. The quantum yield was greatly enhanced by the epitaxial growth of a CdS shell, which was confirmed by X-ray photoelectron spectroscopy (XPS) results. The quantum yield of as-prepared CdTe/CdS core/shell QDs without any post-preparative processing reached 58%. The experimental results illustrate that the QDs with core/shell structure show better photostability than thioglycolic acid (TGA)-capped CdTe QDs. The cyclic voltammograms reveal higher oxidation potentials for CdTe/CdS core/shell QDs than for TGA-capped CdTe QDs, which explains the superior photostability of QDs with a core/shell structure. This enhanced photostability makes these QDs with core/shell structure more suitable for bio-labeling and imaging.     

Chitosan hydrogel films as a template for mild biosynthesis of CdS quantum dots with highly efficient photocatalytic activity

Cadmium sulfide (CdS) semiconducting quantum dots (QDs) were prepared using in situ synthesizing method in crosslinked chitosan hydrogel films under relative mild experimental conditions and characterized by X-ray diffraction (XRD), thermogravimetric analysis (TGA), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The experimental results confirmed that crosslinked chitosan hydrogel films provided a confined matrix for CdS QDs growth in uniform size through chelation and electrostation between cadmium ions and amino groups in chitosan chains. The CdS QDs/chitosan composite films exhibited a highly efficient photocatalytic activity for decolorization of methyl orange (MO) solution under visible light irradiation. The good linearity relationship between ln (C₀/C_i) and irradiation time (t) indicated that the decolorization of MO dye under present experimental conditions followed pseudo-first-order kinetics. These results suggested that CdS QDs/chitosan composite films were suitable material for potential application in decolorization of organic dye pollutants under visible light irradiation.     

InAs/GaAs量子点1.3 μm单光子发射特性

采用双层耦合量子点的分子束外延生长技术生长了InAs/GaAs量子点样品,把量子点的发光波长成功地拓展到1.3 μm.采用光刻的工艺制备了直径为3 μm的柱状微腔,提高了量子点荧光的提取效率.在低温5 K下,测量得到量子点激子的荧光寿命约为1 ns;单量子点荧光二阶关联函数为0.015,显示单量子点荧光具有非常好的单光子特性;利用迈克耳孙干涉装置测量得到单光子的相干时间为22 ps,对应的谱线半高全宽度为30 μeV,且荧光谱线的线型为非均匀展宽的高斯线型.     

多孔硅量子点的受激辐射：陷阱态的作用

经激光辐照和高温退火后能够在硅基上生成氧化多孔硅结构。用514 nm的激光泵浦,观测到该多孔硅的受激辐射。当激励强度超过阈值时,在650～750 nm区域有很强的受激发光峰。这些受激发光峰的半高宽小于0.5 nm。激光辐照和高温退火后,在样品上能形成某些特殊的氧化结构。在傅里叶红外光谱分析中,显示有硅氧双键或硅氧桥键在硅表面形成。计算结果表明：当硅氧双键或硅氧桥键形成时,电子的陷阱态出现在纳晶硅的带隙中。价带顶和陷阱态之间的粒子数反转是解释这种受激辐射的关键。     

Physical reasons of emission transformation in infrared CdSeTe/ZnS quantum dots at bioconjugation

The core/shell CdSeTe/ZnS quantum dots (QDs) with emission at 780–800 nm (1.55–1.60 eV) have been studied by means of photoluminescence (PL) and Raman scattering methods in the nonconjugated state and after conjugation to different antibodies (Ab): (i) mouse monoclonal [8C9] human papilloma virus Ab, anti-HPV 16-E7 Ab, (ii) mouse monoclonal [C1P5] human papilloma virus HPV16 E6+HPV18 E6 Ab, and (iii) pseudo rabies virus (PRV) Ab. The transformations of PL and Raman scattering spectra of QDs, stimulated by conjugated antibodies, have been revealed and discussed.The energy band diagram of core/shell CdSeTe/ZnS QDs has been designed that helps to analyze the PL spectra and their transformations at the bioconjugation. It is shown that the core in CdSeTe/ZnS QDs is complex and including the type II quantum well. The last fact permits to explain the nature of infrared (IR) optical transitions (1.55–1.60 eV) and the high energy PL band (1.88–1.94 eV) in the nonconjugated and bioconjugated QDs. A set of physical reasons has been analyzed with the aim to explain the transformation of PL spectra in bioconjugated QDs. Finally it is shown that two factors are responsible for the PL spectrum transformation at bioconjugation to charged antibodies: (i) the change of energy band profile in QDs and (ii) the shift of QD energy levels in the strong quantum confinement case. The effect of PL spectrum transformation is useful for the study of QD bioconjugation to specific antibodies and can be a powerful technique for early medical diagnostics.     

脉冲激发三能级体系半导体量子点的单光子发射效率

研究了脉冲激发下单个半导体量子点中单光子发射的统计特性.在旋转波近似条件下，由系统粒子数演化主方程并结合量子回归理论推导了二阶相关函数的运动方程，利用此方程讨论了二阶相关函数随输入脉冲面积的关系.在窄脉冲宽度的脉冲激发下，单光子的发射概率p和效率η都随着强度的增强而产生振荡.研究表明，采用窄脉冲宽度，当输入脉冲面积在π附近时可以得到较高的单光子发射效率. 关键词： 半导体量子点 单光子发射 三能级系统