Controlling the spontaneous emission rate of single quantum dots in a two-dimensional photonic crystal

We observe large spontaneous emission rate modification of individual InAs quantum dots (QDs) in a 2D photonic crystal with a modified, high-Q single-defect cavity. Compared to QDs in a bulk semiconductor, QDs that are resonant with the cavity show an emission rate increase of up to a factor of 8. In contrast, off-resonant QDs indicate up to fivefold rate quenching as the local density of optical states is diminished in the photonic crystal. In both cases, we demonstrate photon antibunching, showing that the structure represents an on-demand single photon source with a pulse duration from 210 ps to 8 ns. We explain the suppression of QD emission rate using finite difference time domain simulations and find good agreement with experiment.     

Far field emission of micropillar and planar microcavities lattice-matched to ZnTe

We investigate light emission from ZnTe-based microcavities containing CdTe quantum dots (QDs), with 2D (planar cavity) and 0D (pillar cavities) photonic confinement. The angular distribution from the planar cavity is presented as well as 2D cross-sections of the far field distribution of radiation from the micropillars. The efficient and desirable modification of the isotropic radiation of the QDs is shown for such structures. The diffraction observed is found to be inherent for such experiments with large numerical aperture of the lens and small diameters of the investigated pillars. This diffraction is successfully modeled.     

Effect of temperature and pumping power on the photoluminescence properties of type-II CdTe/CdSe core-shell QDs

CdTe/CdSe core-shell QDs type II was prepared by two steps synthetic process and embedded in polymer host. Emission in the NIR region was recorded. The effect of Ar laser excitation at different powers on the optical properties of the prepared QDs is studied at different temperatures (300-10 K). Amplified spontaneous emission is observed at room temperature and at 10 K. Also, lifetime measurement of prepared QDs was documented using N₂-laser.     

以巯基丙酸为稳定剂的水溶性CdTe量子点的水热合成及表征

以巯基丙酸(MPA)为稳定剂,采用水热合成方法在160 ℃下合成水溶性CdTe量子点。研究了不同反应时间及反应前驱体溶液的不同pH值对合成的CdTe量子点光学性质的影响。结果表明:所制得的CdTe量子点的荧光发射波长在510~661 nm范围内连续可调,并且CdTe量子点的光学性质强烈地依赖于反应前驱体溶液的pH值,最佳pH值为9。透射电子显微镜和X射线衍射分析表明所制备的CdTe量子点的形状接近于球形,粒径分布较均匀。与回流方法制备的水溶性量子点相比,高温条件下的水热合成方法简单,反应时间短,CdTe量子点生长速度快,100 min就可生长到3.5 nm,并且所制得的CdTe量子点荧光强度高,稳定性好,荧光量子产率也较高,最高可达44.6%。     

Advances in photonic crystals with MEMS and with semiconductor quantum dots

We discuss photonic crystals (PCs) with a microelectromechanical system (MEMS) and semiconductor quantum dots (QDs) as novel classes of PC devices. Integration of MEMS structures into PC devices enables one to realize several kinds of functional devices, such as modulators, switches, and tunable filters for highly integrated photonic circuits. We describe the basic concept of MEMS-integrated PC devices and show numerical and experimental demonstrations of MEMS-integrated functional PC devices. On the other hand, QDs are promising candidates for active media in PC devices. Spontaneous emission control of QD emission in PC nanocavities is especially important for novel optoelectronic devices and quantum information devices. In PC nanocavities, the interaction between QD excitons and photons is enhanced dramatically. The control of spontaneous emission spectrum and the enhancement of the luminescence intensity of InAs QDs by PC nanocavities are demonstrated at telecommunication wavelengths. The Purcell effect for ensemble and single QDs in PC nanocavities are also discussed.     

Fabrication of three‐dimensional photonic crystals in quantum‐dot‐based materials

Controlling spontaneous emission (SE) is of fundamental importance to a diverse range of photonic applications including but not limited to quantum optics, low power displays, solar energy harvesting and optical communications. Characterized by photonic bandgap (PBG) property, three‐dimensional (3D) photonic crystals (PCs) have emerged as a promising synthetic material, which can manipulate photons in much the same way as a semiconductor does to electrons. Emission tunable nanocrystal quantum dots (QDs) are ideal point sources to be embedded into 3D PCs towards active devices. The challenge however lies in the combination of QDs with 3D PCs without degradation of their emission properties. Polymer materials stand out for this purpose due to their flexibility of incorporating active materials. Combining the versatile multi‐photon 3D micro‐fabrication techniques, active 3D PCs have been fabricated in polymer‐QD composites with demonstrated control of SE from QDs. With this milestone novel miniaturized photonic devices can thus be envisaged.     

单质碘对水溶性CdTe量子点的荧光猝灭研究

合成了不同尺寸的、巯基丙酸和半胱氨酸修饰的水溶性CdTe量子点,并研究了I2与CdTe量子点的相互作用,实验发现I2能够明显猝灭CdTe量子点的荧光,且猝灭程度与量子点的修饰剂有关,没有表现出明显的尺寸依赖效应。     

Au纳米颗粒和CdTe量子点复合体系发光增强和猝灭效应

利用金属蒸发真空多弧离子源注入机, 将Au离子注入到高纯石英玻璃来制备镶嵌有Au 纳米颗粒的衬底材料, 随后将化学方法合成的CdTe量子点旋涂在玻璃衬底上制备了Au纳米颗粒和CdTe量子点复合体系. 通过对镶嵌有Au纳米颗粒的衬底进行热退火处理来控制Au纳米颗粒的生长和分布, 系统研究了Au纳米颗粒的局域表面等离子体共振对CdTe量子点光致发光性能的影响. 利用光学吸收谱、原子力显微镜、透射电子显微镜和光致发光谱对样品进行了表征和测试. 光致发光谱表明, Au纳米颗粒的局域表面等离子体对CdTe量子点的发光有增强效应也有猝灭效应. 深入分析了Au纳米颗粒和CdTe量子点之间的相互作用过程, 提出了关于Au-CdTe 纳米复合体系中CdTe 发光增强和猝灭的新机理. 该实验结果为利用金属纳米颗粒表面等离子体技术制备高发光性能的光电子器件提供了较好的参考.     

CdTe量子点荧光猝灭法测定微量铅

以CdTe量子点作为荧光探针,基于荧光猝灭法对铅进行了定量检测,考察了缓冲溶液体系、量子点浓度、反应时间等多种因素的影响。实验结果表明,在pH 7.5的0.2mol/L Na2HPO4-NaH2PO4缓冲液中,反应时间为10min,铅浓度为2.0×10-6—3.5×10-5mol/L范围时,其线性回归方程为ΔF=26.35+11.47C(×10-6mol/L),相关系数和检出限分别为0.9991和1.8×10-8mol/L。该方法灵敏度高,为铅的测定提供了新的方法。     

庆大霉素与水溶性CdTe量子点的荧光共振能量转移作用

以巯基丙酸(mercaptopropionic acid,MPA)为稳定剂合成水溶性CdTe最子点(quantum dots,QDs),以CdTe QDs作为能量供体.庆大霉素(Gentamycin,GT)作为能垦受体,建立了荧光共振能量转移(fluorescence resonance energy transfer,FRET)体系.在690 nm处可见发射峰,半峰宽约10 nm,在一定范围内荧光强度与GT的含量旱线性关系,线性范围为2～20 mg·L-1,相关系数r=0.986 7.优化了不同的激发波长、pH、离子强度、时间和温度等凼素对反应的影响,并应用傅里叶变换红外光谱(Fourier transform infrared spectroscopy,FTIR)和高效液相色谱(high-performance liquid chromatography,HPLC)分别表征了化学结构和相对专一性.结果表明巯基丙酸的巯基中S原子和羧基中氧原子与纳米微粒表面的富Cd离子发生了配位作用,CdTe QDs与GT的耦合主要是通过量子点周围巯基丙酸羧基(-COOH)中的氧原子与GT的胺基(-NH2)形成分子问氧键实现的;GT与CdTe QDs的结合率为0.35:1.研究表明GT可以作为检测CdTe QDs标记牛血清白蛋白(bovine serum albumin,BSA)的荧光增敏剂,荧光强度值增强6倍,应用前景广阔.     

Methyl viologen induced fluorescence quenching of CdTe quantum dots for highly sensitive and selective “off-on” sensing of ascorbic acid through redox reaction

Journal of Fluorescence - A turn-on fluorescent sensor based on CdTe quantum dots (QDs) is designed for highly sensitive and selective ascorbic acid (AA) detection. CdTe shows a strong emission...     

CdTe量子点荧光猝灭法测定钴

以CdTe量子点作为荧光探针,基于荧光猝灭法对钴(Ⅱ)进行了定量检测,考察了缓冲溶液体系、量子点浓度、反应时间等多种因素的影响。实验结果表明,在pH8.0的0.2mol/LNa2HPO4-NaH2PO4缓冲液中,反应时间为10min,钴(Ⅱ)浓度为1.6×10-5—20×10-5mol/L范围时,其线性回归方程为F0/F=1.45+0.096Q(10-5mol/L),检出限为3×10-7mol/L。该方法检测范围宽,灵敏度高,为钴的测定提供了新的方法。     

Decay lifetime and evolution of semiconductor quantum dots in photonic crystals

Spontaneous emission from GaAs/AlGaAs quantum dots (QDs) embedded in photonic crystals with a narrow photonic band gap is studied theoretically. The results show that the decay lifetime is very sensitive to the sizes of QDs, and both inhibited and accelerated emission can occur, which had been indicated in a previous experiment. The Weisskopf–Wigner approximation, good for atoms and molecules, may be incorrect for QDs. A damped Rabi oscillation of the excited state with the transition frequency outside the photonic band gap may appear, which is impossible for atoms and molecules.     

巯基乙胺稳定的CdTe量子点荧光猝灭法测定间苯二酚

以CdTe量子点作为荧光探针,基于荧光猝灭法对间苯二酚进行了定量检测,考察了缓冲溶液体系、量子点浓度、反应时间等多种因素的影响.实验结果表明,在pH 6.5的0.2mol/LNa<,2>HPO<,2>-NaH<,2>PO<,4>缓冲液中,反应时间为15min.间苯二酚浓度为1.6×10<'-6>-2.0×10<'-5>...     

水溶性量子点荧光探针用于帕珠沙星的含量测定

文章采用荧光光谱和紫外光谱研究了CdTe量子点(CdTe QDs)与广谱抗菌药物帕珠沙星的相互作用。结果表明,随着帕珠沙星浓度的增加,CdTe QDs荧光强度有规律的降低,但通过透射电镜图对QDs及加入帕珠沙星后的QDs进行比较,发现QDs仍然均一单分散,表明反应的作用机理可能是帕珠沙星促使QDs表面键合的有机分子发生变化,在Cd空位表现出的表面缺损上形成了碲氧复合物,致使荧光猝灭。因此该反应可作为一种新颖的快速检测帕珠沙星含量的方法。在一定条件下,帕珠沙星溶液的浓度与量子点荧光强度成线性关系,线性范围为10.0～850 μg·mL-1,相关系数r为0.995 4,检测限(S/N=3)为3.254×10-3 μg·mL-1。药物对量子点的猝灭常数为2.188×104 L·mol-1。应用到冻干粉针剂和氯化钠注射液中帕珠沙星的含量测定,所得结果与标示量一致。该方法较常用检测方法具有简便、快捷、灵敏、线性范围宽的优点,并有望进一步开展发药物体内显像及作用机理的研究。     

Aqueous synthesis of thiol-capped CdTe quantum dots and its photoluminescence enhancement via room temperature treatment with alkyl chain diamines

In this study the CdTe quantum dots (QDs) are synthesized in aqueous solution with three thiol-contained capping ligands of thioglycollic acid (TGA), 3-mercaptopropionic acid (MPA), and l-cysteine (lCys). The photoluminescence (PL) enhancement of the as-prepared QDs is also conducted via room temperature treatment with alkyl chain diamines. Our measurements on the ultraviolet–visible (UV–vis) absorption and fluorescence emission reveal that both the growth kinetics and the PL efficiency of the QDs vary a lot with the molecular structures of the three involved ligands. In comparison with TGA and lCys, MPA endows the QDs with a wide color tuning range from cyan to deep red and strong PL emission while its full width at half maximum (FWHM) is regretfully large. Notable enhancement on PL emission is achieved for the TGA and MPA capped QDs via room temperature treatment with diamines solutions while in the case of the QDs capped by lCys the enhancement is practically meaningless.     

Synthesis of AS1411-Aptamer-Conjugated CdTe Quantum Dots with High Fluorescence Strength for Probe Labeling Tumor Cells

In this paper, we report microwave-assisted, one-stage synthesis of high-quality functionalized water-soluble cadmium telluride (CdTe) quantum dots (QDs). By selecting sodium tellurite as the Te source, cadmium chloride as the Cd source, mercaptosuccinic acid (MSA) as the capping agent, and a borate-acetic acid buffer solution with a pH range of 5–8, CdTe nanocrystals with four colors (blue to orange) were conveniently prepared at 100 °C under microwave irradiation in less than one hour (reaction time: 10–60 min). The influence of parameters such as the pH, Cd:Te molar ratio, and reaction time on the emission range and quantum yield percentage (QY%) was investigated. The structures and compositions of the prepared CdTe QDs were characterized by transmission electron microscopy, energy-dispersive X-ray spectroscopy, selective area electron diffraction, and X-ray powder diffraction experiments. The formation mechanism of the QDs is discussed in this paper. Furthermore, AS1141-aptamer-conjugated CdTe QDs in the U87MG glioblastoma cell line were assessed with a fluorescence microscope. The obtained results showed that the best conditions for obtaining a high QY of approximately 87 % are a pH of 6, a Cd:Te molar ratio of 5:1, and a 30-min reaction time at 100 °C under microwave irradiation. The results showed that AS1141-aptamer-conjugated CdTe QDs could enter tumor cells efficiently. It could be concluded that a facile high-fluorescence-strength QD conjugated with a DNA aptamer, AS1411, which can recognize the extracellular matrix protein nucleolin, can specifically target U87MG human glioblastoma cells. The qualified AS1411-aptamer-conjugated QDs prepared in this study showed excellent capabilities as nanoprobes for cancer targeting and molecular imaging.     

The double-effect mechanism between Fe3O4 nanoparticles and MSA-capped CdTe QDs

Water-soluble mercaptosuccinic acid (MSA)-capped CdTe quantum dots (QDs) of two sizes and superparamagnetic Fe₃O₄ nanoparticles have been synthesized and used to investigate the effect of the mechanism of Fe₃O₄ nanoparticles on the fluorescence intensity of QDs. In the presence of a low concentration of Fe₃O₄ nanoparticles, the CdTe QDs with smaller particle size exhibit fluorescence quenching while fluorescence enhancement of CdTe QDs with larger particle size was observed, and the fluorescence intensity changes with the excitation wavelength and the concentration of Fe₃O₄ nanoparticles. The mechanism study shows that there is a double-effect between the Fe₃O₄ and CdTe QDs: one is the fluorescence quenching effect due to Fe₃O₄ strong absorption of excitation and emission light, the other is the fluorescence enhancement effect resulting from a localized electromagnetic field caused by the absorption of exciting light. The fluorescence of CdTe QDs with lower concentration of Fe₃O₄ nanoparticles was determined via the synergy of the double-effect. To our best knowledge, this is the first systematic study on the interaction between Fe₃O₄ nanoparticles and CdTe QDs, which finds the fluorescence enhancement effect in the presence of low concentration of Fe₃O₄.     

Microwave-Assisted Aqueous Synthesis of Highly Luminescent Carboxymethyl Chitosan-Coated CdTe/CdS Quantum Dots as Fluorescent Probe for Live Cell Imaging

This paper describes the development of a simplified and rapid method for the aqueous synthesis of quantum dots (QDs) with CdTe cores and gradient CdS external shells (CdTe/CdS QDs) aided by microwave irradiation. Several synthesis parameters, such as molar ratio of reagents, pH, reaction temperature, and reaction time, were studied in details. Under the optimized conditions, highly effective CdTe/CdS QDs could be synthesized in aqueous phase in only 15 min. In order to improve the biocompatibility of the CdTe/CdS QDs, these QDs were then interacted with carboxymethyl chitosan (CMC) so as they could be used as fluorescent probes in the aqueous phase. With the incorporation of CMC, the stability of modified QDs was found to have improved significantly (from 4 months to more than 10 months at room temperature). The photoluminescence quantum yield (PLQY) of the modified QDs could reach 75%, other parameters include a full width at half maximum of the emission (FWHM) spectrum as 40 ~ 60 nm, and an average size, estimated from electron microscopic images, as 3.5 nm. As fluorescent probes, these modified QDs were successfully used for imaging live Madin–Darby canine kidney (MDCK) cells, in which the preliminary results indicated that these modified QDs demonstrated good biocompatibility and showed promising applications for bio-labeling and imaging.     

Photoluminescence properties of a novel conjugate of water-soluble CdTe quantum dots to guanine

A novel conjugate of water-soluble CdTe quantum dots to a small biomolecule guanine has been obtained in aqueous phase. The photoluminescence property and the stability of the conjugate increased comparing to CdTe QDs. The interaction between CdTe QDs and guanine was studied by TEM, fluorescence microscope and photoluminescence (PL), IR, UV-Vis spectra. The effects of reflux time, pH value, ionic strength, and the ratio of CdTe QDs to guanine on the photoluminescence properties of conjugate were investigated in detail. The results show that guanine has a great influence on both the photoluminescence property and stability of thioglycolic acid-stabilized CdTe QDs. The formation of coordination and hydrogen bond between guanine molecules and CdTe including thioglycolic acid on its surface may effectively enhance the PL intensity and stability of CdTe QDs. The maximum PL intensity of the conjugate was obtained on the condition with lower ionic strength, less than 30 min reflux time, neutral pH value and 6/1 as molar ratio of guanine to CdTe.