Carrier-diffusion-limited remote optical addressing of single quantum dots

We present a scheme for remotely addressing single quantum dots (QDs) by means of near-field optical microscopy that simply makes use of the polarization of light. A structure containing self-assembled CdTe QDs is covered with a thin metal film presenting sub-wavelength holes. When the optical tip is positioned some distance away from a hole, surface plasmons in the metal coating are generated which, by turning the polarization plane of the excitation light, transfer the excitation towards a chosen hole and induce emission from the underlying dots. In addition, our procedure gives valuable insight into the diffusion of photo-excited carriers in the QD plane that can put limits to the addressing scheme.     

Quantum confinement in amorphous silicon quantum dots embedded in silicon nitride

Amorphous silicon quantum dots (a-Si QDs) were grown in a silicon nitride film by plasma enhanced chemical vapor deposition. Transmission electron micrographs clearly demonstrated that a-Si QDs were formed in the silicon nitride. Photoluminescence and optical absorption energy measurement of a-Si QDs with various sizes revealed that tuning of the photoluminescence emission from 2.0 to 2.76 eV is possible by controlling the size of the a-Si QD. Analysis also showed that the photoluminescence peak energy E was related to the size of the a-Si QD, a (nm) by E(eV) = 1.56+2.40/a(2), which is a clear evidence for the quantum confinement effect in a-Si QDs.     

Efficient two-photon absorption of CdSe-CdS/ZnS core-multishell quantum dots under the excitation of near-infrared femtosecond pulsed laser

We report that two-photon absorption (TPA) properties of semiconductor CdSe-core CdS/ZnS-multishell quantum dots (QDs) in toluene under excitation of femtosecond laser at 800 nm. The results show efficient TPA process and large TPA cross section of three types of size QDs, which is 1900, 5710, and 16060 GM (1 GM = 10⁻⁵⁰ cm⁴ s photon⁻¹), respectively. TPA cross section dramatically increases with increased core size, showing a strong size-dependence effect. Furthermore, two-photon excitation (TPE) fluorescence intensity not only depends on TPA capacity, but also relies on improved quantum yield resulting from passivation of QD surface by different coated monolayers (MLs). These facts in combination with the narrow fluorescence bandwidth make these QDs as promising probes for multicolor two-photon microscopy.     

Surface plasmon coupled fluorescence in deep-ultraviolet excitation by Kretschmann configuration

We report the experimental demonstration of fluorescence of CdSe quantum dots with surface plasmon excitation in deep-ultraviolet （deep-UV） region. Surface plasmon resonance in deep-UV is excited by aluminum thin film in the Kretschmann-Raether geometry. Considering the oxidation thickness of aluminum, the experimental results of incident angle dependence of reflectance show good agreement with Fresnel theory. Surface plasmon resonance with 19 nm-thick aluminum and 5 nm-thick almnina was excited at the incident angle of 48 degrees for 266 nm excitation. Fluorescence of CdSe quantum dots coated on this aluminum film was observed by the surface plasmon excitation.     

Photostability comparison of CdTe and CdSe/CdS/ZnS quantum dots in living cells under single and two-photon excitations

The photostability is an outstanding feature of quantum dots (QDs) used as fluorescence probes in biological staining and cell imaging. To find out the related factors in the QD photostability, the photobleaching of naked CdTe QDs and BSA coated CdSe/CdS/ZnS QDs in human hepatocellular carcinoma (QGY) cells and human nasopharynx carcinoma (KB) cells were studied under single photon excitation (SPE) and two-photon excitation (TPE). In these two cell lines the cellular QDs were irradiated by a 405 nm continuous wave laser for SPE or an 800 nm femto-second (fs) laser for TPE. The QD photobleaching with the irradiation time was found to fit a biexponential decay. The fast decay plays a dominant role in the bleaching course and thus can be used as the parameter to quantitatively evaluate the QD photostability. The TPE decreased the QD photobleaching as compared to SPE. The BSA coated core/shell QDs had improved the photostability up to 4-5 times than the naked QDs due to the shielding effect of the QD shell. Therefore, it is better to use core/shell structured QDs as the fluorescence probe combining with a TPE manner for those long-term monitoring studies.     

Photoluminescence from single silicon quantum dots excited via surface plasmon polaritons

Single dot spectroscopy of Si quantum dots (QDs) was performed by using surface plasmon polariton (SPP)-mediated excitation in the attenuated total reflection geometry with a MgF₂/Ag film on the base of a prism. Thanks to the 16 times enhancement of the incident electric field and very small background signal, PL from single Si QDs was observed clearly. This proves the usefulness of the technique for the detection of inherently weak emission of Si QDs.     

The influence of the quantum dot/polymethylmethacrylate composite preparation method on the stability of its optical properties under laser radiation

Photoluminescent semiconductor nanocrystals, quantum dots (QDs), are nowadays one of the most promising materials for developing a new generation of fluorescent labels, new types of light-emitting devices and displays, flexible electronic components, and solar panels. In many areas the use of QDs is associated with an intense optical excitation, which, in the case of a prolonged exposure, often leads to changes in their optical characteristics. In the present work we examined how the method of preparation of quantum dot/polymethylmethacrylate (QD/PMMA) composite influenced the stability of the optical properties of QD inside the polymer matrix under irradiation by different laser harmonics in the UV (355 nm) and visible (532 nm) spectral regions. The composites were synthesized by spin-coating and radical polymerization methods. Experiments with the samples obtained by spin-coating showed that the properties of the QD/PMMA films remain almost constant at values of the radiation dose below ~10 fJ per particle. Irradiating the composites prepared by the radical polymerization method, we observed a monotonic increase in the luminescence quantum yield (QY) accompanied by an increase in the luminescence decay time regardless of the wavelength of the incident radiation. We assume that the observed difference in the optical properties of the samples under exposure to laser radiation is associated with the processes occurring during radical polymerization, in particular, with charge transfer from the radical particles inside QDs. The results of this study are important for understanding photophysical properties of composites on the basis of QDs, as well as for selection of the type of polymer and the composite synthesis method with quantum dots that would allow one to avoid the degradation of their luminescence.     

Coupling of spontaneous emission from GaN-AlN quantum dots into silver surface plasmons

We have demonstrated the decay of spontaneous emission (SE) from AlN-GaN quantum dots (QDs) into silver surface plasmon (SP) modes in the ultraviolet at approximately 375-380 nm. Using time-resolved photoluminescence (PL), we show that the electron-hole recombination rate in AlN-GaN QDs is enhanced when SE is resonantly coupled to a metal SP mode, corresponding to the dip in the continuous-wave PL spectrum. Exciton recombination by means of silver SP modes is as much as 3-7 times faster than in normal QD SE and depends strongly on emission wavelength and thickness of the silver.     

Near‐field optical enhancement by lead‐sulfide quantum dots and metallic nanoparticles for SERS

There is a growing interest in using quantum dots (QDs) and metallic nanoparticles (NPs), both for luminescence enhancement and surface‐enhanced Raman scattering (SERS). Here, we study the electromagnetic‐field enhancement that can be generated by lead‐sulfide (PbS) QDs using three‐dimensional finite‐element simulations. We investigate the field enhancement associated with combinations of PbS QDs with metallic NPs and substrates. The results show that high field enhancement can be achieved by combining PbS QDs with metallic NPs of larger sizes. The ideal size for Ag NPs is 25 nm, providing a SERS enhancement factor of ~5*10⁸ for light polarization parallel to the NP dimer axis and a gap of 0.6 nm. For Au NPs, the bigger the size, the higher is the field for the studied diameters, up to 50 nm. The near‐field values for PbS QDs above metallic substrates were found to be lower compared to the case of PbS QD‐metal NP dimers. This study provides the understanding for the design and application of QDs for the enhancement of near‐field phenomena. Copyright © 2013 John Wiley & Sons, Ltd.     

Enhanced photoluminescence of CdSe quantum dots by the coupling of Ag nanocube and Ag film

The coupling of local surface plasmon(LSP) of nanoparticle and surface plasmon(SP) mode produced by metal film can lead to the enhanced electromagnetic field, which has an important application in enhancing the fluorescence of quantum dots(QDs). Herein, the Ag nanocube and Ag film are used to enhance the fluorescence of CdSe QDs. The enhancement is found to relate to the sizes of the Ag nanocube and the thickness of the Ag film. Moreover, we also present the fluorescence enhancement caused by only SP. The result shows that the coupling between metal nanoparticles and metal film can realize larger field enhancement. Numerical simulation verifies that a nanocube can localize a strong electric field around its corner. All the results indicate that the fluorescence of QDs can be efficiently improved by optimizing the parameters of Ag film and Ag cubes.     

Two-photon absorption from single InGaN/GaN quantum dots

We present a study of the time-integrated and time-resolved photoluminescence properties of single-InGaN/GaN quantum dots (QDs) using two-photon spectroscopy. Two samples containing QDs produced by different growth techniques are examined. We find that two-photon excitation results in the suppression of the emission from the underlying quantum well to which the QDs are coupled and yet relatively strong QD emission is observed. This effect is explained in terms of the enhancement of two-photon absorption in QDs due to the full confinement of carriers. Furthermore, evidence of the presence of excited states is revealed from the two-photon photoluminescence excitation spectra presented in the study.     

Si quantum dot structures and their applications

This paper presents briefly the history of emission study in Si quantum dots (QDs) in the last two decades. Stable light emission of Si QDs and NCs was observed in the spectral ranges: blue, green, orange, red and infrared. These PL bands were attributed to the exciton recombination in Si QDs, to the carrier recombination through defects inside of Si NCs or via oxide related defects at the Si/SiOx interface. The analysis of recombination transitions and the different ways of the emission stimulation in Si QD structures, related to the element variation for the passivation of surface dangling bonds, as well as the plasmon induced emission and rare earth impurity activation, have been presented.The different applications of Si QD structures in quantum electronics, such as: Si QD light emitting diodes, Si QD single union and tandem solar cells, Si QD memory structures, Si QD based one electron devices and double QD structures for spintronics, have been discussed as well. Note the significant worldwide interest directed toward the silicon-based light emission for integrated optoelectronics is related to the complementary metal-oxide semiconductor compatibility and the possibility to be monolithically integrated with very large scale integrated (VLSI) circuits. The different features of poly-, micro- and nanocrystalline silicon for solar cells, that is a mixture of both amorphous and crystalline phases, such as the silicon NCs or QDs embedded in a α-Si:H matrix, as well as the thin film 2-cell or 3-cell tandem solar cells based on Si QD structures have been discussed as well. Silicon NC based structures for non-volatile memory purposes, the recent studies of Si QD base single electron devices and the single electron occupation of QDs as an important component to the measurement and manipulation of spins in quantum information processing have been analyzed as well.     

2018年2期电子期刊

光诱导功能退化是胶体量子点在应用中面临的主要挑战之一,本文针对这一问题研究了使用磁控溅射沉积SiO₂薄膜形成钝化层来提高CdSe/ZnS量子点发光稳定性的方法。首先,通过三正辛基膦辅助连续离子层吸附反应方法合成了615 nm发光的红色CdSe/ZnS量子点。然后将量子点旋涂在SiO₂/Si基片上,再通过磁控溅射方法在量子点上沉积了厚度为20 nm的SiO₂薄膜作为钝化层。使用连续波激光光源分别在空气气氛和真空条件下照射样品,研究了经过不同照射时间后钝化和未钝化量子点的稳态光致发光光谱。结果表明,随着照射时间的延长,没有SiO₂钝化的量子点的PL强度显著降低、PL峰值发生蓝移、FWHM不断增大。对比研究发现,由于SiO₂薄膜能够阻挡空气中的水和氧,减缓了量子点表面的光诱导氧化现象,因此显著提高了CdSe/ZnS量子点的稳定性。     

Time-resolved photoluminescence spectroscopy of InAs quantum dots on InP with various InAlGaAs barrier thicknesses

The Optical characteristics of InAs quantum dots (QDs) embeded in InAlGaAs on InP have been investigated by photoluminescence (PL) spectroscopy and time-resolved PL. Four different QD samples are grown by using molecular beam epitaxy, and all the QD samples have five-stacked InAs quantum dot layers with a different InAlGaAs barrier thickness. The PL yield from InAs QDs was increased with an increase in the thickness of the InAlGaAs barrier, and the emission peak positions of all InAs QD samples were measured around 1.5 μm at room temperature. The decay time of the carrier in InAs QDs is decreased abruptly in the QD sample with the 5 nm InAlGaAs barrier. This feature is explained by the tunneling and coupling effect in the vertical direction and probably defect generation.     

Magneto-optical study of nonmagnetic quantum dots coupled to a magnetic semiconductor quantum well

We have investigated a series of double-layer structures consisting of a layer of self-assembled non-magnetic CdSe quantum dots (QDs) separated by a thin ZnSe barrier from a ZnCdMnSe diluted magnetic semiconductor (DMSs) quantum well (QW). In the series, the thickness of the ZnSe barrier ranged between 12 and 40 nm. We observe two clearly defined photoluminescence (PL) peaks in all samples, corresponding to the CdSe QDs and the ZnCdMnSe QW, respectively. The PL intensity of the QW peak is observed to decrease systematically relative to the QD peak as the thickness of the ZnSe barrier decreases, indicating a corresponding increase in carrier tunneling from the QW to the QDs. Furthermore, polarization-selective PL measurements reveal that the degree of polarization of the PL emitted by the CdSe QDs increases with decreasing thickness of the ZnSe barriers. The observed behavior is discussed in terms of anti-parallel spin interaction between carriers localized in the non-magnetic QDs and in the magnetic QWs.     

金属-光折变材料复合全息结构对表面等离激元的波前调控

表面等离激元(surface plasmon polaritons, SPPs)控制具有重要意义.表面电磁波全息法是在金属表面设计能有效控制SPP传输的凹槽阵列结构.本文提出一种新的SPP传输的控制方法,利用金属-光折变材料复合全息结构控制SPP传播.在金属表面覆盖一层光折变材料,两束SPP波在光折变材料内干涉生成全息结构,利用此全息结构能够控制SPP的传播.通过时域有限差分法模拟验证,结果显示,通过金属-光折变材料复合全息结构可以有效地控制SPP波束的传输,实现SPP平面波束的单点聚焦、两点聚焦,以及生成零阶和一阶高斯SPP波束.经过优化发现,光折变材料的最佳厚度为3.3μm,最佳折射率调制度为0.06.现有SPP控制器件主要是通过离子束刻蚀,而金属-光折变材料复合全息结构不需要刻蚀,从而扩展了SPP控制的器件的制作方法,为SPPs的全光控制提供了新的思路,使SPP全光控制成为可能,进一步实现了SPP全光开关等功能.     

Mechanism of fluorescence energy transfer in aqueous solution cadmium sulfide quantum dots

Cadmium sulfide (CdS) quantum dots (QDs) prepared by a convenient chemical method have been characterized using absorption, fluorescence, and photoluminescence excitation techniques. The photoluminescence excitation studies show that there is an electron transfer from the surface adsorbate (thiourea) to CdS QDs in aqueous solution. The excitation band with peak maximum at 5.8 eV is assigned to the electronic transitions in the chemisorbed thiourea, whereas the excitation band between 3.45 and 3.7 eV corresponds to the band-to-band transition within the nanocrystalline CdS host. The absorption spectroscopy of the CdS QD solutions shows a strong absorption peak which is generated from thiourea. The band-edge fluorescence of the CdS QDs has also been investigated. It is shown that the fluorescence property of the CdS QDs can be enhanced by adding cadmium chloride (CdCl₂) solution.     

等离子体增强InAs单量子点荧光辐射的研究

通过测量光致发光(PL)谱、PL时间分辨光谱及不同激发功率下PL发光强度,研究了低温(5 K)下等离子体对InAs单量子点PL光谱的增强效应.采用电子束蒸发镀膜技术在InAs量子点样品表面淀积了5 nm厚度的金膜,形成纳米金岛膜结构.实验发现,金岛膜有利于量子点样品发光强度的增加,最大PL强度增加了约5倍,其主要物理机理是金岛膜纳米结构提高了量子点PL光谱的收集效率.     

Thiol-Capped CdTe Quantum Dots with Two-Photon Excitation for Imaging High Autofluorescence Background Living Cells

To effectively image living cells with quantum dots (QDs), particularly for those cells containing high content of native fluorophores, the two-photon excitation (TPE) with a femto-second 800 nm laser was employed and compared with the single-photon excitations (SPE) of 405 nm and 488 nm in BY-2 Tobacco (BY-2-T) and human hepatocellular carcinoma (QGY) cells, respectively. The 405 nm SPE produced the bright photoluminescence (PL) signals of cellular QDs but also induced a strong autofluorescence(AF) from the native fluorophores like flavins in cells. The AF occupied about 30% and 13% of the total signals detected in QD imaging channel in the BY-2-T and QGY cells, respectively. With the excitation of 488 nm SPE, the PL signals were lower than those excited with the 405 nm SPE, although the AF signals were also reduced. The 800 nm TPE generated the best PL images of intracellular QDs with the highest signal ratio of PL to AF, because the two-photon absorption cross section of QDs is much higher than that of the native fluorophores. By means of the TPE, the reliable cellular imaging with QDs, even for the cells having the high AF background, can be achieved.     

基于量子点-CBP混合层的量子点LED的制备

采用一锅法制备出高质量的具有核壳结构的Cd Se@Zn S、Cd Zn S/Zn S量子点。将量子点混入空穴传输材料CBP中形成复合的有源材料,经过几步简单的旋涂操作,制备出相应的绿光、蓝光量子点LED器件。这种方法利用了油溶性量子点和CBP材料的相容性,减少了旋涂操作的步骤,有利于快速制备基于量子点的电致发光器件。基于两步旋涂操作制备的量子点LED,由于阴极与复合有源层之间的能级差较大,导致需要较高的开启电压。在CBP材料中,注入的载流子有可能会被量子点表面缺陷捕获,形成表面态的发光。表面态发光的相对强度依赖于载流子浓度。