Structural and optical properties of germanium nanostructures on Si(100) and embedded in high-k oxides

The structural and optical properties of Ge quantum dots (QDs) grown on Si(001) for mid-infrared photodetector and Ge nanocrystals embedded in oxide matrices for floating gate memory devices are presented. The infrared photoluminescence (PL) signal from Ge islands has been studied at a low temperature. The temperature- and bias-dependent photocurrent spectra of a capped Si/SiGe/Si(001) QDs infrared photodetector device are presented. The properties of Ge nanocrystals of different size and density embedded in high-k matrices grown using radio frequency magnetron sputtering have been studied. Transmission electron micrographs have revealed the formation of isolated spherical Ge nanocrystals in high-k oxide matrix of sizes ranging from 4 to 18 nm. Embedded nanocrystals in high band gap oxides have been found to act as discrete trapping sites for exchanging charge carriers with the conduction channel by direct tunneling that is desired for applications in floating gate memory devices.     

Ultrafine Cu2ZnSnS4 quantum dots functionalized TiO2 nanotube arrays for potential optoelectronic applications

Tremendous progress has been made in power conversion efficiency (PCE) of thin-film photovoltaics over the past few years, yet most current high-efficient photoactive layer usually contains rare or toxic elements accompanied by expensive and complicated vacuum processes, which increases the cost and limits the scope of the applications in the long run. Here we present a synergistic effect of quantum effect of an earth-abundant and low toxic ultrafine Cu₂ZnSnS₄ (CZTS) quantum dots (QDs) and low charge recombination in one dimensional TiO₂ nanotube arrays for optoelectronic devices. By ligands exchange, the as-obtained ultrafine CZTS QDs have been robustly anchored to a highly ordered TiO₂ nanotube arrays (TNAs) to be served as a function layer in a simple QDs sensitized solar cells. Such ultrafine CZTS QDs based solar cells exhibit significant enhancement up to 457% in PCE compared to that of CZTS QDs with larger size. The CZTS QDs functionalized TNAs has also shown excellent charge transport capability with lower recombination rate than QDs sensitized TiO₂ nanoparticles and it is expected to be used as a low-cost environment-friendly function layer for various potential optoelectronic applications.     

Enhanced photoluminescence of multilayer Ge quantum dots on Si(001) substrates by increased overgrowth temperature

Four-bilayer Ge quantum dots (QDs) with Si spacers were grown on Si(001) substrates by ultrahigh vacuum chemical vapor deposition. In three samples, all Ge QDs were grown at 520 °C, while Si spacers were grown at various temperatures (520 °C, 550 °C, and 580 °C). Enhancement and redshift of room temperature photoluminescence (PL) were observed from the samples in which Si spacers were grown at a higher temperature. The enhancement of PL is explained by higher effective electrons capturing in the larger size Ge QDs. Quantum confinement of the Ge QDs is responsible for the redshift of PL spectra. The Ge QDs’ size and content were investigated by atomic force microscopy and Raman scattering measurements.     

Optical excitations in stoichiometric uncapped ZnS nanostructures

We calculate the optical absorption spectra of low-energy uncapped zinc sulfide nanostructures found by global optimisation (basin-hopping/simulated annealing) using time-dependent density functional theory (TD-DFT) and compare the results with experimental spectra. We predict that for all nanostructures studied the lowest excited state found by TD-DFT corresponds to an exciton with an exciton binding energy that is much larger than that of excitons in bulk zinc sulfide. We further show that for the more symmetrical nanostructures some of the excitons are dark and that the absorption on-sets, the energy of the lowest exciton, for the different nanostructures show no clear evidence of quantum confinement. We propose that this apparent lack of quantum confinement finds its origin in the fact that the lowest exciton is not evenly spread over the whole nanostructure but shows large contributions for specific groups of atoms. Finally, we show that the predicted optical absorption spectra fit with those reported experimentally.     

Miniband-related 1.4–1.8 μm luminescence of Ge/Si quantum dot superlattices

The luminescence properties of highly strained, Sb-doped Ge/Si multi-layer heterostructures with incorporated Ge quantum dots (QDs) are studied. Calculations of the electronic band structure and luminescence measurements prove the existence of an electron miniband within the columns of the QDs. Miniband formation results in a conversion of the indirect to a quasi-direct excitons takes place. The optical transitions between electron states within the miniband and hole states within QDs are responsible for an intense luminescence in the 1.4–1.8 μm range, which is maintained up to room temperature. At 300 K, a light emitting diode based on such Ge/Si QD superlattices demonstrates an external quantum efficiency of 0.04% at a wavelength of 1.55 μm.     

Photoluminescence enhancement of quantum dots on Ag nanoneedles

ABSTRACT: Noble-metal nanostructure allows us to tune optical and electrical properties, which has high utility for real-world application. We studied surface plasmon induced emission of semiconductor quantum dots (QDs) on engineered metallic nanostructures. Highly passive organic ZnS capped CdSe QDs were spin coated on poly-(methyl methacrylate) (PMMA) covered Ag films which brought QDs near to metallic surface. We obtained the enhanced electromagnetic field and reduced fluorescence lifetimes from CdSe/ZnS quantum dots (QDs) due to the strong coupling of emitters wave function with the Ag plasmon resonance. Observed changes include a six-fold increase in the fluorescence intensity and striking reduction in fluorescence lifetimes of CdSe/ZnS QDs on rough Ag nanoneedle compared to the case of smooth surfaces. The advantages of using those nanocomposites are expected for high efficiency light-emitting diodes, platform fabrication of biological and environmental monitoring, and high contrast imaging.     

Water induced protonation of amine-terminated micelles for direct syntheses of ZnO quantum dots and their cytotoxicity towards cancer

This work designs a new strategy for the direct synthesis of different zinc oxide (ZnO) nanostructures at low temperatures. Micelles of dodecylamine (DDA) assembled in an ethanol-water system have been explored as a template to direct the growth of the ZnO nanostructures. The key species for the formation of the ZnO nanostructures, OH(-), can be provided by the water-induced protonation of DDA. The pH of the reaction micro-environment can be regulated by changing the input amount of water and DDA. By controlling the reaction temperature and pH, various ZnO nanostructures, i.e. quantum dots with green or yellow-green emissions, have been prepared. The relationship of the optical properties and the synthetic conditions has been further discussed. This strategy realizes the convenient preparation of ZnO QDs, indicating the potential prospects in the nanotechnology field for their low-cost synthesis. Meanwhile, the cellular toxicity study of ZnO nanoparticles toward cancer cells, including leukemia K562 and K562/A02 cells as well as HepG2 cells, indicates a selective cytotoxic effect of ZnO QDs against a broad range of human cancer cell lines.     

Lead Chalcogenide Quantum Dot-Doped Glasses for Photonic Devices

Tunable absorption and photoluminescence (PL) of lead chalcogenide quantum dots (QDs) doped in glasses due to the quantum confinements effect have been actively investigated for application as saturable absorbers, laser sources, and fiber-optic amplifiers. Optical properties of QDs have been carefully monitored by controlling their sizes through heat treatment and rare-earth ion doping. Two- and three-dimensional precipitation of lead chalcogenide QDs were also realized using silver ion exchange and femtosecond laser irradiation in combination with thermal treatment. Prototypes of microstructured single-mode fibers and tapered fiber amplifiers containing QDs proved potentials of these materials for fiber-optic amplifiers application. Further research works on QD-doped solid core fibers, surface passivation of quantum dots and their application for the mid-infrared optical devices are necessary.     

Various Quantum- and Nano-Structures by III–V Droplet Epitaxy on GaAs Substrates

We report on various self-assembled In(Ga)As nanostructures by droplet epitaxy on GaAs substrates using molecular beam epitaxy. Depending on the growth condition and index of surfaces, various nanostructures can be fabricated: quantum dots (QDs), ring-like and holed-triangular nanostructures. At near room temperatures, by limiting surface diffusion of adatoms, the size of In droplets suitable for quantum confinement can be fabricated and thus InAs QDs are demonstrated on GaAs (100) surface. On the other hand, at relatively higher substrate temperatures, by enhancing the surface migrations of In adatoms, super lower density of InGaAs ring-shaped nanostructures can be fabricated on GaAs (100). Under an identical growth condition, holed-triangular InGaAs nanostructures can be fabricated on GaAs type-A surfaces, while ring-shaped nanostructures are formed on GaAs (100). The formation mechanism of various nanostructures can be understood in terms of intermixing, surface diffusion, and surface reconstruction.     

Quantum dots: synthesis, bioapplications, and toxicity

ABSTRACT: This review introduces quantum dots (QDs) and explores their properties, synthesis, applications, delivery systems in biology, and their toxicity. QDs are one of the first nanotechnologies to be integrated with the biological sciences and are widely anticipated to eventually find application in a number of commercial consumer and clinical products. They exhibit unique luminescence characteristics and electronic properties such as wide and continuous absorption spectra, narrow emission spectra, and high light stability. The application of QDs, as a new technology for biosystems, has been typically studied on mammalian cells. Due to the small structures of QDs, some physical properties such as optical and electron transport characteristics are quite different from those of the bulk materials.     

A study of photoluminescence properties and performance improvement of Cd-doped ZnO quantum dots prepared by the sol-gel method

ABSTRACT: In the present work, ZnO quantum dots (QDs) have been prepared by the sol-gel method, and the performance of the QDs have been improved. The effect of Cd concentration on the structural and luminescent properties of the QDs, as well as the effect of the mass ratio of trioctylphosphine oxide (TOPO)/octadecylamine (ODA), has been investigated. The ZnO and Cd-doped ZnO QDs have hexagonal wurtzite structures and are 3~6 nm in diameter. When the Cd content was increased, the QD particle size was reduced; this effect was confirmed in the corresponding ultraviolet-visible (UV) spectra. The fluorescence intensity was simultaneously enhanced significantly. Both the UV and fluorescence spectra were blue-shifted. The luminous intensity was further enhanced when the QDs were modified with TOPO/ODA. FTIR and XRD techniques proved that the polymer successfully coated the surfaces of the QDs. A TOPO/ODA mass ratio of 1:2 was determined to result in the best optical performance among the different ratios examined. The results showed that the described synthetic method is appropriate for the preparation of doped QDs with a high fluorescence quantum efficiency.     

谷氨酰胺为稳定剂制备硒化镉纳米晶及光谱性质研究

以谷氨酰胺(Gln)为稳定剂合成了硒化镉纳米晶,利用X-射线粉末衍射(XRD)和透射电镜(TEM)对纳米晶结构进行了表征,粒径约为20 nm。通过紫外-可见吸收光谱、激发光谱与发射光谱研究了纳米晶光谱特性。实验结果表明,反应温度过高、反应时间过长都会破坏谷氨酰胺(Gln)的稳定作用,使CdSe聚集,影响其荧光性质。而聚乙二醇(PEG)的加入会使纳米晶的荧光发射明显加强,而且发射峰峰形尖锐。     

Molding the flow of light on the nanoscale: from vortex nanogears to phase-operated plasmonic machinery

Efficient delivery of light into nanoscale volumes by converting free photons into localized charge-density oscillations (surface plasmons) enables technological innovation in various fields from biosensing to photovoltaics and quantum computing. Conventional plasmonic nanostructures are designed as nanoscale analogs of radioantennas and waveguides. Here, we discuss an alternative approach for plasmonic nanocircuit engineering that is based on molding the optical powerflow through 'vortex nanogears' around a landscape of local phase singularities 'pinned' to plasmonic nanostructures. We show that coupling of several vortex nanogears into transmission-like structures results in dramatic optical effects, which can be explained by invoking a hydrodynamic analogy of the 'photon fluid'. The new concept of vortex nanogear transmissions (VNTs) provides new design principles for the development of complex multi-functional phase-operated photonics machinery and, therefore, generates unique opportunities for light generation, harvesting and processing on the nanoscale.     

Multi-scale ordering of self-assembled InAs/GaAs(001) quantum dots

Ordering phenomena related to the self-assembly of InAs quantum dots (QD) grown on GaAs(001) substrates are experimentally investigated on different length scales. On the shortest length-scale studied here, we examine the QD morphology and observe two types of QD shapes, i.e., pyramids and domes. Pyramids are elongated along the [1–10] directions and are bounded by {137} facets, while domes have a multi-facetted shape. By changing the growth rates, we are able to control the size and size homogeneity of freestanding QDs. QDs grown by using low growth rate are characterized by larger sizes and a narrower size distribution. The homogeneity of buried QDs is measured by photoluminescence spectroscopy and can be improved by low temperature overgrowth. The overgrowth induces the formation of nanostructures on the surface. The fabrication of self-assembled nanoholes, which are used as a template to induce short-range positioning of QDs, is also investigated. The growth of closely spaced QDs (QD molecules) containing 2–6 QDs per QD molecule is discussed. Finally, the long-range positioning of self-assembled QDs, which can be achieved by the growth on patterned substrates, is demonstrated. Lateral QD replication observed during growth of three-dimensional QD crystals is reported.     

Silicon and Germanium Nanostructures for Photovoltaic Applications: Ab-Initio Results

Actually, most of the electric energy is being produced by fossil fuels and great is the search for viable alternatives. The most appealing and promising technology is photovoltaics. It will become truly mainstream when its cost will be comparable to other energy sources. One way is to significantly enhance device efficiencies, for example by increasing the number of band gaps in multijunction solar cells or by favoring charge separation in the devices. This can be done by using cells based on nanostructured semiconductors. In this paper, we will present ab-initio results of the structural, electronic and optical properties of (1) silicon and germanium nanoparticles embedded in wide band gap materials and (2) mixed silicon-germanium nanowires. We show that theory can help in understanding the microscopic processes important for devices performances. In particular, we calculated for embedded Si and Ge nanoparticles the dependence of the absorption threshold on size and oxidation, the role of crystallinity and, in some cases, the recombination rates, and we demonstrated that in the case of mixed nanowires, those with a clear interface between Si and Ge show not only a reduced quantum confinement effect but display also a natural geometrical separation between electron and hole.     

Linear and nonlinear optical characteristics of CsPbBr3 perovskite quantum dots-doped borosilicate glasses

CsPbBr₃ perovskite QDs are precipitated in a borosilicate glass matrix, while protects efficiently the QD from photo-induced and chemical degradation. We show that the CsPbBr₃ QD doped glasses exhibit strong visible photoluminescence (PL), which is dependence on the concentration that can be controlled by heat treatment conditions. Due to the stabilization by the glass matrix, we are able to determine the nonlinear optical (NLO) properties with a Z-scan technique. We observe a cross-over from saturated absorption (SA) to reverse saturated absorption (RSA) by either increase the pumping intensity or the QD size, reminiscent of quantum size effect in the NLO response. The RSA is associated with two-photon absorption (TPA) that induces strong upconversion luminescence of QD doped glass samples. Our results imply that the glasses containing CsPbBr₃ QDs may find potential applications from solid state lighting to ultrafast optical switches.     

CdTe量子点的水相制备

在水相中以巯基丙酸作为稳定剂,合成出具有不同荧光发射波长的CdTe量子点（QDs）,利用紫外吸收光谱（UV）、荧光光谱（FS）以及透射电子显微镜（TEM）对CdTeQDs进行了表征。研究了反应温度及pH值对所制备的CdTeQDs光学性质的影响。实验结果表明,合成CdTeQDs的最佳温度为96℃,pH值为10,且随着时间的增加量子点的粒径增大。     

Substrate Temperature Dependent Surface Morphology and Photoluminescence of Germanium Quantum Dots Grown by Radio Frequency Magnetron Sputtering

The visible luminescence from Ge nanoparticles and nanocrystallites has generated interest due to the feasibility of tuning band gap by controlling the sizes. Germanium (Ge) quantum dots (QDs) with average diameter ~16 to 8 nm are synthesized by radio frequency magnetron sputtering under different growth conditions. These QDs with narrow size distribution and high density, characterized using atomic force microscopy (AFM) and field emission scanning electron microscopy (FESEM) are obtained under the optimal growth conditions of 400 °C substrate temperature, 100 W radio frequency powers and 10 Sccm Argon flow. The possibility of surface passivation and configuration of these dots are confirmed by elemental energy dispersive X-ray (EDX) analysis. The room temperature strong visible photoluminescence (PL) from such QDs suggests their potential application in optoelectronics. The sample grown at 400 °C in particular, shows three PL peaks at around ~2.95 eV, 3.34 eV and 4.36 eV attributed to the interaction between Ge, GeO_x manifesting the possibility of the formation of core-shell structures. A red shift of ~0.11 eV in the PL peak is observed with decreasing substrate temperature. We assert that our easy and economic method is suitable for the large-scale production of Ge QDs useful in optoelectronic devices.     

Temperature dependent synthesis and optical properties of CdSe quantum dots

The CdSe quantum dots (QDs) were synthesized at various temperatures in aqueous solution. The as-synthesized QDs were characterized by X-ray diffraction (XRD) method and transmission electron microscopy (TEM), and their optical properties were assessed via ultraviolet–visible (UV–vis) absorption spectrum and fluorescence spectrum. The results showed that the reaction temperature could significantly influence the band gap, particle size, and spectral behaviors of the QDs. With the increase of the temperature from room temperature to 90 °C, the band gap of the QDs linearly decreased, corresponding to an essential increase of particle size as well as variable spectral behaviors. In particular, the starting temperature had an important effect on the QDs synthesis and their optical properties. From a viewpoint of wide controls of fluorescence color and intensity, a reaction temperature range of 17–90 °C was appropriate for the synthesis of the CdSe QDs.     

Quantum Dots in Glasses: Size-Dependent Stokes Shift by Lead Chalcogenide

Size-dependent Stokes shift of PbS quantum dots (QDs) formed in the glasses was investigated. PbS QDs with diameters of 3.5 nm to 13.3 nm were precipitated in silicate glasses with different S/Pb ratios using the conventional thermal treatment method. Absorption and photoluminescence (PL) of PbS QDs were tuned from ~0.9 μm (1.38 eV) to ~2.3 μm (0.54 eV) by adjusting the diameters of PbS QDs from 3.5 nm to 13.3 nm. PL energies of QDs exhibited linear dependence on the absorption energies with a slope of 0.484 for PbS QDs with band gap energies larger than 0.98 eV, and the maximum Stokes shift was found to be 206.2 meV for 3.5 nm-sized PbS QDs. For large PbS QDs with band gap energies smaller than 0.98 eV, Stokes shift was found to be ~20 meV or smaller. The size-dependent Stokes shift indicated that surface defects made the main contribution and relative energy positions of these surface defects were strongly dependent on the size of PbS QDs.