Mid-Infrared Emission From InAs Quantum Dots Grown by Metal–Organic Vapor Phase Epitaxy

We have demonstrated mid-infrared emission from the self-assembled InAs quantum dots grown on InP substrate by metal-organic vapor phase epitaxy using low toxic tertiarybutylarsine and tertiarybutylphosphine as group V sources in pure nitrogen ambient. Emission wavelength of the InAs quantum dots has been extended to mid-infrared region by embedding the InAs quantum dots in graded In_xGa_1-xAs matrix layers. When compared with that of the InAs quantum dots grown on lattice matched In_0.53Ga_0.47As/InP matrix, emission wavelength of the InAs quantum dots red shifted by up to 370 nm when embedded the InAs quantum dots in graded In_0.53rarr0.8Ga_0.47rarr0.2As barriers. The longest emission wavelength of >2.35 mum from the self-assembled InAs quantum dot structure has been measured at 77 K. The full-width at half-maximum of the photoluminescence emission spectrum of the InAs quantum dots is as narrow as 25.5 meV. The results achieved would be promising to high performance mid-infrared quantum dot lasers on InP substrate     

Effects of Magnetic Quantum Dots on Magnetoconductance in Quantum Wires

We present a theoretical study of electronic transport in quantum wires (narrow two-dimensional electron gas) with array of magnetic quantum dots. Each magnetic quantum dot is defined by a small circular region where the strength of perpendicular magnetic field is modulated. By making use of a newly developed calculation method based on the gauge transformations, we calculated the conductance as a function of the external perpendicular magnetic field. Our numerical calculations show that the magnetoconductance is very sensitive to the number of magnetic quantum dots in the field region where the direction of the net magnetic field in dot regions is antiparallel to the external magnetic field.     

The influence of substrate temperature on InAsN quantum dots grown by molecular beam epitaxy

The effect of substrate temperature, 390-480?°C, during molecular beam epitaxy growth of InAsN quantum dots has been studied. The quantum dot formation was studied in situ, and it is shown that the quantum dots are close to fully relaxed within 4 monolayers (ML) of InAsN deposition. Further, the indium concentration was estimated to be 84%, 67%, 55% and 31% for 4?ML thick quantum dots grown at 390, 420, 450 and 480?°C, respectively. Thus, Ga incorporation was demonstrated at all substrate temperatures. The dot diameter and height increased from 23 to 38?nm, and 2.5 to 8.9?nm, respectively, when the growth temperature was increased from 390 to 480?°C. The 5?K photoluminescence intensity and wavelength both increased with substrate temperature.     

Luminescent quantum dots fluorescence resonance energy transfer-based probes for enzymatic activity and enzyme inhibitors

The paper describes the development and characterization of analytical properties of quantum dot-based probes for enzymatic activity and for screening enzyme inhibitors. The luminescent probes are based on fluorescence resonance energy transfer (FRET) between luminescent quantum dots that serve as donors and rhodamine acceptors that are immobilized to the surface of the quantum dots through peptide linkers. Peptide-coated CdSe/ZnS quantum dots were prepared using a one-step ligand exchange process in which RGDC peptide molecules replace trioctylphosphine oxide (TOPO) molecules as the capping ligands of the quantum dots. The peptide molecules were bound to the surface of the CdSe/ZnS quantum dots through the thiol group of the peptide cysteine residue. The peptide-coated quantum dots were labeled with rhodamine to form the FRET probes. The emission quantum yield of the quantum dot FRET probes was 4-fold lower than the emission quantum yield of TOPO-capped quantum dots. However, the quantum dot FRET probes were sufficiently bright to enable quantitative enzyme and enzyme inhibition assays. The probes were used first to test the enzymatic activity of trypsin in solution based on FRET signal changes of the quantum dot-based enzymatic probes in the presence of proteolytic enzymes. For example, exposure of the quantum dot FRET probes to 500 microg/mL trypsin for 15 min resulted in 60% increase in the photoluminescence of the quantum dots and a corresponding decrease in the emission of the rhodamine molecules. These changes resulted from the release of rhodamine molecules from the surface of the quantum dots due to enzymatic cleavage of the peptide molecules. The quantum dot FRET-based probes were used to monitor the enzymatic activity of trypsin and to screen trypsin inhibitors for their inhibition efficiency.     

Detection of bioconjugated quantum dots passivated with different ligands for bio-applications

Bioconjugation of quantum dots has resulted in a significant increase in resolution of biological fluorescent labeling. This intrinsic property of quantum dots can be utilized for sensitive detection of target analytes with high sensitivity; including pathogenic bacteria and cancer monitoring. The quantum dots and quantum dot doped silica nanoparticles exhibit prominent emission peaks when excited at 400 nm but on conjugation to model rabbit antigoat antibodies exhibit diminished intensity of emission peak at 600 nm. It shows that photoluminescence intensity of conjugated quantum dots and quantum dot doped silica nanoparticles could permit the detection of bioconjugation. Samples of conjugated and unconjugated quantum dots and quantum dot doped silica nanoparticles were subjected to enzyme linked immunosorbent assay for further confirmation of bioconjugation. In the present study ligand exchange, bioconjugation, fluorescence detection of bioconjugated quantum dots and quantum dot doped silica nanoparticles and further confirmation of bioconjugation by enzyme linked immunosorbent assay has been described.     

Scanning gate imaging of quantum dots in 1D ultra-thin InAs/InP nanowires

We use a scanning gate microscope (SGM) to characterize one-dimensional ultra-thin (diameter ≈ 30 nm) InAs/InP heterostructure nanowires containing a nominally 300 nm long InAs quantum dot defined by two InP tunnel barriers. Measurements of Coulomb blockade conductance versus backgate voltage with no tip present are difficult to decipher. Using the SGM tip as a charged movable gate, we are able to identify three quantum dots along the nanowire: the grown-in quantum dot and an additional quantum dot near each metal lead. The SGM conductance images are used to disentangle information about individual quantum dots and then to characterize each quantum dot using spatially resolved energy-level spectroscopy.     

Optical properties of HgTe colloidal quantum dots

Room temperature photodetection with HgTe colloidal quantum films is reported between 2 and 5 μm for particles of sizes between ~5 and ~12 nm diameter, and photodetection extends to 7 μm at 80 K. The size-tuning of the absorption of HgTe colloidal quantum dots, their optical cross section and the infrared absorption depth of films are measured. The tuning with radius is empirically given by [see formula in text] where R is in nm. The optical cross section of the colloidal dots at 415 nm is approximately proportional to their volume and given by σ(Hg)(415) = 2.6 ± 0.4 10(-17) cm(2)/mercury atom. The size-dependent optical cross section at the band edge ~1.5 10(-15) cm(2) is consistent with the expected oscillator strength of the quantum dots. The absorption depth of HgTe colloidal dot films is short, about 1-2 μm, which is an advantage for thin film devices. These properties agree rather well with the expectation from the k · p model. HgTe colloidal quantum dot thin films show a strong tuning with temperature with a large positive thermal shift between 0.4 and 0.2 meV K(-1), decreasing with decreasing size within the size range studied and this is attributed primarily to electron-phonon effects.     

Three-dimensional Si/Ge quantum dot crystals

Modern nanotechnology offers routes to create new artificial materials, widening the functionality of devices in physics, chemistry, and biology. Templated self-organization has been recognized as a possible route to achieve exact positioning of quantum dots to create quantum dot arrays, molecules, and crystals. Here we employ extreme ultraviolet interference lithography (EUV-IL) at a wavelength of lambda = 13.5 nm for fast, large-area exposure of templates with perfect periodicity. Si(001) substrates have been patterned with two-dimensional hole arrays using EUV-IL and reactive ion etching. On these substrates, three-dimensionally ordered SiGe quantum dot crystals with the so far smallest quantum dot sizes and periods both in lateral and vertical directions have been grown by molecular beam epitaxy. X-ray diffractometry from a sample volume corresponding to about 3.6 x 10(7) dots and atomic force microscopy (AFM) reveal an up to now unmatched structural perfection of the quantum dot crystal and a narrow quantum dot size distribution. Intense interband photoluminescence has been observed up to room temperature, indicating a low defect density in the three-dimensional (3D) SiGe quantum dot crystals. Using the Ge concentration and dot shapes determined by X-ray and AFM measurements as input parameters for 3D band structure calculations, an excellent quantitative agreement between measured and calculated PL energies is obtained. The calculations show that the band structure of the 3D ordered quantum dot crystal is significantly modified by the artificial periodicity. A calculation of the variation of the eigenenergies based on the statistical variation in the dot dimensions as determined experimentally (+/-10% in linear dimensions) shows that the calculated electronic coupling between neighboring dots is not destroyed due to the quantum dot size variations. Thus, not only from a structural point of view but also with respect to the band structure, the 3D ordered quantum dots can be regarded as artificial crystal.     

Ferromagnetism in One Layer of Self-organized InMnAs Quantum Dots

One layer of self-assembled InMnAs quantum dots with InGaAs barrier was grown on high-resistivity (100) p-type GaAs substrates by molecular beam epitaxy (MBE). A presence of ferromagnetic structure was confirmed in the InMnAs dilute magnetic quantum dots. The one layer of self-assembled InMnAs quantum dots was found to be semiconducting, and have ferromagnetic ordering with a Curie temperature, T _C =80 K. It is likely that the ferromagnetic exchange coupling of sample with T _C =80 K is hole-mediated resulting in Mn substituting Ge. PL emission spectra of InMnAs samples grown at temperature of 210°C and 285°C show that the interband transition peak centered at 1.31 eV comes from the InMnAs quantum dot.     

异质外延自组织量子点弹性应变场分布的研究

通过有限元法,在ANSYS环境下,利用二维模型对自组织应变外延异质结透镜形量子点的应力应变分布情况进行了系统分析。分析过程分别考虑了孤立量子点系统、单层多量子点系统以及量子点超晶格系统3种情况,结果表明单层和超晶格多量子点系统衬底之间存在的长程相互作用力对量子点及其周围的应力应变分布有显著影响。在计算应变对多量子点系统的电子结构的影响时,必须将多量子点系统整体考虑。     

Empirical pseudo-potential studies on electronic structure of semiconducting quantum dots

Theoretical investigations of electronic structure of quantum dots is of current interest in nanophase materials. Empirical theories such as effective mass approximation, tight binding methods and empirical pseudo-potential method are capable of explaining the experimentally observed optical properties. We employ the empirical pseudo-potential to calculate the gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) as a function of shape and size of the quantum dots. Our studies explain the building up of the bulk band structure when the size of the dot is much larger than the bulk Bohr exciton radius. We present our investigations of HOMO-LUMO gap variation with size, for CdSe, ZnSe and GaAs quantum dots. The calculated excitonic energies are sensitive to the shape and size of quantum dots and are in good agreement with experimental HOMO-LUMO gaps for CdSe quantum dots. The agreement improves as experimentally observed lattice contraction is incorporated in pseudo-potential calculations for ZnSe quantum dots. Electronic structure evolution, as the size of quantum dot increases, is presented for CdSe, ZnSe and GaAs quantum dots.     

The influence of post-growth annealing on the optical properties of InAs quantum dot chains grown on pre-patterned GaAs(100)

We report on the effect of post-growth thermal annealing of [011]- ,[011(-)]-, and [010]-oriented quantum dot chains grown by molecular beam epitaxy on GaAs(100) substrates patterned by UV-nanoimprint lithography. We show that the quantum dot chains experience a blueshift of the photoluminescence energy, spectral narrowing, and a reduction of the intersubband energy separation during annealing. The photoluminescence blueshift is more rapid for the quantum dot chains than for self-assembled quantum dots that were used as a reference. Furthermore, we studied polarization resolved photoluminescence and observed that annealing reduces the intrinsic optical anisotropy of the quantum dot chains and the self-assembled quantum dots.     

The effect of nitrogen pressure during molecular beam epitaxy growth of InAsN quantum dots

The influence of N flux during molecular beam epitaxy growth of InAsN quantum dots was studied. Growth of InAsN dots under high N flux was shown to give rise to an abnormal growth behaviour compared to InAs dots and InAsN dots with lower nitrogen content. Cubic In(x)Ga(1-x)N (x = 0.21 ± 0.01) crystallites were found in samples grown with an excessive N?flux. The crystallites are likely to form ～0.6?monolayers (MLs) after the quantum dots have nucleated, when the quantum dot changes growth mode. In addition, it is shown that a bimodal size distribution of InAsN quantum dots was generated in the wetting layer during the dot growth, as opposed to nucleation at N-induced dislocations at the substrate surface. The bimodal distribution may be explained by an increased energy barrier, in the presence of nitrogen, for atomic incorporation into the dots.     

A Ge/Si heterostructure nanowire-based double quantum dot with integrated charge sensor

One proposal for a solid-state-based quantum bit (qubit) is to control coupled electron spins on adjacent semiconductor quantum dots. Most experiments have focused on quantum dots made from III-V semiconductors; however, the coherence of electron spins in these materials is limited by hyperfine interactions with nuclear spins. Ge/Si core/shell nanowires seem ideally suited to overcome this limitation, because the most abundant nuclei in Ge and Si have spin zero and the nanowires can be chemically synthesized defect-free with tunable properties. Here, we present a double quantum dot based on Ge/Si nanowires in which we can completely control the coupling between the dots and to the leads. We also demonstrate that charge on the double dot can be detected by coupling it capacitively to an adjacent nanowire quantum dot. The double quantum dot and integrated charge sensor serve as an essential building block to form a solid-state qubit free of nuclear spin.     

异质外延自组织锥形量子点长程相互作用对弹性应变场分布的影响

利用有限元法,在ANSYS 环境下,利用二维模型对自组织应变外延异质结锥形量子点的应力应变分布情况进行了系统分析.分析过程分别考虑了孤立锥形量子点系统、单层多量子点系统以及量子点超晶格系统三种情况,结果表明,单层和超晶格多量子点系统衬底之间存在的长程相互作用力对量子点及其周围的应力应变分布有显著影响.在计算应变对多量子点系统的电子结构的影响时,必须将多量子点之间的相互作用对应变的贡献考虑进去.     

PbS量子点能级结构的尺寸和配体依赖性及其对异质结电池性能的影响

通过电化学循环伏安测试和吸收光谱测试, 确定了有机配体(油酸)和原子配体(四正丁基碘化铵, TBAI)钝化的不同粒径(2.6~4.5 nm)PbS量子点的导带和价带能级, 并研究了量子点尺寸对PbS/TiO₂异质结电池(空气气氛中制备)性能的影响。结果表明：PbS量子点的能级结构受其粒径大小和表面配体特性的影响。当PbS量子点尺寸从2.6 nm增加至4.5 nm时, 油酸包覆PbS量子点的导带底从-3.67 eV减小到-4.0 eV, 价带顶从-5.19 eV增加到-4.97 eV; 而对于TBAI配体置换的PbS量子点, 其导带底和价带顶则分别从-4.15 eV和-5.61 eV变化至-4.51 eV和-5.46 eV。粒径为3.9 nm的PbS量子点所制备的电池性能最优, 其能量转化效率达到2.32%, 这可归因于其适宜的禁带宽度、结晶质量和良好的PbS/TiO₂界面能级匹配度。     

Exciton storage by Mn(2+) in colloidal Mn(2+)-doped CdSe quantum dots

Colloidal Mn (2+)-doped CdSe quantum dots showing long excitonic photoluminescence decay times of up to tau exc = 15 mus at temperatures over 100 K are described. These decay times exceed those of undoped CdSe quantum dots by approximately 10 (3) and are shown to arise from the creation of excitons by back energy transfer from excited Mn (2+) dopant ions. A kinetic model describing thermal equilibrium between Mn (2+ 4)T 1 and CdSe excitonic excited states reproduces the experimental observations and reveals that, for some quantum dots, excitons can emit with near unity probability despite being approximately 100 meV above the Mn (2+ 4)T 1 state. The effect of Mn (2+) doping on CdSe quantum dot luminescence at high temperatures is thus completely opposite from that at low temperatures described previously.     

Lateral patterning of multilayer InAs/GaAs(001) quantum dot structures by in vacuo focused ion beam

We report on the effects of patterning and layering on multilayer InAs/GaAs(001) quantum dot structures laterally ordered using an in vacuo focused ion beam. The patterned hole size and lateral pattern spacing affected the quantum dot size and the fidelity of the quantum dots with respect to the lateral patterns. 100% pattern fidelity was retained after six layers of dots for a 9.0 ms focused ion beam dwell time and 2.0 μm lateral pattern spacing. Analysis of the change in quantum dot size as a function of pattern spacing provided a means of estimating the maximum average adatom surface diffusion length to be approximately 500 nm, and demonstrated the ability to alter the wetting layer thickness via pattern spacing. Increasing the number of layers from six to 26 resulted in mound formation, which destroyed the pattern fidelity at close pattern spacings and led to a bimodal quantum dot size distribution as measured by atomic force microscopy. The bimodal size distribution also affected the optical properties of the dots, causing a split quantum dot photoluminescence peak where the separation between the split peaks increased with increasing pattern spacing.     

Area preferential nucleation of Ge nano-dots on nano-size porous silicon

The Ge quantum dots on anodized nanometer porous silicon layers are prepared by area preferential nucleation at a low temperature of 720°C. The porous silicon was formed by anodic conversion of p-type (1 0 0)-oriented crystalline silicon in hydrofluoric acid diluted by alcohol. Clear phonon-resolved PL, as a NP transition and its TA phonon replica, was observed from the Ge dots at the temperature of 10 K. We attributed the very large blue-shift in energy of the PL peak to the quantum size effect in Ge dots. The present technique is a potential low-cost method for producing quantum dot arrays.     

Bias-induced photoluminescence quenching of single colloidal quantum dots embedded in organic semiconductors

We demonstrate reversible quenching of the photoluminescence from single CdSe/ZnS colloidal quantum dots embedded in thin films of the molecular organic semiconductor N,N'-diphenyl-N,N'-bis(3-methylphenyl)-(1,1'-biphenyl)-4,4'-diamine (TPD) in a layered device structure. Our analysis, based on current and charge carrier density, points toward field ionization as the dominant photoluminescence quenching mechanism. Blinking traces from individual quantum dots reveal that the photoluminescence amplitude decreases continuously as a function of increasing forward bias even at the single quantum dot level. In addition, we show that quantum dot photoluminescence is quenched by aluminum tris(8-hydroxyquinoline) (Alq3) in chloroform solutions as well as in thin solid films of Alq3 whereas TPD has little effect. This highlights the importance of chemical compatibility between semiconductor nanocrystals and surrounding organic semiconductors. Our study helps elucidate elementary interactions between quantum dots and organic semiconductors, knowledge needed for designing efficient quantum dot organic optoelectronic devices.