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.     

In situ accurate control of 2D-3D transition parameters for growth of low-density InAs/GaAs self-assembled quantum dots

A method to improve the growth repeatability of low-density InAs/GaAs self-assembled quantum dots by molecular beam epitaxy is reported. A sacrificed InAs layer was deposited firstly to determine in situ the accurate parameters of two- to three-dimensional transitions by observation of reflection high-energy electron diffraction patterns, and then the InAs layer annealed immediately before the growth of the low-density InAs quantum dots (QDs). It is confirmed by micro-photoluminescence that control repeatability of low-density QD growth is improved averagely to about 80% which is much higher than that of the QD samples without using a sacrificed InAs layer.     

Growth kinetics of MPS-capped CdS quantum dots in self-assembled thin films

For this study, we prepared colloidal CdS quantum dots using 3-mercaptopropyltrimethoxysilane as capping agent. Colloidal CdS quantum dots were directly deposited on glass substrates by a spin-coating process. Coated substrates were heat-treated between 225°C and 325°C for various heat treatment time intervals to investigate the growth kinetics of the quantum dots. Results showed that sizes of the CdS quantum dots grew approximately from 2.9 to 4.6 nm, and the E_1s1s energy values shifted approximately from 3.3 to 2.7 eV. Results showed that the average size of quantum dots increase by thermal treatment due to Ostwald ripening. The thermal process used to grow the size of quantum dots was examined according to the Lifshitz-Slyozov-Wagner theory. The activation energy of CdS quantum dots in thin films was calculated at approximately 44 kJ/mol.     

Electromodulated reflectance study of self-assembled Ge/Si quantum dots

We perform an electroreflectance spectroscopy of Ge/Si self-assembled quantum dots in the near-infrared and in the mid-infrared spectral range. Up to three optical transitions are observed. The low-energy resonance is proposed to correspond to a band-to-continuum hole transition in the Ge valence band. The other two modulation signals are attributed to the spatially direct transitions between the electrons confined in the L and Δ(4) valleys of the Ge conduction band, and the localized hole states at the Γ point.     

Effects of crossed states on photoluminescence excitation spectroscopy of InAs quantum dots

In this report, the influence of the intrinsic transitions between bound-to-delocalized states (crossed states or quasicontinuous density of electron-hole states) on photoluminescence excitation (PLE) spectra of InAs quantum dots (QDs) was investigated. The InAs QDs were different in size, shape, and number of bound states. Results from the PLE spectroscopy at low temperature and under a high magnetic field (up to 14 T) were compared. Our findings show that the profile of the PLE resonances associated with the bound transitions disintegrated and broadened. This was attributed to the coupling of the localized QD excited states to the crossed states and scattering of longitudinal acoustical (LA) phonons. The degree of spectral linewidth broadening was larger for the excited state in smaller QDs because of the higher crossed joint density of states and scattering rate.     

Impact of N on the atomic-scale Sb distribution in quaternary GaAsSbN-capped InAs quantum dots

The use of GaAsSbN capping layers on InAs/GaAs quantum dots (QDs) has recently been proposed for micro- and optoelectronic applications for their ability to independently tailor electron and hole confinement potentials. However, there is a lack of knowledge about the structural and compositional changes associated with the process of simultaneous Sb and N incorporation. In the present work, we have characterized using transmission electron microscopy techniques the effects of adding N in the GaAsSb/InAs/GaAs QD system. Firstly, strain maps of the regions away from the InAs QDs had revealed a huge reduction of the strain fields with the N incorporation but a higher inhomogeneity, which points to a composition modulation enhancement with the presence of Sb-rich and Sb-poor regions in the range of a few nanometers. On the other hand, the average strain in the QDs and surroundings is also similar in both cases. It could be explained by the accumulation of Sb above the QDs, compensating the tensile strain induced by the N incorporation together with an In-Ga intermixing inhibition. Indeed, compositional maps of column resolution from aberration-corrected Z-contrast images confirmed that the addition of N enhances the preferential deposition of Sb above the InAs QD, giving rise to an undulation of the growth front. As an outcome, the strong redshift in the photoluminescence spectrum of the GaAsSbN sample cannot be attributed only to the N-related reduction of the conduction band offset but also to an enhancement of the effect of Sb on the QD band structure.     

Optical properties of as-grown and annealed InAs quantum dots on InGaAs cross-hatch patterns

InAs quantum dots (QDs) grown on InGaAs cross-hatch pattern (CHP) by molecular beam epitaxy are characterized by photoluminescence (PL) at 20 K. In contrast to QDs grown on flat GaAs substrates, those grown on CHPs exhibit rich optical features which comprise as many as five ground-state emissions from [1-10]- and [110]-aligned QDs, two wetting layers (WLs), and the CHP. When subject to in situ annealing at 700°C, the PL signals rapidly degrades due to the deterioration of the CHP which sets the upper limit of overgrowth temperature. Ex situ hydrogen annealing at a much lower temperature of 350°C, however, results in an overall PL intensity increase with a significant narrowing and a small blueshift of the high-energy WL emission due to hydrogen bonding which neutralizes defects and relieves associated strains.     

Suppression of dislocations by Sb spray in the vicinity of InAs/GaAs quantum dots

The effect of Sb spray prior to the capping of a GaAs layer on the structure and properties of InAs/GaAs quantum dots (QDs) grown by molecular beam epitaxy (MBE) is studied by cross-sectional high-resolution transmission electron microscopy (HRTEM). Compared to the typical GaAs-capped InAs/GaAs QDs, Sb-sprayed QDs display a more uniform lens shape with a thickness of about 3 ~ 4 nm rather than the pyramidal shape of the non-Sb-sprayed QDs. Particularly, the dislocations were observed to be passivated in the InAs/GaAs interface region and even be suppressed to a large extent. There are almost no extended dislocations in the immediate vicinity of the QDs. This result is most likely related to the formation of graded GaAsSb immediately adjacent to the InAs QDs that provides strain relief for the dot/capping layer lattice mismatch.

PACS

81.05.Ea; 81.07.-b; 81.07.Ta     

Strong localization effect and carrier relaxation dynamics in self-assembled InGaN quantum dots emitting in the green

Strong localization effect in self-assembled InGaN quantum dots (QDs) grown by metalorganic chemical vapor deposition has been evidenced by temperature-dependent photoluminescence (PL) at different excitation power. The integrated emission intensity increases gradually in the range from 30 to 160 K and then decreases with a further increase in temperature at high excitation intensity, while this phenomenon disappeared at low excitation intensity. Under high excitation, about 40% emission enhancement at 160 K compared to that at low temperature, as well as a higher internal quantum efficiency (IQE) of 41.1%, was observed. A strong localization model is proposed to describe the possible processes of carrier transport, relaxation, and recombination. Using this model, the evolution of excitation-power-dependent emission intensity, shift of peak energy, and linewidth variation with elevating temperature is well explained. Finally, two-component decays of time-resolved PL (TRPL) with various excitation intensities are observed and analyzed with the biexponential model, which enables us to further understand the carrier relaxation dynamics in the InGaN QDs.     

Long-wavelength room-temperature luminescence from InAs/GaAs quantum dots with an optimized GaAsSbN capping layer

An extensive study on molecular beam epitaxy growth conditions of quaternary GaAsSbN as a capping layer (CL) for InAs/GaAs quantum dots (QD) was carried out. In particular, CL thickness, growth temperature, and growth rate were optimized. Problems related to the simultaneous presence of Sb and N, responsible for a significant degradation of photoluminescence (PL), are thereby solved allowing the achievement of room-temperature (RT) emission. A particularly strong improvement on the PL is obtained when the growth rate of the CL is increased. This is likely due to an improvement in the structural quality of the quaternary alloy that resulted from reduced strain and composition inhomogeneities. Nevertheless, a significant reduction of Sb and N incorporation was found when the growth rate was increased. Indeed, the incorporation of N is intrinsically limited to a maximum value of approximately 1.6% when the growth rate is at 2.0 ML s⁻¹. Therefore, achieving RT emission and extending it somewhat beyond 1.3 μm were possible by means of a compromise among the growth conditions. This opens the possibility of exploiting the versatility on band structure engineering offered by this QD-CL structure in devices working at RT.

PACS

81.15.Hi (molecular beam epitaxy); 78.55.Cr (III-V semiconductors); 73.21.La (quantum dots)     

Temperature dependent optical properties of single, hierarchically self-assembled GaAs/AlGaAs quantum dots

We report on the experimental observation of bright photoluminescence emission at room temperature from single unstrained GaAs quantum dots (QDs). The linewidth of a single-QD ground-state emission (≈ 8.5 meV) is comparable to the ensemble inhomogeneous broadening (≈ 12.4 meV). At low temperature (T  ≤  40 K) photon correlation measurements under continuous wave excitation show nearly perfect single-photon emission from a single GaAs QD and reveal the single photon nature of the emitted light up to 77 K. The QD emission energies, homogeneous linewidths and the thermally activated behavior as a function of temperature are discussed.     

Analysis of the 3D distribution of stacked self-assembled quantum dots by electron tomography

The 3D distribution of self-assembled stacked quantum dots (QDs) is a key parameter to obtain the highest performance in a variety of optoelectronic devices. In this work, we have measured this distribution in 3D using a combined procedure of needle-shaped specimen preparation and electron tomography. We show that conventional 2D measurements of the distribution of QDs are not reliable, and only 3D analysis allows an accurate correlation between the growth design and the structural characteristics.     

Influence of substrate orientation on exciton fine structure splitting of InAs/InP nanowire quantum dots

ABSTRACT: : In this paper, we use an atomistic approach to investigate strain distributions, single particle and many body electronic properties of InAs/InP nanowire quantum dots with substrate orientation varying from [111] to high-index [119], and compared with [001] case. We show that single particle gap for high-index [11k] substrates is increased with respect to [111] and [001] cases, and oscillates with the substrate index due to faceting effects. Surprisingly, the overall shell-like structure of single particle states is preserved even for highly facetted, high-index substrates. On the contrary, we demonstrate that besides two limiting high-symmetry cases, [001] and [111], the bright exciton splitting varies strongly with substrate orientation. For [112]-oriented substrate, the fine structure splitting reaches maximum due to crystal lattice anisotropy despite fully cylindrical isotropic shape of nanowire quantum dot.     

The influence of temperature on the photoluminescence properties of single InAs quantum dots grown on patterned GaAs

ABSTRACT: We report the temperature-dependent photoluminescence of single site-controlled and self-assembled InAs quantum dots. We have used nanoimprint lithography for patterning GaAs(100) templates and molecular beam epitaxy for quantum dot deposition. We show that the influence of the temperature on the photoluminescence properties is similar for quantum dots on etched nanopatterns and randomly positioned quantum dots on planar surfaces. The photoluminescence properties indicate that the prepatterning does not degrade the radiative recombination rate for the site-controlled quantum dots.     

Tunable optical Kerr effects of DNAs coupled to quantum dots

The coupling between DNA molecules and quantum dots can result in impressive nonlinear optical properties. In this paper, we theoretically demonstrate the significant enhancement of Kerr coefficient of signal light using optical pump-probe technique when the pump-exciton detuning is zero, and the probe-exciton detuning is adjusted properly to the frequency of DNA vibration mode. The magnitude of optical Kerr coefficient can be tuned by modifying the intensity of the pump beam. It is shown clearly that this phenomenon cannot occur without the DNA-quantum dot coupling. The present research will lead us to know more about the anomalous nonlinear optical behaviors in the hybrid DNA-quantum dot systems, which may have potential applications in the fields such as DNA detection.     

Increased conductance of individual self-assembled GeSi quantum dots by inter-dot coupling studied by conductive atomic force microscopy

ABSTRACT: The conductive properties of individual self-assembled GeSi quantum dots (QDs) are investigated by conductive atomic force microscopy on single-layer (SL) and bilayer (BL) GeSi QDs with different dot densities at room temperature. By comparing their average currents, it is found that the BL and high-density QDs are more conductive than the SL and low-density QDs with similar sizes, respectively, indicating the existence of both vertical and lateral couplings between GeSi QDs at room temperature. On the other hand, the average current of the BL QDs increases much faster with the bias voltage than that of the SL QDs. Our results suggest that the QDs' conductive properties can be greatly regulated by the coupling effects and bias voltages, which are valuable for potential applications.     

Electrochemical,spectroscopic and morphological characterization of electrostatic self-assembled hybrids of tetracationic phosphonium porphyrins and CdTe quantum dots

Cationic porphyrins (i.e., [Ttolyl(P-(C₆H₅)₃)₄]⁴⁺, where Ttolyl = 5,10,15,20-tetrakis tolylporphyrin and CdTe capped with glutathione) were electrostatically self-assembled via a layer-by-layer methodology onto ITO electrodes and characterized by UV–Vis spectroscopy, cyclic voltammetry, electrochemical impedance spectroscopy (EIS) and SEM-EDX microscopy. Cyclic voltammetry studies of the cationic porphyrin [Ttolyl(P-(C₆H₅)₃)₄]⁴⁺ demonstrated its ability to absorb both glassy carbon and ITO electrodes. The electrochemical properties of the hybrid porphyrin/quantum dot films (i.e., ITO/{[Ttolyl(P-(C₆H₅)₃)₄]⁴⁺/CdTe}_n, where n = 1–5 is the immersion step) were explored in buffer solutions in the presence or absence of the Fe(CN) ₆ ^3? /Fe(CN) ₆ ^4? redox couple at pH 7.0. The resistance to electron transfer determined by cyclic voltammetry and EIS is in agreement with the increase in the UV–Vis absorption of the material adsorbed onto the ITO surface for each newly assembled bilayer. The prepared bilayers exhibited an interesting homogeneous morphological distribution of CdTe quantum dots on the surface, which indicated the ability of [Ttolyl(P-(C₆H₅)₃)₄]⁴⁺ to organize CdTe nanoparticles on the ITO surface. EDX analysis of the bilayers confirmed the presence of Cd, Te, and S from the quantum dot. Linear sweep voltammetry indicated that ITO/{[Ttolyl(P-(C₆H₅)₃)₄]⁴⁺/CdTe}₅ has oxygen reduction electrocatalytic properties and demonstrated a synergetic effect between the cationic porphyrin and the CdTe quantum dot.     

Excitonic effects on the second-order nonlinear optical properties of semi-spherical quantum dots

We study the excitonic effects on the second-order nonlinear optical properties of semi-spherical quantum dots considering, on the same footing, the confinement potential of the electron-hole pair and the Coulomb interaction between them. The exciton is confined in a semi-spherical geometry by means of a three-dimensional semi-parabolic potential. We calculate the optical rectification and second harmonic generation coefficients for two different values of the confinement frequency based on the numerically computed energies and wavefunctions of the exciton. We present the results as a function of the incident photon energy for GaAs/AlGaAs quantum dots ranging from few nanometers to tens of nanometers. We find that the second-order nonlinear coefficients exhibit not only a blue-shift of the order of meV but also a change of intensity compared with the results obtained ignoring the Coulomb interaction in the so-called strong-confinement limit.     

InAs/GaAs quantum dots with wide-range tunable densities by simply varying V/III ratio using metal-organic chemical vapor deposition

The complicated behaviors of InAs/GaAs quantum dots with increasing V/III ratio associated with several competing mechanisms have been described. The results demonstrate that the densities of InAs quantum dots can be tuned in a wide range from 10⁵ to 10¹⁰ cm⁻² by simply manipulating V/III ratio via metal-organic chemical vapor deposition. These results are mainly ascribed to the changes of coverage and In adatom migration length due to the increasing V/III ratio.     

半导体纳米晶体制备及应用进展

综述了量子点的制备及应用进展