STM probe-assisted site-control of self-organized InAs quantum dots on GaAs surfaces

A site-control technique for individual InAs quantum dots (QDs) has been developed by using scanning tunneling microscope (STM) probe-assisted nanolithography and self-organizing molecular-beam epitaxy. We find that nano-scale deposits can be created on a GaAs surface by applying voltage and current pulses between the surface and a tungsten tip of the STM, and that they act as “nano-masks” on which GaAs does not grow directly. Accordingly, subsequent thin GaAs growth produces GaAs nano-holes above the deposits. When InAs is supplied on this surface, QDs are self-organized at the hole sites, while hardly any undesirable Stranski-Krastanov QDs are formed in the flat surface region. Using this technique with nanometer precision, a QD pair with 45-nm pitch is successfully fabricated. An erratum to this article is available at .     

InP基多周期InAs/InAlGaAs量子点阵列的结构和光学性质

在InP（001）衬底上使用分子束外延技术自组织生长了多周期InAs/InAlGaAs量子点阵列结构。根据对透射电镜和光致发光谱结果的分析，认为引入与InP衬底晶格匹配的InAlGaAs缓冲层可以获得较大的InAs量子点结构，而InAlGaAs层的表面特性对InAs量子点的结构及光学性质有很大影响。对InP基InAlGaAs缓冲层上自组织量子点的形核和演化机制进行了探讨，提出量子点的演化过程表现为量子点的合并长大并伴随着自身的徙动，以获得能量最优的分布状态。     

Wavelength controlled InAs/InP quantum dots for telecom laser applications

This article reviews the recent progress in the growth and device applications of InAs/InP quantum dots (QDs) for telecom applications. Wavelength tuning of the metalorganic vapor-phase epitaxy grown single layer and stacked InAs QDs embedded in InGaAsP/InP (1 0 0) over the 1.55-μm region at room temperature (RT) is achieved using ultra-thin GaAs interlayers underneath the QDs. The GaAs interlayers, together with reduced growth temperature and V/III ratio, and extended growth interruption suppress As/P exchange to reduce the QD height in a controlled way. Device quality of the QDs is demonstrated by temperature-dependent photoluminescence (PL) measurements, revealing zero-dimensional carrier confinement and defect-free InAs QDs, and is highlighted by continuous-wave ground-state lasing at RT of narrow ridge-waveguide QD lasers, exhibiting a broad gain spectrum. Unpolarized PL from the cleaved side, important for realization of polarization insensitive semiconductor optical amplifiers, is obtained from closely stacked QDs due to vertical electronic coupling.     

Effects of growth interruption on the evolution of InAs/InP self-assembled quantum dots

We investigated the change in the structural and optical properties of InAs/InP quantum structures during growth interruption (GI) for various times and under various atmospheres in metalorganic chemical vapor deposition. Under AsH₃ + H₂ atmosphere, the mass transport for the 2D-to-3D transition was observed during the GI. Photoluminescence peaks from both quantum dots (QDs) and quantum wells were observed from the premature QD samples. The fully developed QDs showed the two distinct temperature regimes in the PL peak position, full width at half maximum (FWHM) and wavelength-integrated peak intensity. The two characteristic activation energies were obtained from the InAs/InP QDs: ∼10 meV for intra-dot excitation and 90 ∼ 110 meV for the excitation out of the dots, respectively. It was also observed that the QD evolution kinetics could be suppressed in PH₃ + H₂ and H₂ atmospheres. The proper control of GI time and atmosphere might be a useful tool to further improve the properties of QDs.     

Self‐Assembled InAs Quantum Dots on InP(001) for Long‐Wavelength Laser Applications

Self‐assembled InAs quantum dots (QDs) embedded in an InAlGaAs matrix were grown on an InP (001) using a solid‐source molecular beam epitaxy and investigated using transmission electron microscopy (TEM) and photoluminescence (PL) spectroscopy. TEM images indicated that the QD formation was strongly dependent on the growth behaviors of group III elements during the deposition of InAlGaAs barriers. We achieved a lasing operation of around 1.5 µm at room temperature from uncoated QD lasers based on the InAlGaAs‐InAlAs material system on the InP (001). The lasing wavelengths of the ridge‐waveguide QD lasers were also dependent upon the cavity lengths due mainly to the gain required for the lasing operation.     

Light emission by semiconductor structure with quantum well and array of quantum dots

A new type of composite active region of a laser, which contains an In_0.2Ga_0.8As quantum well (QW) and an array of InAs quantum dots (QDs) embedded in GaAs is studied. The QW acts as accumulator of injected carriers, and the QD array is the emitting system located in tunneling proximity to the QW. A theory for the calculation of electron and hole energy levels in the QD is developed. Occupation of the QDs due to the resonance tunneling of electrons and holes from the QW to the QD is considered; the conclusions are compared with the results obtained in studying an experimental laser with a combined active region.     

InAs/InP Self‐Assembled Quantum Dots: Wavelength Tuning and Optical Nonlinearities

Quantum dots (QDs, i.e., semiconductor nanocrystals) can be formed by spontaneous self‐assembly during epitaxial growth of lattice‐mismatched semiconductor systems. InAs QDs embedded in GaInAsP on InP are introduced, which can be continuously wavelength‐tuned over the 1.55 μm region by inserting ultrathin GaAs or GaP interlayers below them. We subsequently introduce a state‐filling optical nonlinearity, which only requires two electron–hole pairs per QD. We employ this nonlinearity for all‐optical switching using a Mach–Zehnder interferometric switch. We find a switching energy as low as 6 fJ.     

Small-signal field effect in GaAs/InAs quantum-dot heterostructures

InAs quantum dots (QDs), incorporated into the space-charge region of an epitaxial n-GaAs film at different distances (5?C300 nm) from the surface, decrease the potential barrier for the electrons located in n-GaAs. For tunnel-thin coating layers this decrease is related to tunneling through QD energy levels. For thick layers this decrease is caused by negative charging of the QDlevels and defects located near QDs. The decrease in the barrier increases the efficiency of electron capture by surface states and shifts the frequency dispersion of mobility under the field effect, related to this capture, toward higher frequencies. When QDs are incorporated near the barrier??s base, they manifest themselves in the relaxation of the small-signal field effect. Some parameters of the QD levels are determined. Defect formation is revealed in the layers adjacent to QDs.     

Ultra-low density InAs quantum dots

We show that InAs quantum dots (QDs) can be grown by molecular beam epitaxy (MBE) with an ultralow density of sin 10⁷ cm^?2 without any preliminary or post-growth surface treatment. The strain-induced QD formation proceeds via the standard Stranski-Krastanow mechanism, where the InAs coverage is decreased to 1.3–1.5 monolayers (MLs). By using off-cut GaAs (100) substrates, we facilitate the island nucleation in this subcritical coverage range without any growth interruption. The QD density dependences on the InAs coverage are studied by photoluminescence, atomic force microscopy, transmission electron microscopy, and are well reproduced by the universal double exponential shapes. This method enables the fabrication of InAs QDs with controllable density in the range 10⁷–10⁸ cm^?2, exhibiting bright photoluminescence.     

Indirect band gaps in quantum dots made from direct-gap bulk materials

The conditions under which the band gaps of free standing and embedded semiconductor quantum dots are direct or indirect are discussed. Semiconductor quantum dots are classified into three categories; (i) free standing dots, (ii) dots embedded in a direct gap matrix, and (iii) dots embedded in an indirect gap matrix. For each category, qualitative predictions are first discussed, followed by the results of both recent experiments and state of the art pseudopotential calculations. We show that:

Improved area density and luminescence properties of InP quantum dots grown on In<Subscript>0.5</Subscript>Al<Subscript>0.5</Subscript>P by metal-organic chemical vapor deposition

We report on the growth of InP self-assembled quantum dots (QDs) on In_0.5Al_0.5P matrices by metal-organic chemical vapor deposition (MOCVD) on (001) GaAs substrates. The effects of the growth temperature and V/III-precursor flow ratio on the areal density and the cathodoluminescence (CL) properties of the grown QDs were systematically studied. We found that, when the growth temperature is ≤630°C, coherent QDs as well as large dislocated InP islands can be observed on the matrix surface. However, by using a two-step growth method, i.e., by growing the InAlP matrix layer at higher temperatures and growing InP QDs at lower temperatures, the formation of large dislocated islands can be effectively suppressed. Moreover, the areal density of the InP QDs is increased as the QD growth temperature is reduced. Furthermore, we found that the V/III ratio used in growing QDs and in growing the InAlP matrix layers has a quite different effect. In growing QDs, decreasing the V/III ratio results in an increase in the CL intensity and a decrease in CL line width; while in growing the InAlP matrix layers, increasing the V/III ratio results in an increase in the CL intensity of the InP QDs.     

Capacitance-voltage analysis of InAs quantum dots grown on InAlAs/InP(0 0 1)

The electronic properties of InAs quantum dots (QDs) grown on InAlAs/InP(0 0 1) were studied by using capacitance-voltage (C-V) analysis and photoluminescence (PL) measurements. The level positions of electrons and holes could be studied separately by using n- and p-type InAlAs matrices, respectively. The holes are found to be more confined than electrons in these kinds of dots.     

Electron microscopy of GaAs Structures with InAs and as quantum dots

An electron-microscopy study of GaAs structures, grown by molecular-beam epitaxy, containing two coupled layers of InAs semiconductor quantum dots (QDs) overgrown with a thin buffer GaAs layer and a layer of low-temperature-grown gallium arsenide has been performed. In subsequent annealing, an array of As nanoinclusions (metallic QDs) was formed in the low-temperature-grown GaAs layer. The variation in the microstructure of the samples during temperature and annealing conditions was examined. It was found that, at comparatively low annealing temperatures (400–500°C), the formation of the As metallic QDs array weakly depends on whether InAs semiconductor QDs are present in the preceding layers or not. In this case, the As metallic QDs have a characteristic size of about 2–3 nm upon annealing at 400°C and 4–5 nm upon annealing at 500°C for 15 min. Annealing at 600°C for 15 min in the growth setup leads to a coarsening of the As metallic QDs to 8–9 nm and to the formation of groups of such QDs in the area of the low-temperature-grown GaAs which is directly adjacent to the buffer layer separating the InAs semiconductor QDs. A more prolonged annealing at an elevated temperature (760°C) in an atmosphere of hydrogen causes a further increase in the As metallic QDs’ size to 20–25 nm and their spatial displacement into the region between the coupled InAs semiconductor QDs.     

Self-organized InAs/GaAs quantum dots multilayers with growth interruption emitting at 1.3 μm

We have grown single, 10 and 20 InAs/GaAs quantum dots (QDs) multilayers by molecular beam epitaxy in Stranski-Krastanov growth mode with and without growth interruption. Multilayer structures of InAs QDs have been studied by photoluminescence (PL) and atomic force microscopy (AFM) techniques. Between 1 and 10 layers of QDs, 10 K PL shows a shift energy, and a PL linewidth reduction. Moreover, AFM image of the 10 layers sample shows that the InAs QDs size remains constant and almost uniform when the growth is without interruption. These effects are attributed to electronic coupling between QDs in the the columns. However, we show the possibility of extending the spectral range of luminescence due to InAs QDs up to 1.3 μm. Realisation of such a wavelength emission is related to formation of lateral associations or coupling of QDs (LAQDs or LCQDs) during InAs deposition when growth interruption (20 s) is used after each InAs QDs layer deposition. The growth interruption applied after the deposition of the InAs layer allows the formation of well-developed InAs dots (large dot size).     

Density Control of InP/GaInP Quantum Dots Grown by Metal-Organic Vapor-Phase Epitaxy

We investigated structural and emission properties of self-organized InP/GaInP quantum dots (QD) grown by metal organic chemical vapor deposition using an amount of deposited In from 7 to 2 monolayers (ML). In the uncapped samples, using atomic force microscopy (AFM), we observed lateral sizes of 100–200 nm, together with a bimodal height distribution having maxima at ～5 and ～15 nm, which we denoted as QDs of type A and B, respectively; and reduction of the density of the type-B dots from 4.4 to 1.6 μm^–2. The reduction of the density of B-type dots were observed also using transmission electron microscopy of the capped samples. Using single dot low-temperature photoluminescence (PL) spectroscopy we demonstrated effects of Wigner localization for the electrons accumulated in these dots.     

Wannier-Stark states in a superlattice of InAs/GaAs quantum dots

Electron and hole emission from states of a ten-layer system of tunneling-coupled vertically correlated InAs/GaAs quantum dots (QDs) is studied experimentally by capacitance—voltage measurements and deep-level transient spectroscopy. The thickness of GaAs interlayers separating sheets of InAs QDs was ≈3 nm, as determined from transmission electron microscope images. It is found that the periodic multimo-dal DLTS spectrum of this structure exhibits a pronounced linear shift as the reverse-bias voltage U _r applied to the structure is varied. The observed behavior is a manifestation of the Wannier—Stark effect in the InAs/GaAs superlattice, where the presence of an external electric field leads to the suppression of coupling between the wave functions of electron states forming the miniband and to the appearance of a series of discrete levels called Wannier—Stark ladder states.     

Influence of bismuth doping of InAs quantum-dot layer on the morphology and photoelectronic properties of Gas/InAs heterostructures grown by metal-organic chemical vapor deposition

GaAs/InAs quantum dot (QD) heterostructures prepared by metalloorganic chemical vapor deposition (MOCVD) are investigated. It is established that the introduction of isovalent bismuth doping during the growth of InAs QD layer results in the suppression of the nanocluster coalescence and favors the formation of more uniform QDs. Bismuth itself is virtually not incorporated into the dots, its role being mainly in limiting the migration mobility of atoms at the surface of the growing layer. A method for investigating the morphology of buried layers of InAs QDs in GaAs matrix by atomic-force microscopy is developed; it relies on the removal of the cap layer by selective chemical etching. The photoluminescence (PL) and photoelectric sensitivity spectra of the fabricated heterostructures and their relation to the morphology of the QD layer are studied. In doped structures, PL and selective photosensitivity owing to the QDs are observed at a wavelength of 1.41 µm with the linewidth of 43 meV at room temperature. Some of the morphological features and photoelectronic properties of the MOCVD-grown heterostructures are related to the formation of a transitional layer at the GaAs/InAs QD interface due to the diffusion-induced mixing of the components.     

Optical properties and structure of InAs quantum dots in near-infrared band

The InAs quantum dots (QDs) grown by molecular beam epitaxy (MBE) are studied as a function of growth temperature at a specific InAs coverage of 2.7 ML. The QDs density is significantly reduced from 8.0 × 1010 to 5.0 × 109 cm-2 as the growth temperature increases from 480℃ to 520℃, while the average QDs diameter and height becomes larger. The effects of the growth temperature on the evolution of bimodal QDs are investigated by combining atomic force microscopy (AFM) and photoluminescence (PL). Results show that the formation of the bimodal QDs depends on the growth temperature: at a growth temperature of 480℃,large QDs result from the small QDs coalition; at a growth temperature of 535℃, the indium desorption and InAs segregation result in the formation of small QDs.     

Green InP/ZnSeS/ZnS Core Multi-Shelled Quantum Dots Synthesized with Aminophosphine for Effective Display Applications

InP quantum dots (QDs) are emerging as promising materials for replacing cadmium-based QDs in view of their heavy metal-free and tunable luminescence. However, the development of InP QD materials still lags due to the expensive and flammable phosphorus precursors, and also the unsatisfactory repeatability caused by the fast nucleation rate. Adopting lowly reactive P precursor aminophosphine can overcome this issue, but their low photoluminescence quantum yield (PLQY) and widening line widths do not apply to the practical application. Through engineering, the core-shell structure of QD, significantly promoted green emissions of QDs were obtained with PLQY of 95% and full width and half maximum (FWHM) of 45 nm, which demonstrated the highest PLQY record obtained from the aminophosphine system. Moreover, due to the residue halogen atoms on the QD surface as inorganic ligands to prevent further oxidization, these InP QDs demonstrated the ultra-long operational lifetime (over 1000 h) for QDs based color enhancement film. By optimizing the device structure, an inverted green InP quantum dot light-emitting diode (QLED) with external quantum efficiency (EQE) of 7.06% was also demonstrated, which showed a significant promise of these InP QDs in highly effective optoelectronic devices.     

Heteroepitaxial growth of InAs on GaAs(0 0 1) by in situ STM located inside MBE growth chamber

The growth of InAs on GaAs(0 0 1) is of great interest primarily due to the self-assembly of arrays of quantum dots (QDs) with excellent opto-electronic properties. However, a basic understanding of their spontaneous formation is lacking. Advanced experimental methods are required to probe these nanostructures dynamically in order to elucidate their growth mechanism. Scanning tunneling microscopy (STM) has been successfully applied to many GaAs-based materials grown by molecular beam epitaxy (MBE). Typical STM–MBE experiments involve quenching the sample and transferring it to a remote STM chamber under arsenic-free ultra-high vacuum. In the case of GaAs-based materials grown at substrate temperatures of 400–600 °C, operating the STM at room temperature ensures that the surface is essentially static on the time scale of STM imaging. To attempt dynamic experiments requires a system in which STM and MBE are incorporated into one unit in order to scan in situ during growth. Here, we discuss in situ STM results from just such a system, covering both QDs and the dynamics of the wetting layer.