Growth and optical characterization of dense arrays of site-controlled quantum dots grown in inverted pyramids

We report on the growth and optical properties of dense arrays of single GaAs/AlGaAs quantum dot (QD) heterostructures with pitches as small as 300 nm. The samples were grown by organometallic chemical vapor deposition in dense inverted pyramids on {1 1 1}B GaAs substrate pre-patterned using electron beam lithography and wet chemical etching. The growth conditions such as deoxidation and growth temperatures, growth rates, and V/III ratio, had to be chosen quite differently from those employed with micron-size pyramids. Low-temperature micro-photoluminescence and cathodoluminescence spectra of the samples show distinct luminescence from the QDs with a linewidth of less than 1 meV and uniform emission energy for an ensemble of 900 QDs. The possibility of incorporating such QD arrays inside optical microcavity structures is also discussed.     

Controlled stacking growth of uniform InAs quantum dots by molecular beam epitaxy

Double-stacked InAs quantum dots (QDs) were grown by molecular beam epitaxy via Stranski–Krastanov growth mode. Transition of the facet formation from {1 3 6} plane to {1 1 0} plane was observed during the stacking growth of InAs QDs by reflection high-energy electron-beam diffraction. The enhanced growth rate and the different facet formation in the stacking growth were caused by tensile strain of the GaAs underlying layer. Low arsenic pressure and low growth rate conditions played an important role for a perfect coupling and uniformity in the size of the stacked QDs. The narrow photoluminescence line width of 17.6 meV was successfully obtained from the stacked InAs QDs.     

Growth of Ge islands on prepatterned Si (0 0 1) substrates

We report on the growth and properties of Ge islands grown on (0 0 1) Si substrates with lithographically defined two-dimensionally periodic pits. After thermal desorption and a subsequent Si buffer layer growth these pits have an inverted truncated pyramid shape. We observe that on such prepatterned substrates lens-like Ge-rich islands grow at the pit bottoms with less Ge deposition than necessary for island formation on flat substrates. This is attributed to the aggregation of Ge at the bottom of the pits, due to Ge migration from the pit sidewalls. At the later stages of growth, dome-like islands with dominant {1,1,3} or {15,3,23}, or other high-index facets [i.e. {15,3,20} facets] are formed on the patterned substrates as shown by surface orientation maps using atomic force microscopy. Furthermore, larger coherent islands can be grown on patterned substrates as compared to Ge deposition on flat ones.     

Electronic states of self-organized InGaAs quantum dots on GaAs (3 1 1)B studied by conductive scanning probe microscope

We have used conductive scanning probe microscope (SPM) in high vacuum and operated at 173 K in order to investigate the electronic properties of self-organized InGaAs quantum dots (QDs) grown on GaAs (3 1 1)B and (0 0 1) substrates. Ordered InGaAs quantum dot arrays on GaAs (3 1 1)B surface were fabricated by atomic-H assisted molecular beam epitaxy (H-MBE), and Si SPM tips coated with Au which warrants electrical conductivity were used to measure simultaneously both the topographic and current images of QDs surface. From the current–voltage (I–V) curves, unique and different plateau features were observed for QDs formed on GaAs (3 1 1)B and (0 0 1) substrates. The results suggested that a high degree of symmetry of InGaAs QDs on (3 1 1)B was responsible for the observed degeneracy of electronic states and artificial atom-like states. We demonstrate that this conductive SPM technique becomes a powerful tool in studies of single electron charging of individual dots.     

Spontaneous one-dimensional lateral alignment of multistacked InGaAs quantum dots on GaAs (n 1 1)B substrates

In_0.45Ga_0.55As/GaAs multistacking quantum dot (QD) structures were fabricated on a GaAs (n 1 1)B (n=2–4) substrate by metalorganic vapor-phase epitaxy. QDs spontaneously aligned in the [0 1 1] direction were observed on stacked QDs, whereas QDs were randomly distributed in the initial In_0.45Ga_0.55As layer growth. The formation mechanism of this self-alignment was studied by changing the number of In_0.45Ga_0.55As/GaAs multilayers and crystallographic arrangement. Photoluminescence spectra showing clear polarization dependence indicate carrier coupling in the QD arrays. This growth technique results in spontaneously aligned InGaAs QDs without any preprocessing technique prior to growth.     

Growth of GaAs/AlGaAs hexagonal pillars on GaAs (1 1 1)B surfaces by selective-area MOVPE

We report on the growth of GaAs and GaAs/AlGaAs heterostructured hexagonal pillar structures using selective area (SA) metalorganic vapor phase epitaxy (MOVPE). By performing growth on SiO₂-masked (1 1 1)B GaAs substrates with circular or hexagonal hole openings, extremely uniform array of hexagonal GaAs/AlGaAs pillars consisting {1 1 0} vertical facets with their diameter of order of 100 nm were obtained. Unexpectedly, strong intense light emission was observed for the room temperature photoluminescence measurement of the pillar arrays in triangular lattice, which is promising for the application to the photonic crystals to enhance the light extraction efficiency from the materials with high refractive index. Furthermore, it was also found that hexagonal pillars with size 60 nm and large aspect ratio (>100) by reducing the size of initial hole size of mask, opening a possibility to grow nanowires using epitaxial growth.     

Atomistic simulation of the surface structure of electrolytic manganese dioxide

Atomistic simulation methods were used to investigate the surface structures and stability of pyrolusite and ramsdellite polymorphs of electrolytic manganese dioxide (EMD). The interactions between the atoms were described using the Born model of Solids. This model was used to calculate the structures and energies of the low index surfaces {0 0 1}, {0 1 0}, {0 1 1}, {1 0 0}, {1 0 1} and {1 1 0} for both pyrolusite and ramsdellite. Pyrolusite is isostructural with rutile and similar to rutile the {1 1 0} surface is found to be the most stable with the relaxed surface energy 2.07 J m⁻². In contrast, for ramsdellite the {1 0 1} surface is the most stable with a surface energy of 1.52 J m⁻². Pyrolusite {1 0 0} and ramsdellite {1 0 0}_b surfaces have equivalent energies of 2.43 J m⁻² and 2.45 J m⁻², respectively and similar surface areas and hence are the likely source for the intergrowths. Finally, comparison of the energies of reduction suggests that the more stable surfaces of pyrolusite are more easily reduced.     

The emission wavelength tuning of InAs/InP quantum dots with thin GaAs, InGaAs, InP capping layers by MOCVD

InAs quantum dots (QDs) were grown on InP substrates by metalorganic chemical vapor deposition. The width and height of the dots were 50 and 5.8 nm, respectively on the average and an areal density of 3.0×10¹⁰ cm⁻² was observed by atomic force microscopy before the capping process. The influences of GaAs, In_0.53Ga_0.47As, and InP capping layers (5–10 ML thickness) on the InAs/InP QDs were studied. Insertion of a thin GaAs capping layer on the QDs led to a blue shift of up to 146 meV of the photoluminescence (PL) peak and an InGaAs capping layer on the QDs led to a red shift of 64 meV relative to the case when a conventional InP capping layer was used. We were able to tune the emission wavelength of the InAs QDs from 1.43 to 1.89 μm by using the GaAs and InGaAs capping layers. In addition, the full-width at half-maximum of the PL peak decreased from 79 to 26 meV by inserting a 7.5 ML GaAs layer. It is believed that this technique is useful in tailoring the optical properties of the InAs QDs at mid-infrared regime.     

Structural and optical properties of In0.5Ga0.5As/GaAs quantum dots in an In0.1Ga0.9As well using repeated depositions of InAs/GaAs short-period superlattices for the application of optical communication

We report structural and optical properties of In_0.5Ga_0.5As/GaAs quantum dots (QDs) in a 100 Å-thick In_0.1Ga_0.9As well grown by repeated depositions of InAs/GaAs short-period superlattices with atomic force microscope, transmission electron microscope (TEM) and photoluminescence (PL) measurement. The QDs in an InGaAs well grown at 510 °C were studied as a function of n repeated deposition of 1 monolayer thick InAs and 1 monolayer thick GaAs for n=5–10. The heights, widths and densities of dots are in the range of 6–22.0 nm, 40–85 nm, and 1.6–1.1×10¹⁰/cm², respectively, as n changes from 5 to 10 with strong alignment along [1 −1 0] direction. Flat and pan-cake-like shape of the QDs in a well is found in TEM images. The bottoms of the QDs are located lower than the center of the InGaAs well. This reveals that there was intermixing—interdiffusion—of group III materials between the InGaAs QD and the InGaAs well during growth. All reported dots show strong 300 K-PL spectrum, and 1.276 μm (FWHM: 32.3 meV) of 300 K-PL peak was obtained in case of 7 periods of the QDs in a well, which is useful for the application to optical communications.     

Excess molar volumes of ternary mixtures {n-butylacetae + 1-butanol + 1, 2-butanediol} and {n-butylacetate + 1-butanol + 1, 3-butanediol} at T = 303.15 K

Excess molar volumes of the ternary systems formed by {n-butylacetate + 1-butanol + 1,2-butanediol } and {n-butylacetate + 1-butanol + 1,3-butanediol} were measured at 303.15 K for the whole composition range. The excess molar volumes, V_m^E, for binary mixtures of {n-butylacetate + 1-butanol, + 1,2-butanediol and + 1,3-butanediol} are positive and for the binary mixtures of {1-butanol + 1,2-butanediol and + 1,3-butanediol} are negative. Several empirical expressions are used to predict and correlate the ternary excess molar volumes from experimental results on the constituted binaries and analyzed to gain insight about liquid mixture interactions.     

InAs/AlAs quantum dots with InGaAs insertion layer: dependence of the indium composition and the thickness

We have systematically studied the effect of an In_xGa_1−xAs insertion layer (IL) on the optical and structural properties of InAs quantum dot (QD) structures. A high density of 9.6×10¹⁰ cm⁻² of InAs QDs with an In_0.3Ga_0.7As IL has been achieved on a GaAs (1 0 0) substrate by metal organic chemical vapor deposition. A photoluminescence line width of 25 meV from these QDs has been obtained. We attribute the high density and high uniformity of these QDs to the use of the IL. Our results show that the InGaAs IL is useful for obtaining high-quality InAs QD structures for devices with a 1.3 μm operation.     

Selective growth of stacked InAs quantum dots by using the templates formed by the Nano-Jet Probe

We have demonstrated the selective area growth of stacked self-assembled InAs quantum dot (QD) arrays in the desired regions on a substrate and confirmed the photoluminescence (PL) emission exhibited by them at room temperature. These InAs QDs are fabricated by the use of a specially designed atomic force microscope cantilever referred to as the Nano-Jet Probe (NJP). By using the NJP, two-dimensional arrays with ordered In nano-dots are fabricated in the desired square regions on a GaAs substrate and directly converted into InAs QD arrays through the subsequent annealing by the irradiation of As flux. By using the converted QD arrays as strain templates, self-organized InAs QDs are stacked. These stacked QDs exhibit the PL emission peak at a wavelength of 1.02 μm.     

Successful growth of two different quantum dots on one substrate

We report the successful growth of ZnSe and ZnTe quantum dots (QDs) embedded in ZnS on GaAs substrate. These QDs have good optical properties and show quantum confinement effect. High-resolution electron scanning microscope studies show that these QDs are grown in Volmer–Weber mode. It is found that the size of the QDs is controlled by the growth duration. When the growth time is short, high density of QDs could be fabricated, but with a long growth time the small QDs get together to form a large cluster. We also show that with this growth method it is possible to grow both ZnSe quantum and ZnTe QDs on one substrate at the same time. For this dual QDs system, two peaks corresponding to the emission from the ZnSe dots (3.0 eV, blue–violet) and ZnTe dots (2.6 eV, green–blue) could be observed at the same time in the photoluminescence measurement.     

Continuous wavelength tuning of InAs quantum dots on InP (1 0 0) and (3 1 1)A substrates by chemical-beam epitaxy

The growth of InAs quantum dots (QDs) on InP (1 0 0) and (3 1 1)A substrates by chemical-beam epitaxy is studied. The InAs QDs are embedded in a GaInAsP layer lattice-matched to InP. We demonstrate an effective way to continuously tune the emission wavelength of InAs QDs grown on InP (1 0 0). With an ultra-thin GaAs layer inserted between the QD layer and the GaInAsP buffer, the peak wavelength from the InAs QDs can be continuously tuned from above 1.6 μm down to 1.5 μm at room temperature. The major role of the thin GaAs layer is to greatly suppress the As/P exchange during the deposition of InAs and subsequent growth interruption under arsenic flux, as well as to consume the segregated In layer floating on the GaInAsP buffer. Moreover, it is found that InP (3 1 1)A substrates are particularly promising for formation of uniform InAs QDs. The growth of InAs on InP (3 1 1)A consists of two stages: nanowire formation due to strain-driven growth instability and subsequent QD formation on top of the wires. The excellent size uniformity of the InAs QDs obtained on InP (3 1 1)A manifests itself in the narrow photoluminescence line width of 26 meV at 4.8 K.     

Transient-enhanced Si diffusion on natural-oxide-covered Si(0 0 1) nano-structures during vacuum annealing

The morphology of annealed patterned Si(0 0 1) wire templates was studied by several techniques. We found an enormous Si-mass transport on the Si surface at usual oxide desorption temperatures around 900°C under UHV conditions. Heat treatment of 5 min transforms the initially rectangular wire profiles with a height of 300 nm to flat (<100 nm) and faceted triangular ridges exhibiting thermodynamically preferred {1 1 1}- and {3 1 1}-facets.It was found that the natural SiO₂ on the predefined wire pattern must be responsible for the degradation of the wire structure. Removing the SiO₂ layer from the Si wires ex situ with an HF dip preserves the rectangular structures during high-temperature annealing. The Si–SiO₂ interface was investigated with high-resolution transmission electron microscopy to image the Si wire surface and the natural oxide layer in detail.     

Coherent dynamics in InGaAs quantum dots and quantum dot molecules

We measure the dephasing time of the exciton ground state transition in InGaAs quantum dots (QD) and quantum dot molecules (QDM) using a sensitive four-wave mixing technique. In the QDs we find experimental evidence that the dephasing time is given only by the radiative lifetime at low temperatures. We demonstrate the tunability of the radiatively limited dephasing time from 400 ps up to 2 ns in a series of annealed QDs with increasing energy separation of 69–330 meV from the wetting layer continuum. Furthermore, the distribution of the fine-structure splitting δ₁ and of the biexciton binding energy δ_B is measured. δ₁ decreases from 96 to with increasing annealing temperature, indicating an improving circular symmetry of the in-plane confinement potential. The biexciton binding energy shows only a weak dependence on the confinement energy, which we attribute to a compensation between decreasing confinement and decreasing separation of electron and hole. In the QDM we measured the exciton dephasing as function of interdot barrier thickness in the temperature range from 5 to 60 K. At 5 K dephasing times of several hundred picoseconds are found. Moreover, a systematic dependence of the dephasing dynamics on the barrier thickness is observed, showing how the quantum mechanical coupling in the molecules affects the exciton lifetime and acoustic-phonon interaction.     

Optical properties of InAs quantum dots in a Si matrix

We report on the optical properties of nanoscale InAs quantum dots in a Si matrix. At a growth temperature of 400°C, the deposition of 7 ML InAs leads to the formation of coherent islands with dimensions in the 2–4 nm range with a high sheet density. Samples with such InAs quantum dots show a luminescence band in the 1.3 μm region for temperatures up to 170 K. The PL shows a pronounced blue shift with increasing excitation density and decays with a time constant of 440 ns. The optical properties suggest an indirect type II transition for the InAs/Si quantum dots. The electronic structure of InAs/Si QDs is discussed in view of available band offset information.     

Formation of InAs quantum dots and wetting layers in GaAs and AlAs analyzed by cross-sectional scanning tunneling microscopy

We have used cross-sectional scanning-tunneling microscopy (X-STM) to compare the formation of self-assembled InAs quantum dots (QDs) and wetting layers on AlAs (1 0 0) and GaAs (1 0 0) surfaces. On AlAs we find a larger QD density and smaller QD size than for QDs grown on GaAs under the same growth conditions (500 °C substrate temperature and 1.9 ML indium deposition). The QDs grown on GaAs show both a normal and a lateral gradient in the indium distribution whereas the QDs grown on AlAs show only a normal gradient. The wetting layers on GaAs and AlAs do not show significant differences in their composition profiles. We suggest that the segregation of the wetting layer is mainly strain-driven, whereas the formation of the QDs is also determined by growth kinetics. We have determined the indium composition of the QDs by fitting it to the measured outward relaxation and lattice constant profile of the cleaved surface using a three-dimensional finite element calculation based on elasticity theory.     

Structural, optical and intraband absorption properties of vertically aligned In0.32Ga0.68As/GaAs quantum dots superlattices

The self-organization growth of In_0.32Ga_0.68As/GaAs quantum dots (QDs) superlattices is investigated by molecular beam epitaxy. It is found that high growth temperature and low growth rate are favorable for the formation of perfect vertically aligned QDs superlattices. The aspect ratio (height versus diameter) of QD increases from 0.16 to 0.23 with increase number of bi-layer. We propose that this shape change play a significant role to improve the uniformity of QDs superlattices. Features in the variable temperature photoluminescence characteristics indicate the high uniformity of the QDs. Strong infrared absorption in the 8–12 μm was observed. Our results suggest the promising applications of QDs in normal sensitive infrared photodetectors.     

Luminescence properties of InAs quantum dots formed by a modified self-assembled method

The luminescence properties of self-assembled InAs quantum dots (QDs) on GaAs (1 0 0) substrates grown by molecular beam epitaxy have been investigated using temperature-dependent photoluminescence (PL) and time-resolved PL (TRPL). InAs QDs were grown using an In-interruption growth technique, in which the indium flux was periodically interrupted. InAs QDs grown using In-interruption showed reduced PL linewidth, redshifted PL emission energy, increased energy level spacing between the ground state and the first excited state, and reduced decay time, indicating an improvement in the size distribution and size/shape of QDs.