Growth conditions effects on optical properties of InAs quantum dots grown by molecular beam epitaxy on GaAs (1 1 3)A substrate

We have investigated the optical properties of InAs/GaAs (1 1 3)A quantum dots grown by molecular beam epitaxy (MBE) with different growth rates by photoluminescence spectroscopy (PL) as a function of the excitation density and the sample temperature (10–300 K). Reflection high-energy electron diffraction (RHEED) is used to investigate the formation process of InAs quantum dots (QDs). A redshift of the InAs QDs PL band emission was observed when the growth rate was increased. This result was explained by the increase of the InAs quantum dot size with increasing growth rate. A significant redshift was observed when the arsenic flux was decreased. The evolution of the PL peak energy with increasing temperature has showed an S-shaped form due to the localization effects and is attributed to the efficient relaxation process of carriers in different InAs quantum dots and to the exciton transfer localized at the wetting layer.     

Effects of growth conditions on the formation of self-assembled InAs quantum dots grown on (1 1 5)A GaAs substrate

Effects of growth conditions on the formation of InAs quantum dots (QDs) grown on GaAs (1 1 5)A substrate were investigated by using the reflection high-energy electron diffraction (RHEED) and photoluminescence spectroscopy (PL). An anomalous evolution of wetting layer was observed when increasing the As/In flux ratio. This is attributed to a change in the surface reconstruction. PL measurements show that QDs emission was strongly affected by the InAs deposited amount. No obvious signature of PL emission QDs appears for sample with 2.2 ML InAs coverage. Furthermore, carrier tunneling from the dots to the non-radiative centers via the inclination continuum band is found to be the dominant mechanism for the InAs amount deposition up to 4.2 MLs.     

Improvement of the optical property and uniformity of self-assembled InAs/InGaAs quantum dots by layer-by-layer temperature and substrate rotation

The influence of layer-by-layer temperature and substrate rotation on the optical property and uniformity of self-assembled InAs/In_0.2Ga_0.8As/GaAs quantum dots (QDs) gown with an As₂ source was investigated. An improvement in the optical property of QDs was obtained by the precise control and optimization of growth temperature utilized for each layer, i.e., InAs QDs, InGaAs quantum wells, GaAs barriers and AlGaAs layers, respectively. By using a substrate rotation, the QD density increased from ∼1.4×10¹⁰ to ∼3.2×10¹⁰ cm⁻² and its size also slightly increased, indicating a good quality of QDs. It is found that the use of an appropriate substrate rotation during growth improves the room-temperature (RT) optical property and uniformity of QDs across the wafer. For the QD sample with a substrate rotation of 6 rpm, the RT photoluminescence (PL) intensity is much higher and the standard deviation of RT-PL full-width at half-maximum is decreased by 35% compared to that grown without substrate rotation.     

Heteroepitaxial growth of thin InAs layers on GaAs(1 0 0) misoriented substrates: A structural and morphological comparison

Thin InAs epilayers were grown on GaAs(1 0 0) substrates exactly oriented and misoriented toward [1 1 1]A direction by atmospheric pressure metalorganic vapor phase epitaxy. InAs growth was monitored by in situ spectral reflectivity. Structural quality of InAs layers were studied by using high-resolution X-ray diffraction. No crystallographic tilting of the layers with respect to any kind of these substrates was found for all thicknesses. This result is discussed in terms of In-rich growth environment. InAs layers grown on 2° misoriented substrate provide an improved crystalline quality. Surface roughness of InAs layers depend on layer thickness and substrate misorientation.     

Cadmium sulfide quantum dots stabilized by castor oil and ricinoleic acid

Castor oil and ricinoleic acid (an isolate of castor oil) are environmentally friendly bio-based organic surfactants that have been used as capping agents to prepare nearly spherical cadmium sulfide quantum dots (QDs) at 230, 250 and 280 °C. The prepared quantum dots were characterized by Ultra violet–visible (UV–vis), Photoluminescence (PL), Transmission Electron Microscopy (TEM), High Resolution Transmission Electron Microscopy (HRTEM) and X-ray diffraction (XRD) giving an overall CdS QDs average size of 5.14±0.39 nm. The broad XRD pattern and crystal lattice fringes in the HRTEM images showed a hexagonal phase composition of the CdS QDs. The calculated/estimated average size of the prepared castor oil capped CdS QDs for various techniques were 4.64 nm (TEM), 4.65 nm (EMA), 5.35 nm (UV–vis) and 6.46 nm (XRD). For ricinoleic acid capped CdS QDs, the average sizes were 5.56 nm (TEM), 4.78 nm (EMA), 5.52 nm (UV–vis) and 8.21 nm (XRD). Optical properties of CdS QDs showed a change of band gap energy from its bulk band gap of 2.42–2.82 eV due to quantum size confinement effect for temperature range of 230–280 °C. Similarly, a blue shift was observed in the photoluminescence spectra. Scanning electron microscope (SEM) observations show that the as-synthesized CdS QDs structures are spherical in shape. Fourier transform infra-red (FTIR) studies confirms the formation of castor oil and ricinoleic acid capped CdS QDs.     

Competing nucleation mechanisms and growth of InAsSbP quantum dots and nano-pits on the InAs(100) surface

InAsSbP quantum dots (QDs) and nano-pits (NPs) are grown on a InAs(100) surface by liquid phase epitaxy (LPE). Their morphology, dimensions and distribution density are investigated by high resolution scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray diffraction and total energy calculations. QDs average density ranges from 5 to 7 × 10⁹ cm^?2, with heights and widths having a Gaussian distribution with sizes from 5 nm to 15 nm and 10 nm to 40 nm respectively. The average pits density is (2–6) × 10¹⁰ cm^?2 with dimensions ranging from 5–30 nm in width and depth. We also find a shift in the absorption edge towards the longer wavelengths together with broadening towards shorter wavelengths indicating that these QDs and lateral overgrown nano-pits are grown at the n-InAs/p-InAsSbP heterojunction interface. Together with total energy calculations, the results indicate that lattice mismatch ratio plays a central role in the growth of these strain-induced nano-objects.     

Physical reasons of emission transformation in infrared CdSeTe/ZnS quantum dots at bioconjugation

The core/shell CdSeTe/ZnS quantum dots (QDs) with emission at 780–800 nm (1.55–1.60 eV) have been studied by means of photoluminescence (PL) and Raman scattering methods in the nonconjugated state and after conjugation to different antibodies (Ab): (i) mouse monoclonal [8C9] human papilloma virus Ab, anti-HPV 16-E7 Ab, (ii) mouse monoclonal [C1P5] human papilloma virus HPV16 E6+HPV18 E6 Ab, and (iii) pseudo rabies virus (PRV) Ab. The transformations of PL and Raman scattering spectra of QDs, stimulated by conjugated antibodies, have been revealed and discussed.The energy band diagram of core/shell CdSeTe/ZnS QDs has been designed that helps to analyze the PL spectra and their transformations at the bioconjugation. It is shown that the core in CdSeTe/ZnS QDs is complex and including the type II quantum well. The last fact permits to explain the nature of infrared (IR) optical transitions (1.55–1.60 eV) and the high energy PL band (1.88–1.94 eV) in the nonconjugated and bioconjugated QDs. A set of physical reasons has been analyzed with the aim to explain the transformation of PL spectra in bioconjugated QDs. Finally it is shown that two factors are responsible for the PL spectrum transformation at bioconjugation to charged antibodies: (i) the change of energy band profile in QDs and (ii) the shift of QD energy levels in the strong quantum confinement case. The effect of PL spectrum transformation is useful for the study of QD bioconjugation to specific antibodies and can be a powerful technique for early medical diagnostics.     

Temperature-dependent photoluminescence of CuInS2 quantum dots

Temperature-dependent photoluminescence (PL) spectroscopy of CuInS₂ core and CuInS₂/ZnS core–shell quantum dots (QDs) was studied for understanding the influence of a ZnS shell on the PL mechanism. The PL quantum yield and lifetime of CuInS₂ core QDs were significantly enhanced after the QD surface was coated with the ZnS shell. The temperature dependences of the PL energy, linewidth, and intensity for the core and core–shell QDs were studied in the temperature range from 92 to 287 K. The temperature-dependent shifts of 98 meV and 35 meV for the PL energies of the QDs were much larger than those of the excitons in their bulk semiconductors. It was surprisingly found that the core and core–shell QDs exhibited a similar temperature dependence of the PL intensity. The PL in the CuInS₂/ZnS core–shell QDs was suggested to originate from recombination of many kinds of defect-related emission centers in the interior of the cores.     

InAs/GaNAs strain-compensated quantum dots stacked up to 50 layers for use in high-efficiency solar cell

We have investigated the effect of strain compensation on the structural and optical properties of multiple stacked InAs quantum dots (QDs) on GaAs (0 0 1) substrates grown by atomic hydrogen-assisted RF-MBE. Strain relaxation was not observed from the reciprocal space mapping, and as a result, dislocations and coalesced islands were not observed in 50 layer-stacked QDs. Thus, the total QD density of as high as 2.5×10¹² cm⁻² was achieved. For QD solar cell characterization, the short-circuit current density increased from 21.0 to 26.4 mA/cm² as the number of stacks was increased from 20 to 50. Further increase of stacks did not affect the open-circuit voltage of ∼0.7 V and diode factor of ∼1.6, which implies that high crystalline quality was maintained even after 50 layers of stacking.     

Quantum dot p-i-n structure in an electric field

Time-resolved photoluminescence (PL), steady-state PL, and electroluminescence (EL) techniques have been used to characterize the carrier relaxation processes and carrier escape mechanisms in self-assembled InAs/GaAs quantum dot (SAQD) p-i-n structures under reverse bias. The measurements were performed between 5 K and room temperature on a ring mesa sample as a function of bias. At 100 K, the PL decay time originating from the n  =  1 SAQD decreases with increasing reverse bias from ∼3 ns under flat band condition to∼ 400 ps for a bias of −3 V. The data can be explained by a simple model based on electron recombination in the quantum dots (QDs) or escape out of the dots. The escape can occur by one of three possible routes: direct tunneling out of the distribution of excited electronic levels, thermally assisted tunneling of ground state electrons through the upper excited electronic states or thermionic emission to the wetting layer.     

Electronic energy alignment at the PbSe quantum dots/ZnO(101̅0) interface

A number of solar energy conversion strategies depend on exciton dissociation across interfaces between semiconductor quantum dots (QDs) and other electron or hole conducting materials. A critical factor governing exciton dissociation and charge transfer in these systems is the alignment of electronic energy levels across the interface. We probe interfacial electronic energy alignment in a model system, sub-monolayer films of PbSe QDs adsorbed on single crystal ZnO(101?0) surfaces using ultraviolet photoemission spectroscopy. We establish electronic energy alignment as a function of quantum dot size and surface chemistry. We find that replacing insulating oleic-acid capping molecules on the QDs by the short hydrazine or ethanedithiol molecules results in pinning of the valence band maximum (VBM) of QDs to ZnO substrate states, independent of QD size. This is in contrast to similar measurements on TiO₂(110) where the alignment of the PbSe QD VBM to that of the TiO₂ substrate depends on QD size. We interpret these findings as indicative of strong electronic coupling of QDs with the ZnO surface but less with the TiO₂ surface. Based on the measured energy alignment, we predict that electron injection from the 1s_e level in photo-excited PbSe QDs to ZnO can occur with small QDs (diameter ? = 3.4 nm), but energetically unfavorably for larger dots (? = 6.7 nm). In the latter, hot electrons above the 1s_e level are necessary for interfacial electron injection.     

Optical investigation of InAs/InP(1 0 0) quantum dots grown by gas source molecular beam epitaxy

We report on the optical characteristics of InAs quantum dots based on the InP(1 0 0) substrate grown by gas source molecular beam epitaxy without assisting any other methods. The photoluminescence was carefully investigated by adjusting the thickness of InAs layers and the growth temperature. A wide range of emitting peaks is obtained with the increase in the thickness of InAs layers. In addition, we find that the morphology and shape of quantum dots also greatly depend on InAs layers. The images of atomic force microscopy show that the quantum dots like forming into quantum dashes elongated along the [0 1 ?1] direction when the thickness of InAs layers increased. A critical thickness of formation quantum dots or quantum dash is obtained. At the same time, we observe that the growth temperature also has a great impact on the emission wavelength peaks. High qualities of InAs/InP(1 0 0) quantum dots providing their emission wavelength in 1.55 μm are obtained, and good performances of quantum dots lasers are fabricated.     

Thermal annealing of GaSb quantum dots in GaAs formed by droplet epitaxy

We investigate effects of annealing on GaSb quantum dots (QDs) formed by droplet epitaxy. Ga droplets grown on GaAs are exposed to Sb molecular beam and then annealed at T_a=340–450 °C for 1 min to form GaSb QDs. An atomic force microscope study shows that with the increase of T_a, the average diameter of dots increases by about 60%, while their density decreases to about 1/3. The photoluminescence (PL) of GaSb QDs is observed at around 1 eV only for those samples annealed above T_a=380 °C, which indicates that the annealing process plays an important role in forming high quality GaSb QDs.     

Influence of growth temperature and deposition duration on the structure,surface morphology and optical properties of InN/YSZ (1 0 0)

InN films with the wurtzite structure have been grown directly on YSZ (1 0 0) substrate by the RF-magnetron sputtering technique. Strongly (0 0 2) oriented films with smooth surfaces (0.7–2.9 nm surface roughness depending on substrate temperature), were grown within 30 min. Films deposited for 60 min developed three-dimensional (3D) pyramidal islands on top of their surfaces, which diminished the residual elastic strain. The optical absorption edge and PL peak energy around 1.7 eV were found to redshift with increasing film thickness and substrate temperature.     

Formation of InAs quantum dots at ultrahigh growth rates

We fabricated quantum dot (QD) structures at ultrahigh growth rates. Smaller fluctuations in QD size were observed when they were grown at a rate of 1.0 ML/s under conventional growth conditions (growth temperature of 500 °C and As₄ flux of 9×10⁻⁶ Torr). For QDs grown at high rates, growth interruption played an important role in the fabrication of QD structures; this was confirmed by carrying out reflection high-energy electron diffraction. Photoluminescence for QDs grown at high and low growth rates, with growth interruption and with low-temperature capping was observed at around 1250 nm at room temperature, indicating that high-quality QDs can be fabricated by employing high growth rates.     

Tailoring of the Wave Function Overlaps and the Carrier Lifetimes in InAs/GaAs1−xSbx Type-II Quantum Dots

Effects of thermal annealing on the emission properties of type-II InAs quantum dots (QDs) covered by a thin GaAs_1−xSb_x layer are investigated by photoluminescence (PL) and time-resolved PL measurements. Apart from large blueshifts and a pronounced narrowing of the QD emission peak, the annealing induced alloy intermixing also leads to enhanced radiative recombination rates and reduced localized states in the GaAs_1−xSb_x layer. We find that the type-II QD structure can sustain thermal annealing up to 850 °C. In particular, we find that it is possible to manipulate between type-I and type-II recombinations in annealed QDs by using different excitation powers. We demonstrate that postgrowth thermal annealing can be used to tailor the band alignment, the wave function overlaps, and hence the recombination dynamics in the InAs/GaAs_1−xSb_x type-II QDs.     

The effect of spacer layer thickness on vertical alignment of InGaAs/GaNAs quantum dots grown on GaAs(3 1 1)B substrate

We fabricated multiple stacked self-organized InGaAs quantum dots (QDs) on GaAs (3 1 1)B substrate by atomic hydrogen-assisted molecular beam epitaxy (H-MBE) to realize an ordered three-dimensional QD array. High quality stacked QDs with good size uniformity were achieved by using strain-compensation growth technique, in which each In_0.35Ga_0.65As QD layer was embedded by GaNAs strain-compensation layer (SCL). In order to investigate the effect of spacer layer thickness on vertical alignment of InGaAs/GaNAs QDs, the thickness of GaNAs SCL was varied from 40 to 20 nm. We observed that QDs were vertically aligned in [3 1 1] direction when viewed along [0 1 −1], while the alignment was inclined when viewed along [−2 3 3] for all samples with different SCL thickness. This is due to their asymmetric shape along [−2 3 3] with two different dominant facets thereby the local strain field around QD extends further outward from the lower-angle facet. Furthermore, the inclination angle of vertical alignment QDs became monotonously smaller from 22° to 2° with decreasing SCL thickness from 40 to 20 nm. These results suggest that the strain field extends asymmetrically resulting in vertically tilted alignment of QDs for samples with thick SCLs, while the propagated local strain field is strong enough to generate the nucleation site of QD formation just above lower QD in the sample with thinner SCLs.     

Near-infrared photoluminescence and thermally stimulated current in Cu3Ga5Se9 layered crystals: A comparative study

Near-infrared photoluminescence (PL) and thermally stimulated current (TSC) spectra of Cu₃Ga₅Se₉ layered crystals grown by Bridgman method have been studied in the photon energy region of 1.35–1.46 eV and the temperature range of 15–115 K (PL) and 10–170 K (TSC). An infrared PL band centered at 1.42 eV was revealed at T = 15 K. Radiative transitions from shallow donor level placed at 20 meV to moderately deep acceptor level at 310 meV were suggested to be the reason of the observed PL band. TSC curve of Cu₃Ga₅Se₉ crystal exhibited one broad peak at nearly 88 K. The thermal activation energy of traps was found to be 22 meV. An energy level diagram demonstrating the transitions in the crystal band gap was plotted taking account of results of PL and TSC experiments conducted below room temperature.     

Re-charging the luminescence states in CdSe/ZnS quantum dots at the conjugation to Osteopontin antibodies

The paper presents the original study of photoluminescence (PL) and Raman scattering spectra of core–shell CdSe/ZnS quantum dots (QDs) covered by the amine-derivatized polyethylene glycol (PEG) with luminescence interface states. First commercially available CdSe/ZnS QDs with emission at 640 nm (1.94 eV) covered by PEG polymer have been studied in nonconjugated states. PL spectra of nonconjugated QDs are characterized by a superposition of PL bands related to exciton emission in a CdSe core and to the hot electron–hole recombination via high energy luminescence states. The study of high energy PL bands in QDs at different temperatures has shown that these PL bands are related to luminescence interface states at the CdSe/ZnS or ZnS/polymer interface. Then CdSe/ZnS QDs have been conjugated with biomolecules—the Osteopontin antibodies. It is revealed that the PL spectrum of bioconjugated QDs changed essentially with decreasing hot electron–hole recombination flow via luminescence interface states. It is shown that the QD bioconjugation process to Osteopontin antibodies is complex and includes the covalent and electrostatic interactions between them. The variation of PL spectra due to the bioconjugation is explained on the basis of electrostatic interaction between the QDs and biomolecule dipoles that stimulates re-charging QD interface states. The study of Raman scattering of bioconjugated CdSe/ZnS QDs has confirmed that the antibody molecules have the electric dipoles. It is shown that CdSe/ZnS QDs with luminescence interface states are promising for the study of bioconjugation effects with specific antibodies and can be a powerful technique in biology and medicine.     

Structural and optical properties of InxGa1−xAs strained layers grown on GaAs substrates by MOVPE

In_xGa_1−xAs/GaAs pseudomorphic structures were grown by metalorganic vapor phase epitaxy. Reciprocal space mapping were recorded in the vicinity of (0 0 4) and (1 1 5) nodes using high resolution X-ray diffraction (HRXRD) in order to determine strain tensor components, indium compositions and thicknesses of alloys. Near-infrared photoluminescence (PL) was performed at 10 K. The impact of strain on PL response was revealed by peak energy positions and line width. In addition, valence-band splitting (VBS) and the shift of the heavy-hole were measured. Besides, photoreflectance (PR) at room temperature was useful to establish experimentally the dependence of VBS and band energy shifts (E₀ and E₀+∆₀) on elastic strain due to lattice mismatches. Other parameters such as the internal electric-field and the electro-optical energy were determined from Franz–Keldysh oscillations analysis. Good correlation between the results obtained from all investigated techniques and theoretical predictions was confirmed.