Sb/As intermixing in self-assembled GaSb/GaAs type II quantum dot systems and control of their photoluminescence spectra

The intermixing of Sb and As atoms induced by rapid thermal annealing (RTA) was investigated for type II GaSb/GaAs self-assembled quantum dots (QD) formed by molecular beam epitaxy growth. Just as in InAs/GaAs QD systems, the intermixing induces a remarkable blueshift of the photoluminescence (PL) peak of QDs and reduces the inhomogeneous broadening of PL peaks for both QD ensemble and wetting layer (WL) as consequences of the weakening of quantum confinement. Contrary to InAs/GaAs QDs systems, however, the intermixing has led to a pronounced exponential increase in PL intensity for GaSb QDs with annealing temperature up to 875 °C. By analyzing the temperature dependence of PL for QDs annealed at 700, 750 and 800 °C, activation energies of PL quenching from QDs at high temperatures are 176.4, 146 and 73.9 meV. The decrease of QD activation energy with annealing temperatures indicates the reduction of hole localization energy in type II QDs due to the Sb/As intermixing. The activation energy for the WL PL was found to drastically decrease when annealed at 800 °C where the QD PL intensity surpassed WL.     

温度对GaSb/GaAs量子点尺寸分布的影响

采用低压金属有机物化学气相沉积 (LP-MOCVD) 法制备GaSb/GaAs量子点。通过对不同生长温度的样品进行分析发现温度的变化对GaSb/GaAs量子点的相位角无明显影响,量子点的形状是透镜型。由于量子点特殊的应力分布,可实现量子点的"自限制"生长。量子点的化学势不连续性以及Ostwald熟化机制的影响使得量子点尺寸分布在一定范围内不连续,会出现两种尺寸模式的量子点生长。Sb原子的表面迁移率对GaSb/GaAs量子点生长有较大的影响。升高温度可有效改善量子点的分立性,在升温过程中量子点体现出其熟化过程,高温时表面原子的解析附作用对量子点尺寸和密度的影响较大。     

Photoluminescence and magneto-optical properties of multilayered type-II ZnTe/ZnSe quantum dots

Multilayered Zn–Se–Te structures grown by migration enhanced epitaxy are studied by temperature- and excitation-dependent photoluminescence (PL) as well as magneto-PL. The PL consists of two bands: a blue band, overlaid with band edge sharp lines, dominant at low temperatures and high excitation, and a green band, which appears at elevated temperature and low excitation. Upon varying excitation intensity by four orders of magnitude, the green band peak energy shifts by ∼60 meV, indicating recombination of excitons in type-II quantum dots (QDs); no significant shift is observed for the blue band. Therefore, the green emission is attributed to ZnTe/ZnSe type-II QDs, which co-exist with isoelectronic centers, responsible for the blue and band edge emissions. The existence of type-II ZnTe/ZnSe QDs is further confirmed by magneto-PL, for which the observed oscillations in the PL intensity as a function of magnetic field is explained in terms of the optical Aharonov–Bohm effect.     

Growth of high-density InGaSb quantum dots on silicon atoms irradiated GaAs substrates

We discuss a technique that allows us to grow high-density GaSb and InGaSb quantum dots (QDs) on (0 0 1)-oriented GaAs substrates. We study the use of Si atom irradiation on the substrate surface as an anti-surfactant before the QDs fabrication. It is clear that the densities of GaSb and InGaSb QDs are drastically enhanced with the Si atom irradiation. Photoluminescence intensities from these QDs are also increased with the Si atom irradiation. These results indicate that the Si atom irradiation technique is useful to improve the properties of the Sb-based QDs.     

InAs/GaAs单量子点中电子/空穴自旋弛豫

利用分子束外延制备了三种类型量子点样品,它们分别是:未掺杂样品、n型Si调制掺杂样品和p型Be调制掺杂样品。在5 K温度下,采用共聚焦显微镜系统,测量了单量子点的光致发光谱和时间分辨光谱, 研究了单量子点中三种类型激子(本征激子、负电荷激子和正电荷激子)的电子/空穴自旋翻转时间。它们的自旋翻转时间常数分别为: 本征激子的自旋翻转时间约16 ns, 正电荷激子中电子的自旋翻转时间约2 ns, 负电荷激子中空穴的自旋翻转时间约50 ps。     

Excitation transfer in novel self-organized quantum dot structures

We report on studies of excitation transfer processes in vertically self-organized pairs of unequal-sized quantum dots (QDs), created in InAs/GaAs bilayers having differing InAs deposition amounts in the first (seed) and subsequent layer. The former and latter enable independent control, respectively, of the density and the size distribution of the second layer QDs. This approach allows us to enhance the average volume and improve the uniformity of InAs QDs, resulting in low-temperature photoluminescence at 1.028 eV with a linewidth of 25 meV for 1.74 ML (seed)/3.00 ML InAs stacking. The optical properties of the formed pairs of unequal-sized QDs with clearly discernible ground-state transition energy depend on the spacer thickness and composition. Photoluminescence results provide evidence for nonresonant energy transfer from the smaller QDs in the seed layer to the larger QDs in the second layer in such asymmetric QD pairs. Transfer times down to 20 ps (36 ML GaAs spacer) are estimated, depending exponentially on the GaAs spacer thickness.     

GaAs间隔层厚度对InAs/GaAs量子点分子光学性质的影响

采用光致荧光发射谱(PL)和时间分辨荧光发射谱(TRPL)研究了GaAs间隔层厚度对自组装生长的双层InAs/GaAs量子点分子光学性质的影响.首先,测量低温下改变激发强度的PL谱,底层量子点和顶层量子点的PL强度比值随激发强度发生变化,表明两层量子点之间的耦合作用和层间载流子的转移随着间隔层厚度变大而变弱.接着测量改变温度的PL谱,量子点荧光光谱峰值位置(Emax)、半峰全宽及积分强度随温度发生变化,表明GaAs间隔层厚度直接影响到量子点内载流子的动力学过程和量子点发光的热淬灭过程.最后,TRPL测量发现60mL比40mL间隔层厚度样品的载流子隧穿时间有明显延长.     

Ground state energy of the electron-hole liquid in type-II (GaAs)m/(AlAs)m quantum wells

The ground state energy of quasi-two-dimensional electron-hole liquid (EHL) at zero temperature is calculated for type-II (GaAs)_m/(AlAs)_m (5≤m≤10) quantum wells (QWs). The correlation effects of Coulomb interaction are taken into account by a random phase approximation of Hubbard. Our EHL ground state energy per electron-hole pair is lower than the exciton energy calculated recently for superlattices, so we expected that EHL is more stable state than excitons at high excitation density. It is also demonstrated that the equilibrium density of EHL in type-II GaAs/AlAs QWs is of one order of magnitude larger than that in type-I GaAs/AlAs QWs.     

Phonon-assisted polar exciton–transitions in self-organized InAs/GaAs quantum dots

Phonon-assisted exciton transitions are investigated for self-organized InAs/GaAs quantum dots (QDs) using selectively excited photoluminescence (PL) and PL excitation spectroscopy. The results unambiguously demonstrate intrinsic recombination in the coherent InAs/GaAs QDs and the absence of a Stokes shift between ground state absorption and emission. Phonon-sidebands corresponding to a phonon energy of 34 meV are resolved and Huang–Rhys parameters of 0.015 and 0.08 are found for phonon-assisted emission and absorption, respectively, which are about one order of magnitude larger than in bulk InAs. Calculations of the exciton–LO–phonon interaction based on an adiabatic approximation and realistic wave functions for ideal pyramidal InAs/GaAs QDs show this enhanced polar coupling to result from the particular confinement and the strain-induced piezoelectric potential in such strained low-symmetry QDs.     

Enhancement of the Coulomb correlations in type-II quantum dots

We report on calculation of binding energies of excitons as well as positively and negatively charged excitons and biexcitons in type-II quantum dots. The shape of the GaSb/GaAs quantum dot is assumed lens-like and the energies are calculated within the Hartree–Fock approximation. A large enhancement of the binding energies has been estimated in comparison with the type-I quantum dots (InAs/GaAs) which is in good agreement with the recent experimental findings.     

Effects of Si-doped GaAs layer on optical properties of InAs quantum dots

We have investigated the optical properties of InAs self-assembled quantum dots (SAQDs) with the Si-doped GaAs barrier layer. Two types of samples are fabricated according to the position of the Si-doped GaAs layer. For type A samples the Si-doped GaAs layer is grown below the QDs, whereas for type B samples the Si-doped GaAs layer is grown above the QDs. For both types of samples the excited-state emissions caused by state filling are observed in photoluminescence (PL) spectra at high excitation power densities. The bandgap renormalization of QDs can be found from the shift of the PL peak energy. Particularly, for type A samples the Si atoms act as nucleation centers during the growth of InAs QDs on the Si-doped GaAs layer and affect the density and the size of the QDs. The Si-doped GaAs layer in type A samples has more effects on the properties of QDs, such as state filling and bandgap renormalization than those of type B samples.     

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.     

Effects of p-type doping on the optical properties of InAs/GaAs quantum dots

The effects of p-type doping on the optical properties of self-organized InAs/GaAs quantum dots (QDs) were investigated by both micro-photoluminescence and degenerated pump–probe reflection measurements. As compared to undoped InAs/GaAs QDs, it was observed that the transitions between the ground and the first excited states of electrons and holes levels appeared at higher energies for p-doped InAs/GaAs QDs. In addition, the PL intensities for both undoped and p-doped QDs were found to decrease when the excitation power exceeded a critical value. The critical excitation power for p-doped QDs appeared to be much lower than that for undoped ones. In the pump–probe experiments, it was revealed that the value and sign of the differential reflectivity depends strongly on excitation wavelength. P-doped QDs exhibited a response behavior that is different from that of undoped ones. It is believed that the large build-in population of holes plays a crucial role in determining the transient reflection spectrum.     

Observation of monolayer-splitting for InAs/GaAs quantum dots

A pronounced modulation is observed in the photoluminescence (PL) spectrum of self-organized InAs/GaAs quantum dots (QDs), recorded at low excitation densities. The clearly distinguishable peaks are identified as a multimodal distribution of the ground state transition energy, originating from a discrete, stepwise variation of the structural properties of the QDs, which is associated with an increase of the QD height in monolayer (ML) steps. The observation of a ML splitting implies a flat QD shape with well-defined upper and lower interfaces as well as negligible indium segregation. The electronic properties of the InAs/GaAs QDs were investigated by PL and PL-excitation spectroscopy and are discussed based on realistic calculations for flat InAs/GaAs QDs with a truncated pyramidal shape based on an extended 8-band k·p model. The calculations predict a red shift of the ground state transition with each additional ML, which saturates for heights above 9 ML, is in good agreement with experiment.     

亚单层InGaAs量子点-量子阱异质结构的时间分辨光致发光谱

测定了亚单层InGaAs/GaAs量子点-量子阱异质结构在5K下的时间分辨光致发光谱.亚单层量 子点的辐射寿命在500 ps 至 800 ps之间，随量子点尺寸的增大而增大，与量子点中激子的 较小的横向限制能以及激子从小量子点向大量子点的隧穿转移有关.光致发光上升时间强烈 依赖于激发强度密度.在弱激发强度密度下，上升时间为 35 ps，纵光学声子发射为主要的 载流子俘获机理.在强激发强度密度下，上升时间随激发强度密度的增加而减小，俄歇过程 为主要的载流子俘获机理.该结果对理解亚单层量子点器件的工作特性非常有用. 关键词： 亚单层 量子点-量子阱 时间分辨光致发光谱     

Quantum-Statistics Behavior of the Exciton-Biexciton System In GaAs/AlAs Type-II Superlattices

We have investigated the quantum-statistics behavior of the exciton-biexciton system from the photoluminescence properties in (GaAs) m /(AlAs) m type-II superlattices with m = 12 and 13 monolayers, where the lowest-energy type-II exciton consists of the n = 1 X electron of AlAs and n = 1 o heavy hole of GaAs. The long exciton lifetime of the order of w s due to the indirect transition nature enables us to obtain precisely the density relation between the exciton and biexciton from the line-shape analysis of time-resolved photoluminescence spectra. In a relatively low exciton-density region, the biexciton density obeys a well-known square law. At an exciton density around 1 2 10 10 cm m 2 , the biexciton density suddenly increases with a threshold-like nature. This behavior, which is realized at a bath temperature up to 8 K under an excitation power of the order of 100 mW/cm 2 , results from the characteristics of Bose-Einstein statistics of the exciton-biexciton system.     

Magneto-optical single dot spectroscopy of GaSb/GaAs type II quantum dots

We have investigated magneto-optical properties of GaSb/GaAs self-assemble type II quantum dots by single dot spectroscopy in magnetic field. We have observed clear Zeeman splitting and diamagnetic shift of GaSb/GaAs quantum dots. The diamagnetic coefficient ranges from 5 to 30 μeV/T². The large coefficient and their large distribution are attributed to the size inhomogeneity and electron localization outside the dot. The g-factor of GaSb/GaAs quantum dots is slightly larger than that of similar type I InGaAs/GaAs quantum dots. In addition, we find almost linear relationship between the diamagnetic coefficient and the g-factor. The linear increase of g-factor with diamagnetic coefficient is due to an increase of spin-orbit interaction with dot size.     

Influence of nanomechanical force on the electronic structure of InAs/GaAs quantum dots

We show nanomechanical force is useful to dynamically control the optical response of self-assembled quantum dots, giving a method to shift electron and heavy hole levels, interval of electron and heavy hole energy levels, and the emission wavelength of quantum dots (QDs). The strain, the electron energy levels, and heavy hole energy levels of InAs/GaAs(001) quantum dots with vertical nanomechanical force are investigated. Both the lattice mismatch and nanomechanical force are considered at the same time. The results show that the hydrostatic and the biaxial strains inside the QDs subjected to nanomechanical force vary with nanomechanical force. That gives the control for tailoring band gaps and optical response. Moreover, due to strain-modified energy, the band edge is also influenced by nanomechanical force. The nanomechanical force is shown to influence the band edge. As is well known, the band offset affects the electronic structure, which shows that the nanomechanical force is proven to be useful to tailor the emission wavelength of QDs. Our research helps to better understand how the nanomechanical force can be used to dynamically control the optics of quantum dots.     

First-principles study of interface relaxation effect on interface and electronic structures of InAs/GaSb superlattices with different interface types

We have implemented first-principles relativistic pseudopotential calculations within general gradient approximation to investigate the structural and electronic properties of quaternary InAs/GaSb superlattices with an InSb or GaAs type of interface. Because of the complexity and low symmetry of the quaternary interfaces, the interface energy and strain in the InAs/GaSb superlattice system have been calculated to determine the equilibrium interface structural parameters. The band structures of InAs/GaSb superlattices with InSb and GaAs interfaces have been calculated with respect to the lattice constant and atomic position relaxations of the superlattice interfaces. The calculation of the relativistic Hartree–Fock pseudopotential in local density approximation has also been performed to verify the calculated band structure results that have been predicted in other empirical theories. The calculated band structures of InAs/GaSb superlattices with different types of interface (InSb or GaAs) have been systematically compared. We find that the virtual–crystal approximation fails to properly describe the quaternary InAs/GaSb superlattice system, and the chemical bonding and ionicity of anion atoms are essential in determining the interface and electronic structures of InAs/GaSb superlattice system.     

The studies of Ge quantum dots on strained Si0.7Ge0.3 layer by photoluminescence and deep level transient spectroscopy

Systematic studies of Ge quantum dots (QDs) grown on strained Si_0.3Ge_0.7 layer have been carried out by photoluminescence (PL) and deep level transient spectroscopy (DLTS). In PL measurements, two peaks around 0.7 eV are distinguished, which are assigned to two types of QDs observed by atomic force microscopy (AFM). Large blueshifts of the PL peaks from small QDs with the increase of excitation power are observed and attributed to the band bending effects typical for type-II band alignment. From DLTS measurements, the energy levels of holes in both types of QDs are derived, which shift with the change of the number of holes in QDs due to their charge energy. By comparing results from PL and DLTS measurements, further understanding of band alignment with the increase of the number of excitons in QDs is deduced.