Temperature dependent time-resolved exciton luminescence in GaAs/AlGaAs quantum wires and dots

Transient photoluminescence of GaAs/AlGaAs quantum wires and quantum dots formed by strain confinement is studied as a function of temperature. At low temperature, luminescent decay times of the wires and dots correspond to the radiative decay times of localized excitons. The radiative decay time can be either longer or shorter than that of the host quantum well, depending on the size of the wires and dots. For small wires and dots (∼ 100 nm stressor), the exciton radiative recombination rate increases due to lateral confinement. Exciton localization due to the fluctuation of quantum well thickness plays an important role in the temperature dependence of luminescent decay time and exciton transfer in quantum wire and dot structures up to at least ∼ 80 K. Lateral exciton transfer in quantum wire and dot structures formed by laterally patterning quantum wells strongly affects the dynamics of wire and dot luminescence. The relaxation time of hot excitons increases with the depth of strain confinement, but we find no convincing evidence that it is significantly slower in quasi 1-D or 0-D systems than in quantum wells.     

Non-exponential decay kinetics: correct assessment and description illustrated by slow luminescence of Si nanostructures

The treatment of time-resolved (TR) photoluminescence (PL) decay kinetics is analysed in details and illustrated by experiments on semiconductor quantum dots, namely silicon nanocrystals (Si NCs). We consider the mono-, stretch- and multi-exponential as well as lognormal (LN) and some complex decay models for continuous and discrete distribution of rates (lifetimes). A particular attention is devoted to the thorough analysis of non-exponential decay kinetics. We explicitly show that a LN distribution of emitter sizes may results in LN distribution of decay rates. On the other hand, the distribution of rates cannot be, strictly speaking, Levy stable distribution (that results in the stretched-exponential decay). We introduce theoretical background and derive expressions to calculate the average decay lifetimes for some common decays with practical examples of their applications. Experimental aspects are discussed with special attention devoted to the major problems of the accurate TR PL data treatment, including background uncertainty, pulse duration, system response function etc. Finally, a thorough literature survey of TR PL in Si NCs is given. The methods and definitions outlined in this systematic review are applicable to various other material systems with slow decay like rare-earth and transition metal-doped materials, amorphous semiconductors, type-II heterostructures, singlet oxygen phosphorescence etc.     

半导体中的自旋弛豫——从体材料到量子阱、量子线、量子点

本文对半导体中的自旋弛豫过程给出一个简要的回顾,介绍了半导体材料从体材料到量子阱、量子线、量子点不同维数的结构中各种自旋弛豫过程,主要关注了自旋去相位和相干控制。对于不同材料中的各种弛豫机制,关注的重点在于如何能够在实验上以一种可以控制的方式来改变可调参数从而达到控制自旋弛豫过程。这些参数主要有电场、磁场、温度、应变、有效g因子等等。本文的组织上,首先介绍研究前景,第1部分简要介绍了自旋弛豫的四种机制。第2部分按照维数的不同将半导体中自旋弛豫分为3个部分:体材料、量子阱、量子线、量子点,在每一部分中又基本上按照电子、空穴、激子的顺序进行了简要的总结:对于不同的载流子,考虑了自旋弛豫对可调参数的依赖关系。这些结果要么试图解释了已有的实验结果,要么从理论上给出预言从而给实验指明了方向,为室温下可以使用的自旋电子学器件设计提供了依据,为固态量子计算和量子信息处理铺平了道路。最后简单地给出展望。     

半导体中的自旋弛豫--从体材料到量子阱、量子线、量子点

本文对半导体中的自旋弛豫过程给出一个简要的回顾,介绍了半导体材料从体材料到量子阱、量子线、量子点不同维数的结构中各种自旋弛豫过程,主要关注了自旋去相位和相干控制。对于不同材料中的各种弛豫机制,关注的重点在于如何能够在实验上以一种可以控制的方式来改变可调参数从而达到控制自旋弛豫过程。这些参数主要有电场、磁场、温度、应变、有效g因子等等。本文的组织上,首先介绍研究前景,第1部分简要介绍了自旋弛豫的四种机制。第2部分按照维数的不同将半导体中自旋弛豫分为3个部分:体材料、量子阱、量子线、量子点,在每一部分中又基本上按照电子、空穴、激子的顺序进行了简要的总结:对于不同的载流子,考虑了自旋弛豫对可调参数的依赖关系。这些结果要么试图解释了已有的实验结果,要么从理论上给出预言从而给实验指明了方向,为室温下可以使用的自旋电子学器件设计提供了依据,为固态量子计算和量子信息处理铺平了道路。最后简单地给出展望。     

Electronic excitation energy transfer between CdS quantum dots and carbon nanotubes

Stationary and transient photoluminescence of CdS quantum dots deposited on silicon substrates and carbon nanotubes is investigated. The photoluminescence spectrum of quantum dots on a silicon substrate is dominated by a band originating from electron transitions between the quantum-confinement levels in the dots. When the quantum dots are deposited on carbon nanotubes, the intensity of this band decreases significantly. Furthermore, the kinetics of the photoluminescence decay becomes faster, which brings evidence of an additional channel for the quantum-dot deexcitation. The analysis of the experimental data demonstrates that the Förster energy transfer from CdS quantum dots to carbon nanotubes is most probably responsible for this channel. The efficiency of this process exceeds 60%.     

Temperature dependence of photoluminescence of semiconductor quantum dots upon indirect excitation in a SiO2 dielectric matrix

The processes of excitation and relaxation of confined excitons in semiconductor quantum dots upon indirect high-energy excitation have been considered. The temperature behavior of photoluminescence of quantum dots in a SiO₂ dielectric matrix has been described using a model accounting for the process of population of quantum-dot triplet states upon excitation transfer through mobile excitons of the matrix. Analytical expressions that take into account the two-stage and three-stage schemes of relaxation transitions have been obtained. The applicability of these expressions for analyzing fluorescence properties of semiconductor quantum dots has been demonstrated using the example of silicon and carbon nanoparticles in the thin-film SiO₂ matrix. It has been shown that the complex character of the temperature dependences of the photoluminescence upon indirect excitation can be an indication of a multistage relaxation of excited states of the matrix and quantum dots. The model concepts developed in this study allow one to predict the form of temperature dependences of the photoluminescence for different schemes of indirect excitation of quantum dots.

     

Carrier capture and relaxation of self-assembled ZnTe/ZnSe quantum dots prepared under Volmer–Weber and Stranski–Krastanow growth modes

The carrier capture and relaxation of type II ZnTe/ZnSe quantum dots have been investigated with ultrafast time-resolved photoluminescence upconversion. The carrier capture times were 7 and 38 ps for the Volmer–Weber mode and Stranski–Krastanow mode, respectively. We found that the carrier relaxation of QDs exhibits faster decay under the Volmer–Weber growth mode than under the Stranski–Krastanow growth mode. We attribute the difference of carrier relaxation to the wetting layer formed in the Stranski–Krastanow growth mode.     

The polaronic nature of intraband relaxation in InAs/GaAs self-assembled quantum dots

Polaron relaxation processes in a series of n-type InAs quantum dots (QDS) have been investigated using energy-dependent far-infrared pump–probe spectroscopy. For energies up to 53 meV, polarons decay to 2 longitudinal acoustic phonons; above this energy additional decay channels open resulting in a reduction of the decay time. Inter-state transfer has been observed between closely spaced p-like excited states, with the measured transfer times in good agreement with calculations assuming acoustic phonon assisted transfer. Finally, for QDs containing 2 electrons we observe evidence of a spin-flip process resulting in long (700 ps) relaxation times.     

CdSeS合金结构量子点的多激子俄歇复合过程

多激子效应通常是指吸收单个光子产生多个激子的过程,该效应不仅可以为研究基于量子点的太阳能电池开拓新思路,还可以为提高太阳能电池的光电转换效率提供新方法.但是,超快多激子产生和复合机制尚不明确.这里以CdSeS合金结构量子点为研究对象,研究了其多激子生成和复合动力学.稳态吸收光谱显示, 510, 468和430 nm附近的稳态吸收峰,分别对应1S_(3/2)(h)-1S(e)(或1S), 2S_(3/2)(h)-1S(e)(或2S)和1P_P(3/2)(h)-1P(e)(或1P)激子的吸收带.通过飞秒时间分辨瞬态吸收光谱和纳秒时间分辨荧光光谱两种时间分辨光谱技术对CdSeS合金结构量子点的超快动力学进行了探究,结果显示, 1S激子的双激子复合时间大概是80 ps,这一时间比传统量子点的双激子复合时间(小于50 ps)延长了近一倍,结合最近发展的超快界面电荷分离技术,在激子湮灭之前将其利用起来,这一时间的延长将有很大的应用前景;其中,在2S和1P激子中除上述双激子复合外,还存在一个通过声子耦合路径的空穴弛豫过程,时间大概是5—6 ps.最后,利用纳秒时间分辨荧光光谱得到该样品体系单激子复合的时间约为200 ns.     

Millisecond fluorescence in InAs quantum dots embedded in AlAs

The temperature dependence of steady-state and time-resolved photoluminescence from self-assembled InAs quantum dots embedded in AlAs has been studied. Millisecond-long nonexponential photoluminescence decay is observed in the temperature range of 4.2–50 K. At higher temperatures, the decay time decreases to a few nanoseconds. The experimental results are interpreted using a model of singlet–triplet splitting of exciton levels in small dots in a dense quantum dot system with local carrier transfer between dots.     

Control of type-I and type-II band alignments in AlInAs/AlGaAs self-assembled quantum dots by changing AlGaAs compositions

Type-I and type-II band alignments were successfully controlled by changing composition and growth temperature in AlInAs/AlGaAs self-assembled quantum dots. The Al composition dependence of the photoluminescence peak shift clearly indicated the crossover from type-I to type-II band line up and a long decay time of 30 ns was obtained by time-resolved photoluminescence at 8 K for the sample with type-II band alignment grown under optimized conditions. A much longer decay component of 500 ns was also observed from the same structure, but it may be due to slow relaxation of carriers trapped in AlGaAs matrix.     

Quantum beats of fine-structure states in InP quantum dots

Different types of quantum beats were experimentally observed in the photoluminescence kinetics of semiconductor nanostructures with InP quantum dots characterized by strong inhomogeneous broadening of the optical transitions. Specific types of beats were selected by varying the magnitude and orientation of the magnetic field, the applied bias voltage, and the frequencies of the exciting and detected light. Parameters of the fine structure of electrons and holes in the system under study and characteristic relaxation times of the spin coherence are determined from the experimental data.     

分子束外延生长ZnSe自组织量子点光、电行为研究

分别应用光致发光、电容电压和深能级瞬态傅里叶谱技术详细研究ZnSe自组织量子点样品的光学和电学行为.光致发光温度关系表明ZnSe量子点的光致发光热猝火过程机理.两步猝火过程的理论较好模拟和解释了相关的实验数据.电容电压测量表明样品表观载流子积累峰出现的深度(样品表面下约100nm处)大约是ZnSe量子点层的位置.深能级瞬态傅里叶谱获得的ZnSe量子点电子基态能级位置为ZnSe导带下的011eV,这与ZnSe量子点光致发光热猝火模型得到的结果一致.     

Photoluminescence kinetics of structures with InAs quantum dots for IR photodetectors

The experimental results of a photoluminescence kinetics study of InAs/GaAs structures with quantum dots grown by metal-organic vapor-phase epitaxy are shown. The measurements have revealed the fast capture of excited carriers from the GaAs barrier to quantum dots and slow interlevel relaxation inside the quantum dots.     

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.     

Magnetic Circular Polarization of Exciton Photoluminescence

Experimental and theoretical studies of circular polarization of photoluminescence of excitons (MCPL) in semiconductors placed in an external magnetic field are reviewed. The advantage of the MCPL method is its relative simplicity. In particular, it does not require spectral resolution of the Zeeman sublevels of an exciton and may be applied to a wide class of objects having broad photoluminescence spectral lines or bands: in bulk semiconductors with excitons localized on the defects of the crystal lattice and composition fluctuations, in structures with quantum wells and quantum dots of types I and II, in two-dimensional transition metals dichalcogenides and quantum microcavities. The basic mechanisms of the magnetic circular polarization of luminescence are considered. It is shown that either known mechanisms should be modified or additional mechanisms of the MCPL should be developed to describe the polarized photoluminescence in newly invented nanosystems.     

Dynamics of carriers photogenerated in a dot-in-a-well nanostructure

We review our recent results on the investigation of carrier dynamics of semiconductor nanostructures, i.e., dot-in-a-well. We introduced a technique based on the measurement of time-resolved differential photoluminescence spectra induced by subpicosecond pump and probe laser pulses. In this technique, the temporal resolution was achieved by adjusting the temporal delay between the pump and probe pulses. Using such a new technique, we measured the exciton decay times and then studied the dependences of integrated photoluminescence intensity and photoluminescence linewidth on temperature in InAs quantum dots embedded in InGaAs/GaAs quantum wells. We gave consistent interpretations to our experimental results.     

High quantum yield ZnO quantum dots synthesizing via an ultrasonication microreactor method

Green emission ZnO quantum dots were synthesized by an ultrasonic microreactor. Ultrasonic radiation brought bubbles through ultrasonic cavitation. These bubbles built microreactor inside the microreactor. The photoluminescence properties of ZnO quantum dots synthesized with different flow rate, ultrasonic power and temperature were discussed. Flow rate, ultrasonic power and temperature would influence the type and quantity of defects in ZnO quantum dots. The sizes of ZnO quantum dots would be controlled by those conditions as well. Flow rate affected the reaction time. With the increasing of flow rate, the sizes of ZnO quantum dots decreased and the quantum yields first increased then decreased. Ultrasonic power changed the ultrasonic cavitation intensity, which affected the reaction energy and the separation of the solution. With the increasing of ultrasonic power, sizes of ZnO quantum dots first decreased then increased, while the quantum yields kept increasing. The effect of ultrasonic temperature on the photoluminescence properties of ZnO quantum dots was influenced by the flow rate. Different flow rate related to opposite changing trend. Moreover, the quantum yields of ZnO QDs synthesized by ultrasonic microreactor could reach 64.7%, which is higher than those synthesized only under ultrasonic radiation or only by microreactor.     

Intraband carrier relaxation in quantum dots mediated by surface plasmon-phonon excitations

A new mechanism of the intraband carrier relaxation in quantum dots embedded into a heterostructure at a relatively large distance from its doped elements is proposed. The relaxation process is related to the coupling between the electronic subsystem of a quantum dot and surface plasmon-phonon excitations of the doped components of the heterostructure via the electric potential produced by these excitations. It is found that, in layered heterostructures, the dispersion relations of the surface plasmon-LO-phonon modes display critical points giving rise to pronounced singularities in the relaxation rate spectra. The estimates of the relaxation rates for InAs quantum dots embedded into a GaAs heterostructure have shown high efficiency of the proposed mechanism even when the quantum dots are located at a distance of up to 100 nm from the doped regions of the heterostructure. When this distance lies in the range of a few tens of nanometers, this mechanism appears to be predominant. Possible manifestations of the relaxation mechanism under consideration in the photoluminescence spectra of quantum dots are discussed.     

Optical transitions and carrier dynamics in self-organized InAs quantum dots grown on In0.52Al0.48As/InP(0 0 1)

Optical transitions in self-organized InAs quantum dots (QDs) grown on In_0.52Al_0.48As layer lattice matched to InP(0 0 1) substrate, have been studied by continuous wave (cw) photoluminescence (PL) and time-resolved PL. The dependence of the PL transition on excitation power and photoluminescence excitation measurements clearly shows that the multi-component cw-PL spectrum is related to emission coming from ground and related excited states of QDs with heights varying by monolayer fluctuations. While decay times measured by time-resolved PL are in the nanosecond range for the ground states, shorter decay times related to relaxation of carriers down directly to the ground state are determined for the excited states.