Si quantum dot structures and their applications

This paper presents briefly the history of emission study in Si quantum dots (QDs) in the last two decades. Stable light emission of Si QDs and NCs was observed in the spectral ranges: blue, green, orange, red and infrared. These PL bands were attributed to the exciton recombination in Si QDs, to the carrier recombination through defects inside of Si NCs or via oxide related defects at the Si/SiOx interface. The analysis of recombination transitions and the different ways of the emission stimulation in Si QD structures, related to the element variation for the passivation of surface dangling bonds, as well as the plasmon induced emission and rare earth impurity activation, have been presented.The different applications of Si QD structures in quantum electronics, such as: Si QD light emitting diodes, Si QD single union and tandem solar cells, Si QD memory structures, Si QD based one electron devices and double QD structures for spintronics, have been discussed as well. Note the significant worldwide interest directed toward the silicon-based light emission for integrated optoelectronics is related to the complementary metal-oxide semiconductor compatibility and the possibility to be monolithically integrated with very large scale integrated (VLSI) circuits. The different features of poly-, micro- and nanocrystalline silicon for solar cells, that is a mixture of both amorphous and crystalline phases, such as the silicon NCs or QDs embedded in a α-Si:H matrix, as well as the thin film 2-cell or 3-cell tandem solar cells based on Si QD structures have been discussed as well. Silicon NC based structures for non-volatile memory purposes, the recent studies of Si QD base single electron devices and the single electron occupation of QDs as an important component to the measurement and manipulation of spins in quantum information processing have been analyzed as well.     

Temperature Dependence of Photoluminescence from Single and Ensemble InAs/GaAs Quantum Dots

We investigate the temperature dependence of photoluminescence from single and ensemble InAs/GaAs quantum dots systematically. As temperature increases, the exciton emission peak for single quantum dot shows broadening and redshift. For ensemble quantum dots, however, the exciton emission peak shows narrowing and fast redshift. We use a simple steady-state rate equation model to simulate the experimental data of photoluminescence spectra. It is confirmed that carrier-phonon scattering gives the broadening of the exciton emission peak in single quantum dots while the effects of carrier thermal escape and retrapping play an important role in the narrowing and fast redshift of the exciton emission peak in ensemble quantum dots.     

Spectral diffusion in nitride quantum dots: Emission energy dependent linewidths broadening via giant built‐in dipole moments

We present a study about the origin of the huge emission linewidths broadening commonly observed for wurtzite GaN/AlN quantum dots. Our analysis is based on a statistically significant number of quantum dot spectra measured by an automatized µ‐photoluminescence mapping system applying image recognition techniques. A clear decrease of the single quantum dot emission linewidths is observed with rising overall exciton emission energy. 8‐band k · p based model calculations predict a corresponding decrease of the built‐in exciton dipole moments with increasing emission energy in agreement with the measured behavior for the emission linewidths. Based on this proportionality we explain the particular susceptibility of nitride quantum dots to spectral diffusion causing the linewidth broadening via the linear quantum‐confined Stark effect. This is the first statistical analysis of emission linewidths that identifies the giant excitonic dipole moments as their origin and estimates the native defect‐induced electric field strength to ～2 MV/m. Our observation is in contrast to less‐polar quantum dot systems as e.g. arsenides that exhibit a naturally lower vulnerability to emission linewidth broadening due to almost negligible exciton dipole moments. (© 2014 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Single InAs/InP quantum dot spectroscopy in 1.3–1.55 μm telecommunication band

We present an optical spectroscopy and photon correlation measurement at telecommunication wavelengths performed on single InAs/InP quantum dots. Two main approaches brought high optical quality: an application of a ‘double-cap’ growth method to metalorganic chemical vapor deposition, and fabrication of a small mesa structure using low-damage wet chemical etching. Sharp and discrete exciton transition lines have been observed on the single quantum dots, which widely cover the spectral range of 1.3–1.55 μm. Using a pulsed excitation source and gated single-photon detection modules, we observed a photon antibunching behavior for an isolated exciton emission line, indicating nonclassical light emission near the wavelength of 1.3 μm.     

Resonantly driven exciton Rabi oscillation in single quantum dots emitting at 1300 nm

We report on the resonance fluorescence(RF) from single In As quantum dots(QDs) emitting at the telecom band of 1300 nm. The InAs/GaAs QDs are embedded in a planar optical microcavity and the RF is measured by an orthogonal excitation-detection geometry for deeply suppressing the residual laser scattering. An ultra-weak He–Ne laser is necessary to be used as a gate laser for obtaining RF. Rabi oscillation with more than one period is observed through the picosecond(ps) pulsed laser excitation. The resonant control of exciton opens up new possibilities for realizing the on-demand single photon emission and quantum manipulation of solid-state qubits at telecom band.     

Electroluminescence of single CdSe nanocrystals induced by scanning tunneling microscope

Electroluminescence intensity of single CdSe nanocrystals (NCs) excited by the tunnel current of a scanning tunneling microscope (STM) was measured. Samples with NCs do not exhibit plasmon emission. This enables one to measure pure emission from a single NC. Electroluminescence, measured in time, differs considerably from that of photoluminescence in similar NCs. This difference in temporal behavior results from the difference in physical conditions of experiments on photo- and electroluminescence.     

Abnormal Energy Dependence of Photoluminescence Decay Time in InGaN Epilayer

We employ photoluminescence (PL) and time-resolved PL to study exciton localization effect in InGaN epilayers.By measuring the exciton decay time as a function of the monitored emission energy at different temperatures,we have found unusual behaviour of the energy dependence in the PL decay process. At low temperature, the measured PL decay time increases with the emission energy. It decreases with the emission energy at 200K, and remains nearly constant at the intermediate temperature of 12OK. We have studied the dot size effect on the radiative recombination time by calculating the temperature dependence of the exciton recombination lifetime in quantum dots, and have found that the observed behaviour can be well correlated to the exciton localization in quantum dots. This suggestion is further supported by steady state PL results.     

Magnetooptics and dynamics of a magnetic polaron in semimagnetic CdSe/ZnMnSe quantum dots

The magnetooptics and picosecond dynamics of the radiative recombination of excitons in self-assembled semimagnetic CdSe/ZnMnSe quantum dots is studied at low temperatures. The behavior of individual quantum dots in a magnetic field and with an increase in temperature is indicative of a strong exchange interaction of excitons and magnetic Mn ions giving rise to a quasi-zero-dimensional exciton magnetic polaron. When the exciton energy exceeds the intracenter transition energy in Mn, the energy is rapidly transferred from excitons to Mn ions (faster than 20 ps). In the opposite case, a substantial red shift (～15 meV) of the emission line maximum is observed during the exciton lifetime ～500 ps, presenting the dynamics of the formation of a magnetic polaron with a characteristic time of ～110 ps.     

CdSe量子点的光物理性质研究与荧光杂化纤维的制备

半导体纳米晶体（NCs）具有良好的光稳定性,广泛的发射持久性和高消光系数,在过去几年被广泛研究报道,其中,硒化镉半导体纳米晶体(CdSe NCs)被广泛用于电子照明、太阳能发电、光电传感等领域。然而CdSe NCs的电学、热力学和光物理性质具有较强的尺寸依赖性,在传统的制备方法及应用中容易出现晶体表面缺陷和悬空键以及较为严重的生物毒性和环境毒性。为了实现量子点在各个领域的应用,必须严格控制CdSe NCs的发光波长,尺寸分布以及荧光性能。本研究通过高温热注射法合成了单分散的胶体发光CdSe NCs,使用表面配体对CdSe NCs进行修饰,研究了不同烷基链长度的配体对CdSe NCs尺寸分布和荧光性能的影响,并通过改变溶剂配比制备了纺丝溶液,将其与聚乙烯吡咯烷酮（PVP）进行杂化,制备了PVP/CdSe QDs荧光杂化纤维。结果表明,与传统CdSe NCs相比,经表面配体的修饰的CdSe NCs在有机溶液中因分子间吸附的降低在溶液中有良好的稳定性,具有可调节的溶解度,弥补了缺陷和悬空键造成的荧光性能下降。在CdSe晶体结构的形成过程中,表面配体也有着显著的调控作用。并且更为重要的是,该研究将表面配体修饰与杂化相结合,改善了表面配体的附着,在杂化材料的制备过程中避免了硒化镉纳米晶体与高分子基体直接接触,为荧光团提供了良好的发光微环境,保证了CdSe NCs的荧光性能,使杂化纤维具有良好而稳定的荧光性能。同时,PVP的引入使CdSe NCs的生物毒性和环境毒性得以改善,使材料更加环境友好且具有更好的生物相容性,大大提升了材料的应用范围。事实证明,PVP/CdSe QDs杂化微纤维杂化相容性和分散性良好,具有优异的荧光性能和材料成型性,纤维合成方式简便易行且造价低廉,可应用于溶液处理,光学照明,电极材料,和生物成像等各个领域。     

Interferometric spectroscopy for excitons in InP single quantum dots

Dynamical dephasing processes of an exciton and a charged exciton in single InP quantum dots were studied by using interferometric spectroscopy. Interferometric spectroscopy enabled us to observe with high sensitivity the dephasing of exciton or other exciton complexes in single quantum dots. In order to observe the dephasing of the exciton or exciton complexes, emitted single-photons generated from single InP quantum dots were detected through the Michelson interferometer. The contrast of the interferometric signal due to the exciton and the charged exciton shows non-exponential decay under band-to-band excitation for the GaInP matrix. The band-to-band excitation generates carriers trapped in the matrix and the trapped carriers modulate the energy of the quantum dots because of the quantum-confined Stark effect. Therefore the non-exponential decays are caused by energy fluctuation due to the trap carriers in the long timescale.     

神经网络法研究多溴代二苯胺热力学性质

通过时间分辨光谱技术详细地研究了ZnCuInS/ZnSe/ZnS量子点的激子弛豫动力学. 基于速率分布模型,波长依赖的发射动力学表明本征激子、界面缺陷态中的激子、给-受体对态中的激子都会参与量子点的发光过程,整个发光过程主要依赖于给-受体对态发射. 瞬态吸收数据表明激发后本征激子和界面缺陷物种可能会同时出现,在高激发光强下,光强依赖的俄歇复合过程也存在于量子点中     

Cancellation of fine-structure splitting in quantum dots by a magnetic field

We demonstrate control of the fine-structure splitting of the exciton emission lines in single InAs quantum dots by the application of an in-plane magnetic field. The composition of the barrier material and the size and symmetry of the quantum dot are found to determine decrease or increase in the linear polarization splitting of the dominant exciton emission lines with increasing magnetic field. This enables the selection of dots for which the splitting can to be tuned to zero, within the resolution of our experiments. General differences in the g-factors and exchange splittings are found for different types of dot.     

ZnO对硫硒化镉量子点玻璃发光性能的影响

以CdS、Se、Zn粉和玻璃基质为原料,采用高温熔融法制备了CdS_xSe_(1-x)量子点硅酸盐玻璃,研究了ZnO含量对CdS_xSe_(1-x)量子点发光玻璃微观结构及发光性能的影响。结果表明:ZnO对CdS_xSe_(1-x)量子点玻璃的发光性能有显著的影响,紫外-可见吸收光谱和荧光光谱分析结果说明在470 nm蓝光激发下,掺Zn O的CdS_xSe_(1-x)量子点玻璃中CdS_xSe_(1-x)量子点处于强限域区,出现了强烈的带边激子发射现象,证明量子点具有明显的量子尺寸效应。当样品中ZnO的质量分数为13%时,荧光光谱峰强最大,半峰宽最窄。     

Phonon-mediated coupling of InGaAs/GaAs quantum-dot excitons to photonic crystal cavities

We demonstrate that the emission characteristics of site-controlled InGaAs/GaAs single quantum dots embedded in photonic crystal slab cavities correspond to single confined excitons coupled to cavity modes, unlike previous reports of similar systems based on self-assembled quantum dots. By using polarization-resolved photoluminescence spectroscopy at different temperatures and a theoretical model, we show that the exciton-cavity interaction range is limited to the phonon sidebands. Photon-correlation and pump-power dependence experiments under nonresonant excitation conditions further establish that the cavity is fed only by a single exciton.     

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.     

平均探测时间:研究单个量子点荧光现象的另一种思路

Due to photoluminescence intermittency of single colloidal quantum dots (QDs), the traditional exponential fluorescence lifetime analysis is not perfect to characterize QDs'' fluorescent emission behavior. In this work we used the time-tagged time-resolved (TTTR) mode to record the fluorescent photons from single QDs. We showed that this method is compatible with the traditional lifetime analysis. In addition, by constructing the trajectory over time and the distribution of average arrival time (AAT) of the fluorescent photons, more details about the emission behavior of QDs were revealed.     

Study of isolated cubic GaN quantum dots by low-temperature cathodoluminescence

We report single dot spectroscopy of cubic GaN/AlN self-assembled quantum dots. Typical linewidths of the zero-phonon line between 2 and 8 meV are observed and interpreted in terms of charge fluctuations around a given quantum dot. The phonon sideband contribution in this emission, even at low temperature, reveals the importance of the acoustic phonon broadening mechanism which controls the exciton dephasing and may impose the real limits to the optical properties of GaN single QDs emission.     

Optical study of single InAs on In0.12Ga0.88As self-assembled quantum dots: biexciton binding energy dependence on the dots size

Single self-assembled InAs quantum dots embedded in a In_0.12Ga_0.88As quantum well and emitting in the near infrared have been optically investigated. The dependence on the excitation power of the single quantum dot photoluminescence has been used to identify the emission of the biexciton complex. The biexciton binding energy, which has been measured for a dozen dots, increases with increasing exciton transition energy for the dot sizes investigated in the present work, as a consequence of stronger confinement in a smaller quantum dot. The obtained data is compared with experimental results available in the literature for InAs quantum dots. PACS 78.67.Hc; 73.21.La; 78.55.Cr     

New mechanism of surface polariton resonance at an isolated interface between transparent dielectric media (non-Tamm quasistationary surface polariton states)

A system of quantum dots on the basis of Al_xIn_1-xAs/Al_yGa_1-y As solid solutions has been studied. The usage of broadband Al_xIn_1-x solid solutions as the basis of quantum dots makes it possible to expand considerably the spectral emission range into the short-wave region, including the wavelength region near 770 nm being of interest for the design of aerospace systems of quantum cryptography. The optical characteristics of single Al_xIn_1-xAs quantum dots grown according to the Stranski–Krastanov mechanism are studied by the cryogenic microphotoluminescence method. The fine structure of exciton states of quantum dots is studied in the wavelength region near 770 nm. It is shown that the splitting of exciton states is comparable with the natural width of exciton lines, which is of great interest for the design of emitters of pairs of entangled photons on the basis of Al_xAs_1-x quantum dots.     

High efficiency carrier multiplication in PbSe nanocrystals: implications for solar energy conversion

We demonstrate for the first time that impact ionization (II) (the inverse of Auger recombination) occurs with very high efficiency in semiconductor nanocrystals (NCs). Interband optical excitation of PbSe NCs at low pump intensities, for which less than one exciton is initially generated per NC on average, results in the formation of two or more excitons (carrier multiplication) when pump photon energies are more than 3 times the NC band gap energy. The generation of multiexcitons from a single photon absorption event is observed to take place on an ultrafast (picosecond) time scale and occurs with up to 100% efficiency depending upon the excess energy of the absorbed photon. Efficient II in NCs can be used to considerably increase the power conversion efficiency of NC-based solar cells.