Correlations between antibunching and blinking of photoluminescence from a single CdSe quantum dot

The antibunching and blinking from a single CdSe/ZnS nanocrystal with an emission wavelength of 655 nm were investigated under different excitation powers. The decay process of the photoluminescence from nanocrystal was fitted into a stretched exponential, and the small lifetime and the small stretching exponent under a high excitation power were explained by using nonradiative multi-channel model. The probability of distributions for off-times from photoluminescence intermittence was fitted into the power law, and the power exponents were explained by using a tunneling model. For higher excitation power, the Auger-assisted tunneling model takes effect, where the tunneling rate increases and the observed lifetime decreases. For weak excitation power, the electron directly tunnels between the nanocrystal and trapping state without Auger assistance. The correlation between antibunching and blinking from the same nanocrystal was analyzed.     

Antibunching and blinking from a single colloidal CdSe quantum dot

We have investigated the optical properties of single CdSe/ZnS nanocrystals by conducting combinations of experiments on antibunching and photoluminescence intermittence under different experimental conditions.Based on photoluminescence in an antibunching experiment,we analyzed the emission lifetime of QDs by using stretched exponentials.The difference between the parameters obtained from average lifetimes and stretched exponents were analyzed by considering the effect of nonradiative emission.An Auger-assisted tunneling model was used to explain the power law exponents of off time distribution.The power law exponent under high excitation power was correlated with a higher Auger ionization rate.Using the parameters obtained from stretched exponential function and power law,the antibunching phenomena at different time and under different excitation intensity were analyzed.     

Single-Photon Emission at Liquid Nitrogen Temperature from a Single InAs/GaAs Quantum Dot

We report on the single photon emission from single InAs/GaAs self-assembled Stranski-Krastanow quantum dots up to 80 K under pulsed and continuous wave excitations. At temperature 8OK, the second-order correlation function at zero time delay, g^（2）（0）, is measured to be 0.422 for pulsed excitation. At the same temperature under continuous wave excitation, the photon antibunching effect is observed. Thus, our experimental results demonstrate a promising potential application of self-assembled InAs/GaAs quantum dots in single photon emission at liquid nitrogen temperature.     

氧化硅稳定的氧化锡量子点薄膜的制备及其光学性能

 用溶胶-凝胶-水热过程制备了氧化硅稳定的氧化锡量子点,然后将其分散到氧化硅溶液中,用旋转涂膜的方法制备光学性能良好的氧化硅稳定的氧化锡量子点薄膜。X射线衍射和高分辨透射电镜表征显示氧化锡量子点具有良好的四方金红石晶型,平均粒径约4.0 nm。室温光致发光显示这种氧化硅稳定的氧化锡量子点薄膜在356 nm和388 nm处分别有很强的激子发光和缺陷态发光。根据透射谱拟合得到了氧化锡量子点薄膜的光学禁带宽度,其值约为3.96 eＶ。     

Photon antibunching in the photoluminescence spectra of a single carbon nanotube

We report the first observation of photon antibunching in the photoluminescence from single carbon nanotubes. The emergence of a fast luminescence decay component under strong optical excitation indicates that Auger processes are partially responsible for inhibiting two-photon generation. Additionally, the presence of exciton localization at low temperatures ensures that nanotubes emit photons predominantly one by one. The fact that multiphoton emission probability can be smaller than 5% suggests that carbon nanotubes could be used as a source of single photons for applications in quantum cryptography.     

Effect of a buffer layer between the shell and ligand on the optical properties of an exciton and biexciton in type-II quantum dot nanocrystals

In this study, we have investigated the effect of the buffer layers on the electronic and optical properties of an exciton (X) and a biexciton (XX) in a type-II CdTe/CdSe quantum dot nanocrystal. In an experimental study, it has been reported that when a CdTe/CdSe quantum dot nanocrystal is coated by a ZnTe material as a buffer layer, the photoluminescence quantum yield is growing from 4 to 20%. We have confirmed theoretically this improvement and extended the calculations to an XX structure. In the calculations, two different semiconductor materials, CdS and ZnTe, have been considered for the buffer layer. We have theoretically shown that the buffer layer causes an increase in the radiative oscillator strength of both X and XX. When the ZnTe is used as the buffer layer, the oscillator strength becomes stronger when compared to CdSe buffer material because of higher conduction band offset between CdSe and ZnTe.     

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     

巯基丙酸分子对CdSe核壳量子点和 ZnO纳米粒子薄膜之间电荷转移的影响

通过稳态光谱和时间分辨荧光光谱研究了巯基丙酸(MPA)分子对由量子点到ZnO纳米粒子薄膜的电荷转移过程的影响。研究发现,相对于CdSe纳米粒子薄膜样品,没有MPA分子参与作用的CdSe/ZnO薄膜样品和有MPA分子连接的CdSe/MPA/ZnO薄膜样品中都存在从CdSe量子点到ZnO纳米粒子薄膜的有效电荷分离过程,但是相对于CdSe/ZnO样品, CdSe/MPA/ZnO样品中电荷转移速率明显变小。这表明MPA分子本身它并不能促进CdSe到ZnO电荷分离过程,因此可以认为用金属氧化物薄膜直接吸附量子点吸收材料,将能获得高功率转换效率的量子点敏化太阳能电池。     

Growth and time-resolved photoluminescence study of self-organized CdSe quantum dots in ZnSe

Employing two different growth methods: standard molecular beam epitaxy (MBE) and low-temperature atomic layer epitaxy (ALE) with subsequent annealing, we have obtained high-quality quantum dot structures consisting of CdSe embedded in ZnSe. Single dot emission lines are observed in micro-luminescence. The samples have been investigated by further optical methods including time-resolved photoluminescence under resonant excitation at 4.2 K. Distinct properties of systems with three-dimensional confinement are observed such as the suppression of the interaction between isolated quantum dots (QDs). In standard quantum wells tunneling/hopping processes generally lead to a pronounced red shift of the luminescence over time due to a lateral localization of excitons in potential fluctuations. A much less pronounced red shift is observed for the QDs reflecting only the different lifetimes of single dots and higher excited states. The red shift completely vanishes under resonant excitation that selectively excites only a few QDs of the ensemble in the layer. Typical behaviour is also observed from the halfwidth of the quantum dot emission.     

Resonance in quantum dot fluorescence in a photonic bandgap liquid crystal host

Microcavity resonance is demonstrated in nanocrystal quantum dot fluorescence in a one-dimensional (1D) chiral photonic bandgap cholesteric-liquid crystal host under cw excitation. The resonance demonstrates coupling between quantum dot fluorescence and the cholesteric microcavity. Observed at a band edge of a photonic stop band, this resonance has circular polarization due to microcavity chirality with 4.9 times intensity enhancement in comparison with polarization of the opposite handedness. The circular-polarization dissymmetry factor g(e) of this resonance is ~1.3. We also demonstrate photon antibunching of a single quantum dot in a similar glassy cholesteric microcavity. These results are important in cholesteric-laser research, in which so far only dyes were used, as well as for room-temperature single-photon source applications.     

Purcell effect in triangular plasmonic nanopatch antennas with three-layer colloidal quantum dots

A model describing a plasmonic nanopatch antenna based on triangular silver nanoprisms and multilayer cadmium chalcogenide quantum dots is introduced. Electromagnetic-field distributions in nanopatch antennas with different orientations of the quantum-dot dipoles are calculated for the first time with the finite element method for numerical electrodynamics simulations. The energy flux through the surface of an emitting quantum dot is calculated for the configurations with the dot in free space, on an aluminum substrate, and in a nanopatch antenna. It is shown that the radiative part of the Purcell factor is as large as 1.7 × 10₂ The calculated photoluminescence lifetimes of a CdSe/CdS/ZnS colloidal quantum dot in a nanopatch antenna based on a silver nanoprism agree well with the experimental results.     

Efficient Quantum Dot Light-Emitting Diodes Based on Well-Type Thick-Shell CdxZn1−xS/CdSe/CdyZn1−yS Quantum Dots

Device grade quantum dots (QDs) require QDs ensembles to retain their original superior optical properties as in solution. QDs with thick shells are proven effective in suppressing the inter-dot interaction and preserving the emission properties for QDs solids. However, lattice strain–induced defects may form as the shell grows thicker, resulting in a notable photoluminescence quenching. Herein, a well-type Cd_xZn_1−xS/CdSe/Cd_yZn_1−yS QDs is proposed, where ternary alloys CdZnS are adopted to match the lattice parameter of intermediate CdSe by separately adjusting the x and y parameters. The resultant thick-shell Cd_0.5Zn_0.5S/CdSe/Cd_0.73Zn_0.27S QDs reveal nonblinking properties with a high PL QY of 99% in solution and 87% in film. The optimized quantum dot light-emitting diodes (QLEDs) exhibit a luminance of 31547.5 cd m⁻² at the external quantum efficiency maximum of 21.2% under a bias of 4.0 V. The shell thickness shows great impact on the degradation of the devices. The T₅₀ lifetime of the QLEDs with 11.2 nm QDs reaches 251 493 h, which is much higher than that of 6.5 and 8.4 nm QDs counterparts. The performances of the well-type thick-shell QLEDs are comparable to state-of-the-art devices, suggesting that this type of QDs is a promising candidate for efficient optoelectronic devices.     

Temperature dependent single photon emission in InP/GaInP quantum dots

Intensity correlation measurements on single InP/GaInP quantum dots (QDs) show antibunching at zero delay time, indicative of single photon emission. The antibunching time τ_R increases or decreases with temperature depending on the QD size as a result of the competition between: (1) thermal excitation of holes dominant in smaller QDs and (2) dark-to-bright exciton transition dominant in larger QDs. The antibunching minimum g⁽²⁾(0) remains below 0.2 up to 45 K.     

Time-Resolved Fluorescence Spectroscopy Study on the Photophysical Behavior of Quantum Dots

Room-temperature time-resolved luminescence measurements on single CdSe/ZnS quantum dots (QDs) are presented. Fluorescence emission spectra were recorded over periods of up to 30 minutes with a time resolution as small as 6 ms. For QDs in ambient air, a clear 30–40 nm blue shift in the emission wavelength is observed, before the luminescence stops after about 2–3 minutes because of photobleaching. In a nitrogen atmosphere, the blue shift is absent while photobleaching occurs after much longer times (i.e., 10–15 minutes). These observations are explained by photoinduced oxidation. The CdSe surface is oxidized during illumination in the presence of oxygen. This effectively results in shrinkage of the CdSe core diameter by almost 1 nm and consequently in a blue shift. The faster fading of the luminescence in air suggests that photoinduced oxidation results in the formation of non-radiative recombination centers at the CdSe/CdSeO_x interface. In a nitrogen atmosphere, photoinduced oxidation is prevented by the absence of oxygen. Additionally, a higher initial light output for CdSe/ZnS QDs in air is observed. This can be explained by a fast reduction of the lifetime of the long-lived defect states of CdSe QDs by oxygen.     

Competition in the carrier capture between InGaAs/AlGaAs quantum dots and deep point defects

The presence of an extrinsic photoluminescence (PL) band peaked at 1.356 eV at low temperature is observed, on a large number of self-assembled InAs and In_0.5Ga_0.5As quantum dot (QD) structures, when exciting just below the GaAs absorption edge. A detailed optical characterization allows us to attribute the 1.356 eV PL band to the radiative transition between the conduction band and the doubly ionized Cu _Ga acceptor in GaAs. A striking common feature is observed in all investigated samples, namely a resonant quenching of the QD-PL when exciting on the excited level of this deep defect. Moreover, the photoluminescence excitation (PLE) spectrum of the 1.356 eV emission turns out to be almost specular to the QD PLE. This correlation between the PL efficiency of the QDs and the Cu centers evidences a competition in the carrier capture arising from a resonant coupling between the excited level of the defect and the electronic states of the wetting layer on which the QDs nucleate. The estimated Cu concentration is compatible with a contamination during the epitaxial growth. Received 13 November 2001 / Received in final form 28 May 2002 Published online 19 July 2002     

Time-resolved four-wave-mixing of exciton transitions in GaAs/AlGaAs quantum wells: Novel effects in the lineshape

We investigate coherent exciton transitions in GaAs/Al _x Ga_1–x As quantum wells using subpicosecond four-wave-mixing spectroscopy. In a first part, we show that the four-wave-mixing lineshape deviates considerably from earlier predictions when the detailed structure of the excitons is taken into account, and we study the density dependence and excitation energy dependence in detail. In a second part, we discuss the observation of quantum beats due to the coherent superposition of different excitonic transitions and show how the analysis of the lineshape can yield information about relaxation processes.Dedicated to H.-J. Queisser on the occasion of his 60th birthday     

Photoluminescence spectroscopy of CdSe nanoparticles embedded in transparent glass

In this paper we present photoluminescence measurements of CdSe nanoparticles embedded in transparent glass. Sample is prepared using an original technique, which combines both heat treatment and ultraviolet laser irradiation. Photoluminescence spectra displayed one main emission band at 2.14 eV. We identify this bands energy as basic interband transition in CdSe nanoparticle. We calculated energy of basic (1s_h–1s_e) transition in spherical CdSe quantum dot (QD), within infinite potential barrier, in effective-mass approximation. On the basis of this model, average radius of synthesized CdSe QDs is about 3 nm, which is in consistence with AFM measurements and UV–VIS absorption measurements.     

Exciton tunnelling in ZnCdSe quantum well/CdSe quantum dots

Exciton tunnelling through a ZnSe barrier layer of various thicknesses is investigated in a Zn_0.72Cd_0.28Se/CdSe coupled quantum well/quantum dots (QW/QDs) structure using photoluminescence (PL) spectra and near resonant pump-probe technique. Fast exciton tunnelling from quantum well to quantum dots is observed by transient differential transmission. The tunnelling time is 1.8, 4.4 and 39 ps for barrier thickness of 10, 15 and 20 nm, respectively.     

Photon-emission properties of quantum-dot-based single-photon sources under different excitations

The photon-emission efficiencies and photon indistinguishabilities of a single-photon source, which employs a cavity coupled with a quantum dot, are studied under above-band and resonant excitations. The results are obtained by solving master equations and by applying the quantum regression theorem. According to the study, the photon indistinguishability increases with the Purcell factor under resonant excitation, which is consistent with the increase in emission efficiency; however, these two figures of merit are inconsistent for the above-band excitation scheme. Moreover, the efficiencies, defined as the average photon number emitted in one excitation cycle, are almost the same for the two different excitation schemes, whereas the excitation power needed to reach that efficiency is much lower under resonant excitation than that for above-band excitation. These results will be helpful in improving the performances of the applications concerning indistinguishability and efficiency.     

Second-Order Correlation Function of the Photon Emission from a Single Quantum Dot

The photon correlation of photon emission from a single quantum dot with cw excitation and pulsed excitation is investigated in details. To calculate the second-order correlation function for optical pumping, we deduce rate equations with a simplified two-level model under cw excitation and present the master equation approach in the interaction picture to the study of evolution of a three-level system under pulsed excitation. In addition, we report photon correlation measurements on a single self-assembled In0.5Ga0.5As quantum dot, which show strong antibunching behaviour under both the conditions of cw and pulsed excitations. The calculated results are in agreement with the experimental measurements.