CdTe/CdS核壳结构量子点超快载流子动力学

在水相合成CdTe以及CdTe/CdS核壳结构量子点基础上, 利用基于抽运-探测技术的瞬态差分透射技术研究了CdTe量子点以及不同CdS壳层厚度的CdTe/CdS量子点的最低激子能态的超快激发与弛豫动力学. 研究表明:相比于CdTe,CdTe/CdS量子点的电子空穴由于空间分离,其所需的激发时间要长于电子空穴空间重叠态所需要的激发时间.随着壳层厚度的增加, 量子点表面的钝化有效地减少了表面态相关弛豫机理,并延长相对应的弛豫时间.     

低强度飞秒激光激发下CdTe和CdTe/CdS核壳量子点的荧光上转换研究

利用400 nm和800 nm不同波长的低强度飞秒激光,对CdTe和CdTe/CdS核壳量子点溶胶进行激发,研究其稳态和时间分辨荧光性质.800 nm飞秒激光激发下,CdTe和CdTe/CdS核壳量子点产生上转换发光现象,上转换荧光峰与400 nm激发下的荧光峰相比蓝移最多达15 nm,而且蓝移值与荧光量子产率有关.变功率激发确认激发光功率与上转换荧光强度间满足二次方关系,时间分辨荧光的研究表明荧光动力学曲线服从双e指数衰减.提出表面态辅助的双光子吸收模型是低激发强度上转换发光的主要机理.CdTe和CdT 关键词： CdTe量子点 CdTe/CdS核壳量子点 时间分辨荧光 上转换荧光     

水溶性TGA-CdTe量子点的超快弛豫动力学过程探究

本文以三个不同粒径(1^#:2.3 nm, 2^#:2.8 nm和3^#:3.5 nm)的巯基乙酸包覆的CdTe量子点(thioglycolic acid capped CdTe quantum dots, TGA-CdTe QDs)样品为研究对象, 其时间相关单光子计数(time-correlated single photon counting, TCSPC)实验得到的时间分辨光谱显示, 三个量子点的荧光平均寿命依次是～6 ns, ～10 ns和～12 ns, 其动力学过程包括慢过程和快过程两部分. 随其粒径尺寸的增加, 其慢过程延长, 快过程在变短. 然后, 通过瞬态吸收和荧光上转换两种基于飞秒的时间分辨光谱技术, 对TGA-CdTe量子点的带间弛豫过程做了探究. 实验结果显示, 三个TGA-CdTe量子点样品, 随其粒径增大, 最高激发态和最低激发态填充速率减慢, 其中, 最高激发态从0.33 ps增加至0.79 ps; 最低激发态从0.53 ps增至～1 ps. 另外, 由瞬态吸收和荧光上转换两种时间分辨手段相结合, 可得到CdTe量子点带间弛豫的完整图像, 结果显示了TGA-CdTe 量子点的一个本征特征:即在基态漂白恢复过程中的初始上升阶段, 荧光上转换信号要慢于瞬态吸收信号. 这可以为量子点在光电转换应用上提供帮助.     

水溶性CdTe量子点的稳态和纳秒时间分辨光致发光光谱

报道了以飞秒脉冲激光为激发光源的水溶性CdTe量子点(QDs)的稳态荧光光谱和纳秒时间分辨荧光光谱.实验发现CdTe量子点的荧光光谱峰值位置随激发波长变化发生明显移动，激发脉冲波长越长，荧光峰位红移越大.荧光动力学实验数据显示，在400nm和800nm脉冲激光激发下，水溶性CdTe量子点的荧光光谱中均含有激子态和诱捕态两个衰减成分，两者的发射峰相距很近，诱捕态的发射峰波长较长.在800nm脉冲激光激发下的诱捕态成分占总荧光强度的比重比400nm激发下的约高3倍，其相对强度的这种变化导致了稳态荧光发射峰位的红移. 关键词： CdTe 量子点 时间分辨 荧光光谱 上转换荧光     

室温下CdSe胶体量子点超快自旋动力学

利用时间分辨法拉第旋转光谱技术研究了室温下CdSe胶体量子点的自旋相干特性.获得了不同磁场下的自旋退相干时间,并分析了自旋退相干的物理机理.零磁场时量子点激子自旋退相干时间为102 ps,主要受电子与核自旋之间的超精细相互作用所影响.当外加横向磁场强度为250 mT时,激子自旋退相干时间为294 ps;增大磁场强度,自旋退相干时间逐渐减小.在较强磁场环境中(≥250mT),量子点激子自旋动力学由非均匀退相干机制所主导.     

The third-order optical nonlinearity and upconversion luminescence of CdTe quantum dots under femtosecond laser excitation

The aqueous CdTe quantum dots (QDs) were synthesized by the electrostatic reaction method. The optical properties of CdTe QDs were investigated by femtosecond Z-scan and time-resolved luminescence technique in nonresonant spectral region. The nonlinear absorption and refraction are ascribed to two-photon absorption, and time-resolved upconversion photoluminescence produces biexponential decay pattern at infrared femtosecond laser excitation. Upconversion luminescence is composed of a band-edge excitonic state and a photoinduced trapping state. The short-lived band-edge excitonic emission is independent of the detection wavelengths, and long-lived species becomes even longer with the increase of detection wavelengths, which indicates the size dependence of surface excitonic emission. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.     

PbTe/CdTe量子点的光学增益

PbTe/CdTe量子点是一类新型异系低维结构材料,实验发现具有强的室温中红外光致发光现象.为研究这一材料体系的发光特性,建立了理论模型,计算了PbTe/CdTe量子点的光学跃迁和增益.模型基于k·p包络波函数方法并考虑了PbTe能带结构的各向异性.分析了量子点光学增益与量子点尺寸、注入载流子浓度的关系.结果表明,当注入载流子浓度在(0.3—3)×10¹⁸cm^-3范围时,尺寸为15—20nm的量子点可以产生 关键词： PbTe/CdTe量子点 光学增益 铅盐矿半导体     

Study on the interaction of CdTe quantum dots with ferulic acid and protocatechuic aldehyde by optical spectroscopy

Luminescent CdTe quantum dots (QDs) were synthesized using thioglycolic acid (TGA) as a stabilizing agent in aqueous medium and were characterized by Fourier transform infrared spectroscopy (FTIR), atomic force microscopy (AFM), and transmission electron microscopy (TEM). In weak basic media the fluorescence of TGA-CdTe QDs was quenched notably by ferulic acid (FA) and protocatechuic aldehyde (PA), and the quenching values were proportional to the concentration of the quenchers in a certain range. The addition of bovine serum albumin (BSA) to TGA-CdTe QDs-FA and TGA-CdTe QDs-PA systems rendered a large recovery of the fluorescence of TGA-CdTe QDs.     

Ultrafast electron spin dynamics in bulk CdTe investigated by femtosecond pump-probe reflection spectroscopy

The transient spin polarization dynamics in bulk cadmium telluride (CdTe) at 70 K is investigated by the circularly polarized pump-probe reflection technique. A general expression is derived from the rate equations of a two-level system with small signal approximation to describe the light-helicity-dependent reflection spectrum. The initial degree of electron spin polarization in the excited state and the electron spin relaxation time in bulk CdTe at low temperature with different carrier density are analyzed according to this model. Our experimental results reveal that the D?yakonov–Perel? mechanism based on a fully microscopic kinetic spin Bloch equation (microscopic KSBE) approach dominates in the electron spin relaxation process in bulk CdTe crystal.     

Sonoelectrochemical synthesis of water-soluble CdTe quantum dots

A facile and fast one-pot method has been developed for the synthesis of CdTe quantum dots (QDs) in aqueous phase by a sonoelectrochemical route without the protection of N₂. The morphology, structure and composition of the as-prepared products were investigated by high resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and energy dispersive X-ray spectrometer (EDS). The influences of current intensity, current pulse width, and reaction temperature on the photoluminescence (PL) and quantum yield (QY) of the products were studied. The experimental results showed that the water-soluble CdTe QDs with high PL qualities can be conveniently synthesized without precursor preparation and N₂ protection, and the PL emission wavelength and QY can be effectively controlled by adjusting some parameters. This method can be expected to prepare other QDs as promising building blocks in solar cell, photocatalysis and sensors.     

Elementary relaxation processes investigated by femtosecond photoelectron spectroscopy of two‐dimensional materials

Elementary scattering processes in solid matter occur on ultrafast timescales and photoelectron spectroscopy in the time domain represents an excellent tool for their analysis. Conventional photoemission accesses binding energies of electronic states and their momentum dispersion. The use of femtosecond laser pulses in pump‐probe experiments allows obtaining direct insights to the energy and momentum dependence of ultrafast dynamics. This article introduces the elementary interaction processes and emphasizes recent work performed in this rapidly developing field. Decay processes in the low excitation limit are addressed, where electrons decay according to their interaction with carriers in equilibrium. Here, hot electron relaxation in epitaxial metallic film is reviewed. In the limit of an intense optical excitation, scattering of the excited electrons among each other establishes a non‐equilibrium state. Results on charge‐density wave materials and the effect of coherent nuclear motion on the electronic structure, which can break low symmetry ground states, are discussed. Figure reprinted with permission from [71].     

CdTe量子点-铜酞菁复合体系荧光共振能量转移的研究

以波长为780 nm、重复频率为76 MHz、脉宽为130 fs的飞秒激光作为激发光源, 采用超快时间分辨光谱技术研究了CdTe量子点-铜酞菁复合体系的荧光共振能量转移. 实验结果表明, 在780 nm的双光子激发条件下, 复合体系中CdTe量子点的荧光寿命随着铜酞菁溶液浓度的增加而减少, 荧光共振能量转移效率增加. 同时也研究了激发功率对荧光共振能量转移效率的影响. 结果表明, 随着激发光功率的增加, 复合体系溶液中CdTe量子点的荧光寿命增加, 荧光共振能量转移效率减小, 其物理机理是因为高激发功率下的热效应和由双光子诱导的高阶激发态的跃迁. 当激发光功率为200 mW时, 双光子荧光共振能量转移效率为43.8%. 研究表明CdTe量子点-铜酞菁复合体系是非常有潜力的第三代光敏剂.     

Absorption spectroscopy of single InAs self-assembled quantum dots

Excitonic transitions of single InAs self-assembled quantum dots were directly measured at 4.2 K in an optical transmission experiment. We use the Stark effect in order to tune the exciton energy of a single quantum dot into resonance with a narrow-band laser. With this method, sharp resonances in the transmission spectra are observed. The oscillator strengths as well as the homogeneous line widths of the single-dot optical transitions are obtained. A clear saturation in the absorption is observed at modest laser powers.     

水溶性CdTe量子点的三阶光学非线性极化特性

利用超短脉冲Z扫描技术和光学Kerr效应研究了以巯基丙酸为稳定剂的CdTe量子点水溶液的三阶光学非线性极化特性. 在532nm,30ps和800nm,130fs脉冲激光激发下, 发现分别具有正负相反取值的三阶光学非线性折射率,自由载流子吸收和双光子吸收分别是这两种脉冲激光激发下三阶光学非线性吸收的起因. 测量得到CdTe量子点的三阶光学非线性极化率约为CS₂的32倍, 在520—700nm光谱区的CdTe量子点的光学响应时间小于400fs. 关键词： CdTe量子点(QDs) Z扫描 三阶光学非线性极化特性 双光子吸收     

Photoluminescence quenching of CdTe/CdS core-shell quantum dots in aqueous solution by ZnO nanocrystals

Photoluminescence (PL) properties of 3-mercaptopropionic acid (MPA) coated CdTe/CdS core-shell quantum dots (QDs) in aqueous solution in the presence of ZnO colloidal nanocrystals were studied by steady-state and time-resolved PL spectroscopy. The PL quenching of CdTe/CdS core-shell QDs with addition of purified ZnO nanocrystals resulted in a decrease in PL lifetime and a small red shift of the PL band. It was found that CdTe(1.5 nm)/CdS type II core-shell QDs exhibited higher efficiency of PL quenching than the CdTe(3.0 nm)/CdS type I core-shell QDs, indicating an electron transfer process from CdTe/CdS core-shell QDs to ZnO nanocrystals. The experimental results indicated that the efficient electron transfer process from CdTe/CdS core-shell QDs to ZnO nanocrystals could be controlled by changing the CdTe core size on the basis of the quantum confinement effect.     

壳聚糖包覆的CdTe量子点荧光猝灭法测定吉米沙星

以壳聚糖包覆的CdTe量子点为荧光探针,基于荧光猝灭法建立了吉米沙星定量测定方法。结果表明,体系的荧光强度与吉米沙星浓度在3.46×10-9～3.46×10-7 g.L-1范围内呈良好的线性关系(r=0.999 2),线性回归方程为F0/F=1.063 7+0.016 7c(g.L-1)。对2.77×10-7 g.L-1吉米沙星溶液进行7次平行测定的相对标准偏差为2.7%,基于荧光猝灭法相关理论证明了该相互作用过程为静态猝灭。本方法灵敏度高,检测线性范围宽,为吉米沙星定量测定提供了简便可靠的方法。     

Size-dependent optical properties and carriers dynamics in CdSe/ZnS quantum dots

Size-dependence of optical properties and energy relaxation in CdSe/ZnS quantum dots （QDs） were investigated by two-colour femtosecond （fs） pump-probe （400/800 nm） and picosecond time-resolved photoluminescence （ps TRPL） experiments. Pump-probe measurement results show that there are two components for the excited carriers relaxation, the fast one with a time constant of several ps arises from the Auger-type recombination, which shows almost particle sizeindependence. The slow relaxation component with a time constant of several decades of ns can be clearly determined with ps TRPL spectroscopy in which the slow relaxation process shows strong particle size-dependence. The decay time constants increase from 21 to 34 ns with the decrease of particle size from 3.2 to 2.1 nm. The room-temperature decay lifetime is due to the thermal mixing of bright and dark excitons, and the size-dependence of slow relaxation process can be explained very well in terms of simple three-level model.     

Chemiluminescence resonance energy transfer in the luminol-CdTe quantum dots conjugates

The luminol-CdTe quantum dots (QDs) conjugates were prepared through the reaction between -NH₂ and -COOH. The resonance energy transfer between chemiluminescence donor (luminol-H₂O₂ system) and quantum dots (QDs, with different emission peaks) acceptors (CRET) was investigated. The luminescence of QDs in luminol-QDs conjugates in the process of CRET was influenced by the molar ratio of luminol/QDs. It could reach higher luminescence intensity while the luminol/QDs value was 1/1. Quantum yield of QDs and overlapping areas between the emission spectrum of luminol and adsorption spectrum of QDs played important roles in the CRET efficiency of luminol-QDs conjugates. The higher CRET efficiency (21.2%) was observed when the 540 nm QDs were used as acceptors. This work will offer helpful knowledge for the CRET studies based on QDs.     

Coherent spectroscopy of semiconductor quantum dots

Coherent spectroscopy of semiconductor quantum dots, such as photon echo, accumulated photon echo, interferometric coherency measurement, quantum beat and coherent phonon measurement, are reviewed in relation to the historical progress in the coherent spectroscopy of semiconductors.     

水溶性CdTe:Mn量子点的双光子吸收

采用激发波长800 nm、脉宽50 fs、重复频率1 kHz的Ti:sapphire放大飞秒激光器作为激发光源,利用开孔Z扫描技术研究了不同粒径的CdTe:Mn量子点的非线性吸收性质。理论计算结果表明,同一生长时间CdTe:Mn量子点的双光子吸收系数是CdTe量子点的1.1倍,其双光子吸收系数随量子点尺寸的减小而增大,这是由于CdTe:Mn量子点非线性吸收属于反饱和吸收,掺杂了Mn元素,减小了表面缺陷浓度,表明掺杂量子点具有很好的双光子吸收现象。