Fluorescence Intermittency in Monolayer WSe_2

Fluorescence intermittent dynamics of single quantum emitters in monolayer WSe2 are investigated via measuring spectrally resolved time traces and time-dependent fluorescence intensity trajectories. Analysis of fluorescence trajectories and spectral shifting reveal a correlation between the fluorescence intermittency and spectral diffusion.A model of an inverse power law can be used to understand the observed blinking dynamics.     

Enhanced fluorescence intermittency of CdSe-ZnS quantum-dot clusters

Fluorescence intermittency, or blinking, of individual close-packed clusters containing two or more CdSe-ZnS quantum dots (QDs) was investigated. The QD clusters exhibited rapid, intense blinking that was distinct from that of isolated QDs blinking independently. This enhanced blinking is suggested to occur when the QDs in the cluster become electronically coupled. The nature of this coupling is not known, though electrons trapped from QDs when they blink off may play a role by altering the electronic environment of neighboring QDs and enhancing their fluorescence properties.     

Calculation of the quantum efficiency for the absorption on confinement levels in quantum dots

The quantum efficiency of the absorption on quantum confinement levels is investigated. This is achieved by modeling the electron confinement in a spherical quantum dot (QD). The confinement levels are calculated using both infinite and finite rectangular quantum wells. The spectral internal quantum efficiency is evaluated within both the models, by computing Einstein’s coefficients for the transitions between confinement levels. The size of QDs (1–3 nm radius) leads to negligible many body effects. The nature of the QD material and of the matrix embedding is taken into account in the finite rectangular quantum well approximation and introduces only a small correction. The temperature dependence of the efficiency is also taken into account. A numerical application is performed for a silicon QD of 2.5 nm radius, embedded in amorphous silica. It is proved that the absorption threshold shifts toward the far infrared limit and that the spectral internal quantum efficiency reaches 4–5% at the threshold.     

Models of Semiconductor Quantum Dots Blinking based on Spectral Diffusion

Optics and Spectroscopy - Three models of single colloidal quantum dot emission fluctuations (blinking) based on spectral diffusion were considered analytically and numerically. It was shown that...     

室温下表面极化效应对量子点带隙和吸收峰波长的影响

对于离散在本底介质中的纳米晶体量子点,考虑表面极化效应,通过像电荷法建立极化势能项,应用微扰法求解激子的薛定谔方程,得到了与本底介电系数直接相关的量子点带隙解析表达式.对不同本底中尺寸依赖的量子点带隙、第一吸收峰波长、第一吸收峰波长移动进行的计算表明,表面极化效应对量子点的带隙和第一吸收峰波长有明显的影响.随着本底介电系数的增大,量子点的带隙减小,第一吸收峰波长红移.量子点在不同本底中的第一吸收峰波长移动会在某个固定粒径达到最大值,最大值对应的粒径取决于量子点种类.     

Laser light scattering and correlation techniques for characterization of colloidal suspensions

Particle motion in colloidal suspensions causes Doppler shifts in scattered laser light. For pure diffusion, the resulting spectral broadening may be measured by intensity interferometry and photon correlation techniques. Measured line widths or decay times yield particle size information. Electrophoretic mobilities may be determined, if an electric field is applied to the suspension. However, resulting line shifts can be extremely small and real-time optical phase processing may be required to resolve it. Finally, information about particle interactions may be obtained by studying angular cross sections or by photon correlation measurements on a small number of particles, i.e. using a very small scattering volume.Dedicated to Professor Harry Thomas on the occasion of his 60th birthday     

界面电子转移对量子点荧光闪烁行为的影响

利用激光扫描共聚焦显微系统分别测量了CdSe/ZnS量子点在SiO2玻片表面、铟锡氧化物(ITO)纳米粒子表面和聚甲基丙烯酸甲酯(PMMA)薄膜表面上的荧光闪烁行为.研究发现,不同界面环境中量子点的亮态发光持续时间的概率密度都服从指数修正的幂律分布P(t)∝t-αexp(-t/μ).与处于SiO2玻片表面的情况相比,在ITO表面上的单量子点具有非常短暂的亮态发光持续时间,而在PMMA表面的单量子点亮态发光持续时间最长.这种荧光闪烁行为的不同主要归因于量子点与三种材料之间的界面电子转移特性.     

R6G单分子表面增强共振拉曼散射光谱探测研究

以共焦显微系统为平台,研究了不同浓度的R6G银溶胶的表面增强共振拉曼散射(SERRS)光谱, 结果表明不同浓度溶液中的R6G分子表现出了不同的光谱特性。在浓度为10-13mol·L-1的R6G银溶胶中 得到了R6G单分子的表面增强共振拉曼散射光谱,观察到了一些光谱非均匀变化现象,如谱色散、谱线的 强度起伏、拉曼谱的偏振化以及分子的闪烁等,并对这些现象进行了分析,证明得到的是R6G单分子的 SERRS光谱。文章还对单分子检测中的一些关键问题进行了分析与讨论,确定了单分子SERRS光谱检测的 适当条件。     

Blueshifts of emission energy from InAs quantum dots in GaAs matrix due to narrowed interdot spacing: a token of the integrity of a nanostructure

The shifts of emission energy from InAs quantum dots (QDs) in the GaAs matrix due to change in the QD stacking period have been numerically analyzed by investigating the strain modified shifts of band edges. Narrower stacking results in a blueshift of emission energy from direct band gap transition provided the QD spacing is wide enough to avoid electronic coupling. Through a comparison with existing experimental results in the literature, processing methods and variables that have benefits in achieving a blueshift have been inferred. A blueshift through decreased QD spacing has been proposed as a token of the integrity of a processed QD nanostructure . PACS 68.65.+g; 78.66.Fd     

Recognition of spectrally degraded and frequency-shifted vowels in acoustic and electric hearing

The present study measured the recognition of spectrally degraded and frequency-shifted vowels in both acoustic and electric hearing. Vowel stimuli were passed through 4, 8, or 16 bandpass filters and the temporal envelopes from each filter band were extracted by half-wave rectification and low-pass filtering. The temporal envelopes were used to modulate noise bands which were shifted in frequency relative to the corresponding analysis filters. This manipulation not only degraded the spectral information by discarding within-band spectral detail, but also shifted the tonotopic representation of spectral envelope information. Results from five normal-hearing subjects showed that vowel recognition was sensitive to both spectral resolution and frequency shifting. The effect of a frequency shift did not interact with spectral resolution, suggesting that spectral resolution and spectral shifting are orthogonal in terms of intelligibility. High vowel recognition scores were observed for as few as four bands. Regardless of the number of bands, no significant performance drop was observed for tonotopic shifts equivalent to 3 mm along the basilar membrane, that is, for frequency shifts of 40%-60%. Similar results were obtained from five cochlear implant listeners, when electrode locations were fixed and the spectral location of the analysis filters was shifted. Changes in recognition performance in electrical and acoustic hearing were similar in terms of the relative location of electrodes rather than the absolute location of electrodes, indicating that cochlear implant users may at least partly accommodate to the new patterns of speech sounds after long-time exposure to their normal speech processor.     

On-axis spectral shifts and spectral switches of Gaussian Schell-model beams focused by an astigmatic aperture lens

Starting from the propagation law of partially coherent light, the on-axis spectral shifts and spectral switches of Gaussian Schell-model (GSM) beams focused by an astigmatic aperture lens are studied. It is shown that, as compared with an aberration-free case whose spectral shifts and spectral switches are induced by spatial correlation and aperture diffraction, the spectral shifts and spectral switches of GSM beams also depend upon the astigmatism of the lens for an astigmatism case. Detailed numerical calculations are made to illustrate the behavior of spectral shifts and spectral switches of GSM beams focused by an astigmatic aperture lens.     

Spectral anomalies due to temporal correlation in a white-light interferometer

We present what we believe to be the first experimental demonstration of anomalous spectral behavior such as spectral shifts and spectral switches due to temporal correlation around the intensity minima in a white-light interferometer. Unusual behavior in the number of spectral fringes, measured within the source bandwidth, as a function of path delay between the interfering beams is also reported. Experimental observations match well with the spectra calculated by using the interference law in the spectral domain.     

Semi-empiric approach to the calculation of H2O and CO2 line broadening and shifting

A semi-empiric approach to the calculation of spectral line half-widths and shifts is proposed. This approach is based on the Anderson approximation and includes the correction factors, the parameters of which can be determined by fitting the broadening or shifting coefficients to the experimental data. This allows sufficiently accurate predictions of the parameters of line profiles that were not measured. The coefficients of CO₂ and H₂O spectral line broadening and shifting due to air and nitrogen pressure are calculated, as well as the coefficients of their temperature dependence. The calculated coefficients agree satisfactorily with measured values.     

Spectral characterization of diffusion with chemical shift resolution: Highly concentrated water-in-oil emulsion

We present a modulated gradient spin-echo method, which uses a train of sinusoidally shaped gradient pulses separated by 180° radio-frequency (RF) pulses. The RF pulses efficiently refocus chemical shifts and de-phasing due to susceptibility differences, resulting in undistorted, high-resolution diffusion weighted spectra. This allows for the simultaneous spectral characterization of the diffusion of several molecular species with different chemical shifts. The technique is robust against susceptibility artifacts, field inhomogeneity and imperfections in the gradient generating equipment. The feasibility of the technique is demonstrated by measuring the diffusion of water, oil, and water-soluble salt in a highly concentrated water-in-oil emulsion. The diffusion of water and salt reveal precise information about the droplet size distribution below the μm-range. Common droplet size distribution explains both the data for water with finite long-range diffusion and the data for salt with negligible long-range diffusion. The results of water diffusion show that the technique is efficient in deconvolving the effects of molecular exchange between droplets and restricted diffusion within droplets. The effects of water exchange suggest that droplets of different sizes are uniformly distributed within the sample.     

Influence of the shallow impurity environment on the luminescence of single-quantum dots

The evolution of low-temperature photoluminescence (PL) spectra of single GaAs/AlGaAs quantum dots (QD) is studied as a function of laser excitation power. At very low powers, where multi-exciton occupation of the QD can be excluded, an unexpected and pronounced spectral evolution is observed. In this weak excitation regime, a significant difference in the fine structure of single-QD spectra is observed not only among different, structurally identical QDs of the same sample, but also among spectra taken from the same single QD excited above and below the AlGaAs barrier. A time-resolved, two-color pump and probe PL experiment on a single QD indicates relaxation times between the different spectral shapes in the ms-range. A model, taking into account the influence of the shallow impurities in the environment of each QD, explains the experimental results.     

Charge distribution in a Kondo-correlated quantum dot

We report on direct measurement of charge and its distribution in a Kondo correlated quantum dot (QD). A noninvasive potential-sensitive detector, in proximity with a QD, reveals that, although the conductance of the QD is significantly enhanced as it enters the Kondo regime, the average charge remains unaffected. This demonstrates the separation between spin and charge degrees of freedom. We find, however, under certain conditions, an abrupt redistribution of charge in the QD, taking place with an onset of Kondo correlation. This suggests a correlation between the spin and charge degrees of freedom.     

Quantum Discord Dynamics of Three Qubits in Non-Markovian Environments

We investigate the dynamics of palrwise quantum discord （QD） for a mixed three-qubit W-type state in three independent non-Markovian reservoirs at zero temperature, each of which is modeled by a leaky cavity with Lorentzian spectral density. The influence of the environment＇s amount of non-Markovianity, the detuning between the qubit frequency and the cavity centre frequency, and the purity of the initial state on the QD dynamics are analyzed in detail. It is found that in the non-Maxkovian regime the system-reservoir interactions induce QD revivals and oscillations no matter whether the detuning is zero or not. Moreover, QD can be preserved for a long time if the non-Markovian condition and the detuning condition are satisfied simultaneously.     

Diffusion-controlled electron transfer processes and power-law statistics of fluorescence intermittency of nanoparticles

A mechanism involving diffusion-controlled electron transfer processes in Debye and non-Debye dielectric media is proposed to elucidate the power-law distribution for the lifetime of a blinking quantum dot. This model leads to two complementary regimes of power law with a sum of the exponents equal to 2, and to a specific value for the exponent in terms of a distribution of the diffusion correlation times. It also links the exponential bending tail with energetic and kinetic parameters.     

Second-harmonic generation in asymmetric quantum dots in the presence of a static magnetic field

The second-harmonic generation(SHG) coefficient in an asymmetric quantum dot(QD) with a static magnetic field is theoretically investigated.Within the framework of the effective-mass approximation,we obtain the confined wave functions and energies of electrons in the QD.We also obtain the SHG coefficient by the compact-density-matrix approach and the iterative method.The numerical results for the typical GaAs/AlGaAs QD show that the SHG coefficient depends strongly on the magnitude of magnetic field,parameters of the asymmetric potential and the radius of the QD.The resonant peak shifts with the magnetic field or the radius of the QD changing.     

Modeling of exciton diffusion in amorphous organic thin films

Time-resolved photoluminescence spectroscopy of amorphous organic thin films of aluminum tris-(8-hydroxyquinoline) show emission spectra that redshift with time following excitation by ultrafast laser pulses. Based on reports of similar phenomena in other materials, we attribute this effect to the exciton diffusion between energetically dissimilar molecules by means of F?rster transfer. In analyzing results at 295, 180, 75, and 35 K, we show that existing theoretical treatments of exciton diffusion require two modifications to self-consistently fit our data: one must include spatial disorder in the model, and the energy dependence of F?rster transfer must be calculated using the donor-acceptor spectral overlap, instead of a Boltzman distribution. Monte Carlo simulations utilizing these changes yield results that are self-consistent with the observed spectral shifts.