- 标题
- 摘要
- 关键词
- 实验方案
- 产品
-
Photoluminescence Intensity Enhancement of Single Silicon Quantum Dots on a Metal Membrane with a Spacer
摘要： Silicon quantum dots (Si QDs) featuring high photoluminescence (PL) intensity are necessary for the realization of different photonic and photovoltaic devices, such as light-emitting diodes (LEDs) and luminescent solar concentrators (LSCs). Herein, Si QDs on a (cid:1)100–200 nm thin silicon dioxide membrane with a metal back-coating are prepared. The dots are formed from the device layer of a silicon-on-insulator (SOI) wafer by etching and thermal oxidation. Aluminum is sputtered on the backside of the membrane, acting as a back-surface mirror, changing the local density of optical modes, as well as the local excitation ?eld. The PL properties of such Si QDs are then characterized at the single-particle level. It is found that the PL yield of single Si QDs on the membrane is enhanced by approximately one order of magnitude, compared with that of Si QDs outside the membrane under the same excitation power. These results indicate that advances in nanofabrication can substantially improve the optical properties of Si QDs, thus paving the way for their application.
关键词： membranes,quantum dots,silicon,blinking,photoluminescence
更新于2025-11-21 11:24:58
-
Increase of photoluminescence blinking frequency of 3C–SiC nanocrystals with excitation power
摘要： Super-resolution optical fluctuation imaging is dependent on the blinking frequency of fluorophores. Consequently, improvement of the photoluminescence (PL) blink frequency is important. This is achieved for 3C–SiC nanocrystals (NCs) by simply increasing the excitation power. Using an excitation of 488 nm with powers of 5 μW to 50 μW, individual 3C–SiC NC always exhibits PL blinking with a short on-state sojourn time (< 0.1 s). A fast Fourier transform method is exploited to determine the PL switching frequency. It is found that the frequency of the bright state increases from 2 Hz to 20 Hz as the excitation power increases from 5 μW to 50 μW, which is explained by the Auger photonionization model.
关键词： photoluminescence,nanocrystals,Auger photonionization,blinking
更新于2025-11-20 15:33:11
-
Stark Effect and Environment-Induced Modulation of Emission in Single Halide Perovskite Nanocrystals
摘要： Organic-inorganic halide perovskites have emerged as promising materials for next generation solar cells. In nanostructured form also, these materials are excellent candidates for optoelectronic applications such as lasers and light emitting diodes for displays and lighting. While great progress has been achieved so far in optimizing the intrinsic photophysical properties of perovskite nanocrystals (NCs), in working opto-electronic devices external factors, such as the effects of conducting environment and of the applied electric field on exciton generation and photon emission have been largely unexplored. Here, we use NCs of the all-inorganic perovskite CsPbBr3 dispersed polyvinyl carbazole, a hole-conductor, and in polymethyl methacrylate, an insulator, to examine the effects of applied electric field and conductivity of the matrix on the perovskite photophysics at single-particle level. We found that the conducting environment causes a significant decrease of photoluminescence (PL) brightness of individual NCs due the appearance of intermediate-intensity emitting states with significantly shortened lifetime. Applied electric field has a similar effect and, in addition, causes a non-linear spectral-shift of the PL maxima, a combination of linear and quadratic Stark effect caused by environment-induced polarity and field-related polarizability. The environment and electric field effects are explained by ionization of the NCs through hole transfer and emission of the resulting negatively-charged excitons.
关键词： ionization,halide perovskite nanocrystals,single-particle spectroscopy,Stark effect,blinking
更新于2025-09-23 15:23:52
-
Redox-state dependent blinking of single photosystem I trimers at around liquid-nitrogen temperature
摘要： Efficient light harvesting in a photosynthetic antenna system is disturbed by a ragged and fluctuating energy landscape of the antenna pigments in response to the conformation dynamics of the protein. This situation is especially pronounced in Photosystem I (PSI) containing red shifted chlorophylls (red Chls) with the excitation energy much lower than the primary donor. The present study was conducted to clarify light-harvesting dynamics of PSI isolated from Synechocystis sp. PCC6803 by using single-molecule spectroscopy at liquid?nitrogen temperatures. Fluorescence emission at around 720 nm from the red Chls in single PSI trimers was monitored at 80–100 K. Intermittent variations in the emission intensities, so-called blinking, were frequently observed. Its time scale lay in several tens of seconds. The blinking amplitude depended on the redox state of the phylloquinone (A1). Electrochromic shifts of Chls induced by the negative charge on A1 were calculated based on the X-ray crystallographic structure. A Chl molecule, Chl-A839 (numbering according to PDB 5OY0), bound near A1 was found to have a large electrochromic shift. This Chl has strong exciton coupling with neighboring Chl (A838) whose site energy was predicted to be determined by interaction with an arginine residue (ArgF84) [Adolphs et al., 2010]. A possible scenario of the blinking was proposed. Conformational fluctuations of ArgF84 seesaw the excitation-energy of Chl-A838, which perturbs the branching ratio of excitation-energy between the red Chl and the cationic form of P700 as a quencher. The electrochromic shift of Chl-A839 enhances the effect of the conformation dynamics of ArgF84.
关键词： Cryogenic microscope,Phylloquinone,Fluorescence blinking,Site energy,Single-molecule spectroscopy,Electrochromic shift
更新于2025-09-23 15:23:52
-
Mechanism of photoluminescence intermittency in organic-inorganic perovskite nanocrystals
摘要： Lead halide perovskite nanocrystals have demonstrated their potential as active materials for optoelectronic applications over the past few years. Nevertheless one issue which hampers their applicability has to do with the observation of photoluminescence intermittency, commonly referred to as blinking, as in their inorganic counterparts. Such behavior, reported for structures well above the quantum confinement regime, has been discussed to be strongly related with the presence of charge carrier traps. In this work we analyze the characteristics of this intermittency and explore the dependence with the surrounding atmosphere, showing evidence for the critical role played by the presence of oxygen. We discuss a possible mechanism in which a constant creation/annihilation of halide-related carrier traps takes place under light irradiation, the dominant rate being determined by the atmosphere.
关键词： photoluminescence,Hybrid organic inorganic perovskites,spectroscopy,nanocrystal,blinking
更新于2025-09-23 15:23:52
-
A method for the statistical evaluation of the fluorescence intensity of single blinking quantum dots using a confocal fluorescence microscope
摘要： The evaluation of the fluorescence intensity of single quantum dots (QDs) using a confocal fluorescence microscope can provide an alternative approach for estimating the effects of environmental changes or surface modifications on the fluorescence intensity of single QDs. In the case of blinking QDs, irregular blinking would significantly influence the intensity evaluation results that are based on the analysis of one or a few single QDs. In this regard, statistical intensity evaluations based on a large number of single QDs would be helpful to estimate an approximate intensity value of single QDs with reduced effects of blinking on the evaluation results. Herein, we developed a convenient method to statistically evaluate the fluorescence intensity of a large number of single blinking QDs using Gaussian distribution. Based on the intensity analysis of thousands of single QDs, the fluorescence intensity of the single QDs evaluated using a confocal fluorescence microscope was approximately 4090 with little data fluctuation induced by blinking.
关键词： confocal fluorescence microscope,statistical evaluation,fluorescence intensity,single blinking quantum dots,Gaussian distribution
更新于2025-09-23 15:19:57
-
CuInS <sub/>2</sub> -Doped ZnS Quantum Dots Obtained via Non-Injection Cation Exchange Show Reduced but Heterogeneous Blinking and Provide Insights into Their Structurea??Optical Property Relationships
摘要： Cadmium-free CuInS2-doped ZnS quantum dots (QDs) are synthesized through a 2-step non-injection synthetic method. The resulting QDs are small (8 nm or less) and relatively isotropic with photoluminescence quantum yields (PL QY) up to almost 70% and emission peaks in the 560-600 nm window, depending on the amount of Zn precursor added. The results indicate small CuInS2 ‘clusters’ within a zinc-blende ZnS lattice are the radiative recombination centers in the nanoparticle. Interestingly, higher ensemble photoluminescence quantum yields (PL QY) result when cation exchange is less extensive (~80 % ZnS composition), while a reduction in blinking is observed when ZnS composition exceeds 99%. A wide heterogeneity in blinking behavior from QD-to-QD is evident and a subpopulation statistical analysis shows that the on-state dwell times change from multiexponential (or inverse power law) behavior towards more mono-exponential behavior for particles that spend more of their time in the on-state. These results indicate that, as the number of CuInS2 emitting centers is reduced, the number of pathways leading to the off-state decreases, and a model is proposed to relate this behavior to the QD structure. These results provide a novel route towards CuInS2-doped visible-light emitting ZnS QDs with high quantum yield and reduced blinking and provides insight into how the composition of dopant and host matrix affects the radiative recombination mechanisms in single particles.
关键词： non-injection cation exchange,CuInS2-doped ZnS,blinking,structure-optical property relationships,quantum dots
更新于2025-09-23 15:19:57
-
An experimental study on the blinking suppression mechanism of organic-inorganic formamidinium lead halide perovskite quantum dots on N-Type semiconductors
摘要： Lead halide perovskite has emerged as a potential material for a wide range of applications, including solar cells, light-emitting diode displays, lasing, and single photon emitters. To optimize their utilization in optoelectronic devices, the fundamental photophysical properties, especially their charge carrier transition and blinking behaviors, must be elucidated. In this study, we investigate the blinking behaviors of single formamidinium bromide perovskite quantum dots (FAPbBr3 PQDs) on the n-type TiO2 substrate. It is suggested that the electrons from TiO2 fill the trap states of FAPbBr3 PQD during Fermi-level equilibrium, which can reduce the possibility of capturing the hot electrons from PQD into the trap states. In addition, charge separation and charge recombination processes between PQD and TiO2 are expected to shorten the duration of the OFF state, thus stabilizing the fluorescence of PQDs.
关键词： optoelectronic devices,TiO2 substrate,charge carrier transition,perovskite quantum dots,blinking suppression
更新于2025-09-23 15:19:57
-
Influence of morphology on the blinking mechanisms and the excitonic fine structure of single colloidal nanoplatelets
摘要： Colloidal semiconductor nanoplatelets with a similar electronic structure as quantum wells have recently emerged as exciting materials for optoelectronic applications. Here we investigate how morphology affects important photoluminescence properties of single CdSe and core/shell CdSe/CdZnS nanoplatelets. By analyzing photoluminescence intensity-lifetime correlation and second-order photon correlation results, we demonstrate that, irrespective of the morphology, Auger recombination plays only a minor role in dictating the blinking behavior of the nanoplatelets. We find that a rough shell induces additional non-radiative channels presumably related to defects or traps of an imperfect shell. Furthermore, polarization-resolved spectroscopy analysis reveals exciton fine-structure splitting of the order of several tens of meV in rough-shell nanoplatelets at room temperature, which is attributed to exciton localization and is substantiated by theoretical calculations taking into account the nanoplatelet shape and electron–hole exchange interaction.
关键词： exciton fine structure,photoluminescence,nanoplatelets,blinking,Auger recombination
更新于2025-09-19 17:15:36
-
Lifetime super-resolution optical fluctuation imaging
摘要： In this paper, we propose a promising super-resolution imaging scheme in fluorescence lifetime domain (lifetime super-resolution optical fluctuation imaging, ltSOFI). ltSOFI has the potential to obtain super-resolution images by taking advantage of fluorescence lifetime blinking under wide-field lifetime detection. The proof-of-concept for ltSOFI was demonstrated through numerical simulation of high-order cumulant analysis on fluorescence lifetime blinking emitters. As a tentative experimental demonstration, we obtained super-resolution lifetime imaging from time-lapse FLIM recording of HeLa cells expressing a cAMP sensor using ltSOFI method. ltSOFI is expected to initiate a new dimension in the lifetime domain for blinking-based super-resolution microscopy.
关键词： fluorescence fluctuation,lifetime blinking,super-resolution
更新于2025-09-19 17:15:36