All‐optical modulation based on silicon quantum dot doped SiOx:Si‐QD waveguide

All‐optical modulation based on silicon quantum dot doped SiO_x:Si‐QD waveguide is demonstrated. By shrinking the Si‐QD size from 4.3 nm to 1.7 nm in SiO_x matrix (SiO_x:Si‐QD) waveguide, the free‐carrier absorption (FCA) cross section of the Si‐QD is decreased to 8 × 10⁻¹⁸ cm² by enlarging the electron/hole effective masses, which shortens the PL and Auger lifetime to 83 ns and 16.5 ps, respectively. The FCA loss is conversely increased from 0.03 cm⁻¹ to 1.5 cm⁻¹ with the Si‐QD size enlarged from 1.7 nm to 4.3 nm due to the enhanced FCA cross section and the increased free‐carrier density in large Si‐QDs. Both the FCA and free‐carrier relaxation processes of Si‐QDs are shortened as the radiative recombination rate is enlarged by electron–hole momentum overlapping under strong quantum confinement effect. The all‐optical return‐to‐zero on‐off keying (RZ‐OOK) modulation is performed by using the SiO_x:Si‐QD waveguides, providing the transmission bit rate of the inversed RZ‐OOK data stream conversion from 0.2 to 2 Mbit/s by shrinking the Si‐QD size from 4.3 to 1.7 nm.     

Fabrication of three‐dimensional photonic crystals in quantum‐dot‐based materials

Controlling spontaneous emission (SE) is of fundamental importance to a diverse range of photonic applications including but not limited to quantum optics, low power displays, solar energy harvesting and optical communications. Characterized by photonic bandgap (PBG) property, three‐dimensional (3D) photonic crystals (PCs) have emerged as a promising synthetic material, which can manipulate photons in much the same way as a semiconductor does to electrons. Emission tunable nanocrystal quantum dots (QDs) are ideal point sources to be embedded into 3D PCs towards active devices. The challenge however lies in the combination of QDs with 3D PCs without degradation of their emission properties. Polymer materials stand out for this purpose due to their flexibility of incorporating active materials. Combining the versatile multi‐photon 3D micro‐fabrication techniques, active 3D PCs have been fabricated in polymer‐QD composites with demonstrated control of SE from QDs. With this milestone novel miniaturized photonic devices can thus be envisaged.     

Multicolor Light‐Emitting Diodes with MoS2 Quantum Dots

Molybdenum disulfide (MoS₂) quantum dots (QDs) are known for their excitation‐wavelength‐dependent photoluminescent (PL) properties. However, the mechanism of this phenomenon is still unclear. Here, small size MoS₂ QDs with a narrow size distribution are synthesized. Based on the decay study and PL dynamics, a reasonable radiation model is presented to understand the special PL properties, i.e., the carrier recombination in the localized surface defect states generated the PL. Accordingly, this optical property is used to fabricate multicolor light‐emitting devices with the same MoS₂ QDs. The emission color covers the full visible spectrum from blue to red, only by adjusting the thickness of the down‐conversion QD layers.     

A method to obtain ground state electroluminescence from 1.3μm emitting InAs/GaAs quantum dots grown by molecular beam epitaxy

1.3μm emitting InAs/GaAs quantum dots(QDs) have been grown by molecular beam epitaxy and QD light emitting diodes(LEDs) have been fabricated.In the electroluminescence spectra of QD LEDs,two clear peaks corresponding to the ground state emission and the excited state emission are observed.It was found that the ground state emission could be achieved by increasing the number of QDs contained in the active region because of the state filling effect.This work demonstrates a way to control and tune the emitting wavelength of QD LEDs and lasers.     

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.     

Optimum Quantum Yield of the Light Emission from 2 to 10 nm Hydrosilylated Silicon Quantum Dots

Optimizing the light‐emitting efficiency of silicon quantum dots (Si QDs) has been recently intensified by the demand of the practical use of Si QDs in a variety of fields such as optoelectronics, photovoltaics, and bioimaging. It is imperative that an understanding of the optimum light‐emitting efficiency of Si QDs should be obtained to guide the design of the synthesis and processing of Si QDs. Here an investigation is presented on the characteristics of the photoluminescence (PL) from hydrosilylated Si QDs in a rather broad size region (≈2–10 nm), which enables an effective mass approximation model to be developed, which can very well describe the dependence of the PL energy on the QD size for Si QDs in the whole quantum‐confinement regime, and demonstrates that an optimum PL quantum yield (QY) appears at a specific QD size for Si QDs. The optimum PL QY results from the interplay between quantum‐confinement effect and surface effect. The current work has important implications for the surface engineering of Si QDs. To optimize the light‐emission efficiency of Si QDs, the surface of Si QDs must be engineered to minimize the formation of defects such as dangling bonds at the QD surface and build an energy barrier that can effectively prevent carriers in Si QDs from tunneling out.     

Ultrasensitive PbS‐Quantum‐Dot Photodetectors for Visible–Near‐Infrared Light Through Surface Atomic‐Ligand Exchange

A surface atomic‐ligand exchange method is applied the first time in the construction of photodetectors (PDs) based on PbS quantum dots (QDs) for ultrasensitivity. The device thus produces a high photosensitivity to visible and near‐infrared light with a photoresponsivity up to 7.5 × 10³ A W^?1 and a high stability in air. In particular, these PbS‐QD‐based PDs show the capability of following a pulse light with a frequency up to 100 kHz well at a relatively fast response time/recovery time of ≈4/40 μs, much faster than most previous QD‐based PDs. The short response time is attributed to modification for the surface of the PbS‐QDs by cetyltrimethylammonium bromide treatment, which effectively improves the contact between the QDs and the Au electrodes, leading to extracting a high carrier mobility (≈0.142 cm² V^?1 s^?1). These findings show the great potential of PbS‐QDs as high‐speed nano‐photodetectors, and, more importantly, demonstrate the importance of the surface atomic‐ligand exchange method in the construction of QD‐based devices.     

Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO2 Interface in Quantum Dot‐Sensitized Solar Cells

Quantum dot‐sensitized solar cells (QDSSCs) have emerged as a promising solar architecture for next‐generation solar cells. The QDSSCs exhibit a remarkably fast electron transfer from the quantum dot (QD) donor to the TiO₂ acceptor with size quantization properties of QDs that allows for the modulation of band energies to control photoresponse and photoconversion efficiency of solar cells. To understand the mechanisms that underpin this rapid charge transfer, the electronic properties of CdSe and PbSe QDs with different sizes on the TiO₂ substrate are simulated using a rigorous ab initio density functional method. This method capitalizes on localized orbital basis set, which is computationally less intensive. Quite intriguingly, a remarkable set of electron bridging states between QDs and TiO₂ occurring via the strong bonding between the conduction bands of QDs and TiO₂ is revealed. Such bridging states account for the fast adiabatic charge transfer from the QD donor to the TiO₂ acceptor, and may be a general feature for strongly coupled donor/acceptor systems. All the QDs/TiO₂ systems exhibit type II band alignments, with conduction band offsets that increase with the decrease in QD size. This facilitates the charge transfer from QDs donors to TiO₂ acceptors and explains the dependence of the increased charge transfer rate with the decreased QD size.     

High‐Responsivity Photodetectors Based on Formamidinium Lead Halide Perovskite Quantum Dot–Graphene Hybrid

Highly performance photodetector requires a wide range of responses of the incident photons and converts them to electrical signals efficiently. Here, a photodetector based on formamidinium lead halide perovskite quantum dots (e.g., FAPbBr₃ QDs)–graphene hybrid, aiming to take the both advantages of the two constituents. The FAPbBr₃ QD–graphene layer not only benefits from the high mobility and wide spectral absorption of the graphene material but also from the long charge carrier lifetime and low dark carrier concentration of the FAPbBr₃ QDs. The photodetector based on FAPbBr₃ QD–graphene hybrid exhibits a broad spectral photoresponse ranging from 405 to 980 nm. A photoresponsivity of 1.15 × 10⁵AW⁻¹ and an external quantum efficiency as high as 3.42 × 10⁷% are obtained under an illumination power of 3 µW at 520 nm wavelength. In detail, a high responsivity is achieved in 405–538 nm, while a relatively low but fast response is observed in 538–980 nm. The photoelectric conversion mechanism of this hybrid photodetector is investigated in the view of built‐in electric field from the QD–graphene contact which improves the photoconductive gain.     

State‐of‐the‐Art and Trends in Synthesis,Properties, and Application of Quantum Dots‐Based Nanomaterials

Quantum dots (QDs) with a nanoscale size range have attracted significant attention in various areas of nanotechnology due to their unique properties. Different strategies for the synthesis of QD nanoparticles are reported in which various factors, such as size, impurities, shape, and crystallinity, affect the QDs fundamental properties. Consequently, to obtain QDs with appropriate physical properties, it is required to select a synthesis method which allows enough control over the surface chemistry of QDs through fine‐tuning of the synthesis parameters. Moreover, QDs nanocrystals are recently used in multidisciplinary research integrated with biological interfaces. The state‐of‐the‐art methods for synthesizing QDs and bioconjugation strategies to provide insight into various applications of these nanomaterials are discussed herein.     

Mussel‐Inspired Polymer Grafting on CsPbBr3 Perovskite Quantum Dots Enhancing the Environmental Stability

Mussel‐inspired chemistry, motivated by the adhesive proteins secreted by mussels for attachment to wet surfaces, is an emerging technique for manipulating the surface properties of a variety of materials. Here, a facile mussel‐inspired poly(N‐vinyl pyrrolidone) (PVP) polymer encapsulation with trivial influence on inherent optical properties of perovskite quantum dots (QDs) is demonstrated to efficiently combat the low intrinsic thermal, chemical, and photostability of CsPbBr₃ QDs. The suitability of photopolymer‐processed PVP‐CsPbBr₃ QDs flexible films as color components in white light–emitting devices is substantiated.     

Flexible Ti‐Doped FeOOH Quantum Dots/Graphene/Bacterial Cellulose Anode for High‐Energy Asymmetric Supercapacitors

Ti‐doped FeOOH quantum dots (QD) decorated on graphene (GN) sheets are designed and fabricated by a facile and scalable synthesis route. Importantly, the Ti‐doped FeOOH QD/GN are successfully dispersed within bacterial cellulose (BC) substrate as bending anode with large loading mass for flexible supercapacitor. By virtue of its favorable architecture, this composite electrode exhibits a remarkable areal capacitance of 3322 mF cm^?2 at 2 mA cm^?2, outstanding cycle performance (94.7% capacitance retention after 6000 cycles), and excellent mechanical strength (68.7 MPa). To push the energy density of flexible supercapacitors, the optimized asymmetric supercapacitor using Mn₃O₄/GN/BC as positive electrode and Ti‐doped FeOOH QD/GN/BC as negative electrode can be cycled reversibly in the operating voltage range of 0–1.8 V and displays ultrahigh areal energy density of 0.541 mWh cm^?2, ultrahigh volumetric energy density of 9.02 mWh cm^?3, reasonable cycling performance (9.4% decay in specific capacitance after 5000 cycles), and good capacitive retention at bending state.     

Identifying multi‐excitons in quantum dots: the subtle connection between electric dipole moments and emission linewidths

The emission linewidths of excitonic complexes confined in quantum dots (QDs) mirror their interaction with a defect‐induced, fluctuating charge environment, a phenomenon known as spectral diffusion. Interestingly, extended excitonic complexes that comprise several interacting excitons exhibit significantly smaller emission linewidths if compared to the optical fingerprint of their building block, a sole exciton. Hence, it is not the absolute, but the relative electric dipole moment that governs the directly accessible emission linewidths. Exemplarily we investigate this matter based on differing exciton and biexciton emission linewidths of single GaN QDs with varying emission energies, i.e. QD dimensions. Our results establish the full width at half maximum (FWHM) or any other linewidths criterion for the identification of excitonic complexes, a technique that can directly be applied to polar but even non‐polar QD materials. Additionally, we find an emission energy dependent trend for the FWHM ratios of the biexciton and the exciton (XX_FWHM/X_FWHM) in perfect agreement with their relative dipole moment ratios as derived from our 8‐band‐ k · p based treatment of the Coulomb and exchange interaction within these multi‐particle complexes. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

超小晶粒锡掺杂CsPbBr3蓝光量子点的合成及其光学性能研究

近年来,铅卤钙钛矿CsPbX₃ (X=Cl,Br或I)因其具有荧光波段可调、荧光量子产率高(Photoluminescence quantum yield,PLQY)以及荧光半峰宽窄等优点而被广泛应用于光电器件领域.然而,与PLQY接近于100%的绿光和红光相比,蓝光卤素钙钛矿的PLQY仍比较低.在此,采用过饱和结晶的方法在室温下合成了粒径低于4 nm的超小晶粒锡(Sn)掺杂CsPbBr₃量子点,并对其结构特性和光学特性进行了研究.结果表明:随着SnBr₂添加量的增大,量子点晶粒的粒径略微减小,荧光发射峰发生蓝移,粒径由3.33 nm (SnBr₂为0.03 mmol)减小到2.23 nm(SnBr₂为0.06 mmol时),对应的荧光发射峰由490 nm蓝移至472 nm.当SnBr₂添加量为0.05 mmol时合成的超小晶粒锡掺杂CsPbBr₃量子点显示出最优的光学性能,其粒径约为2.91 nm,对应的XRD各晶面衍射峰强度最强,...     

半导体自组织量子点量子发光机理与器件

介绍了自组织量子点单光子发光机理及器件研究进展.主要内容包括：半导体液滴自催化外延GaAs纳米线中InAs量子点和GaAs量子点的单光子发光效应、自组织InAs/GaAs量子点与分布布拉格平面微腔耦合结构的单光子发光效应和器件制备,单量子点发光的共振荧光测量方法、量子点单光子参量下转换实现的纠缠光子发射、单光子的量子存储效应以及量子点单光子发光的光纤耦合输出芯片制备等.     

量子点背光技术的研究进展

量子点材料因具有发光波长可调,色度纯,量子效率高等优异特性而受到广泛关注,在光致发光高色彩显示方面有着巨大的应用潜力。本文综述了量子点背光技术的研究进展,主要对比了QDs On-Chip、QDs On-Surface及QDs On-Edge 3种量子点背光主流技术的基本原理及结构,并分析了它们在液晶显示领域的应用,未来前景及面临的挑战;然后介绍了几种新型的量子点背光技术,并对两种量子点背光新技术进行重点说明:一种是采用低温注塑成型工艺将量子点与高分子材料均匀混合为一体,用于制备直下式背光的量子点体散射型结构扩散板;另一种新技术是采用丝网印刷或喷墨打印工艺将量子点转印至导光板表面,形成应用于侧入式背光的量子点网点微结构导光板。这两种背光都具有制备工艺简单、成本低、生产效率高等特点,对高色域液晶显示的研究及发展意义深远。     

Near‐field optical enhancement by lead‐sulfide quantum dots and metallic nanoparticles for SERS

There is a growing interest in using quantum dots (QDs) and metallic nanoparticles (NPs), both for luminescence enhancement and surface‐enhanced Raman scattering (SERS). Here, we study the electromagnetic‐field enhancement that can be generated by lead‐sulfide (PbS) QDs using three‐dimensional finite‐element simulations. We investigate the field enhancement associated with combinations of PbS QDs with metallic NPs and substrates. The results show that high field enhancement can be achieved by combining PbS QDs with metallic NPs of larger sizes. The ideal size for Ag NPs is 25 nm, providing a SERS enhancement factor of ~5*10⁸ for light polarization parallel to the NP dimer axis and a gap of 0.6 nm. For Au NPs, the bigger the size, the higher is the field for the studied diameters, up to 50 nm. The near‐field values for PbS QDs above metallic substrates were found to be lower compared to the case of PbS QD‐metal NP dimers. This study provides the understanding for the design and application of QDs for the enhancement of near‐field phenomena. Copyright © 2013 John Wiley & Sons, Ltd.     

Quantum Dots Microstructural Metrology: From Time-Resolved Spectroscopy to Spatially Resolved Electron Microscopy

Colloidal quantum dots (QDs) have unique optical and electrical properties with promising applications in next-generation semiconductor technologies, including displays, lighting, solar cells, photodetectors, and image sensors. Advanced analytical tools to probe the optical, morphological, structural, compositional, and electrical properties of QDs and their ensemble solid films are of paramount importance for the understanding of their device performance. In this review, comprehensive studies on the state-of-the-art metrology approaches used in QD research are introduced, with particular focus on time-resolved (TR) and spatially resolved (SR) spectroscopy and microscopy. Through discussing these analysis techniques in different QD system, such as various compositions, sizes, and shell structures, the critical roles of these TR-spectroscopic and SR-microscopic techniques are highlighted, which provide the structural, morphological, compositional, optical, and electrical information to precisely design QDs and QD solid films. The employment of TR and SR analysis in integrated QD device systems is also discussed, which can offer detailed microstructural information for achieving high performance in specific applications. In the end, the current limitations of these analytical tools are discussed, and the future development of the possibility of interdisciplinary research in both QD fundamental and applied fields is prospected.     

Development and Investigation of Ultrastable PbS/CdS/ZnS Quantum Dots for Near‐Infrared Tumor Imaging

Achieving bright, reliable, robust, and stable probes for in vivo imaging is becoming extremely urgent for the cancer imaging research community. To date very few works have reported on elucidating in the varied and chemically complex biological milieu. The authors report detailed investigations of the synthesis of near‐infrared, water dispersive, strongly luminescent, and highly stable PbS/CdS/ZnS core/shell/shell quantum dots (QDs). These QDs are extremely stable, they could keep their initial morphology, dispersion status, and photoluminescence (PL) in phosphate buffered saline buffer for as long as 14 months. The QDs also show excellent photostability and could keep ≈80% of their initial PL intensity after 1 h continuous, strong UV illumination. More interestingly, they show negligible toxicity to cultured cells even at high QDs concentration. Given these outstanding properties, the QDs are explored for in vivo, tumor imaging in mice. With one order of magnitude lower QD concentration (0.04 mg mL^–1), significantly weaker laser intensity (0.04 W cm^–2 vs ≈1 W cm^–2), and considerably shorter signal integration time (≤1 ms vs hundreds of ms) as compared to the best reported rare earth doped nanoparticles, the QDs show high emission intensity even at injection depth of ≈2.5 mm.     

The influence of the quantum dot/polymethylmethacrylate composite preparation method on the stability of its optical properties under laser radiation

Photoluminescent semiconductor nanocrystals, quantum dots (QDs), are nowadays one of the most promising materials for developing a new generation of fluorescent labels, new types of light-emitting devices and displays, flexible electronic components, and solar panels. In many areas the use of QDs is associated with an intense optical excitation, which, in the case of a prolonged exposure, often leads to changes in their optical characteristics. In the present work we examined how the method of preparation of quantum dot/polymethylmethacrylate (QD/PMMA) composite influenced the stability of the optical properties of QD inside the polymer matrix under irradiation by different laser harmonics in the UV (355 nm) and visible (532 nm) spectral regions. The composites were synthesized by spin-coating and radical polymerization methods. Experiments with the samples obtained by spin-coating showed that the properties of the QD/PMMA films remain almost constant at values of the radiation dose below ~10 fJ per particle. Irradiating the composites prepared by the radical polymerization method, we observed a monotonic increase in the luminescence quantum yield (QY) accompanied by an increase in the luminescence decay time regardless of the wavelength of the incident radiation. We assume that the observed difference in the optical properties of the samples under exposure to laser radiation is associated with the processes occurring during radical polymerization, in particular, with charge transfer from the radical particles inside QDs. The results of this study are important for understanding photophysical properties of composites on the basis of QDs, as well as for selection of the type of polymer and the composite synthesis method with quantum dots that would allow one to avoid the degradation of their luminescence.