High-Sensitivity Fluorescence Lifetime Thermal Sensing Based on CdTe Quantum Dots

The potential use of CdTe quantum dots as luminescence nano-probes for lifetime fluorescence nano-thermometry is demonstrated. The maximum thermal sensitivity achievable is strongly dependent on the quantum dot size. For the smallest sizes (close to 1 nm) the lifetime thermal sensitivity overcomes those of conventional nano-probes used in fluorescence lifetime thermometry.     

Nanoscale Thermometry with a Quantum Dot

A two-terminal quantum dot bridging a temperature difference can operate as a thermometer by probing the Fermi-Dirac distributions of the electron gas on both sides of the quantum dot. This thermometry requires that the dot’s energy levels are spaced in energy by many kT and that the intrinsic energetic width of the energy resonances are either much larger or much smaller than kT. We compare these two regimes of operation and discuss the intermediate regime which separates them. Quantum-dot thermometry can assist in mesoscopic thermal experiments where short-distance temperature gradients elude most thermometry techniques.     

Self-assembled InAs/GaAs quantum dots covered by different strain reducing layers exhibiting strong photo- and electroluminescence in 1.3 and 1.55 microm bands

The effect of different InGaAs and GaAsSb strain reducing layers on photoluminescence and electroluminescence from self-assembled InAs/GaAs quantum dots grown by metal-organic vapour phase epitaxy was investigated. The aim was to shift their luminescence maximum towards optical communication wavelengths at 1.3 or 1.55 microm. Results show that covering by InGaAs strain reducing layer provides stronger shift of photoluminescence maximum (up to 1.55 microm) as compared to GaAsSb one with similar strain in the structure. This is caused by the increase of quantum dot size during InGaAs capping and reduction of quantum confinement of the electron wave function which spreads into the cap. Unfortunately, the weaker electron confinement in quantum dots is a reason of a considerable blue shift of electroluminescence from these InGaAs structures since optical transitions move to InGaAs quantum well. Although strong electroluminescence at 1300 nm was achieved from quantum dots covered by both types of strain reducing layers, the GaAsSb strain reducing layer is more suitable for long wavelength electroluminescence due to higher electron confinement potential allowing suppression of thermal carrier escape from quantum dots.     

Simultaneous Local Heating/Thermometry Based on Plasmonic Magnetochromic Nanoheaters

A crucial challenge in nanotherapies is achieving accurate and real‐time control of the therapeutic action, which is particularly relevant in local thermal therapies to minimize healthy tissue damage and necrotic cell deaths. Here, a nanoheater/thermometry concept is presented based on magnetoplasmonic (Co/Au or Fe/Au) nanodomes that merge exceptionally efficient plasmonic heating and simultaneous highly sensitive detection of the temperature variations. The temperature detection is based on precise optical monitoring of the magnetic‐induced rotation of the nanodomes in solution. It is shown that the phase lag between the optical signal and the driving magnetic field can be used to detect viscosity variations around the nanodomes with unprecedented accuracy (detection limit 0.0016 mPa s, i.e., 60‐fold smaller than state‐of‐the‐art plasmonic nanorheometers). This feature is exploited to monitor the viscosity reduction induced by optical heating in real‐time, even in highly inhomogeneous cell dispersions. The magnetochromic nanoheater/thermometers show higher optical stability, much higher heating efficiency and similar temperature detection limits (0.05 °C) compared to state‐of‐the art luminescent nanothermometers. The technological interest is also boosted by the simpler and lower cost temperature detection system, and the cost effectiveness and scalability of the nanofabrication process, thereby highlighting the biomedical potential of this nanotechnology.     

Temperature‐Dependent Exciton and Trap‐Related Photoluminescence of CdTe Quantum Dots Embedded in a NaCl Matrix: Implication in Thermometry

Temperature‐dependent optical studies of semiconductor quantum dots (QDs) are fundamentally important for a variety of sensing and imaging applications. The steady‐state and time‐resolved photoluminescence properties of CdTe QDs in the size range from 2.3 to 3.1 nm embedded into a protective matrix of NaCl are studied as a function of temperature from 80 to 360 K. The temperature coefficient is found to be strongly dependent on QD size, with the highest sensitivity obtained for the smallest size of QDs. The emission from solid‐state CdTe QD‐based powders is maintained with high color purity over a wide range of temperatures. Photoluminescence lifetime data suggest that temperature dependence of the intrinsic radiative lifetime in CdTe QDs is rather weak, and it is mostly the temperature‐dependent nonradiative decay of CdTe QDs which is responsible for the thermal quenching of photoluminescence intensity. By virtue of the temperature‐dependent photoluminescence behavior, high color purity, photostability, and high photoluminescence quantum yield (26%–37% in the solid state), CdTe QDs embedded in NaCl matrices are useful solid‐state probes for thermal imaging and sensing over a wide range of temperatures within a number of detection schemes and outstanding sensitivity, such as luminescence thermochromic imaging, ratiometric luminescence, and luminescence lifetime thermal sensing.     

量子点材料应用于发光二极管的研究进展

量子点材料因具有独特的光学特性而被广泛应用于发光领域,用其作发光层可制成量子点发光二极管。与有机电致发光二极管相比,量子点发光二极管具有发光光谱窄、色域广、稳定性好、寿命长、制作成本低等优势。本文介绍了量子点发光器件在国内外的热点研究方向及取得的成果,并对其发展前景进行展望。     

A Tunneling Dielectric Layer Free Floating Gate Nonvolatile Memory Employing Type‐I Core–Shell Quantum Dots as Discrete Charge‐Trapping/Tunneling Centers

A nonvolatile memory with a floating gate structure is fabricated using ZnSe@ZnS core–shell quantum dots as discrete charge‐trapping/tunneling centers. Systematical investigation reveals that the spontaneous recovery of the trapped charges in the ZnSe core can be effectively avoided by the type‐I energy band structure of the quantum dots. The surface oleic acid ligand surrounding the quantum dots can also play a role of energy barrier to prevent unintentional charge recovery. The device based on the quantum dots demonstrates a large memory window, stable retention, and good endurance. What is more, integrating charge‐trapping and tunneling components into one quantum dot, which is solution synthesizable and processible, can largely simplify the processing of the floating gate nonvolatile memory. This research reveals the promising application potential of type‐I core–shell nanoparticles as the discrete charge‐trapping/tunneling centers in nonvolatile memory in terms of performance, cost, and flexibility.     

Controlled photonic manipulation of proteins and other nanomaterials

The ability to controllably handle the smallest materials is a fundamental enabling technology for nanoscience. Conventional optical tweezers have proven useful for manipulating microscale objects but cannot exert enough force to manipulate dielectric materials smaller than about 100 nm. Recently, several near-field optical trapping techniques have been developed that can provide higher trapping stiffness, but they tend to be limited in their ability to reversibly trap and release smaller materials due to a combination of the extremely high electromagnetic fields and the resulting local temperature rise. Here, we have developed a new form of photonic crystal "nanotweezer" that can trap and release on-command Wilson disease proteins, quantum dots, and 22 nm polymer particles with a temperature rise less than ~0.3 K, which is below the point where unwanted fluid mechanical effects will prevent trapping or damage biological targets.     

Spin state readout by quantum jump technique: for the purpose of quantum computing

Utilizing the Pauli-blocking mechanism we show that shining circular polarized light on a singly-charged quantum dot induces spin dependent fluorescence. Employing the quantum-jump technique we demonstrate that this resonance luminescence, due to a spin dependent optical excitation, serves as an excellent readout mechanism for measuring the spin state of a single electron confined to a quantum dot.     

Two-fold emission from the S-shell of PbSe/CdSe core/shell quantum dots

The optical properties of PbSe/CdSe core/shell quantum dots with core sizes smaller than 4 nm in the 5-300 K range are reported. The photoluminescence spectra show two peaks, which become increasingly separated in energy as the core diameter is reduced below 4 nm. It is shown that these peaks are due to intrinsic exciton transitions in each quantum dot, rather than emission from different quantum dot sub-ensembles. Most likely, the energy separation between the peaks is due to inter-valley coupling between the L-points of PbSe. The temperature dependence of the relative intensities of the peaks implies that the two emitting states are not in thermal equilibrium and that dark exciton states must play an important role.     

Competition between surface trapping and nonradiative energy transfer to gold nanofilm

Nonradiative resonant energy transfer from CdSeS quantum dot to gold nanofilm was investigated by taking nanosecond and picosecond time resolved photoluminescence measurements. Surface plasma resonant absorption peak of gold nanofilm was adjusted to meet the near resonant conditions with the fluorescence peak of quantum dot by changing the thickness. Surface trapping state was proved to be the origin of the long lifetime component by comparing fresh and eight months aged quantum dot. It was observed that the excitonic state lifetime of the quantum dots was reduced by nonradiative resonant energy transfer to gold nanofilm. Nonradiative resonant energy transfer time, which was comparable with the surface trapping time, was calculated based on the data of picosecond photoluminescence measurements. No nonradiative energy transfer from surface trapping state to gold nanofilm, thus the lifetime of surface trapping state was not affected obviously. It is suggested that in the assembly combined with quantum dot and gold nanostructure, nonradiative energy transfer will occur after the population of excitonic state, and compete with surface trapping process. The interactions between surface trapping state and gold nanoflim were not exhibited.     

光激发下Li6Gd(BO3)3:Ce晶体发光和衰减的温度依赖特性

研究了80-500K范围内，光激发下Li6Gd（BO3）3：Ce晶体发光和衰减的温度依赖特性．在346nm光激发下，热猝灭占优势，发光随温度升高而降低．在274nm光激发下，发光由Gd^3＋向Ce^3＋的能量传递和热猝灭共同决定：低于200K时，能量传递占支配地位，发光随温度升高而增强；高于200K时，热猝灭占优势，发光随温度升高而减弱．225K以下，辐射跃迁占优势，衰减随温度升高而略有增大；225K以上，无辐射跃迁占优势，衰减随温度升高而减小．利用经典的热猝灭公式和Arrhenius公式，获取的激活能分别为0．33和0．32eV．     

Layer-by-layer assembly of multicolored semiconductor quantum dots towards efficient blue, green, red and full color optical films

Multicolored semiconductor quantum dots have shown great promise for construction of miniaturized light-emitting diodes with compact size, low weight and cost, and high luminescent efficiency. The unique size-dependent luminescent property of quantum dots offers the feasibility of constructing single-color or full-color output light-emitting diodes with one type of material. In this paper, we have demonstrated the facile fabrication of blue-, green-, red-?and full-color-emitting semiconductor quantum dot optical films via a layer-by-layer assembly technique. The optical films were constructed by alternative deposition of different colored quantum dots with a series of oppositely charged species, in particular, the new use of cationic starch on glass substrates. Semiconductor ZnSe quantum dots exhibiting blue emission were deposited for fabrication of blue-emitting optical films, while semiconductor CdTe quantum dots with green and red emission were utilized for construction of green-?and red-emitting optical films. The assembly of integrated blue, green and red semiconductor quantum dots resulted in full-color-emitting optical films. The luminescent optical films showed very bright emitting colors under UV irradiation, and displayed dense, smooth and efficient luminous features, showing brighter luminescence in comparison with their corresponding quantum dot aqueous colloid solutions. The assembled optical films provide the prospect of miniaturized light-emitting-diode applications.     

Optical properties of HgTe colloidal quantum dots

Room temperature photodetection with HgTe colloidal quantum films is reported between 2 and 5 μm for particles of sizes between ~5 and ~12 nm diameter, and photodetection extends to 7 μm at 80 K. The size-tuning of the absorption of HgTe colloidal quantum dots, their optical cross section and the infrared absorption depth of films are measured. The tuning with radius is empirically given by [see formula in text] where R is in nm. The optical cross section of the colloidal dots at 415 nm is approximately proportional to their volume and given by σ(Hg)(415) = 2.6 ± 0.4 10(-17) cm(2)/mercury atom. The size-dependent optical cross section at the band edge ~1.5 10(-15) cm(2) is consistent with the expected oscillator strength of the quantum dots. The absorption depth of HgTe colloidal dot films is short, about 1-2 μm, which is an advantage for thin film devices. These properties agree rather well with the expectation from the k · p model. HgTe colloidal quantum dot thin films show a strong tuning with temperature with a large positive thermal shift between 0.4 and 0.2 meV K(-1), decreasing with decreasing size within the size range studied and this is attributed primarily to electron-phonon effects.     

Damage-free top-down processes for fabricating two-dimensional arrays of 7 nm GaAs nanodiscs using bio-templates and neutral beam etching

The first damage-free top-down fabrication processes for a two-dimensional array of 7 nm GaAs nanodiscs was developed by using ferritin (a protein which includes a 7 nm diameter iron core) bio-templates and neutral beam etching. The photoluminescence of GaAs etched with a neutral beam clearly revealed that the processes could accomplish defect-free etching for GaAs. In the bio-template process, to remove the ferritin protein shell without thermal damage to the GaAs, we firstly developed an oxygen-radical treatment method with a low temperature of 280?°C. Then, the neutral beam etched the defect-free nanodisc structure of the GaAs using the iron core as an etching mask. As a result, a two-dimensional array of GaAs quantum dots with a diameter of ～ 7 nm, a height of ～ 10 nm, a high taper angle of 88° and a quantum dot density of more than 7 × 10(11) cm(-2) was successfully fabricated without causing any damage to the GaAs.     

Protein‐Directed Synthesis of NIR‐Emitting,Tunable HgS Quantum Dots and their Applications in Metal‐Ion Sensing

The development of luminescent mercury sulfide quantum dots (HgS QDs) through the bio‐mineralization process has remained unexplored. Herein, a simple, two‐step route for the synthesis of HgS quantum dots in bovine serum albumin (BSA) is reported. The QDs are characterized by UV–vis spectroscopy, Fourier transform infrared (FT‐IR) spectroscopy, luminescence, Raman spectroscopy, transmission electron microscopy (TEM), X‐ray photoelectron spectroscopy (XPS), circular dichroism (CD), energy dispersive X‐ray analysis (EDX), and picosecond‐resolved optical spectroscopy. Formation of various sizes of QDs is observed by modifying the conditions suitably. The QDs also show tunable luminescence over the 680–800 nm spectral regions, with a quantum yield of 4–5%. The as‐prepared QDs can serve as selective sensor materials for Hg(II) and Cu(II), based on selective luminescence quenching. The quenching mechanism is found to be based on Dexter energy transfer and photoinduced electron transfer for Hg(II) and Cu(II), respectively. The simple synthesis route of protein‐capped HgS QDs would provide additional impetus to explore applications for these materials.     

The influence of post-growth annealing on the optical properties of InAs quantum dot chains grown on pre-patterned GaAs(100)

We report on the effect of post-growth thermal annealing of [011]- ,[011(-)]-, and [010]-oriented quantum dot chains grown by molecular beam epitaxy on GaAs(100) substrates patterned by UV-nanoimprint lithography. We show that the quantum dot chains experience a blueshift of the photoluminescence energy, spectral narrowing, and a reduction of the intersubband energy separation during annealing. The photoluminescence blueshift is more rapid for the quantum dot chains than for self-assembled quantum dots that were used as a reference. Furthermore, we studied polarization resolved photoluminescence and observed that annealing reduces the intrinsic optical anisotropy of the quantum dot chains and the self-assembled quantum dots.     

Perovskite Quantum Dots with Near Unity Solution and Neat‐Film Photoluminescent Quantum Yield by Novel Spray Synthesis

In this study, a novel perovskite quantum dot (QD) spray‐synthesis method is developed by combining traditional perovskite QD synthesis with the technique of spray pyrolysis. By utilizing this new technique, the synthesis of cubic‐shaped perovskite QDs with a homogeneous size of 14 nm is demonstrated, which shows an unprecedented stable absolute photoluminescence quantum yield ≈100% in the solution and even in the solid‐state neat film. The highly emissive thin films are integrated with light emission devices (LEDs) and organic light emission displays (OLEDs). The color conversion type QD‐LED (ccQD‐LED) hybrid devices exhibit an extremely saturated green emission, excellent external quantum efficiency of 28.1%, power efficiency of 121 lm W^?1, and extraordinary forward‐direction luminescence of 8 500 000 cd m^?2. The conceptual ccQD‐OLED hybrid display also successfully demonstrates high‐definition still images and moving pictures with a 119% National Television System Committee 1931 color gamut and 123% Digital Cinema Initiatives‐P3 color gamut. These very‐stable, ultra‐bright perovskite QDs have the properties necessary for a variety of useful applications in optoelectronics.     

Effects of separate carrier generation on the emission properties of InAs/GaAs quantum dots

Individual quantum dots have been studied by means of microphotoluminescence with dual-laser excitation. The additional infrared laser influences the dot charge configuration and increases the dot luminescence intensity. This is explained in terms of separate generation of excess electrons and holes into the dot from the two lasers. With increasing dot density and/or sample temperature, the increase of the luminescence intensity vanishes progressively, while the possibility to control the dot charge remains.     

Nanoassembled Peptide Biosensors for Rapid Detection of Matrilysin Cancer Biomarker

Early detection of cancer is likely to be one of the most effective means of reducing the cancer mortality rate. Hence, simple and ultra‐quick methods for noninvasive detection of early‐stage tumors are highly sought‐after. In this study, a nanobiosensing platform with a rapid response time of nearly 30 s is introduced for the detection of matrilysin—the salivary gland cancer biomarker—with a limit of detection as low as 30 nm . This sensing platform is based on matrilysin‐digestible peptides that bridge gold nanoparticle (AuNPs) cores (≈30–50 nm) and carbon quantum dot (CDs) satellites (≈9 nm). A stepwise synthesis procedure is used for self‐assembly of AuNP‐peptide‐CDs, ensuring their long‐term stability. The AuNP‐peptide‐CDs produce ideal optical signals, with noticeable fluorescence quenching effects. Upon peptide cleavage by matrilysin, CDs leave the surface of AuNPs, resulting in ultra‐fast detectable violet and visible fluorescent signals.