Efficiency of Cathodoluminescence Emission by Nitrogen‐Vacancy Color Centers in Nanodiamonds

Correlated electron microscopy and cathodoluminescence (CL) imaging using functionalized nanoparticles is a promising nanoscale probe of biological structure and function. Nanodiamonds (NDs) that contain CL‐emitting color centers are particularly well suited for such applications. The intensity of CL emission from NDs is determined by a combination of factors, including particle size, density of color centers, efficiency of energy deposition by electrons passing through the particle, and conversion efficiency from deposited energy to CL emission. This paper reports experiments and numerical simulations that investigate the relative importance of each of these factors in determining CL emission intensity from NDs containing nitrogen‐vacancy (NV) color centers. In particular, it is found that CL can be detected from NV‐doped NDs with dimensions as small as ≈40 nm, although CL emission decreases significantly for smaller NDs.     

Entangling a single NV centre with a superconducting qubit via parametric couplings between photons and phonons in a hybrid system

We propose an efficient scheme for generating entangled states between a single nitrogen-vacancy (NV) centre in diamond and a superconducting qubit in a hybrid set-up. In this device, the NV centre and the superconducting qubit couple to a nanomechanical resonator and a superconducting coplanar waveguide cavity, respectively, while the microwave cavity and the mechanical resonator are parametrically coupled with a tunable coupling strength. We show that, highly entangled states between the NV centre and the superconducting qubit can be achieved, by means of the Jaynes–Cummings interactions in the NV-resonator and qubit-cavity subsystems which transfer the entanglement between the vibration phonons and the cavity photons to the NV centre and the superconducting qubit. This work may provide interesting applications in quantum computation and communication with single NV spins and superconducting qubits.     

Spectrally and spatially resolved cathodoluminescence of nanodiamonds: local variations of the NV(0) emission properties

Here we report the spectrally and spatially resolved cathodoluminescence of diamond nanoparticles using focused fast electron beams in a transmission electron microscope. We demonstrate the possibility of quickly detecting various individual colour centres of different kinds on wide areas (several micrometres square) contained in nanoparticles separated by subwavelength distances. Among them, nanoparticles containing one or more neutral nitrogen-vacancy (NV(0)) intensity maxima have been seen, attributable to individual emitters. Thanks to a spatial resolution which is solely limited by charge carrier diffusion in the case of a fast electron (80 keV) setup, the spectra of two individual NV(0) emitters separated by 80 nm inside a nanoparticle have been spatially discerned. A shift of the zero phonon line (ZPL) between the two emitters, which we attribute to internal stress, is shown to arise even within the same nanoparticle. Detailed emission spectra (ZPL, phonon lines and Huang-Rhys factor, directly linked to the relaxation energy of the colour centre) in 51 individual NV(0) centres have been measured in 39 particles. The ZPL and Huang-Rhys factor are found to be measurably dispersed, while the phonon energies keep constant.     

Unraveling In Vivo Brain Transport of Protein‐Coated Fluorescent Nanodiamonds

Nanotheranostics, combining diagnostics and therapy, has the potential to revolutionize treatment of neurological disorders. But one of the major obstacles for treating central nervous system diseases is the blood–brain barrier (BBB) preventing systemic delivery of drugs and optical probes into the brain. To overcome these limitations, nanodiamonds (NDs) are investigated in this study as they are a powerful sensing and imaging platform for various biological applications and possess outstanding stable far‐red fluorescence, do not photobleach, and are highly biocompatible. Herein, fluorescent NDs encapsulated by a customized human serum albumin–based biopolymer (polyethylene glycol) coating (dcHSA‐PEG) are taken up by target brain cells. In vitro BBB models reveal transcytosis and an additional direct cell–cell transport via tunneling nanotubes. Systemic application of dcHSA‐NDs confirms their ability to cross the BBB in a mouse model. Tracking of dcHSA‐NDs is possible at the single cell level and reveals their uptake into neurons and astrocytes in vivo. This study shows for the first time systemic NDs brain delivery and suggests transport mechanisms across the BBB and direct cell–cell transport. Fluorescent NDs are envisioned as traceable transporters for in vivo brain imaging, sensing, and drug delivery.     

Quality of Information Flow in the Backend of a Product Development Process: a Case Study

The increasing need for products that are able to reliably deliver complex functionality with a high degree of innovation presents a major challenge to the modern day product creation processes. In order to be able to use information on the field behaviour of previous products in the design of new products, increasingly detailed information needs to be retrieved from the market in an increasingly shorter time. The purpose of this study is to analyse, in a typical case in the consumer electronics industry, whether the underlying business process is able to generate this information with adequate quality sufficiently quickly. Information models of the company's service centre and call centre were developed using the concepts of maturity index on reliability. The results showed that the structure of the information handling process resulted in a massive data loss (up to 60% of the data gathered by the service centres) and also in serious data quality degradation. Would this information have not been lost, it could have been used by development teams for preventive and corrective actions. Copyright © 2004 John Wiley & Sons, Ltd.     

烯烃配位聚合及催化剂基础研究进展：活性中心浓度测定

从动力学研究角度出发,指出催化活性中心浓度测定对于烯烃配位聚合反应机理和催化剂研究的重要意义。简要介绍了在烯烃配位聚合领域中应用的各种活性中心浓度测定方法,并对这些方法的特点及存在问题进行了分析和讨论。     

Nanodiamond‐Based Theranostic Platform for Drug Delivery and Bioimaging

Nanodiamonds (NDs) are promising candidates for biomedical application due to their excellent biocompatibility and innate physicochemical properties. In this Concept article, nanodiamond‐based theranostic platforms, which combine both drug delivery features and bioimaging functions, are discussed. The latest developments of therapeutic strategies are introduced and future perspectives for theranostic NDs are addressed.     

Ultrahigh hardness of carbon steel surface realized by novel solid carburizing with rapid diffusion of carbon nanostructures

In this study, a novel rapid solid carburizing process with a large diffusion depth using nano-diamonds(NDs) was conducted for low carbon steel. Changes of annealed NDs were obtained by Raman spectroscopy and transmission electron microscopy(TEM), and the results suggested that the NDs experience a stripping process before a special solid-reaction with surface iron atoms from steel substrate. Onionlike carbon(OLC) derived from the annealed NDs provided broken graphitic ribbons as carbon sources that accelerated the rate of adsorption and diffusion. Examination of the surface layer at equilibrium using TEM and X-ray photoelectron spectroscopy(XPS) also revealed the special state of carbon, and an ultrafine mixed phase microstructure was obtained by rapid solid-phase transformation. As a result, a surface hardened layer with ultrahigh hardness and a smooth transition region were realized. We believe that these kinds of diamond or graphitic structures with high activity states have an important influence not only on adsorption and diffusion but also on this special solid-phase transformation.     

Ultrasmall Cu2‐xS Nanodots for Highly Efficient Photoacoustic Imaging‐Guided Photothermal Therapy

Monodisperse, ultrasmall (<5 nm) Cu_2?xS nanodots (u‐Cu_2?xS NDs) with significantly strong near‐infrared absorption and conversion are successfully demonstrated for effective deep‐tissue photoacoustic imaging‐guided photothermal therapy both in vitro and in vivo. Owing to ultrasmall nanoparticle size and high water dispersibility as well as long stability, such nanodots possess a prolonged circulation in blood and good passive accumulation within tumors through the enhanced permeability and retention effect. These u‐Cu_2?xS NDs have negligible side effects to both blood and normal tissues according to in vivo toxicity evaluations for up to 3 months, showing excellent hemo/histocompatibility. Furthermore, these u‐Cu_2?xS NDs can be thoroughly cleared through feces and urine within 5 days, showing high biosafety for further potential clinical translation. This novel photoacoustic imaging‐guided photothermal therapy based on u‐Cu_2?xS NDs composed of a single component shows great prospects as a multifunctional nanoplatform with integration and multifunction for cancer diagnosis and therapy.     

Size-controlled MoS<Subscript>2</Subscript> nanodots supported on reduced graphene oxide for hydrogen evolution reaction and sodium-ion batteries

Transition metal dichalcogenide nanodots (NDs) have received considerable interest.We report a facile bottom-up synthetic route for MoS2 NDs by using molybdenum pentachloride and L-cysteine as precursors in oleylamine.The synthesis of NDs with a narrow size distribution ranging from 2.2 to 5.3 nm,was tailored by controlling the reaction time.Because of its coating characteristics,oleyalmine leads to uniformity and monodispersity of the NDs.Moreover,the NDs synthesized have large specific surface areas providing active sites.Graphene possesses outstanding conductivity.Combining the advantages of the two materials,the 0D/2D material exhibits superior electrochemical performance because of the 2D permeable channels for ion adsorption,energy storage,and conversion.The as-prepared MoS2/rGO (～2.2 nm) showed a stable capacity of 220 mAh·g-1 after 10,000 cycles at the current density of 20 A·g-1.Furthermore,a reversible capacity ～140 mAh·g-1 was obtained at a much higher current density of 40 A·g-1.Additionally,this composite exhibited superior catalytic performance evidenced by a small overpotential (222 mV) to afford 10 mA·cm-2,and a small Tafel slope (59.8 mV·decade-1) with good acid-stability.The facile approach may pave the way for the preparation of NDs with these nanostructures for numerous applications.     

Elucidation of Photoluminescence Blinking Mechanism and Multiexciton Dynamics in Hybrid Organic–Inorganic Perovskite Quantum Dots

Halide perovskites (ABX₃) have emerged as promising materials in the past decade owing to their superior photophysical properties, rendering them potential candidates as solar cells, light‐emitting diode displays, and lasing materials. To optimize their utilization into optoelectronic devices, fundamental understanding of the optical behaviors is necessary. To reveal the comprehensive structure–property relationship, CH₃NH₃PbBr₃ (MAPbBr₃) perovskite quantum dots (PQDs) of three different sizes are prepared by controlling the precipitation temperature. Photoluminescence (PL) blinking, a key process that governs the emission efficiency of the PQD materials, is investigated in detail by the time‐resolved spectroscopic measurements of individual dots. The nature of the generated species in the course of blinking events is identified, and the mechanism governing the PL blinking is studied as a function of PQD sizes. Further, the practical applicability of MAPbBr₃ PQDs is assessed by studying the multiexciton dynamics under high photoexcitation intensity under which most of the display devices work. Ultrafast transient absorption spectroscopy helped in uncovering the volume‐dependent Auger recombination rates, which are further explored by comparing the early‐time transitions related to surface trap states and higher band states.     

Smart Nanovehicles Based on pH‐Triggered Disassembly of Supramolecular Peptide‐Amphiphiles for Efficient Intracellular Drug Delivery

A novel type of nanovehicle (NV) based on stimuli‐responsive supramolecular peptide‐amphiphiles (SPAs, dendritic poly (L‐lysine) non‐covalently linked poly (L‐leucine)) is developed for intracellular drug delivery. To determine the pH‐dependent mechanism, the supramolecular peptide‐amphiphile system (SPAS) is investigated at different pH conditions using a variety of physical and chemical approaches. The pH‐triggered disassembly of SPAS can be attributed to the disappearance of non‐covalent interactions within SPAs around the isoelectric point of poly (L‐leucine). SPAS is found to encapsulate guest molecules at pH 7.4 but release them at pH 6.2. In this way, SPAS is able to act as a smart NV to deliver its target to tumor cells using intracellular pH as a trigger. The DOX‐loaded NVs are approximately 150 nm in size. In vitro release profiles and confocal laser scanning microscopy (CLSM) images of HepG2 cells confirm that lower pH conditions can trigger the disassembly of NVs and so achieve pH‐dependent intracellular DOX delivery. In vitro cytotoxicity of the DOX‐loaded NVs to HepG2 cells demonstrate that the smart NVs enhance the efficacy of hydrophobic DOX. Fluorescence‐activated cell sorting (FACS) and CLSM results show that the NVs can enhance the endocytosis of DOX into HepG2 cells considerably and deliver DOX to the nuclei.     

Application of the TOC thinking processes to challenging assumptions of profit and cost centre performance measurement

The interaction of the measurement criteria of cost centres and profit centres, and the resultant effect on organizational profit is examined by applying the Theory of Constraints thinking processes. Three cases are described based on the assumptions that a profit centre should maximize profit and a cost centre should at least recover its costs. These cases illustrate that there will exist conflict between profit centres and cost centres due to disagreement about transfer pricing and hourly tariffs; that some outsourcing decisions taken in isolation can lead to a spiral of declining competitiveness; and that the attempts by a cost centre to maximize cost recovery leads to a lower profit for the organization. The thinking process logic trees show that these negative effects are caused by the application of wrong measurement criteria.     

In vivo Metabolic Imaging of Insulin with Multiphoton Fluorescence of Human Insulin–Au Nanodots

Functional human insulin–Au nanodots (NDs) are synthesized for the in vivo imaging of insulin metabolism. Benefiting from its efficient red to near infrared fluorescence, deep tissue subcellular uptake of insulin–Au NDs can be clearly resolved through a least‐invasive harmonic generation and two‐photon fluorescence (TPF) microscope. In vivo investigations on mice ear and ex vivo assays on human fat tissues conclude that cells with rich insulin receptors have higher uptake of administrated insulin. Interestingly, the insulin–Au NDs can even permeate into lipid droplets (LDs) of adipocytes. Using this newly discovered metabolic phenomenon of insulin, it is found that enlarged adipocytes in type II diabetes mice have higher adjacent/LD concentration contrast with small‐sized ones in wild type mice. For human clinical samples, the epicardial adipocytes of patients with diabetes and coronary artery disease (CAD) also show elevated adjacent/LD concentration contrast. As a result, human insulin–Au nanodots provide a new approach to explore subcellular insulin metabolism in model animals or patients with metabolic or cardiovascular diseases.     

Fe3Si nanodots epitaxially grown on Si(111) substrates using ultrathin SiO2 film technique

Ultrahigh density (> 10¹² cm⁻²) Fe₃Si nanodots (NDs) are epitaxially grown on Si(111) substrates by codeposition of Fe and Si on the ultrathin SiO₂ films with ultrahigh density nanovoids. We used two kinds of methods for epitaxial growth: molecular beam epitaxy (MBE) and solid phase epitaxy. For MBE, low temperature (< 300 °C) growth of the Fe₃Si NDs is needed to suppress the interdiffusion between Fe atoms deposited on the surfaces and Si atoms in the substrate. These epitaxial NDs exhibited the ferromagnetism at low temperatures, which were expected in terms of the application to the magnetic memory device materials.     

One-pot synthesis of MoSe<Subscript>2</Subscript> hetero-dimensional hybrid self-assembled by nanodots and nanosheets for electrocatalytic hydrogen evolution and photothermal therapy

We designed and prepared a hetero-dimensional hybrid (HDH) based on molybdenum selenide (MoSe2) nanodots (NDs) anchored in few-layer MoSe2 nanosheets (NSs) (MoSe2 HDH) via a one-pot hydrothermal process.The MoSe2 HDH exhibits excellent electrocatalytic activity toward hydrogen evolution reaction (HER).This is because,on the one hand,the edge-abundant features of MoSe2 NDs and the unique defect-rich structure at the interface of MoSe2 NSs/NDs could bring in more active sites for HER;on the other hand,the random stacking of the flake-like MoSe2 NSs on the surface of the supporting electrode may achieve efficient charge transport.Additionally,the MoSe2 HDH shows good water stability,desirable biocompatibility,and high near infrared (NIR) photothermal conversion efficiency.Therefore,the MoSe2 HDH is investigated as a nanomedicine in NIR photothermal therapy (PTT) for cancer.Specifically,the MoSe2 HDH can be applied as a dual-modal probe for computed tomography (CT) and photoacoustic tomography (PA) imaging owing to its strong X-ray attenuation ability and NIR absorption.Therefore,the MoSe2 HDH,combining PTr with CT/PA imaging into one system,holds great potential for imaging-guided cancer theranostics.This work may provide an ingenious strategy to prepare other hetero-dimensional layered transition metal dichalcogenides.     

Functional Nanovalves on Protein‐Coated Nanoparticles for In vitro and In vivo Controlled Drug Delivery

A multifunctional mesoporous drug delivery system that contains fluorescent imaging molecules, targeting proteins, and pH‐sensitive nanovalves is developed and tested. Three nanovalve‐mesoporous silica nanoparticle (NV‐MSN) systems with varied quantities of nanovalves on the surface are synthesized. These systems are characterized and tested to optimize the trade‐off between the coverage of nanovalves on the MSNs to effectively trap and deliver cargo, and the remaining underivatized silanol groups that can be used for protein attachments. The NV‐MSN system that has satisfactory coverage for high loading and spare silanols is chosen, and transferrin (Tf) is integrated into the system. Abiotic studies are performed to test the operation of the nanovalve in the presence of the protein. In vitro studies are carried out to demonstrate the autonomous activation and function of the nanovalves in the system under biological conditions. Enhanced cellular uptake of the Tf‐modified MSNs is seen using fluorescence microscopy and flow cytometry in MiaPaCa‐2 cells. The MSNs are then tested using SCID mice, which show that both targeted and untargeted NV‐MSN systems are fully functional to effectively deliver cargo. These new multifunctional nanoparticles serve proof of concept of nanovalve functionality in the presence of large proteins and demonstrate another dimension of MSN‐based theranostic platforms.     

Improving Defect‐Based Quantum Emitters in Silicon Carbide via Inorganic Passivation

Defect‐based color centers in wide‐bandgap crystalline solids are actively being explored for quantum information science, sensing, and imaging. Unfortunately, the luminescent properties of these emitters are frequently degraded by blinking and photobleaching that arise from poorly passivated host crystal surfaces. Here, a new method for stabilizing the photoluminescence and charge state of color centers based on epitaxial growth of an inorganic passivation layer is presented. Specifically, carbon antisite‐vacancy pairs (CAV centers) in 4H‐SiC, which serve as single‐photon emitters at visible wavelengths, are used as a model system to demonstrate the power of this inorganic passivation scheme. Analysis of CAV centers with scanning confocal microscopy indicates a dramatic improvement in photostability and an enhancement in emission after growth of an epitaxial AlN passivation layer. Permanent, spatially selective control of the defect charge state can also be achieved by exploiting the mismatch in spontaneous polarization at the AlN/SiC interface. These results demonstrate that epitaxial inorganic passivation of defect‐based quantum emitters provides a new method for enhancing photostability, emission, and charge state stability of these color centers.     

Ultrahigh Photocatalytic Rate at a Single‐Metal‐Atom‐Oxide

Metal oxides, as one of the mostly abundant and widely utilized materials, are extensively investigated and applied in environmental remediation and protection, and in energy conversion and storage. Most of these diverse applications are the result of a large diversity of the electronic states of metal oxides. Noticeably, however, many metal oxides present obstacles for applications in catalysis, mainly due to the lack of efficient active sites with desired electronic states. Here, the fabrication of single‐tungsten‐atom‐oxide (STAO) is demonstrated, in which the metal oxide's volume reaches its minimum as a unit cell. The catalytic mechanism in the STAO is determined by a new single‐site physics mechanism, named as quasi‐atom physics. The photogenerated electron transfer process is enabled by an electron in the spin‐up channel excited from the highest occupied molecular orbital to the lowest unoccupied molecular orbital +1 state, which can only occur in STAO with W⁵⁺. STAO results in a record‐high and stable sunlight photocatalytic degradation rate of 0.24 s^?1, which exceeds the rates of available photocatalysts by two orders of magnitude. The fabrication of STAO and its unique quasi‐atom photocatalytic mechanism lays new ground for achieving novel physical and chemical properties using single‐metal‐atom oxides (SMAO).     

Blinking statistics of silicon quantum dots

The blinking statistics of numerous single silicon quantum dots fabricated by electron-beam lithography, plasma etching, and oxidation have been analyzed. Purely exponential on- and off-time distributions were found consistent with the absence of statistical aging. This is in contrast to blinking reports in the literature where power-law distributions prevail as well as observations of statistical aging in nanocrystal ensembles. A linear increase of the switching frequency with excitation power density indicates a domination of single-photon absorption processes, possibly through a direct transfer of charges to trap states without the need for a bimolecular Auger mechanism. Photoluminescence saturation with increasing excitation is not observed; however, there is a threshold in excitation (coinciding with a mean occupation of one exciton per nanocrystal) where a change from linear to square-root increase occurs. Finally, the statistics of blinking of single quantum dots in terms of average on-time, blinking frequency and blinking amplitude reveal large variations (several orders) without any significant correlation demonstrating the individual microscopic character of each quantum dot.