Despite the interest in improving the sensitivity of optical sensors using plasmonic nanoparticles (NPs) (rods, wires, and stars), the full structural characterization of complex shape nanostructures is challenging. Here, we derive from a single scanning transmission electron microscope diffraction map (4D-STEM) a detailed determination of both the 3D shape and atomic arrangement of an individual 6-branched AuAg nanostar (NS) with high-aspect-ratio legs. The NS core displays an icosahedral structure, and legs are decahedral rods attached along the 5-fold axes at the core apexes.
View Article and Find Full Text PDFWe report the synthesis of near-infrared (IR)-emitting core/shell/shell quantum dots of CuInZnS/ZnSe/ZnS and their phase transfer to water. The intermediate ZnSe shell was added to inhibit the migration of ions from the standard ZnS shell into the emitting core, which often leads to a blue shift in the emission profile. By engineering the interface between the core and terminal shell layer, the optical properties can be controlled, and emission was maintained in the near-IR region, making the materials attractive for biological applications.
View Article and Find Full Text PDFKnowledge of the nucleosynthetic isotope composition of the outermost protoplanetary disk is critical to understand the formation and early dynamical evolution of the Solar System. We report the discovery of outer disk material preserved in a pristine meteorite based on its chemical composition, organic-rich petrology, and N-rich, deuterium-rich, and O-poor isotope signatures. We infer that this outer disk material originated in the comet-forming region.
View Article and Find Full Text PDFWe describe a new synthetic methodology for the preparation of high quality, emission tuneable InP-based quantum dots (QDs) using a solid, air- and moisture-tolerant primary phosphine as a group-V precursor. This presents a significantly simpler synthetic pathway compared to the state-of-the-art precursors currently employed in phosphide quantum dot synthesis which are volatile, dangerous and air-sensitive, P(Si(CH)).
View Article and Find Full Text PDFUnderstanding the growth mechanisms of III-nitride nanowires is of great importance to realise their full potential. We present a systematic study of silane-assisted GaN nanowire growth on -sapphire substrates by investigating the surface evolution of the sapphire substrates during the high temperature annealing, nitridation and nucleation steps, and the growth of GaN nanowires. The nucleation step - which transforms the AlN layer formed during the nitridation step to AlGaN - is critical for subsequent silane-assisted GaN nanowire growth.
View Article and Find Full Text PDFExisting barriers to efficient deep ultraviolet (UV) light-emitting diodes (LEDs) may be reduced or overcome by moving away from conventional planar growth and toward three-dimensional nanostructuring. Nanorods have the potential for enhanced doping, reduced dislocation densities, improved light extraction efficiency, and quantum wells free from the quantum-confined Stark effect. Here, we demonstrate a hybrid top-down/bottom-up approach to creating highly uniform AlGaN core-shell nanorods on sapphire repeatable on wafer scales.
View Article and Find Full Text PDFFluorescent InP-based quantum dots have emerged as valuable nanomaterials for display technologies, biological imaging, and optoelectronic applications. The inclusion of zinc can enhance both their emissive and structural properties and reduce interfacial defects with ZnS or CdS shells. However, the sub-particle distribution of zinc and the role this element plays often remains unclear, and it has previously proved challenging to synthesise Zn-alloyed InP-based nanoparticles using aminophosphine precursors.
View Article and Find Full Text PDFMetal-organic frameworks (MOFs) are among the most promising materials for next-generation energy storage systems. However, the impact of particle morphology on the energy storage performances of these frameworks is poorly understood. To address this, here we use coordination modulation to synthesise three samples of the conductive MOF Cu(HHTP) (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) with distinct microstructures.
View Article and Find Full Text PDFAnaerobic nitrate-dependent iron(ii) oxidation is a process common to many bacterial species, which promotes the formation of Fe(iii) minerals that can influence the fate of soil and groundwater pollutants, such as arsenic. Herein, we investigated simultaneous nitrate-dependent Fe(ii) and As(iii) oxidation by sp. strain ST3 with the aim of studying the Fe biominerals formed, their As immobilization capabilities and the metabolic effect on cells.
View Article and Find Full Text PDFNew scalable precursor chemistries for quantum dots are highly desirable and ionic liquids are viewed as an attractive alternative to existing solvents, as they are often considered green and recyclable. Here we report the synthesis of HgTe quantum dots with emission in the near-IR region using a phosphonium based ionic liquid, and without standard phosphine capping agents.
View Article and Find Full Text PDFThe performance of transistors designed specifically for high-frequency applications is critically reliant upon the semi-insulating electrical properties of the substrate. The suspected formation of a conductive path for radio frequency (RF) signals in the highly resistive (HR) silicon substrate itself has been long held responsible for the suboptimal efficiency of as-grown GaN high electron mobility transistors (HEMTs) at higher operating frequencies. Here, we reveal that not one but two discrete channels distinguishable by their carrier type, spatial extent, and origin within the metal-organic vapor phase epitaxy (MOVPE) growth process participate in such parasitic substrate conduction.
View Article and Find Full Text PDFIntegrating diamond with GaN high electron mobility transistors (HEMTs) improves thermal management, ultimately increasing the reliability and performance of high-power high-frequency radio frequency amplifiers. Conventionally, an amorphous interlayer is used before growing polycrystalline diamond onto GaN in these devices. This layer contributes significantly to the effective thermal boundary resistance (TBR) between the GaN HEMT and the diamond, reducing the benefit of the diamond heat spreader.
View Article and Find Full Text PDFMetal sulfide and metal oxide alloys of the form Mo W S and Mo W O (0 ≤ ≤ 1) are synthesized with varying nominal stoichiometries ( = 0, 0.25, 0.50, 0.
View Article and Find Full Text PDFWhen approaching the atomically thin limit, defects and disorder play an increasingly important role in the properties of two-dimensional (2D) materials. While defects are generally thought to negatively affect superconductivity in 2D materials, here we demonstrate the contrary in the case of oxygenation of ultrathin tantalum disulfide (TaS). Our first-principles calculations show that incorporation of oxygen into the TaS crystal lattice is energetically favorable and effectively heals sulfur vacancies typically present in these crystals, thus restoring the electronic band structure and the carrier density to the intrinsic characteristics of TaS.
View Article and Find Full Text PDFZinc nitride (ZnN) colloidal quantum dots are composed of nontoxic, low-cost, and earth-abundant elements. The effects of quantum confinement on the optical properties and charge dynamics of these dots are studied using steady-state optical characterization and ultrafast fluence-dependent transient absorption. The absorption and emission energies are observed to be size-tunable, with the optical band gap increasing from 1.
View Article and Find Full Text PDFAccurately determining the morphology and hence the true surface areas of catalytic nanoparticles remains challenging. For many chemically synthesised nanoparticle suspensions conventional BET surface area measurements are often not feasible due to the large quantities of material required. For platinum, a paradigmatic catalyst, this issue is further complicated by the propensity of this metal to form porous aggregate structures comprised of smaller (ca.
View Article and Find Full Text PDFHot carrier generation by light in various semiconductors and metallic nanostructures is important for many photocatalytic and photochemical processes, including water and hydrogen splitting. Here, we report on investigations of hot electron generation and extraction from Pt decorated SiO2-Au nanoparticles using the degradation of methylene blue dye as a test-bed. Enhanced catalytic activity was found with an increase of Pt loading on the surface of the heterostructures.
View Article and Find Full Text PDFThe synthesis of colloidal semiconductor nanocrystals (NCs) from single-source precursors offers simplified manufacturing processes at the cost of reduced atom efficiency. Self-capping routes have the potential to maximise this efficiency although investigation has so far been limited to organic solvents. Here we present the synthesis of copper sulfide NCs the decomposition of a copper dithiocarbamate complex in water.
View Article and Find Full Text PDFAchieving control of the surface chemistry of colloidal quantum dots (CQDs) is essential to fully exploit their properties in solar cells, but direct measurement of the chemistry and electronic structure in the outermost atomic layers is challenging. Here we probe the surface oxidation and passivation of cation-exchanged PbS/CdS core/shell CQDs with sub nm-scale precision using synchrotron-radiation-excited depth-profiling photoemission. We investigate the surface composition of the topmost 1-2.
View Article and Find Full Text PDFIncorporation of CdS quantum dots is shown to significantly promote photocatalytic hydrogen production from water over single-layer MoS in a remote manner via their dispersions on a carbon nanotube as a nanocomposite: the hydrogen evolution rate is found to be critically dependent on the content and structural integrity of the carbon nanotube such that the double-walled carbon nanotube shows superior H production to a single-walled carbon nanotube because the inner carbon tubules survive from the structural damage during functionalization.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2016
The charge dynamics at the surface of the transparent conducting oxide and photoanode material ZnO are investigated in the presence and absence of light-harvesting colloidal quantum dots (QDs). The time-resolved change in surface potential upon photoexcitation has been measured in the m-plane ZnO (101[combining macron]0) using a laser pump-synchrotron X-ray probe methodology. By varying the oxygen annealing conditions, and hence the oxygen vacancy concentration of the sample, we find that dark carrier lifetimes at the ZnO surface vary from hundreds of μs to ms timescales, i.
View Article and Find Full Text PDFWe report single molecular sheets of niobate prepared by a simple bottom-up approach using hydrothermal synthesis of niobium ethoxide with the aid of triethanolamine as a structural modifier: the high kinetic stability of these molecular entities against self-assembly allows them to mix well with other colloids and facilitates their extensive electronic interactions and thus photocatalytic hydrogen evolution activity from water is much enhanced over composite of single niobate sheets with graphene and MoS2 due to efficient electron transfer and charge separation.
View Article and Find Full Text PDFA series of highly efficient semiconductor nanocrystal (NC) photocatalysts have been synthesized by growing wurtzite-ZnO tetrahedrons around pre-formed CdS, CdSe, and CdTe quantum dots (QDs). The resulting contact between two small but high-quality crystals creates novel CdX/ZnO heterostructured semiconductor nanocrystals (HSNCs) with extensive type-II nanojunctions that exhibit more efficient photocatalytic decomposition of aqueous organic molecules under UV irradiation. Catalytic testing and characterization indicate that catalytic activity increases as a result of a combination of both the intrinsic chemistry of the chalcogenide anions and the heterojunction structure.
View Article and Find Full Text PDFThe application of indium-free quaternary chalcogenides, such as Cu(2)ZnSnS(4) (CZTS), in photovoltaics has created tremendous interest in recent years. In this paper we develop a method to synthesize high quality CZTS nanoparticles with thermodynamically stable kesterite and wurtzite phases via a simple, one-pot, low-cost solution method.
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