Colloidal nanocrystals (NCs, i.e., crystalline nanoparticles) have become an important class of materials with great potential for applications ranging from medicine to electronic and optoelectronic devices. Today's strong research focus on NCs has been prompted by the tremendous progress in their synthesis. Impressively narrow size distributions of just a few percent, rational shape-engineering, compositional modulation, electronic doping, and tailored surface chemistries are now feasible for a broad range of inorganic compounds. The performance of inorganic NC-based photovoltaic and light-emitting devices has become competitive to other state-of-the-art materials. Semiconductor NCs hold unique promise for near- and mid-infrared technologies, where very few semiconductor materials are available. On a purely fundamental side, new insights into NC growth, chemical transformations, and self-organization can be gained from rapidly progressing in situ characterization and direct imaging techniques. New phenomena are constantly being discovered in the photophysics of NCs and in the electronic properties of NC solids. In this Nano Focus, we review the state of the art in research on colloidal NCs focusing on the most recent works published in the last 2 years.
Bulk quantities of defect-free silicon (Si) nanowires with nearly uniform diameters ranging from 40 to 50 angstroms were grown to a length of several micrometers with a supercritical fluid solution-phase approach. Alkanethiol-coated gold nanocrystals (25 angstroms in diameter) were used as uniform seeds to direct one-dimensional Si crystallization in a solvent heated and pressurized above its critical point. The orientation of the Si nanowires produced with this method could be controlled with reaction pressure. Visible photoluminescence due to quantum confinement effects was observed, as were discrete optical transitions in the ultraviolet-visible absorbance spectra.
Ligand-stabilized copper selenide (Cu2−xSe) nanocrystals, approximately 16 nm in diameter, were synthesized by a colloidal hot injection method and coated with amphiphilic polymer. The nanocrystals readily disperse in water and exhibit strong near infrared (NIR) optical absorption with a high molar extinction coefficient of 7.7 × 107 cm−1 M−1 at 980 nm. When excited with 800 nm light, the Cu2−xSe nanocrystals produce significant photothermal heating with a photothermal transduction efficiency of 22%, comparable to nanorods and nanoshells of gold (Au). In vitro photothermal heating of Cu2−xSe nanocrystals in the presence of human colorectal cancer cell (HCT-116) led to cell destruction after 5 minutes of laser irradiation at 33 W/cm2, demonstrating the viabilitiy of Cu2−xSe nanocrystals for photothermal therapy applications.
Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of perovskite nanocrystals and understanding of their properties and applications. In this comprehensive review, researchers having expertise in different fields (chemistry, physics, and device engineering) of metal-halide perovskite nanocrystals have joined together to provide a state of the art overview and future prospects of metal-halide perovskite nanocrystal research.
Reversible electrochemical injection of discrete numbers of electrons into sterically stabilized silicon nanocrystals (NCs) (approximately 2 to 4 nanometers in diameter) was observed by differential pulse voltammetry (DPV) in N,N'-dimethylformamide and acetonitrile. The electrochemical gap between the onset of electron injection and hole injection-related to the highest occupied and lowest unoccupied molecular orbitals-grew with decreasing nanocrystal size, and the DPV peak potentials above the onset for electron injection roughly correspond to expected Coulomb blockade or quantized double-layer charging energies. Electron transfer reactions between positively and negatively charged nanocrystals (or between charged nanocrystals and molecular redox-active coreactants) occurred that led to electron and hole annihilation, producing visible light. The electrogenerated chemiluminescence spectra exhibited a peak maximum at 640 nanometers, a significant red shift from the photoluminescence maximum (420 nanometers) of the same silicon NC solution. These results demonstrate that the chemical stability of silicon NCs could enable their use as redox-active macromolecular species with the combined optical and charging properties of semiconductor quantum dots.
Chalcopyrite copper indium sulfide (CuInS2) and copper indium gallium selenide (Cu(InxGa(1-x))-Se2; CIGS) nanocrystals ranging from approximately 5 to approximately 25 nm in diameter were synthesized by arrested precipitation in solution. The In/Ga ratio in the CIGS nanocrystals could be controlled by varying the In/Ga reactant ratio in the reaction, and the optical properties of the CulnS2 and CIGS nanocrystals correspond to those of the respective bulk materials. Using methods developed to produce uniform, crack-free micrometer-thick films, CulnSe2 nanocrystals were tested in prototype photovoltaic devices. As a proof-of-concept, the nanocrystal-based devices exhibited a reproducible photovoltaic response.
To utilize high-capacity Si anodes in next-generation Li-ion batteries, the physical and chemical transformations during the Li-Si reaction must be better understood. Here, in situ transmission electron microscopy is used to observe the lithiation/delithiation of amorphous Si nanospheres; amorphous Si is an important anode material that has been less studied than crystalline Si. Unexpectedly, the experiments reveal that the first lithiation occurs via a two-phase mechanism, which is contrary to previous understanding and has important consequences for mechanical stress evolution during lithiation. On the basis of kinetics measurements, this behavior is suggested to be due to the rate-limiting effect of Si-Si bond breaking. In addition, the results show that amorphous Si has more favorable kinetics and fracture behavior when reacting with Li than does crystalline Si, making it advantageous to use in battery electrodes. Amorphous spheres up to 870 nm in diameter do not fracture upon lithiation; this is much larger than the 150 nm critical fracture diameter previously identified for crystalline Si spheres.
Hydrophobic dodecanethiol-capped silver nanocrystals ranging from 50 to 80 Å in diameter were synthesized using arrested growth methods. Size-selective precipitation was employed to isolate nanocrystals homogeneous in size and shape which exhibited close-packed structural order after drying on a carbon or mica substrate. Elemental analysis, H NMR and FTIR spectroscopies were used to characterize the compositional features of the adsorbed thiolate ligands on nanocrystals suspended in solution and condensed in nanocrystal films. Small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM) were used to probe the structure of both individual nanocrystals and superlattices, and to estimate the energetic interactions between these sterically stabilized particles. In terms of these measurements, the effects of the capping ligand coverage, particle faceting and shape, and interparticle attractions on superlattice formation are elucidated. In particular, the concept of nanocrystals as “soft spheres” which order with an effective hard sphere diameter is introduced. In addition, the ways in which nanocrystals deviate from such an ideal model are discussed.
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