In this study, we conducted a high-pressure investigation of CuSe nanostructures with pyramid- and plate-like morphologies, created through cation exchange from zinc-blende CdSe nanocrystals and wurtzite CdSe nanoplatelets respectively. Using a diamond anvil cell setup at the APS synchrotron, we observed the phase transitions in the CuSe nanostructures up to 40 GPa, identifying a novel CsCl-type lattice with 3̅ symmetry above 4 GPa. This CsCl-type structure, previously unreported in copper selenides, was partially retained after decompression.
View Article and Find Full Text PDFThe two-dimensional CsPbBr nanoplatelets have a quantum well electronic structure with a band gap tunable with sample thicknesses in discreet steps based upon the number of monolayers. The polarized optical properties of CsPbBr nanoplatelets are studied using fluorescence anisotropy and polarized transient absorption spectroscopies. Polarized spectroscopy shows that they have absorption and emission transitions which are strongly plane-polarized.
View Article and Find Full Text PDFSynthesizing patchy particles with predictive control over patch size, shape, placement and number has been highly sought-after for nanoparticle assembly research, but is fraught with challenges. Here we show that polymers can be designed to selectively adsorb onto nanoparticle surfaces already partially coated by other chains to drive the formation of patchy nanoparticles with broken symmetry. In our model system of triangular gold nanoparticles and polystyrene-b-polyacrylic acid patch, single- and double-patch nanoparticles are produced at high yield.
View Article and Find Full Text PDFNanoscale hyperspectral techniques-such as electron energy loss spectroscopy (EELS)-are critical to understand the optical response in plasmonic nanostructures, but as systems become increasingly complex, the required sampling density and acquisition times become prohibitive for instrumental and specimen stability. As a result, there has been a recent push for new experimental methodologies that can provide comprehensive information about a complex system, while significantly reducing the duration of the experiment. Here, we present a pan-sharpening approach to hyperspectral EELS analysis, where we acquire two datasets from the same region (one with high spatial resolution and one with high spectral fidelity) and combine them to achieve a single dataset with the beneficial properties of both.
View Article and Find Full Text PDFSolid-solid phase transitions are processes ripe for the discovery of correlated atomic motion in crystals. Here, we monitor an order-disorder transition in real-time in nanoparticles of the super-ionic solid, CuSe. The use of in-situ high-resolution transmission electron microscopy allows the spatiotemporal evolution of the phase transition within a single nanoparticle to be monitored at the atomic level.
View Article and Find Full Text PDFZnO has industrial utility as a solid sorbent for the removal of polluting sulfur compounds from petroleum-based fuels. Small ZnO nanoparticles may be more effective in terms of sorption capacity and ease of sulfidation as compared to bulk ZnO. Motivated by this promise, here, we study the sulfidation of ZnO NPs and uncover the solid-state mechanism of the process by crystallographic and optical absorbance characterization.
View Article and Find Full Text PDFThe search for ion-conductive solid electrolytes for Li batteries is an important scientific and technological challenge with economic and sustainable energy implications. In this study, nanocrystals (NCs) of the ion conductor copper selenide (Cu Se) were doped with Li by the process of cation exchange. Li Cu Se alloy NCs were formed at intermediate stages of the reaction, which was followed by phase segregation into Li Se and Cu Se domains.
View Article and Find Full Text PDFJ Phys Chem Lett
April 2018
An optically modulated scanning tunneling microscopy technique developed for measurement of single-molecule optical absorption is used here to image the light absorption by individual Au nanoislands and Au nanostructures. The technique is shown to spatially map, with nanometer resolution, localized surface plasmons (LSPs) excited within the nanoislands. Electrodynamic simulations demonstrate the correspondence of the measured images to plasmonic near-field intensity maps.
View Article and Find Full Text PDFSuper-ionic solids, which exhibit ion mobilities as high as those in liquids or molten salts, have been employed as solid-state electrolytes in batteries, improved thermoelectrics and fast-ion conductors in super-capacitors and fuel cells. Fast-ion transport in many of these solids is supported by a disordered, 'liquid-like' sub-lattice of cations mobile within a rigid anionic sub-lattice, often achieved at high temperatures or pressures via a phase transition. Here we show that ultrasmall clusters of copper selenide exhibit a disordered cationic sub-lattice under ambient conditions unlike larger nanocrystals, where Cu ions and vacancies form an ordered super-structure similar to the bulk solid.
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