Morphological control of nanocrystals has become increasingly important, as many of their physical and chemical properties are highly shape dependent. Nanocrystal shape control for both single- and multiple-material systems, however, remains empirical and challenging. New methods need to be explored for the rational synthetic design of heterostructures with controlled morphology. Overgrowth of a different material on well-faceted seeds, for example, allows for the use of the defined seed morphology to control nucleation and growth of the secondary structure. Here, we have used highly faceted cubic Pt seeds to direct the epitaxial overgrowth of a secondary metal. We demonstrate this concept with lattice-matched Pd to produce conformal shape-controlled core-shell particles, and then extend it to lattice-mismatched Au to give anisotropic growth. Seeding with faceted nanocrystals may have significant potential towards the development of shape-controlled heterostructures with defined interfaces.
We present a novel method for synthesizing graphene sheets in the gas phase using a substrate-free, atmospheric-pressure microwave plasma reactor. Graphene sheets were synthesized by passing liquid ethanol droplets into an argon plasma. The graphene sheets were characterized by transmission electron microscopy, electron energy loss spectroscopy, Raman spectroscopy, and electron diffraction. We prove that graphene can be created without three-dimensional materials or substrates and demonstrate a possible avenue to the large-scale synthesis of graphene.
The manipulation of the bandgap of graphene by various means has stirred great interest for potential applications. Here we show that treatment of graphene with xenon difluoride produces a partially fluorinated graphene (fluorographene) with covalent C-F bonding and local sp(3)-carbon hybridization. The material was characterized by Fourier transform infrared spectroscopy, Raman spectroscopy, electron energy loss spectroscopy, photoluminescence spectroscopy, and near edge X-ray absorption spectroscopy. These results confirm the structural features of the fluorographane with a bandgap of 3.8 eV, close to that calculated for fluorinated single layer graphene, (CF)(n). The material luminesces broadly in the UV and visible light regions, and has optical properties resembling diamond, with both excitonic and direct optical absorption and emission features. These results suggest the use of fluorographane as a new, readily prepared material for electronic, optoelectronic applications, and energy harvesting applications.
The ability of electron microscopes to analyze all the atoms in individual nanostructures is limited by lens aberrations. However, recent advances in aberration-correcting electron optics have led to greatly enhanced instrument performance and new techniques of electron microscopy. The development of an ultrastable electron microscope with aberration-correcting optics and a monochromated high-brightness source has significantly improved instrument resolution and contrast. In the present work, we report information transfer beyond 50 pm and show images of single gold atoms with a signal-to-noise ratio as large as 10. The instrument's new capabilities were exploited to detect a buried Sigma3 {112} grain boundary and observe the dynamic arrangements of single atoms and atom pairs with sub-angstrom resolution. These results mark an important step toward meeting the challenge of determining the three-dimensional atomic-scale structure of nanomaterials.
Direct imaging of surface molecules and the interfaces between soft and hard materials on functionalized nanoparticles is a great challenge using modern microscopy techniques. We show that graphene, a single atomic layer of sp(2)-bonded carbon atoms, can be employed as an ultrathin support film that enables direct imaging of molecular layers and interfaces in both conventional and atomic-resolution transmission electron microscopy. An atomic-resolution imaging study of the capping layers and interfaces of citrate-stabilized gold nanoparticles is used to demonstrate this novel capability. Our findings reveal the unique potential of graphene as an ideal support film for atomic-resolution transmission electron microscopy of hard and soft nanomaterials.
Rapid prototyping of bottom-up nanostructure circuits is demonstrated, utilizing metal deposition and patterning methodology based on combined focused ion and electron beam induced decomposition of a metal−organic precursor gas. Ohmic contacts were fabricated using electron beam deposition, followed by the faster process of ion beam deposition for interconnect formation. Two applications of this method are demonstrated: three-terminal transport measurements of Y-junction carbon nanotubes and fabrication of nanocircuits for determination of electromechanical degradation of silver nanowires.
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