Topological defects are singularities within a field that cannot be removed by continuous transformations. The definition of these irregularities requires an ordered reference configuration, calling into question whether they exist in disordered materials, such as glasses. However, recent work suggests that well-defined topological defects emerge in the dynamics of glasses, even if they are not evident in the static configuration.
View Article and Find Full Text PDFSheet-like colloidal assemblies represent model systems to investigate the structure and properties of two-dimensional materials. Here, we report a simple yet versatile method for the preparation of colloidal monolayer sheet-like assemblies that affords control over the size, crystalline order, flexibility, and defect density. The protocol that we report relies on self-assembly of colloids as a sessile drop of dispersion is evaporated on an oil-covered substrate.
View Article and Find Full Text PDFThe deformation mechanism in amorphous solids subjected to external shear remains poorly understood because of the absence of well-defined topological defects mediating the plastic deformation. The notion of soft spots has emerged as a useful tool to characterize the onset of irreversible rearrangements and plastic flow, but these entities are not clearly defined in terms of geometry and topology. In this study, we unveil the phenomenology of recently discovered, precisely defined topological defects governing the microscopic mechanical and yielding behavior of a model 3D glass under shear deformation.
View Article and Find Full Text PDFThe efficiency of an organic solar cell is highly dependent on the complex, interpenetrating morphology, and molecular order within the composite phases of the bulk heterojunction (BHJ) blend. Both these microstructural aspects are strongly influenced by the processing conditions and chemical design of donor/acceptor materials. To establish improved structure-function relationships, it is vital to visualize the local microstructural order to provide specific local information about donor/acceptor interfaces and crystalline texture in BHJ blend films.
View Article and Find Full Text PDFThe waveguide modes in chemically-grown silver nanowires on silicon nitride substrates are observed using spectrally- and spatially-resolved cathodoluminescence (CL) excited by high-energy electrons in a scanning electron microscope. The presence of a long-range, travelling surface plasmon mode modulates the coupling efficiency of the incident electron energy into the nanowires, which is observed as oscillations in the measured CL with the point of excitation by the focused electron beam. The experimental data are modeled using the theory of surface plasmon polariton modes in cylindrical metal waveguides, enabling the complex mode wavenumbers and excitation strength of the long-range surface plasmon mode to be extracted.
View Article and Find Full Text PDFThis study describes the capabilities and limitations of carrying out total scattering experiments on the Powder Diffraction (PD) beamline at the Australian Synchrotron, ANSTO. A maximum instrument momentum transfer of 19 Å can be achieved if the data are collected at 21 keV. The results detail how the pair distribution function (PDF) is affected by Q, absorption and counting time duration at the PD beamline, and refined structural parameters exemplify how the PDF is affected by these parameters.
View Article and Find Full Text PDFQuasiperiodicity is a form of spatial order that has been observed in quasicrystalline matter but not light. We construct a quasicrystalline surface out of a light emitting diode. Using a nanoscale waveguide as a microscope (NSOM), we directly image the light field at the surface of the diode.
View Article and Find Full Text PDFThe mechanical properties of crystals are controlled by the translational symmetry of their structures. But for glasses with a disordered structure, the link between the symmetry of local particle arrangements and stability is not well established. In this contribution, we provide experimental verification that the centrosymmetry of nearest-neighbor polyhedra in a glass strongly correlates with the local mechanical stability.
View Article and Find Full Text PDFWe developed a series of highly crystalline double-cable conjugated polymers for application in single-component organic solar cells (SCOSCs). These polymers contain conjugated backbones as electron donor and pendant perylene bisimide units (PBIs) as electron acceptor. PBIs are connected to the backbone via alkyl units varying from hexyl (C H ) to eicosyl (C H ) as flexible linkers.
View Article and Find Full Text PDFThe evolution of polygonal-shaped nanoholes on the (100) surface of germanium, aided by focused ion beam induced self-organization, is presented. The energetic beam of ions creates a viscous phase which, at a thermodynamical minimum, leads to surface self-organization. A directed viscous-flow along the predefined nanoholes provides well-ordered polygonal nanostructures, ranging from triangles to hexagons and octagons, as desired.
View Article and Find Full Text PDFNanoparticle dimers composed of different metals or metal oxides, as well as different shapes and sizes, are of wide interest for applications ranging from nanoplasmonic sensing to nanooptics to biomedical engineering. Shaped nanoparticles, like triangles and nanorods, can be particularly useful in applications due to the strong localized plasmonic hot-spot that forms at the tips or corners. By placing catalytic, but traditionally weakly- or non-plasmonic nanoparticles, such as metal oxides and metals like palladium, in these hot-spots, an enhanced function for sensing, photocatalysis or optical use is predicted.
View Article and Find Full Text PDFThe excitability of local surface plasmon modes in radial trimers composed of gold nanorods was mapped using hyperspectral cathodoluminescence (CL) in the scanning electron microscope. In symmetric trimers, the local plasmon resonances could be excited most effectively at the ends of individual rods. Introducing asymmetry into the structure breaks the degeneracy of the dipole modes and changes the excitability of transverse dipole modes in different directions.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2018
Here, we systematically study the effect of fluorination on the performance of all-polymer solar cells by employing a naphthalene diimide (NDI)-based polymer acceptor with thiophene-flanked phenyl co-monomer. Fluorination of the phenyl co-monomer with either two or four fluorine units is used to create a series of acceptor polymers with either no fluorination (PNDITPhT), bifluorination (PNDITF2T), or tetrafluorination (PNDITF4T). In blends with the donor polymer PTB7-Th, fluorination results in an increase in power conversion efficiency from 3.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
September 2017
Local structure and symmetry are keys to understanding how a material is formed and the properties it subsequently exhibits. This applies to both crystals and amorphous and glassy materials. In the case of amorphous materials, strong links between processing and history, structure and properties have yet to be made because measuring amorphous structure remains a significant challenge.
View Article and Find Full Text PDFAsymmetric nanoparticle trimers composed of particles with increasing diameter act as "plasmonic lenses" and have been predicted to exhibit ultrahigh confinement of electromagnetic energy in the space between the two smallest particles. Here we present an electrostatic self-assembly approach for creating gold nanoparticle trimers with an assembly yield of over 60%. We demonstrate that the trimer assembly leads to characteristic red-shifts and show the localization of the relevant plasmon modes by means of cathodoluminescence and electron energy loss spectroscopy.
View Article and Find Full Text PDFThe aqueous dispersibility of carbon-based nanomaterials, namely graphene oxide (GO), reduced graphene oxide (rGO) and carbon nanotubes (CNTs), can be controlled by light via the photoisomerisation of a photoswitchable surfactant molecule adsorbed to the surface of these materials. By incorporating a cationic azobenzene photosurfactant into these systems, GO, rGO and CNT dispersions can be separated and redispersed on command utilising UV radiation at 365 nm, whereby the surfactant molecules change from the trans to the cis isomer. This increases their aqueous solubility and in turn, alters their adsorption affinity for the GO and rGO sheets such that the ratio of free to adsorbed surfactant molecules changes significantly, allowing for reversible phase separation of the colloids.
View Article and Find Full Text PDFActa Crystallogr A Found Adv
September 2015
The interpretation of angular symmetries in electron nanodiffraction patterns from thin amorphous specimens is examined. It is found that in general there are odd symmetries in experimental electron nanodiffraction patterns. Using simulation, it is demonstrated that this effect can be attributed to dynamical scattering, rather than other divergences from the ideal experimental conditions such as probe-forming lens aberrations and camera noise.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2015
Porosity loss, also known as physical aging, in glassy polymers hampers their long term use in gas separations. Unprecedented interactions of porous aromatic frameworks (PAFs) with these polymers offer the potential to control and exploit physical aging for drastically enhanced separation efficiency. PAF-1 is used in the archetypal polymer of intrinsic microporosity (PIM), PIM-1, to achieve three significant outcomes.
View Article and Find Full Text PDFAging in super glassy polymers such as poly(trimethylsilylpropyne) (PTMSP), poly(4-methyl-2-pentyne) (PMP), and polymers with intrinsic microporosity (PIM-1) reduces gas permeabilities and limits their application as gas-separation membranes. While super glassy polymers are initially very porous, and ultra-permeable, they quickly pack into a denser phase becoming less porous and permeable. This age-old problem has been solved by adding an ultraporous additive that maintains the low density, porous, initial stage of super glassy polymers through absorbing a portion of the polymer chains within its pores thereby holding the chains in their open position.
View Article and Find Full Text PDFHigh-resolution radial distribution functions of as-implanted and thermally relaxed amorphous silicon created by ion implantation were measured using tilted-illumination selected area electron diffraction at room temperature. The diffracted intensities were measured out to a maximum scattering vector 2 sin(θ)/λ of 3.3-3.
View Article and Find Full Text PDFPhase retrieval is widely used in phase contrast microscopy. Here we present an autofocus algorithm that allows the phase of the exit wave function, from a single-material object, to be reconstructed at medium resolution from a single phase contrast image without any a priori knowledge of the imaging system or object. The algorithm is demonstrated on coherent out-of-focus electron micrographs of 30 nm latex sphere calibration standards, giving <10% RMS error over a large defocus range.
View Article and Find Full Text PDFThe intermediate voltage electron microscope-tandem user facility in the Electron Microscopy Center at Argonne National Laboratory is described. The primary purpose of this facility is electron microscopy with in situ ion irradiation at controlled sample temperatures. To illustrate its capabilities and advantages a few results of two outside user projects are presented.
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