Confined linear carbon chains as a route to bulk carbyne.

Strong chemical activity and extreme instability in ambient conditions characterize carbyne, an infinite sp(1) hybridized carbon chain. As a result, much less has been explored about carbyne as compared to other carbon allotropes such as fullerenes, nanotubes and graphene. Although end-capping groups can be used to stabilize carbon chains, length limitations are still a barrier for production, and even more so for application. We report a method for the bulk production of long acetylenic linear carbon chains protected by thin double-walled carbon nanotubes. The synthesis of very long arrangements is confirmed by a combination of transmission electron microscopy, X-ray diffraction and (near-field) resonance Raman spectroscopy. Our results establish a route for the bulk production of exceptionally long and stable chains composed of more than 6,000 carbon atoms, representing an elegant forerunner towards the final goal of carbyne's bulk production.

Defect-Free Carbon Nanotube Coils.

Carbon nanotubes are promising building blocks for various nanoelectronic components. A highly desirable geometry for such applications is a coil. However, coiled nanotube structures reported so far were inherently defective or had no free ends accessible for contacting. Here we demonstrate the spontaneous self-coiling of single-wall carbon nanotubes into defect-free coils of up to more than 70 turns with identical diameter and chirality, and free ends. We characterize the structure, formation mechanism, and electrical properties of these coils by different microscopies, molecular dynamics simulations, Raman spectroscopy, and electrical and magnetic measurements. The coils are highly conductive, as expected for defect-free carbon nanotubes, but adjacent nanotube segments in the coil are more highly coupled than in regular bundles of single-wall carbon nanotubes, owing to their perfect crystal momentum matching, which enables tunneling between the turns. Although this behavior does not yet enable the performance of these nanotube coils as inductive devices, it does point a clear path for their realization. Hence, this study represents a major step toward the production of many different nanotube coil devices, including inductors, electromagnets, transformers, and dynamos.

Near-field Raman spectroscopy of nanocarbon materials.

Nanocarbon materials, including sp(2) hybridized two-dimensional graphene and one-dimensional carbon nanotubes, and sp(1) hybridized one-dimensional carbyne, are being considered for the next generation of integrated optoelectronic devices. The strong electron-phonon coupling present in these nanocarbon materials makes Raman spectroscopy an ideal tool to study and characterize the material and device properties. Near-field Raman spectroscopy combines non-destructive chemical, electrical, and structural specificity with nanoscale spatial resolution, making it an ideal tool for studying nanocarbon systems. Here we use near-field Raman spectroscopy to study strain, defects, and doping in different nanocarbon systems.

Individual Template-Stripped Conductive Gold Pyramids for Tip-Enhanced Dielectrophoresis.

Gradient fields of optical, magnetic, or electrical origin are widely used for the manipulation of micro- and nanoscale objects. Among various device geometries to generate gradient forces, sharp metallic tips are one of the most effective. Surface roughness and asperities present on traditionally produced tips reduce trapping efficiencies and limit plasmonic applications. Template-stripped, noble metal surfaces and structures have sub-nm roughness and can overcome these limits. We have developed a process using a mix of conductive and dielectric epoxies to mount template-stripped gold pyramids on tungsten wires that can be integrated with a movable stage. When coupled with a transparent indium tin oxide (ITO) electrode, the conductive pyramidal tip functions as a movable three-dimensional dielectrophoretic trap which can be used to manipulate submicrometer-scale particles. We experimentally demonstrate the electrically conductive functionality of the pyramidal tip by dielectrophoretic manipulation of fluorescent beads and concentration of single-walled carbon nanotubes, detected with fluorescent microscopy and Raman spectroscopy.

Measuring coherence functions using non-parallel double slits.

We present an experimental method for the fast measurement of both the spectral (spatial) and complex degrees of coherence of an optical field using only a binary amplitude mask and a detector array. We test the method by measuring a two-dimensional spectral degree of coherence function created by a broadband thermal source. The results are compared to those expected by the van Cittert-Zernike theorem and found to agree well in both amplitude and phase.

Demonstration of zero optical backscattering from single nanoparticles.

We present the first experimental demonstration of zero backscattering from nanoparticles at optical frequencies as originally discussed by Kerker et al. [ Kerker , M. ; Wang , D. ; Giles , C. J. Opt. Soc. A 1983 , 73 , 765 ]. GaAs pillars were fabricated on a fused silica substrate and the spectrum of the backscattered radiation was measured in the wavelength range 600-1000 nm. Suppression of backscattering occurred at ~725 nm, agreeing with calculations based on the discrete dipole approximation. Particles with zero backscattering provide new functionality for metamaterials and optical antennas.

Self-similar gold-nanoparticle antennas for a cascaded enhancement of the optical field.

We experimentally demonstrate cascaded field enhancement by means of gold nanoparticle dimer and trimer antennas. The local field enhancement is probed by single-molecule fluorescence using fluorophores with high intrinsic quantum efficiency (Q(0)>80%). Using a self-similar trimer antenna consisting of 80, 40, and 20 nm gold nanoparticles, we demonstrate a fluorescence enhancement of 40 and a spatial confinement of 15 nm. Compared with a single gold nanoparticle, the self-similar trimer antenna improves the enhancement-confinement ratio by more than an order of magnitude. Self-similar antennas hold promise for high-resolution imaging and spectroscopy, ultrasensitive detection, and efficient single-photon sources.

Highly reproducible near-field optical imaging with sub-20-nm resolution based on template-stripped gold pyramids.

With a template-stripping fabrication technique, we demonstrate the mass fabrication of high-quality, uniform, ultrasharp (10 nm) metallic probes suitable for single-molecule fluorescence imaging, tip-enhanced Raman spectroscopy (TERS), and other near-field imaging techniques. We achieve reproducible single-molecule imaging with sub-20-nm spatial resolution and an enhancement in the detected fluorescence signal of up to 200. Similar results are obtained for TERS imaging of carbon nanotubes. We show that the large apex angle (70.5°) of our pyramidal tip is well suited to scatter the near-field optical signal into the far-field, leading to larger emission enhancement and hence to a larger quantum yield. Each gold or silver pyramidal probe is used on-demand, one at a time, and the unused tips can be stored for extended times without degradation or contamination. The high yield (>95%), reproducibility, durability, and massively parallel fabrication (1.5 million identical probes over a wafer) of the probes hold promise for reliable optical sensing and detection and for cementing near-field optical imaging and spectroscopy as a routine characterization technique.

Near-field quantification of complement receptor 1 (CR1/CD35) protein clustering in human erythrocytes.

We investigate the distribution of the membrane protein complement receptor 1 (CR1/CD35) in human erythrocyte membrane ghosts using scanning near-field optical microscopy. Recent studies have demonstrated that levels of Aß peptide, associated with Alzheimers disease (AD) and present in brain and peripheral blood, vary significantly when bound by complement C3b-dependent adherence to CR1. It is unknown why patients with AD have a markedly impaired ability to bind Aß to CR1 via this mechanism, but one possibility is a defect in the localization and/or conformation of CR1 in the membrane. Scanning near-field optical microscopy does not require the harsh preparation of electron microscopy techniques and may therefore be better suited for measuring membrane protein distributions. The clustering phenomenon of CR1 identified in electron microscopy studies is confirmed and quantified. The standard deviation of the inter-cluster spacing of CR1 is constant (79 ± 9 nm) across erythrocytes with between 61 and 124 clusters per membrane ghost.