Polydiacetylenes (PDAs) form a unique class of polymeric materials that couple highly aligned and conjugated backbones with tailorable pendant sidegroups and terminal functionalities. They can be structured in the form of bulk materials, multilayer and monolayer films, polymerized vesicles, and even incorporated into inorganic host matrices to form nanocomposites. The resulting materials exhibit an array of spectacular properties, beginning most notably with dramatic chromogenic transitions that can be activated optically, thermally, chemically, and mechanically. Recent studies have shown that these transitions can even be controlled and observed at the nanometre scale. These transitions have been harnessed for the purpose of chemical and biomolecular sensors, and on a more fundamental level have led to new insights regarding chromogenic phenomena in polymers. Other recent studies have explored how the strong structural anisotropy that these materials possess leads to anisotropic nanomechanical behaviour. These recent advances suggest that PDAs could be considered as a potential component in nanostructured devices due to the large number of tunable properties. In this paper, we provide a succinct review of the latest insights and applications involving PDA. We then focus in more detail on our work concerning ultrathin films, specifically structural properties, mechanochromism, thermochromism, and in-plane mechanical anisotropy of PDA monolayers. Atomic force microscopy (AFM) and fluorescence microscopy confirm that films 1-3 monolayers thick can be organized into highly ordered domains,with the conjugated backbones parallel to the substrate. The number of stable layers is controlled by the head-group functionality. Local mechanical stress applied by AFM and near-field optical probes induces the chromogenic transition in the film at the nanometre scale. The transition R680 Topical Review involves substantial optical and structural changes in a highly compressed form. Thermochromism is also studied using spectroscopic ellipsometry and fluorescence intensity measurements, and reveals that ultrathin films can reversibly attain an intermediate phase before irreversibly transforming to a final stable state. Further AFM studies also reveal the relation between the highly anisotropic film structure and its nanomechanical properties. In particular, friction at the nanometre scale depends dramatically upon the angle between the polymer backbone and the sliding direction, with the maximum found when sliding perpendicular to the backbones. The observed threefold anisotropy in mechanical dissipation also leads to contrast in the phase response of intermittent-contact AFM, indicating for the first time that in-plane anisotropy of polymeric systems in general can be investigated using this technique.

Recent studies have demonstrated that carbon, in the form of diamond, can be functionalized with molecular and/or biomolecular species to yield interfaces exhibiting extremely high stability and selectivity in binding to target biomolecules in solution. However, diamond and most other crystalline forms of carbon involve high-temperature deposition or processing steps that restrict their ability to be integrated with other materials. Here, we demonstrate that photochemical functionalization of amorphous carbon films followed by covalent immobilization of DNA yields highly stable surfaces with excellent biomolecular recognition properties that can be used for real-time biological detection. Carbon films deposited onto substrates at 300 K were functionalized with organic alkenes bearing protected amine groups and characterized using X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy. The functionalized carbon surfaces were covalently linked to DNA oligonucleotides. Measurements show very high selectivity for binding to the complementary sequence, and a high density of hybridizing DNA molecules. Samples repeatedly hybridized and denatured 25 times showed no significant degradation. The ability to use amorphous carbon films as a basis for real-time biosensing is demonstrated by coating quartz crystal microbalance (QCM) crystals with a thin carbon film and using this for covalent modification with DNA. Measurements of the resonance frequency show the ability to detect DNA hybridization in real time with a detection limit of <3% of a monolayer, with a high degree of reversibility. These results demonstrate that functionalized films of amorphous carbon can be used as a chemically stable platform for integrated biosensing using only room-temperature processing steps.

Exposing single-walled carbon nanotubes to room-temperature UV-generated ozone leads to an irreversible increase in their electrical resistance. We demonstrate that the increased resistance is due to ozone oxidation on the sidewalls of the nanotubes rather than at the end caps. Raman and X-ray photoelectron spectroscopies show an increase in the defect density due to the oxidation of the nanotubes. Using ultraviolet photoelectron spectroscopy, we show that these defects represent the removal of pi-conjugated electron states near the Fermi level, leading to the observed increase in electrical resistance. Oxidation of carbon nanotubes is an important first step in many chemical functionalization processes. Because the oxidation rate can be controlled with short exposures, UV-generated ozone offers the potential for use as a low-thermal-budget processing tool.

We demonstrate the electrically addressable biomolecular functionalization of single-walled carbon nanotube electrodes and vertically aligned carbon nanofiber electrodes. The method uses an electrochemical reaction in which nitro groups on specific nanostructures are reduced to amino groups and then used to covalently link DNA to only these nanostructures. We demonstrate fabrication of a four-element array of distinct DNA oligonucleotides on carbon nanotube electrodes and the addressable functionalization of submicron bundles of <100 nm diameter vertically aligned carbon nanofibers. DNA hybridization shows that the DNA-modified nanoscale structures have excellent biological selectivity.

Optoelectronic measurements of carbon nanotube transistors have shown a wide variety of sensitivites to the incident light. Direct photocurrent processes compete with a number of extrinsic mechanisms. Here we show that visible light absorption in the silicon substrate generates a photovoltage that can electrically gate the nanotube device. The photocurrent induced by the changing gate voltage can be significantly larger than that due to direct electron-hole pair generation in the nanotube. The dominance of photogating in these devices is confirmed by the power and position dependence of the resulting photocurrent. The power dependence is strongly nonlinear and photocurrents are measured through the device even when the laser illuminates up to 1mm from the nanotube.

State-of-the-art microfabricated ion traps for quantum information research are approaching nearly one hundred control electrodes. We report here on the development and testing of a new architecture for microfabricated ion traps, built around ball-grid array (BGA) connections, that is suitable for increasingly complex trap designs. In the BGA trap, through-substrate vias bring electrical signals from the back side of the trap die to the surface trap structure on the top side. Gold-ball bump bonds connect the back side of the trap die to an interposer for signal routing from the carrier. Trench capacitors fabricated into the trap die replace area-intensive surface or edge capacitors. Wirebonds in the BGA architecture are moved to the interposer. These last two features allow the trap die to be reduced to only the area required to produce trapping fields. The smaller trap dimensions allow tight focusing of an addressing laser beam for fast single-qubit rotations. Performance of the BGA trap as characterized with 40 Ca + ions is comparable to previous surface-electrode traps in terms of ion heating rate, mode frequency stability, and storage lifetime. We demonstrate two-qubit entanglement operations with 171 Yb + ions in a second BGA trap.

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Biological cells are complex objects that have the potential to act as templates for the subsequent construction of nanoscale structures. We demonstrate the ability to controllably and reversibly manipulate individual, live bacterial cells across micron-sized electrical gaps, and to detect bridging directly through changes in the electrical response. Our model system, Bacillus mycoides, is a rod-shaped bacterium approximately 800 nm wide and 5 microm long, similar in size and shape to many inorganic nanowires.