Guiding epitaxial crystallization of amorphous solids at the nanoscale: Interfaces, stress, and precrystalline order.

The crystallization of amorphous solids impacts fields ranging from inorganic crystal growth to biophysics. Promoting or inhibiting nanoscale epitaxial crystallization and selecting its final products underpin applications in cryopreservation, semiconductor devices, oxide electronics, quantum electronics, structural and functional ceramics, and advanced glasses. As precursors for crystallization, amorphous solids are distinguished from liquids and gases by the comparatively long relaxation times for perturbations of the mechanical stress and for variations in composition or bonding. These factors allow experimentally controllable parameters to influence crystallization processes and to drive materials toward specific outcomes. For example, amorphous precursors can be employed to form crystalline phases, such as polymorphs of Al2O3, VO2, and other complex oxides, that are not readily accessible via crystallization from a liquid or through vapor-phase epitaxy. Crystallization of amorphous solids can further be guided to produce a desired polymorph, nanoscale shape, microstructure, or orientation of the resulting crystals. These effects enable advances in applications in electronics, magnetic devices, optics, and catalysis. Directions for the future development of the chemical physics of crystallization from amorphous solids can be drawn from the structurally complex and nonequilibrium atomic arrangements in liquids and the atomic-scale structure of liquid-solid interfaces.

Non-Invasive MRI of Blood-Cerebrospinal Fluid Barrier Function.

The blood-cerebrospinal fluid barrier (BCSFB) is a highly dynamic transport interface that serves brain homeostasis. To date, however, understanding of its role in brain development and pathology has been hindered by the absence of a non-invasive technique for functional assessment. Here we describe a method for non-invasive measurement of BSCFB function by using tracer-free MRI to quantify rates of water delivery from arterial blood to ventricular cerebrospinal fluid. Using this method, we record a 36% decrease in BCSFB function in aged mice, compared to a 13% decrease in parenchymal blood flow, itself a leading candidate biomarker of early neurodegenerative processes. We then apply the method to explore the relationship between BCSFB function and ventricular morphology. Finally, we provide proof of application to the human brain. Our findings position the BCSFB as a promising new diagnostic and therapeutic target, the function of which can now be safely quantified using non-invasive MRI.

Two-party secret key distribution via a modified quantum secret sharing protocol.

We present and demonstrate a novel protocol for distributing secret keys between two and only two parties based on N-party single-qubit Quantum Secret Sharing (QSS). We demonstrate our new protocol with N = 3 parties using phase-encoded photons. We show that any two out of N parties can build a secret key based on partial information from each other and with collaboration from the remaining N - 2 parties. Our implementation allows for an accessible transition between N-party QSS and arbitrary two party QKD without modification of hardware. In addition, our approach significantly reduces the number of resources such as single photon detectors, lasers and dark fiber connections needed to implement QKD.

A short-pulse X-ray beamline for spectroscopy and scattering.

Experimental facilities for picosecond X-ray spectroscopy and scattering based on RF deflection of stored electron beams face a series of optical design challenges. Beamlines designed around such a source enable time-resolved diffraction, spectroscopy and imaging studies in chemical, condensed matter and nanoscale materials science using few-picosecond-duration pulses possessing the stability, high repetition rate and spectral range of synchrotron light sources. The RF-deflected chirped electron beam produces a vertical fan of undulator radiation with a correlation between angle and time. The duration of the X-ray pulses delivered to experiments is selected by a vertical aperture. In addition to the radiation at the fundamental photon energy in the central cone, the undulator also emits the same photon energy in concentric rings around the central cone, which can potentially compromise the time resolution of experiments. A detailed analysis of this issue is presented for the proposed SPXSS beamline for the Advanced Photon Source. An optical design that minimizes the effects of off-axis radiation in lengthening the duration of pulses and provides variable X-ray pulse duration between 2.4 and 16 ps is presented.

Nanomembrane-based materials for Group IV semiconductor quantum electronics.

Strained-silicon/relaxed-silicon-germanium alloy (strained-Si/SiGe) heterostructures are the foundation of Group IV-element quantum electronics and quantum computation, but current materials quality limits the reliability and thus the achievable performance of devices. In comparison to conventional approaches, single-crystal SiGe nanomembranes are a promising alternative as substrates for the epitaxial growth of these heterostructures. Because the nanomembrane is truly a single crystal, in contrast to the conventional SiGe substrate made by compositionally grading SiGe grown on bulk Si, significant improvements in quantum electronic-device reliability may be expected with nanomembrane substrates. We compare lateral strain inhomogeneities and the local mosaic structure (crystalline tilt) in strained-Si/SiGe heterostructures that we grow on SiGe nanomembranes and on compositionally graded SiGe substrates, with micro-Raman mapping and nanodiffraction, respectively. Significant structural improvements are found using SiGe nanomembranes.

Compact ultrahigh vacuum sample environments for x-ray nanobeam diffraction and imaging.

X-ray nanobeams present the opportunity to obtain structural insight in materials with small volumes or nanoscale heterogeneity. The effective spatial resolution of the information derived from nanobeam techniques depends on the stability and precision with which the relative position of the x-ray optics and sample can be controlled. Nanobeam techniques include diffraction, imaging, and coherent scattering, with applications throughout materials science and condensed matter physics. Sample positioning is a significant mechanical challenge for x-ray instrumentation providing vacuum or controlled gas environments at elevated temperatures. Such environments often have masses that are too large for nanopositioners capable of the required positional accuracy of the order of a small fraction of the x-ray spot size. Similarly, the need to place x-ray optics as close as 1 cm to the sample places a constraint on the overall size of the sample environment. We illustrate a solution to the mechanical challenge in which compact ion-pumped ultrahigh vacuum chambers with masses of 1-2 kg are integrated with nanopositioners. The overall size of the environment is sufficiently small to allow their use with zone-plate focusing optics. We describe the design of sample environments for elevated-temperature nanobeam diffraction experiments demonstrate in situ diffraction, reflectivity, and scanning nanobeam imaging of the ripening of Au crystallites on Si substrates.

Optical design of the short pulse x-ray imaging and microscopy time-angle correlated diffraction beamline at the Advanced Photon Source.

The short pulse x-ray imaging and microscopy beamline is one of the two x-ray beamlines that will take full advantage of the short pulse x-ray source in the Advanced Photon Source (APS) upgrade. A horizontally diffracting double crystal monochromator which includes a sagittally focusing second crystal will collect most of the photons generated when the chirped electron beam traverses the undulator. A Kirkpatrick-Baez mirror system after the monochromator will deliver to the sample a beam which has an approximately linear correlation between time and vertical beam angle. The correlation at the sample position has a slope of 0.052 ps/µrad extending over an angular range of 800 µrad for a cavity deflection voltage of 2 MV. The expected time resolution of the whole system is 2.6 ps. The total flux expected at the sample position at 10 keV with a 0.9 eV energy resolution is 5.7 × 10(12) photons/s at a spot having horizontal and vertical full width at half maximum of 33 µm horizontal by 14 µm vertical. This new beamline will enable novel time-dispersed diffraction experiments on small samples using the full repetition rate of the APS.

Extraordinary optical transmission of multimode quantum correlations via localized surface plasmons.

We demonstrate the transduction of macroscopic quantum correlations by Ag localized surface plasmons (LSPs). Quantum noise reduction, or squeezed light, generated through four-wave mixing in Rb vapor, is coupled to a Ag nanohole array designed to exhibit LSP-mediated extraordinary-optical transmission spectrally coincident with the squeezed light source at 795 nm. This first demonstration of the coupling of quantum light into LSPs conserves spatially dependent quantum information, allowing for parallel quantum protocols in on-chip subwavelength quantum information processing.

Bright source of spectrally uncorrelated polarization-entangled photons with nearly single-mode emission.

We present results of a bright polarization-entangled photon source operating at 1552 nm via type-II collinear degenerate spontaneous parametric down-conversion in a periodically poled potassium titanyl phosphate crystal. We report a conservative inferred pair generation rate of 123,000 pairs/s/mW into collection modes. Minimization of spectral and spatial entanglement was achieved by group velocity matching the pump, signal, and idler modes and through properly focusing the pump beam. By utilizing a pair of calcite beam displacers, we are able to overlap photons from adjacent down-conversion processes to obtain polarization-entanglement visibility of 94.7+/-1.1% with accidentals subtracted.

Risk management measures for chemicals: the "COSHH essentials" approach.

"COSHH essentials" was developed in Great Britain to help duty holders comply with the Control of Substances Hazardous to Health (COSHH) Regulations. It uses a similar approach to that described in the new European "REACH" Regulation (Registration, Evaluation, Authorisation and Restriction of Chemicals; EC No. 1907/2006 of the European Parliament), insofar as it identifies measures for managing the risk for specified exposure scenarios. It can therefore assist REACH duty holders with the identification and communication of appropriate risk-management measures. The technical basis for COSHH essentials is explained in the original papers published in the Annals of Occupational Hygiene. Its details will, therefore, not be described here; rather, its ability to provide a suitable means for communicating risk-management measures will be explored. COSHH essentials is a simple tool based on an empirical approach to risk assessment and risk management. The output is a "Control Guidance Sheet" that lists the "dos" and "don'ts" for control in a specific task scenario. The guidance in COSHH essentials recognises that exposure in the workplace will depend not just on mechanical controls, but also on a number of other factors, including administrative and behavioural controls, such as systems of work, supervision and training. In 2002, COSHH essentials was made freely available via the internet (http://www.coshh-essentials.org.uk/). This electronic delivery enabled links to be made between product series that share tasks, such as drum filling, and with ancillary guidance, such as setting up health surveillance for work with a respiratory sensitiser. COSHH essentials has proved to be a popular tool for communicating good control practice. It has attracted over 1 million visits to its site since its launch. It offers a common benchmark of good practice for chemical users, manufacturers, suppliers and importers, as well as regulators and health professionals.

A spectroscopic investigation of the shape dependency of gold nanoparticles grown on roughened surfaces.

We present an investigation of the optical excitation of surface plasmons on Au films deposited on roughened surfaces by using a glancing angle deposition technique. By adjusting the deposition parameters of calcium fluoride and Au thin films, the spectral position of the surface plasmon resonances can be shifted through the green and into the near infrared region. In particular, we find that a rougher surface with obliquely deposited Au produces distinct spheroid-shaped nanoparticles (NPs). This results in stronger resonances with narrower linewidths, whereas smoother films result in broad red-shifted absorption. Imaging with an atomic force microscope and a scanning electron microscope provides information of NP geometry which are used as inputs for theoretical simulations of the observed spectra. The consequence of geometry distributions and inter-particle interactions are discussed. The ability to control the shape, therefore the optical response, of Au NPs over an arbitrarily large active area is of paramount importance in nano-science, especially in biological sensing applications and surface enhanced Raman scattering.

Microscopic and macroscopic signatures of antiferromagnetic domain walls.

Magnetotransport measurements on small single crystals of Cr, the elemental antiferromagnet, reveal the hysteretic thermodynamics of the domain structure. The temperature dependence of the transport coefficients is directly correlated with the real-space evolution of the domain configuration as recorded by x-ray microprobe imaging, revealing the effect of antiferromagnetic domain walls on electron transport. A single antiferromagnetic domain wall interface resistance is deduced to be of order 5 x 10(-5) mu Omega cm(2) at a temperature of 100 K.

Sculpting semiconductor heteroepitaxial islands: from dots to rods.

In the Ge on Si model heteroepitaxial system, metal patterns on the silicon surface provide unprecedented control over the morphology of highly ordered Ge islands. Island shape including nanorods and truncated pyramids is set by the metal species and substrate orientation. Analysis of island faceting elucidates the prominent role of the metal in promoting growth of preferred facet orientations while investigations of island composition and structure reveal the importance of Si-Ge intermixing in island evolution. These effects reflect a remarkable combination of metal-mediated growth phenomena that may be exploited to tailor the functionality of island arrays in heteroepitaxial systems.

Shear modulus and plasticity of a driven charge density wave.

We have probed the effects of transverse variations in pinning strength on charge-density-wave (CDW) structure in NbSe3 by x-ray micro-beam diffraction. In ribbonlike crystals having a large longitudinal step in thickness, the CDW first depins on the thick side of the step, causing rotations of the CDW wave vector. By measuring these rotations as a function of position and electric field, the corresponding shear strains are determined, allowing the CDW's shear modulus to be estimated. These results demonstrate the usefulness of x-ray microdiffraction as a tool in studying collective dynamics in electronic crystals.

Internal contamination of gloves: routes and consequences.

The effect of internal glove contamination was investigated using N-methyl pyrrolidone (NMP) as a biological marker to assess systemic absorption when wearing internally contaminated gloves, and when not wearing gloves but subjected to the same challenge contaminant. The routes by which the insides of gloves become contaminated were also investigated. The area of dermal contamination was quantified using a fluorescent tracer dye and a surface monitoring fluorimeter. The main routes of internal glove contamination were found to be self-contamination, cuff entry and failed gloves. Wearing internally contaminated gloves led to higher systemic absorption than was gained from the equivalent skin contamination when not wearing gloves. Repeat wetting of fingers with aqueous NMP, when gloves were not worn, gave higher systemic absorption than the equivalent continuous exposure, probably due to the low volatility of NMP leading to increased concentration and longer residence time on the skin.

Crystallization of charge holes in the spin ladder of Sr14Cu24O41.

Determining the nature of the electronic phases that compete with superconductivity in high-transition-temperature (high-T(c)) superconductors is one of the deepest problems in condensed matter physics. One candidate is the 'stripe' phase, in which the charge carriers (holes) condense into rivers of charge that separate regions of antiferromagnetism. A related but lesser known system is the 'spin ladder', which consists of two coupled chains of magnetic ions forming an array of rungs. A doped ladder can be thought of as a high-T(c) material with lower dimensionality, and has been predicted to exhibit both superconductivity and an insulating 'hole crystal' phase in which the carriers are localized through many-body interactions. The competition between the two resembles that believed to operate between stripes and superconductivity in high-T(c) materials. Here we report the existence of a hole crystal in the doped spin ladder of Sr14Cu24O41 using a resonant X-ray scattering technique. This phase exists without a detectable distortion in the structural lattice, indicating that it arises from many-body electronic effects. Our measurements confirm theoretical predictions, and support the picture that proximity to charge ordered states is a general property of superconductivity in copper oxides.

Probing large area surface plasmon interference in thin metal films using photon scanning tunneling microscopy.

The interference of surface plasmons can provide important information regarding the surface features of the hosting thin metal film. We present an investigation of the interference of optically excited surface plasmons in the Kretschmann configuration in the visible spectrum. Large area surface plasmon interference regions are generated at several wavelengths and imaged with the photon scanning tunneling microscope. Furthermore, we discuss the non-retarded dispersion relations for the surface plasmons in the probe-metal system modeled as confocal hyperboloids of revolution in the spheroidal coordinate systems.

A toolkit for dermal risk assessment and management: an overview.

The European Research project RISKOFDERM (QLK4-CT-1999-01107) has two major goals. One is the development of a conceptual model for dermal risk assessment for regulatory purposes, such as the registration of new chemicals. The other goal is to develop a simple-to-use toolkit for assessment and management of health risks from occupational dermal exposure. This toolkit was constructed by analysing the major determinants of dermal hazard and dermal exposure. The results were combined in the form of a decision-tree that leads the user of the toolkit through a number of questions on the hazardous properties of the chemical in use, and on the exposure situation. The toolkit translates the information given by the user into broad data categories of hazard and exposure that lead to a rough estimate of health risk from dermal exposure. This is done separately for local skin effects and skin allergy on the one hand, and systemic effects after skin penetration on the other hand. After going through the decision-tree, the user is advised to act to control the risk, and to read general information on dermal exposure and a statement describing the uncertainty of the risk estimate produced by the toolkit. The final version of the toolkit will be available for use on portable or stationary computers and runs the decision algorithms in the background so that the non-expert user only will see the judgements, the recommendations and the general information. The toolkit will be evaluated before release by experts on the various elements included in the toolkit and by field experts in its practical use. The toolkit is an attempt to adapt elements of exact science to a situation where the necessary input data are of limited quality and are only estimates. The toolkit does not claim to give precise answers based on imprecise information. The purpose is to enable the user to estimate the order of magnitude of hazard, exposure and risk, and to encourage the user to deal with the issues of dermal hazard, exposure and control.

X-ray microdiffraction images of antiferromagnetic domain evolution in chromium.

Magnetic x-ray diffraction combined with x-ray focusing optics was used to image individual antiferromagnetic spin density wave domains in a chromium single crystal at the micron scale. The cross section for nonresonant magnetic x-ray scattering depends on the antiferromagnetic modulation vector and spin polarization direction and allows these quantities to be extracted independently. The technique was used to show that the broadening of the nominally first-order "spin-flip" transition at 123 kelvin, at which the spins rotate by 90 degrees C, originates at the walls between domains with orthogonal modulation vectors. During cooling, the transition begins at these walls and progresses inward. The modulation vector domains are themselves unchanged.