Solubility, speciation and local environment of chlorine in zirconolite glass–ceramics for the immobilisation of plutonium residues

The immobilisation and disposal of fissile materials from civil and defence nuclear programmes requires compatible, passively safe and proliferation resistant wasteforms. In this study, we demonstrate the application of an albite glass–zirconolite ceramic material for immobilisation of chloride contaminated plutonium oxide residues in the United Kingdom. The chlorine solubility limit in the albite glass phase was determined to be 1.0 ± 0.1 wt%, above the maximum envisaged chorine inventory of 0.5 wt%, attainable at a 20 wt% PuO2 incorporation rate within the ceramic. Cl K-edge of X-ray Absorption Near Edge Spectroscopy (XANES) was exploited to confirm partitioning of Cl to the glass phase, speciated as the chloride anion, with exsolution of crystalline NaCl above the chlorine solubility limit. Combinatorial fitting of Cl XANES data, utilising a library of chemically plausible reference spectra, demonstrated the association of Cl with Na and Ca modifier cations, with environments characteristic of the aluminosilicate chloride minerals eudialyte, sodalite, chlorellestadite and afghanite. Adventitious incorporation of Ca, Zr and Ti within the albite glass phase apparently assists chlorine solubility, by templating a local chemical environment characteristic of the mineral reference compounds. The partitioning of Ce, as a Pu analogue, within the glass–ceramic was not adversely impacted by incorporation of Cl. The significance of this research is in demonstrating the compatibility of the glass–ceramic wasteform toward Cl solubility at the expected incorporation rate, below the determined solubility limit. Thus, an upstream heat treatment facility to remove chloride contamination, as specified in the current conceptual flowsheet, would not be required from the perspective of wasteform compatibility, thus providing scope to de-risk the technology roadmap and reduce the projected capital and operational plant costs

Synthesis and characterisation of the hollandite solid solution Ba1.2-xCsxFe2.4-xTi5.6+xO16 for partitioning and conditioning of radiocaesium

The geological disposal of high level radioactive waste requires careful budgeting of the heat load produced by radiogenic decay. Removal of high-heat generating radionuclides, such as 137 Cs, reduces the heat load in the repository allowing the remaining high level waste to be packed closer together therefore reducing demand for repository space and the cost of the disposal of the remaining wastes. Hollandites have been proposed as a possible host matrix for the long-term disposal of Cs separated from HLW raffinate. The incorporation of Cs into the hollandite phase is aided by substitution of cations on the B-site of the hollandite structure, including iron. A range of Cs containing iron hollandites were synthesised via an alkoxide-nitrate route and the structural environment of Fe in the resultant material characterised by Mössbauer and X-ray Absorption Near Edge Spectroscopy. The results of spectroscopic analysis found that Fe was present as octahedrally co-ordinated Fe (III) in all cases and acts as an effective charge compensator over a wide solid solution range

Navigating data governance associated with real-world data for public benefit: an overview in the UK and future considerations

Real-world data encompass data primarily captured for the provision or operation of services, for example, electronic health records for direct care purposes, but which may have secondary uses for informing research or commissioning. Public benefit is potentially forfeited by the underutilisation of real-world data for secondary uses, in part due to risk aversion when faced with the prospect of navigating necessary and important data governance processes. Such processes can be perceived as complex, daunting, time-consuming and exposing organisations to risk. By providing an overview description and discussion around the role of six key legal and information governance frameworks and their role regarding responsible data access, linkage and sharing, our intention is to make data governance a less daunting prospect and reduce the perception that it is a barrier to secondary uses, thus enabling public benefit

True Superconductivity in a 2D "Superconducting-Insulating" System

We present results on disordered amorphous films which are expected to undergo a field-tuned Superconductor-Insulator Transition. Based on low-field data and I-V characteristics, we find evidence of a low temperature Metal-to-Superconductor transition. This transition is characterized by hysteretic magnetoresistance and discontinuities in the I-V curves. The metallic phase just above the transition is different from the "Fermi Metal" before superconductivity sets in.Comment: 3 pages, 4 figure

Can Short-Range Interactions Mediate a Bose Metal Phase in 2D?

We show here based on a 1-loop scaling analysis that short-range interactions are strongly irrelevant perturbations near the insulator-superconductor (IST) quantum critical point. The lack of any proof that short-range interactions mediate physics which is present only in strong coupling leads us to conclude that short-range interactions are strictly irrelevant near the IST quantum critical point. Hence, we argue that no new physics, such as the formation of a uniform Bose metal phase can arise from an interplay between on-site and nearest-neighbour interactions.Comment: 3 pages, 1 .eps file. SUbmitted to Phys. Rev.

Polarization coupling and pattern selection in a type-II optical parametric oscillator

We study the role of a direct intracavity polarization coupling in the dynamics of transverse pattern formation in type-II optical parametric oscillators. Transverse intensity patterns are predicted from a stability analysis, numerically observed, and described in terms of amplitude equations. Standing wave intensity patterns for the two polarization components of the field arise from the nonlinear competition between two concentric rings of unstable modes in the far field. Close to threshold a wavelength is selected leading to standing waves with the same wavelength for the two polarization components. Far from threshold the competition stabilizes patterns in which two different wavelengths coexist.Comment: 14 figure

Companions of Stars: From Other Stars to Brown Dwarfs to Planets: The Discovery of the First Methane Brown Dwarf

The discovery of the first methane brown dwarf provides a framework for describing the important advances in both fundamental physics and astrophysics that are due to the study of companions of stars. I present a few highlights of the history of this subject along with details of the discovery of the brown dwarf Gliese 229B. The nature of companions of stars is discussed with an attempt to avoid biases induced by anthropocentric nomenclature. With the newer types of remote reconnaissance of nearby stars and their systems of companions, an exciting and perhaps even more profound set of contributions to science is within reach in the near future. This includes an exploration of the diversity of planets in the universe and perhaps soon the first solid evidence for biological activity outside our Solar System.Comment: 31 pages, 13 figure

Grain boundary pinning and glassy dynamics in stripe phases

We study numerically and analytically the coarsening of stripe phases in two spatial dimensions, and show that transient configurations do not achieve long ranged orientational order but rather evolve into glassy configurations with very slow dynamics. In the absence of thermal fluctuations, defects such as grain boundaries become pinned in an effective periodic potential that is induced by the underlying periodicity of the stripe pattern itself. Pinning arises without quenched disorder from the non-adiabatic coupling between the slowly varying envelope of the order parameter around a defect, and its fast variation over the stripe wavelength. The characteristic size of ordered domains asymptotes to a finite value $R_g \sim \lambda_0\ \epsilon^{-1/2}\exp(|a|/\sqrt{\epsilon})$, where$\epsilon\ll 1$is the dimensionless distance away from threshold,$\lambda_0$the stripe wavelength, and$a$ a constant of order unity. Random fluctuations allow defect motion to resume until a new characteristic scale is reached, function of the intensity of the fluctuations. We finally discuss the relationship between defect pinning and the coarsening laws obtained in the intermediate time regime.Comment: 17 pages, 8 figures. Corrected version with one new figur

Balloon Measurements of Cosmic Ray Muon Spectra in the Atmosphere along with those of Primary Protons and Helium Nuclei over Mid-Latitude

We report here the measurements of the energy spectra of atmospheric muons and of the cosmic ray primary proton and helium nuclei in a single experiment. These were carried out using the MASS superconducting spectrometer in a balloon flight experiment in 1991. The relevance of these results to the atmospheric neutrino anomaly is emphasized. In particular, this approach allows uncertainties caused by the level of solar modulation, the geomagnetic cut-off of the primaries and possible experimental systematics to be decoupled in the comparison of calculated fluxes of muons to measured muon fluxes. The muon observations cover the momentum and depth ranges of 0.3-40 GeV/c and 5-886 g/cmsquared, respectively. The proton and helium primary measurements cover the rigidity range from 3 to 100 GV, in which both the solar modulation and the geomagnetic cut-off affect the energy spectra at low energies.Comment: 31 pages, including 17 figures, simplified apparatus figure, to appear in Phys. Rev.

Cosmological evolution of interacting dark energy in Lorentz violation

The cosmological evolution of an interacting scalar field model in which the scalar field interacts with dark matter, radiation, and baryon via Lorentz violation is investigated. We propose a model of interaction through the effective coupling $\bar{\beta}$. Using dynamical system analysis, we study the linear dynamics of an interacting model and show that the dynamics of critical points are completely controlled by two parameters. Some results can be mentioned as follows. Firstly, the sequence of radiation, the dark matter, and the scalar field dark energy exist and baryons are sub dominant. Secondly, the model also allows the possibility of having a universe in the phantom phase with constant potential. Thirdly, the effective gravitational constant varies with respect to time through $\bar{\beta}$. In particular, we consider a simple case where $\bar{\beta}$ has a quadratic form and has a good agreement with the modified $\Lambda$CDM and quintessence models. Finally, we also calculate the first post--Newtonian parameters for our model.Comment: 14 pages, published versio