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

XCDCC: Core Excitation in the Breakup of Exotic Nuclei

The eXtended Continuum Discretized Coupled Channel (XCDCC) method is developed to treat reactions where core degrees of freedom play a role. The projectile is treated as a multi-configuration coupled channels system generated from a valence particle coupled to a deformed core which is allowed to excite. The coupled channels initial state breaks up into a coupled channels continuum which is discretized into bins, similarly to the original CDCC method. Core collective degrees of freedom are also included in the interaction of the core and the target, so that dynamical effects can occur during the reaction. We present results for the breakup of $^{17}$C=$^{16}$C+n and $^{11}$Be=$^{10}$Be+n on $^{9}$Be. Results show that the total cross section increases with core deformation. More importantly, the relative percentage of the various components of the initial state are modified during the reaction process through dynamical effects. This implies that comparing spectroscopic factors from structure calculations with experimental cross sections requires more detailed reaction models that go beyond the single particle model.Comment: 14 pages, revtex, submitted to Phys Rev

The thermal decomposition of studtite: analysis of the amorphous phase

Studtite is known to exist at the back-end of the nuclear fuel cycle as an intermediate phase formed in the reprocessing of spent nuclear fuel. In the thermal decomposition of studtite, an amorphous phase is obtained at calcination temperatures between 200 and 500 °C. This amorphous compound, referred to elsewhere in the literature as U2O7, has been characterised by analytical spectroscopic methods. The local structure of the amorphous compound has been found to contain uranyl bonding by X-ray absorption near edge (XANES), Fourier transform infrared and Raman spectroscopy. Changes in bond distances in the uranyl group are discussed with respect to studtite calcination temperature. The reaction of the amorphous compound with water to form metaschoepite is also discussed and compared with the structure of schoepite and metaschoepite by X-ray diffraction. A novel schematic reaction mechanism for the thermal decomposition of studtite is proposed

B(E1) Strengths from Coulomb Excitation of 11Be

The $B$(E1;$1/2^+\to1/2^-$) strength for $^{11}$Be has been extracted from intermediate energy Coulomb excitation measurements, over a range of beam energies using a new reaction model, the extended continuum discretized coupled channels (XCDCC) method. In addition, a measurement of the excitation cross section for $^{11}$Be+$^{208}$Pb at 38.6 MeV/nucleon is reported. The $B$(E1) strength of 0.105(12) e$^2$fm$^2$ derived from this measurement is consistent with those made previously at 60 and 64 MeV/nucleon, i n contrast to an anomalously low result obtained at 43 MeV/nucleon. By coupling a multi-configuration description of the projectile structure with realistic reaction theory, the XCDCC model provides for the first time a fully quantum mechanical description of Coulomb excitation. The XCDCC calculations reveal that the excitation process involves significant contributions from nuclear, continuum, and higher-order effects. An analysis of the present and two earlier intermediate energy measurements yields a combined B(E1) strength of 0.105(7) e$^2$fm$^2$. This value is in good agreement with the value deduced independently from the lifetime of the $1/2^-$ state in $^{11}$Be, and has a comparable p recision.Comment: 5 pages, 2 figures, accepted for publication in Phys. Lett.

Red Queen Coevolution on Fitness Landscapes

Species do not merely evolve, they also coevolve with other organisms. Coevolution is a major force driving interacting species to continuously evolve ex- ploring their fitness landscapes. Coevolution involves the coupling of species fit- ness landscapes, linking species genetic changes with their inter-specific ecological interactions. Here we first introduce the Red Queen hypothesis of evolution com- menting on some theoretical aspects and empirical evidences. As an introduction to the fitness landscape concept, we review key issues on evolution on simple and rugged fitness landscapes. Then we present key modeling examples of coevolution on different fitness landscapes at different scales, from RNA viruses to complex ecosystems and macroevolution.Comment: 40 pages, 12 figures. To appear in "Recent Advances in the Theory and Application of Fitness Landscapes" (H. Richter and A. Engelbrecht, eds.). Springer Series in Emergence, Complexity, and Computation, 201

Breakup reaction models for two- and three-cluster projectiles

Breakup reactions are one of the main tools for the study of exotic nuclei, and in particular of their continuum. In order to get valuable information from measurements, a precise reaction model coupled to a fair description of the projectile is needed. We assume that the projectile initially possesses a cluster structure, which is revealed by the dissociation process. This structure is described by a few-body Hamiltonian involving effective forces between the clusters. Within this assumption, we review various reaction models. In semiclassical models, the projectile-target relative motion is described by a classical trajectory and the reaction properties are deduced by solving a time-dependent Schroedinger equation. We then describe the principle and variants of the eikonal approximation: the dynamical eikonal approximation, the standard eikonal approximation, and a corrected version avoiding Coulomb divergence. Finally, we present the continuum-discretized coupled-channel method (CDCC), in which the Schroedinger equation is solved with the projectile continuum approximated by square-integrable states. These models are first illustrated by applications to two-cluster projectiles for studies of nuclei far from stability and of reactions useful in astrophysics. Recent extensions to three-cluster projectiles, like two-neutron halo nuclei, are then presented and discussed. We end this review with some views of the future in breakup-reaction theory.Comment: Will constitute a chapter of "Clusters in Nuclei - Vol.2." to be published as a volume of "Lecture Notes in Physics" (Springer

Personalized brain stimulation of memory networks

Available online 13 September 2022Background: The finding that transcranial magnetic stimulation (TMS) can enhance memory performance via stimulation of parietal sites within the Cortical-Hippocampal Network counts as one of the most exciting findings in this field in the past decade. However, the first independent effort aiming to fully replicate this finding found no discernible influence of TMS on memory performance. Objective: We examined whether this might relate to interindividual spatial variation in brain connectivity architecture, and the capacity of personalisation methodologies to overcome the noise inherent across independent scanners and cohorts. Methods: We implemented recently detailed personalisation methodology to retrospectively compute individual-specific parietal targets and then examined relation to TMS outcomes. Results: Closer proximity between actual and novel fMRI-personalized targets associated with greater improvement in memory performance. Conclusion: These findings demonstrate the potential importance of aligning brain stimulation targets according to individual-specific differences in brain connectivity, and extend upon recent findings in prefrontal cortex.Robin F.H. Cash, Joshua Hendrikse, Kavisha B Fernando, Sarah Thompson, Chao Suo, Alex Fornito, Murat Yücel, Nigel C. Rogasch, Andrew Zalesky, James P. Coxo

A terminal assessment of stages theory : introducing a dynamic states approach to entrepreneurship

Stages of Growth models were the most frequent theoretical approach to understanding entrepreneurial business growth from 1962 to 2006; they built on the growth imperative and developmental models of that time. An analysis of the universe of such models (N=104) published in the management literature shows no consensus on basic constructs of the approach, nor is there any empirical confirmations of stages theory. However, by changing two propositions of the stages models, a new dynamic states approach is derived. The dynamic states approach has far greater explanatory power than its precursor, and is compatible with leading edge research in entrepreneurship

Twenty Years of the Polyvinyl Chloride Sustainability Challenges

Intense campaigning pressure on the UK PVC sector up to the late 1990s forced strategic engagement with sustainable development. Simplified outcomes from a detailed, consensus-based analysis by science-based NGO The Natural Step (TNS) took the form of five TNS Sustainability Challenges for PVC published in 2000. UK manufacturing companies initially used these Challenges to direct strategic progress. The Challenges have since been progressively taken up across European PVC value chains. The VinylPlus® programme uses an updated version of the five Challenges as a basis for voluntary commitments and transparent auditing of progress against published targets. Initial framing of the five TNS Sustainability Challenges for PVC were drafted consciously for generic relevance to other materials. Assessing the sustainability performance of some alternative materials to PVC against the five Sustainability Challenges reveals different sustainability performance in a range of potential applications. This highlights the danger inherent in automatic selection or deselection of materials in the absence of assessment of options on a ‘level playing field’ of sustainability principles. The five TNS Sustainability Challenges for PVC remain valid today and into the longer-term future as a basis for making stepwise, profitable progress towards the goal of sustainability for PVC and other materials