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Influence of P{sub 2}O{sub 5} and Al{sub 2}O{sub 3} content on the structure of erbium-doped borosilicate glasses and on their physical, thermal, optical and luminescence properties
Highlights: • Reorganization of the glass structure induced by the addition of P{sub 2}O{sub 5} or Al{sub 2}O{sub 3}. • Emission properties related to the presence of P or Al in the Er{sup 3+} coordination shell. • Declustering observed upon addition of P{sub 2}O{sub 5}. • No declustering upon addition of Al{sub 2}O{sub 3}. - Abstract: The effect of P{sub 2}O{sub 5} and/or Al{sub 2}O{sub 3} addition in Er-doped borosilicate glasses on the physical, thermal, optical, and luminescence properties is investigated. The changes in these glass properties are related to the glass structure modifications induced by the addition of P{sub 2}O{sub 5} and/or Al{sub 2}O{sub 3}, which were probed by FTIR, {sup 11}B MAS NMR and X-ray photoelectron spectroscopies. Variations of the polymerization degree of the silicate tetrahedra and modifications in the {sup [3]}B/{sup [4]}B ratio are explained by a charge compensation mechanism due to the formation of AlO{sub 4}, PO{sub 4} groups and the formation of Al-O-P linkages in the glass network. From the absorption and luminescence properties of the Er{sup 3+} ions at 980 nm and 1530 nm, declustering is suspected for the highest P{sub 2}O{sub 5} concentrations while for the highest Al{sub 2}O{sub 3} concentrations no declustering is observed.
Erbium-doped borosilicate glasses containing various amounts of P{sub 2}O{sub 5} and Al{sub 2}O{sub 3}: Influence of the silica content on the structure and thermal, physical, optical and luminescence properties
Highlights: • Er{sup 3+} doped borosilicate glasses were processed with different compositions and characterizations. • An increase in the SiO{sub 2} content leads to a silicate-rich environment around the Er{sup 3+} site. • An increase in the SiO{sub 2} content decreases the Er{sup 3+} absorption cross-section at 980 nm. • Glasses with 60 mol% of SiO{sub 2} exhibit a stronger emission intensity at 1530 nm than glasses with x = 50. • Highest 1.5 μm emission intensity was achieved for the Al and P containing glass with 60 mol% of SiO{sub 2}. - Abstract: The influence of the silica content on several properties of Er-doped borosilicate glasses in the presence of various amounts of P{sub 2}O{sub 5} and Al{sub 2}O{sub 3} has been investigated. The introduction of P{sub 2}O{sub 5} and/or Al{sub 2}O{sub 3} are responsible for structural modifications in the glass network through a charge-compensation mechanism related to the formation of negatively-charged PO{sub 4} and AlO{sub 4} groups or through the formation of AlPO{sub 4}-like structural units. In this paper, we show that an increase in the SiO{sub 2} content leads to a silicate-rich environment around the Er{sup 3+} site, resulting in an increased dependence of the Er{sup 3+} ions optical and luminescence properties on the P{sub 2}O{sub 5} and/or Al{sub 2}O{sub 3} concentration. The highest emission intensity at 1.5 μm was achieved for the glass with an equal proportion of P and Al in the glass system with 60 mol% of SiO{sub 2}.
3D probabilistic fracture mechanics / computational fluid dynamics simulation of a reactor pressure vessel under transient conditions
Reactor pressure vessels (RPVs) are safety-critical light-water-reactor components that, under irradiation, experience long-term material degradation in the form of embrittlement. This can increase their susceptibility to fracture under thermal-shock conditions, which could occur during off-normal transients such as loss-of-coolant accidents (LOCAs). During a LOCA, the most severe conditions for the RPV occur when emergency core cooling water is injected through the cold legs into the water-and-steam-filled RPV. The rapid cooling of the downcomer and internal RPV surface causes decreased temperature and elevated thermally driven tensile stresses in the RPV wall. This, combined with long-term material embrittlement, may cause fracture initiation at pre-existing flaws, challenging the integrity of the RPV. Assessing RPV integrity during transients with a large spatial variation in the coolant temperature requires a modeling approach that considers the effects of spatially varying coolant temperature on the fracture probability of a population of flaws distributed throughout the RPV, accounting for spatially varying embrittlement. Here, the present study addresses this need by demonstrating first-of-its-kind coupling of a high-fidelity 3D computational fluid dynamics code with 3D probabilistic fracture mechanics This was accomplished using representative models of a pressurized-water reactor subjected to small- and medium-break LOCA conditions, both of which can result in large spatial temperature variations. While the observed impact of accounting for 3D effects was minimal under the small-break LOCA this study indicates a significant increase in the probability of fracture initiation under the medium-break LOCA when 3D effects are considered, relative to a spatially uniform cooling scenario.
Surface-wave-assisted nonreciprocity in spatio-temporally modulated metasurfaces
Emerging photonic functionalities are mostly governed by the fundamental principle of Lorentz reciprocity. Lifting the constraints imposed by this principle could circumvent deleterious effects that limit the performance of photonic systems. Most efforts to date have been limited to waveguide platforms. Here, we propose and experimentally demonstrate a spatiotemporally modulated metasurface capable of complete violation of Lorentz reciprocity by reflecting an incident beam into far-field radiation in forward scattering, but into near-field surface waves in reverse scattering. These observations are shown both in nonreciprocal beam steering and nonreciprocal focusing. We also demonstrate nonreciprocal behavior of propagative-only waves in the frequency- and momentum-domains, and simultaneously in both. We develop a generalized Bloch-Floquet theory which offers physical insights into Lorentz nonreciprocity for arbitrary spatial phase gradients, and its predictions are in excellent agreement with experiments. Our work opens exciting opportunities in applications where free-space nonreciprocal wave propagation is desired.
Expanding applications of SERS through versatile nanomaterials engineering
Nanomaterials engineering and synthetic chemistry continues to expand the range of applications for surface-enhanced Raman scattering spectroscopy.
Enabling quantitative analysis of complex polymer blends by infrared nanospectroscopy and isotopic deuteration
Atomic-force microscopy coupled with infrared spectroscopy (AFM-IR) deciphers surface morphology of thin-film polymer blends and composites by simultaneously mapping physical topography and chemical composition. However, acquiring quantitative phase and composition information from multi-component blends can be challenging using AFM-IR due to the possible overlapping infrared absorption bands between different species. Isotope labeling one of the blend components introduces a new type of bond (carbon-deuterium vibration) that can be targeted using AFM-IR and responds at wavelengths sufficiently shifted toward unoccupied regions (around 2200 cm –1 ). In this project, AFM-IR was used to probe the surface morphology and chemical composition of three polymer blends containing deuterated polystyrene; each blend is expected to exhibit various degrees of miscibility. AFM-IR results successfully demonstrated that deuterium labeling prevents infrared spectral overlap and enables the visualization of blend phases that could not normally be distinguished by other scanning probe techniques. The nanoscale domain composition was resolved by fast infrared spectrum analysis. Overall, we presented isotope labeling as a robust approach for circumventing obstacles preventing the quantitative analysis of multiphase systems by AFM-IR.
Femtosecond laser structuring of silver-containing glass: Silver redistribution, selective etching, and surface topology engineering
Femtosecond direct laser writing in silver-containing phosphate glasses allows for the three-dimensional (3D) implementation of complex photonic structures. Sample translation along or perpendicular to the direction of the beam propagation has been performed, which led to the permanent formation of fluorescent structures, either corresponding to a tubular shape or to two parallel planes at the vicinity of the interaction voxel, respectively. These optical features are related to significant modifications of the local material chemistry. Indeed, silver depletion areas with a diameter below 200 nm were evidenced at the center of the photo-produced structures while photo-produced luminescence properties are attributed to the formation of silver clusters around the multiphoton interaction voxel. The laser-triggered oxidation-reduction processes and the associated photo-induced silver redistribution are proposed to be at the origin of the observed original 3D luminescent structures. Thanks to such material structuring, surface engineering has been also demonstrated. Selective surface chemical etching of the glass has been obtained subsequently to laser writing at the location of the photo-produced structures, revealing features with nanometric depth profiles and radial dimensions strongly related to the spatial distributions of the silver clusters.
Work function tuning at Au-HfO{sub 2} interfaces using organophosphonate monolayers
We show that introducing organophosphonate nanomolecular monolayers (NMLs) at Au-HfO{sub 2} interfaces shift the effective work function by 0.2 eV ≥ ΔΦ{sub eff} ≥ −0.6 eV, due to NML body and bonding dipoles. Electron spectroscopy of NML-Au, NML-HfO{sub 2,} and Au-NML-HfO{sub 2} structures indicate that the Au-NML bond strength is the major factor. Au-NML covalent bonding yields ΔΦ{sub eff} ∼ − 0.2 eV, while weak bonding yields ΔΦ{sub eff} ∼ 0.6 eV. In contrast, NMLs on HfO{sub 2} decrease Φ{sub eff} by ∼0.4 eV due to competing contributions from NML-HfO{sub 2} bonding strength and NML orientation. These findings are relevant for nanomolecularly tailoring the electronic properties of metal–ceramic interfaces for applications.
On-lattice kinetic Monte Carlo approaches for modeling molecular anisotropy in resveratrol crystallization
Stilbenes are a class of organic compounds with broad-ranging pharmaceutical and agricultural applications, which are typically isolated and purified through recrystallization. We are motivated by reducing experimental waste and optimizing yield via developing predictive simulations for processing-dependent crystal morphologies. Using resveratrol as a model stilbene system, we have developed an approach for simulating crystallization with molecular resolution using on-lattice kinetic Monte Carlo. In this work, we highlight modifications to the Stochastic Parallel PARticle Kinetic Simulator (SPPARKS) software package, which were essential to this application. Key enhancements include the incorporation of non-orthogonal cell shapes and monomer anisotropy approximations using bound hard spheres. This new SPPARKS application has been applied to resveratrol with attachment energy libraries obtained from density functional theory, resulting in excellent agreement with experimental morphology prediction.
Passive radiative thermal management using phase-change metasurfaces
Abstract Realizing innovative composite materials with passive thermal management capabilities and minimal ecological footprints is a challenging but much sought-after goal that would have a transformative effect on renewable energy sciences. We demonstrate an environmentally friendly metasurface utilizing vanadium dioxide (VO 2 ) that offers responsiveness to ambient temperature and potentially long-term stability. The metasurface enables passive thermal management by self-adjusting its absorptivity and emissivity response over a broad bandwidth ranging from visible to mid-infrared (IR) wavelengths. Above the VO 2 phase transition the metasurface exhibits increased mid-IR emissivity and reduced visible/near-IR absorptivity, creating an efficient radiative emission channel in the first atmospheric transparency window with reduced absorption of solar radiation. In contrast, below VO 2 ’s transition temperature, the metasurface increasingly absorbs sun light while minimizing mid-IR radiative heat losses. Moreover, a functional silicon layer eliminates the need for an additional capping layer commonly employed to protect VO 2 from environmental degradation. The additional protective layer often impedes the use and performance of VO 2 based devices in terrestrial as well as spacecraft applications. Therefore, the proposed durable and eco-friendly metasurface will be an excellent candidate for essential passive thermal regulation systems across residential and terrestrial applications.
Superiority of compensatory reserve measurement compared with the Shock index for early and accurate detection of reduced central blood volume status
Shock index (SI) equals the ratio of heart rate (HR) to systolic blood pressure (SBP) with clinical evidence that it is more sensitive for trauma patient status assessment and prediction of outcome compared with either HR or SBP alone. We used lower body negative pressure (LBNP) as a human model of central hypovolemia and compensatory reserve measurement (CRM) validated for accurate tracking of reduced central blood volume to test the hypotheses that SI: (1) presents a late signal of central blood volume status; (2) displays poor sensitivity and specificity for predicting the onset of hemodynamic decompensation; and (3) cannot identify individuals at greatest risk for the onset of circulatory shock. We measured HR, SBP, and CRM in 172 human subjects (19–55 years) during progressive LBNP designed to determine tolerance to central hypovolemia as a model of hemorrhage. Subjects were subsequently divided into those with high tolerance (HT) (n = 118) and low tolerance (LT) (n = 54) based on completion of 60 mm Hg LBNP. The time course relationship between SI and CRM was determined and receiver operating characteristic (ROC) area under the curve (AUC) was calculated for sensitivity and specificity of CRM and SI to predict hemodynamic decompensation using clinically defined thresholds of 40% for CRM and 0.9 for SI. The time and level of LBNP required to reach a SI = 0.9 (~60 mm Hg LBNP) was significantly greater (p < 0.001) compared with CRM that reached 40% at ~40 mm Hg LBNP. Shock index did not differ between HT and LT subjects at 45 mm Hg LBNP levels. ROC AUC for CRM was 0.95 (95% CI = 0.94–0.97) compared with 0.91 (0.89–0.94) for SI (p = 0.0002). Despite high sensitivity and specificity, SI delays time to detect reductions in central blood volume with failure to distinguish individuals with varying tolerances to central hypovolemia.
Developing a Marine Energy Workforce Pipeline through STEM Education
Marine Energy is a nascent but growing industry and will need a strong workforce to be successful. This paper examines the resources and programs needed to achieve the industry's goals.
Wireless Temperature Sensing using Permanent Magnets for Multiple Points Undergoing Repeatable Motions.
Abstract not provided.
COVID-19 Exposure Assessment Tool (CEAT): Exposure quantification based on ventilation, infection prevalence, group characteristics, and behavior
The coronavirus disease 2019 (COVID-19) Exposure Assessment Tool (CEAT) allows users to compare respiratory relative risk to severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) for various scenarios, providing understanding of how combinations of protective measures affect risk. CEAT incorporates mechanistic, stochastic, and epidemiological factors including the (i) emission rate of virus, (ii) viral aerosol degradation and removal, (iii) duration of activity/exposure, (iv) inhalation rates, (v) ventilation rates (indoors/outdoors), (vi) volume of indoor space, (vii) filtration, (viii) mask use and effectiveness, (ix) distance between people (taking into account both near-field and far-field effects of proximity), (x) group size, (xi) current infection rates by variant, (xii) prevalence of infection and immunity in the community, (xiii) vaccination rates, and (xiv) implementation of COVID-19 testing procedures. CEAT applied to published studies of COVID-19 transmission events demonstrates the model’s accuracy. We also show how health and safety professionals at NASA Ames Research Center used CEAT to manage potential risks posed by SARS-CoV-2 exposures.
In vitro selection and analysis of SARS-CoV-2 nirmatrelvir resistance mutations contributing to clinical virus resistance surveillance
To facilitate the detection and management of potential clinical antiviral resistance, in vitro selection of drug-resistant severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) against the virus M pro inhibitor nirmatrelvir (Paxlovid active component) was conducted. Six M pro mutation patterns containing T304I alone or in combination with T21I, L50F, T135I, S144A, or A173V emerged, with A173V+T304I and T21I+S144A+T304I mutations showing >20-fold resistance each. Biochemical analyses indicated inhibition constant shifts aligned to antiviral results, with S144A and A173V each markedly reducing nirmatrelvir inhibition and M pro activity. SARS-CoV-2 surveillance revealed that in vitro resistance–associated mutations from our studies and those reported in the literature were rarely detected in the Global Initiative on Sharing All Influenza Data database. In the Paxlovid Evaluation of Protease Inhibition for COVID-19 in High-Risk Patients trial, E166V was the only emergent resistance mutation, observed in three Paxlovid-treated patients, none of whom experienced COVID-19–related hospitalization or death.
An oral SARS-CoV-2 M[superscript pro] inhibitor clinical candidate for the treatment of COVID-19
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Solid Electrolytes as Thermally Activated Ionic Switches.
Abstract not provided.