Complementarity of neutron reflectometry and ellipsometry for the study of atmospheric reactions at the air–water interface

The combined application of neutron reflectometry (NR) and ellipsometry to determine the oxidation kinetics of organic monolayers at the air–water interface is described for the first time. This advance was possible thanks to a new miniaturised reaction chamber that is compatible with the two techniques and has controlled gas delivery. The rate coefficient for the oxidation of methyl oleate monolayers by gas-phase O3 determined using NR is (5.4 ± 0.6) × 10−10 cm2 per molecule per s, which is consistent with the value reported in the literature but is now better constrained. This highlights the potential for the investigation of faster atmospheric reactions in future studies. The rate coefficient determined using ellipsometry is (5.0 ± 0.9) × 10−10 cm2 per molecule per s, which indicates the potential of this more economical, laboratory-based technique to be employed in parallel with NR. In this case, temporal fluctuations in the optical signal are attributed to the mobility of islands of reaction products. We outline how such information may provide critical missing information in the identification of transient reaction products in a range of atmospheric surface reactions in the future

Night-time oxidation of surfactants at the air–water interface: effects of chain length, head group and saturation

Reactions of the key atmospheric night-time oxidant NO3 with organic monolayers at the air–water interface are used as proxies for the ageing of organic-coated aqueous aerosols. The surfactant molecules chosen for this study are oleic acid (OA), palmitoleic acid (POA), methyl oleate (MO) and stearic acid (SA) to investigate the effects of chain length, head group and degree of unsaturation on the reaction kinetics and products formed. Fully and partially deuterated surfactants were studied using neutron reflectometry (NR) to determine the reaction kinetics of organic monolayers with NO3 at the air–water interface for the first time. Kinetic modelling allowed us to determine the rate coefficients for the oxidation of OA, POA and MO monolayers to be (2.8 ± 0.7) × 10−8 cm2 molecule−1 s−1, (2.4 ± 0.5) × 10−8 cm2 molecule−1 s−1 and (3.3 ± 0.6) × 10−8 cm2 molecule−1 s−1, respectively. The corresponding uptake coefficients were found to be (2.1 ± 0.5) × 10−3, (1.7 ± 0.3) × 10−3 and (2.1 ± 0.4) × 10−3. For the much slower NO3-initiated oxidation of the saturated surfactant SA we found a loss rate of (5 ± 1) × 10−12 cm2 molecule−1 s−1 which we consider to be an upper limit for the reactive loss, and estimated an uptake coefficient of (5 ± 1) × 10−7. Our investigations demonstrate that NO3 will contribute substantially to the processing of unsaturated surfactants at the air–water interface during night-time given its reactivity is ca. two orders of magnitude higher than that of O3. Furthermore, the relative contributions of NO3 and O3 to the oxidative losses vary massively between species that are closely related in structure: NO3 reacts ca. 400 times faster than O3 with the common model surfactant oleic acid, but only ca. 60 times faster with its methyl ester MO. It is therefore necessary to perform a case-by-case assessment of the relative contributions of the different degradation routes for any specific surfactant. The overall impact of NO3 on the fate of saturated surfactants is slightly less clear given the lack of prior kinetic data for comparison, but NO3 is likely to contribute significantly to the loss of saturated species and dominate their loss during night-time. The retention of the organic character at the air–water interface differs fundamentally between the different surfactant species: the fatty acids studied (OA and POA) form products with a yield of ∼ 20% that are stable at the interface while NO3-initiated oxidation of the methyl ester MO rapidly and effectively removes the organic character (≤ 3% surface-active products). The film-forming potential of reaction products in real aerosol is thus likely to depend on the relative proportions of saturated and unsaturated surfactants as well as the head group properties. Atmospheric lifetimes of unsaturated species are much longer than those determined with respect to their reactions at the air–water interface, so that they must be protected from oxidative attack e.g. by incorporation into a complex aerosol matrix or in mixed surface films with yet unexplored kinetic behaviour

Improvement of accuracy of multi-scale models of Li-ion batteries by applying operator splitting techniques

In this work operator splitting techniques have been applied successfully to improve the accuracy of multi-scale Lithium-ion (Li-ion) battery models. A slightly simplified Li-ion battery model is derived, which can be solved on one time scale and multiple time scales. Different operator splitting schemes combined with different approximations are compared with the non-splitted reference solution in terms of stability, accuracy and processor cost. It is shown, that the reverse Strang–Marchuk splitting combined with the implicit scheme to solve the diffusion operator and Newton method to approximate the non-linear source term can improve the accuracy of the commonly applied vertical (sequential) multi-scale models by almost 3 times without considerably increasing the processor cost. © 2016 The Author

Analysis of ASTEC-Na capabilities for simulating a loss of flow CABRI experiment

Abstract This paper presents simulation results of the CABRI BI1 test using the code ASTEC-Na, currently under development, as well as a comparison of the results with available experimental data. The EU-JASMIN project (7th FP of EURATOM) centres on the development and validation of the new severe accident analysis code ASTEC-Na (Accident Source Term Evaluation Code) for sodium-cooled fast reactors whose owner and developer is IRSN. A series of experiments performed in the past (CABRI/SCARABEE experiments) and new experiments to be conducted in the new experimental sodium facility KASOLA have been chosen to validate the developed ASTEC-Na code. One of the in-pile experiments considered for the validation of ASTEC-Na thermal–hydraulic models is the CABRI BI1 test, a pure loss-of-flow transient using a low burnup MOX fuel pin. The experiment resulted in a channel voiding as a result of the flow coast-down leading to clad melting. Only some fuel melting took place. Results from the analysis of this test using SIMMER and SAS-SFR codes are also presented in this work to check their suitability for further code benchmarking purposes

Air quality and mental illness: Role of bioaerosols, causal mechanisms and research priorities

BACKGROUND: Poor air quality can both trigger and aggravate lung and heart conditions, as well as affecting child development. It can even lead to neurological and mental health problems. However, the precise mechanisms by which air pollution affect human health are not well understood. AIMS: To promote interdisciplinary dialogue and better research based on a critical summary of evidence on air quality and health, with an emphasis on mental health, and to do so with a special focus on bioaerosols as a common but neglected air constituent. METHOD: A rapid narrative review and interdisciplinary expert consultation, as is recommended for a complex and rapidly changing field of research. RESULTS: The research methods used to assess exposures and outcomes vary across different fields of study, resulting in a disconnect in bioaerosol and health research. We make recommendations to enhance the evidence base by standardising measures of exposure to both particulate matter in general and bioaerosols specifically. We present methods for assessing mental health and ideal designs. There is less research on bioaerosols, and we provide specific ways of measuring exposure to these. We suggest research designs for investigating causal mechanisms as important intermediate steps before undertaking larger-scale and definitive studies. CONCLUSIONS: We propose methods for exposure and outcome measurement, as well as optimal research designs to inform the development of standards for undertaking and reporting research and for future policy

Evidence for proton acceleration up to TeV energies based on VERITAS and Fermi-LAT observations of the Cas A SNR

We present a study of $\gamma$-ray emission from the core-collapse supernova remnant Cas~A in the energy range from 0.1GeV to 10TeV. We used 65 hours of VERITAS data to cover 200 GeV - 10 TeV, and 10.8 years of \textit{Fermi}-LAT data to cover 0.1-500 GeV. The spectral analysis of \textit{Fermi}-LAT data shows a significant spectral curvature around $1.3 \pm 0.4_{stat}$ GeV that is consistent with the expected spectrum from pion decay. Above this energy, the joint spectrum from \textit{Fermi}-LAT and VERITAS deviates significantly from a simple power-law, and is best described by a power-law with spectral index of $2.17\pm 0.02_{stat}$ with a cut-off energy of $2.3 \pm 0.5_{stat}$ TeV. These results, along with radio, X-ray and $\gamma$-ray data, are interpreted in the context of leptonic and hadronic models. Assuming a one-zone model, we exclude a purely leptonic scenario and conclude that proton acceleration up to at least 6 TeV is required to explain the observed $\gamma$-ray spectrum. From modeling of the entire multi-wavelength spectrum, a minimum magnetic field inside the remnant of $B_{\mathrm{min}}\approx150\,\mathrm{\mu G}$ is deduced.Comment: 33 pages, 9 Figures, 6 Table

Demonstration of stellar intensity interferometry with the four VERITAS telescopes

High angular resolution observations at optical wavelengths provide valuable insights in stellar astrophysics, directly measuring fundamental stellar parameters, and probing stellar atmospheres, circumstellar disks, elongation of rapidly rotating stars, and pulsations of Cepheid variable stars. The angular size of most stars are of order one milli-arcsecond or less, and to spatially resolve stellar disks and features at this scale requires an optical interferometer using an array of telescopes with baselines on the order of hundreds of meters. We report on the successful implementation of a stellar intensity interferometry system developed for the four VERITAS imaging atmospheric-Cherenkov telescopes. The system was used to measure the angular diameter of the two sub-mas stars $\beta$ Canis Majoris and $\epsilon$ Orionis with a precision better than 5%. The system utilizes an off-line approach where starlight intensity fluctuations recorded at each telescope are correlated post-observation. The technique can be readily scaled onto tens to hundreds of telescopes, providing a capability that has proven technically challenging to current generation optical amplitude interferometry observatories. This work demonstrates the feasibility of performing astrophysical measurements with imaging atmospheric-Cherenkov telescope arrays as intensity interferometers and the promise for integrating an intensity interferometry system within future observatories such as the Cherenkov Telescope Array.Comment: Accepted for publication in Nature Astronomy (2020

Measurement of the extragalactic background light spectral energy distribution with VERITAS

The extragalactic background light (EBL), a diffuse photon field in the optical and infrared range, is a record of radiative processes over the Universe's history. Spectral measurements of blazars at very high energies ($>$100 GeV) enable the reconstruction of the spectral energy distribution (SED) of the EBL, as the blazar spectra are modified by redshift- and energy-dependent interactions of the gamma-ray photons with the EBL. The spectra of 14 VERITAS-detected blazars are included in a new measurement of the EBL SED that is independent of EBL SED models. The resulting SED covers an EBL wavelength range of 0.56--56 $\mu$m, and is in good agreement with lower limits obtained by assuming that the EBL is entirely due to radiation from cataloged galaxies.Comment: Accepted for publication in The Astrophysical Journa