Correlating atom probe tomography with x-ray and electron spectroscopies to understand microstructure-activity relationships in electrocatalysts

The search for a new energy paradigm with net-zero carbon emissions requires new technologies for energy generation and storage that are at the crossroad between engineering, chemistry, physics, surface and materials sciences. To keep pushing the inherent boundaries of device performance and lifetime, we need to step away from a cook-and-look approach and aim to establish the scientific ground to guide the design of new materials. This requires strong efforts in establishing bridges between microscopy and spectroscopy techniques, across multiple scales. Here, we discuss how the complementarities of X-ray- and electron-based spectroscopies and atom probe tomography can be exploited in the study of surfaces and sub-surfaces to understand structure-property relationships in electrocatalysts

Radio emission models of Colliding-Wind Binary Systems

We present calculations of the spatial and spectral distribution of the radio emission from a wide WR+OB colliding-wind binary system based on high-resolution hydrodynamical simulations and solutions to the radiative transfer equation. We account for both thermal and synchrotron radio emission, free-free absorption in both the unshocked stellar wind envelopes and the shocked gas, synchrotron self-absorption, and the Razin effect. The applicability of these calculations to modelling radio images and spectra of colliding-wind systems is demonstrated with models of the radio emission from the wide WR+OB binary WR147. Its synchrotron spectrum follows a power-law between 5 and 15 GHz but turns down to below this at lower and higher frequencies. We find that while free-free opacity from the circum-binary stellar winds can potentially account for the low-frequency turnover, models that also include a combination of synchrotron self-absorption and Razin effect are favoured. We argue that the high-frequency turn down is a consequence of inverse-Compton cooling. We present our resulting spectra and intensity distributions, along with simulated MERLIN observations of these intensity distributions. From these we argue that the inclination of the WR147 system to the plane of the sky is low. We summarise by considering extensions of the current model that are important for models of the emission from closer colliding wind binaries, in particular the dramatically varying radio emission of WR140.Comment: 18 pages, 18 figures; Accepted by Astronomy and Astrophysics, July 8, 200

An Eccentric Binary Millisecond Pulsar in the Galactic Plane

Binary pulsar systems are superb probes of stellar and binary evolution and the physics of extreme environments. In a survey with the Arecibo telescope, we have found PSR J1903+0327, a radio pulsar with a rotational period of 2.15 ms in a highly eccentric (e = 0.44) 95-day orbit around a solar mass companion. Infrared observations identify a possible main-sequence companion star. Conventional binary stellar evolution models predict neither large orbital eccentricities nor main-sequence companions around millisecond pulsars. Alternative formation scenarios involve recycling a neutron star in a globular cluster then ejecting it into the Galactic disk or membership in a hierarchical triple system. A relativistic analysis of timing observations of the pulsar finds its mass to be 1.74+/-0.04 Msun, an unusually high value.Comment: 28 pages, 4 figures inc Supplementary On-Line Material. Accepted for publication in Science, published on Science Express: 10.1126/science.115758

The epidemiology of Plasmodium falciparum and Plasmodium vivax in East Sepik Province, Papua New Guinea, pre- and post-implementation of national malaria control efforts

Background In the past decade, national malaria control efforts in Papua New Guinea (PNG) have received renewed support, facilitating nationwide distribution of free long-lasting insecticidal nets (LLINs), as well as improvements in access to parasite-confirmed diagnosis and effective artemisinin-combination therapy in 2011–2012. Methods To study the effects of these intensified control efforts on the epidemiology and transmission of Plasmodium falciparum and Plasmodium vivax infections and investigate risk factors at the individual and household level, two cross-sectional surveys were conducted in the East Sepik Province of PNG; one in 2005, before the scale-up of national campaigns and one in late 2012-early 2013, after 2 rounds of LLIN distribution (2008 and 2011–2012). Differences between studies were investigated using Chi square (χ2), Fischer’s exact tests and Student’s t-test. Multivariable logistic regression models were built to investigate factors associated with infection at the individual and household level. Results The prevalence of P. falciparum and P. vivax in surveyed communities decreased from 55% (2005) to 9% (2013) and 36% to 6%, respectively. The mean multiplicity of infection (MOI) decreased from 1.8 to 1.6 for P. falciparum (p = 0.08) and from 2.2 to 1.4 for P. vivax (p  50% of household members with Plasmodium infection). Conclusion After the scale-up of malaria control interventions in PNG between 2008 and 2012, there was a substantial reduction in P. falciparum and P. vivax infection rates in the studies villages in East Sepik Province. Understanding the extent of local heterogeneity in malaria transmission and the driving factors is critical to identify and implement targeted control strategies to ensure the ongoing success of malaria control in PNG and inform the development of tools required to achieve elimination. In household-based interventions, diagnostics with a sensitivity similar to (expert) microscopy could be used to identify and target high rate households

PSR J1856+0245: Arecibo Discovery of a Young, Energetic Pulsar Coincident with the TeV Gamma-ray Source HESS J1857+026

We present the discovery of the Vela-like radio pulsar J1856+0245 in the Arecibo PALFA survey. PSR J1856+0245 has a spin period of 81ms, a characteristic age of 21kyr, and a spin-down luminosity Edot = 4.6 x 10^36 ergs/s. It is positionally coincident with the TeV gamma-ray source HESS J1857+026, which has no other known counterparts. Young, energetic pulsars create wind nebulae, and more than a dozen pulsar wind nebulae have been associated with very-high-energy (100GeV-100TeV) gamma-ray sources discovered with the HESS telescope. The gamma-ray emission seen from HESS J1857+026 is potentially produced by a pulsar wind nebula powered by PSR J1856+0245; faint X-ray emission detected by ASCA at the pulsar's position supports this hypothesis. The inferred gamma-ray efficiency is epsilon_gamma = L_gamma/Edot = 3.1% (1-10TeV, for a distance of 9kpc), comparable to that observed in similar associations.Comment: 13 pages, 1 figure, accepted for publication in The Astrophysical Journal Letter

Probing catalytic surfaces by correlative scanning photoemission electron microscopy and atom probe tomography

The chemical composition and the electronic state of the surface of alloys or mixed oxides with enhanced electrocatalytic properties are usually heterogeneous at the nanoscale. The non-uniform distribution of the potential across their surface affects both activity and stability. Studying such heterogeneities at the relevant length scale is crucial for understanding the relationships between structure and catalytic behaviour. Here, we demonstrate an experimental approach combining scanning photoemission electron microscopy and atom probe tomography performed at identical locations to characterise the surface's structure and oxidation states, and the chemical composition of the surface and sub-surface regions. Showcased on an Ir-Ru thermally grown oxide, an efficient catalyst for the anodic oxygen evolution reaction, the complementary techniques yield consistent results in terms of the determined surface oxidation states and local oxide stoichiometry. Significant chemical heterogeneities in the sputter-deposited Ir-Ru alloy thin films govern the oxide's chemistry, observed after thermal oxidation both laterally and vertically. While the oxide grains have a composition of Ir0.94Ru0.06O2, the composition in the grain boundary region varies from Ir0.70Ru0.30O2 to Ir0.40Ru0.60O2 and eventually to Ir0.75Ru0.25O2 from the top surface into the depth. The influence of such compositional non-uniformities on the catalytic performance of the material is discussed, along with possible engineering levers for the synthesis of more stable and reactive mixed oxides. The proposed method provides a framework for investigating materials of interest in the field of electrocatalysis and beyond

The fitness of African malaria vectors in the presence and limitation of host behaviour

<p>Background Host responses are important sources of selection upon the host species range of ectoparasites and phytophagous insects. However little is known about the role of host responses in defining the host species range of malaria vectors. This study aimed to estimate the relative importance of host behaviour to the feeding success and fitness of African malaria vectors, and assess its ability to predict their known host species preferences in nature.</p> <p>Methods Paired evaluations of the feeding success and fitness of African vectors Anopheles arabiensis and Anopheles gambiae s.s in the presence and limitation of host behaviour were conducted in a semi-field system (SFS) at Ifakara Health Institute, Tanzania. In one set of trials, mosquitoes were released within the SFS and allowed to forage overnight on a host that was free to exhibit natural behaviour in response to insect biting. In the other, mosquitoes were allowed to feed directly on from the skin surface of immobile hosts. The feeding success and subsequent fitness of vectors under these conditions were investigated on 6 host types (humans, calves, chickens, cows, dogs and goats) to assess whether physical movements of preferred host species (cattle for An. arabiensis, humans for An. gambiae s.s.) were less effective at preventing mosquito bites than those of common alternatives.</p> <p>Results Anopheles arabiensis generally had greater feeding success when applied directly to host skin than when foraging on unrestricted hosts (in five of six host species). However, An. gambiae s.s obtained blood meals from free and restrained hosts with similar success from most host types (four out of six). Overall, the blood meal size, oviposition rate, fecundity and post-feeding survival of mosquito vectors were significantly higher after feeding on hosts free to exhibit behaviour, than those who were immobilized during feeding trials.</p> <p>Conclusions Allowing hosts to move freely during exposure to mosquitoes was associated with moderate reductions in mosquito feeding success, but no detrimental impact to the subsequent fitness of mosquitoes that were able to feed upon them. This suggests that physical defensive behaviours exhibited by common host species including humans do not impose substantial fitness costs on African malaria vectors.</p&gt

Study of measured pulsar masses and their possible conclusions

We study the statistics of 61 measured masses of neutron stars (NSs) in binary pulsar systems, including 18 double NS (DNS) systems, 26 radio pulsars (10 in our Galaxy) with white dwarf (WD) companions, 3 NSs with main-sequence companions, 13 NSs in X-ray binaries, and one undetermined system. We derive a mean value of M = 1.46 +/- 0.30 solar masses. When the 46 NSs with measured spin periods are divided into two groups at 20 milliseconds, i.e., the millisecond pulsar (MSP) group and others, we find that their mass averages are, respectively, M=1.57 +/- 0.35 solar masses and M=1.37+/- 0.23 solar masses. In the framework of the pulsar recycling hypothesis, this suggests that an accretion of approximately 0.2 solar mass is sufficient to spin up a neutron star and place it in the millisecond pulsar group. An empirical relation between the accreting mass and MSP spin period is \Delta M=0.43 (solar mass)(P/1 ms)^{-2/3}. UNlike the standard recycling process, if a MSP is formed by the accretion induced collapse (AIC) of a white dwarf with a mass less than Chandrasekha limit, e.g. 1.35 solar mass, then the binary MSPs involved in AICs is not be higher than 20%, which imposes a constraint on the AIC origin of MSPs.Comment: 6 pages, 5 figures, in press, Astronomy and Astrophysics 2011, 527, 8