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

Arecibo Pulsar Survey Using ALFA. I. Survey Strategy and First Discoveries

We report results from the initial stage of a long-term pulsar survey of the Galactic plane using the Arecibo L-band Feed Array (ALFA), a seven-beam receiver operating at 1.4 GHz with 0.3 GHz bandwidth. The search targets Galactic latitudes |b| < 5 deg in the longitude ranges 32 deg < l < 77 deg and 168 deg < l < 77 deg. Data discussed here were collected over a 100 MHz passband centered on 1.42 GHz using a spectrometer that recorded 256 channels every 64 microsec. In a preliminary, standard period-DM analysis, we have detected 29 previously known pulsars and discovered 11 new ones. One of these, with a period of 69 ms and a low characteristic age of 82 kyr, is a plausible candidate for association with the unidentified EGRET source 3EG J1928+1733. Another is a non-recycled pulsar in a relativistic binary with orbital period of 3.98 hr. We also search the data for isolated dispersed pulses, a technique that yielded discovery of an extremely sporadic radio emitter with a spin period of 1.2 s. Simulations we have carried out indicate that about 1000 new pulsars will be found in the ALFA survey. In addition to providing a large sample for use in population analyses and for probing the magnetoionic interstellar medium, the survey maximizes the chances of finding rapidly spinning millisecond pulsars and pulsars in compact binary systems. Our search algorithms will exploit the multiple data streams from ALFA to discriminate between radio frequency interference and celestial signals, including pulsars and possibly new classes of transient radio sources.Comment: 10 pp, 9 figures, accepted by the Astrophysical Journa

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 Binary Companion of Young, Relativistic Pulsar J1906+0746

PSR J1906+0746 is a young pulsar in the relativistic binary with the second-shortest known orbital period, of 3.98 hours. We here present a timing study based on five years of observations, conducted with the 5 largest radio telescopes in the world, aimed at determining the companion nature. Through the measurement of three post-Keplerian orbital parameters we find the pulsar mass to be 1.291(11) M_sol, and the companion mass 1.322(11) M_sol respectively. These masses fit well in the observed collection of double neutron stars, but are also compatible with other white dwarfs around young pulsars such as J1906+0746. Neither radio pulsations nor dispersion-inducing outflows that could have further established the companion nature were detected. We derive an HI-absorption distance, which indicates that an optical confirmation of a white dwarf companion is very challenging. The pulsar is fading fast due to geodetic precession, limiting future timing improvements. We conclude that young pulsar J1906+0746 is likely part of a double neutron star, or is otherwise orbited by an older white dwarf, in an exotic system formed through two stages of mass transfer.Comment: 13 pages, 10 figures. Accepted for Ap