Publications

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

No abstract is provided for this article.

Size-controlled model Pt nanoparticle catalysts, synthesized by colloidal chemistry, were used to study the hydrogenative reforming of three C6 hydrocarbons in mixtures with 5:1 excess of H2: methylcyclopentane, n-hexane and 2-methylpentane. We found a strong particle size dependence on the distribution of different reaction products for the hydrogenolysis of methylcyclopentane. The reactions of 50 Torr methylcyclopentane in 250 Torr H2 at 320 °C, using 1.5 and 3.0 nm Pt nanoparticles produced predominantly C6 isomers, especially 2-methylpentane, whereas 5.2 and 11.3 nm Pt nanoparticles were more selective for the formation of benzene. For the hydrogenolysis of n-hexane and 2-methylpentane, strong particle size effects on the turnover rates were observed. Hexane and 2-methylpentane reacted up to an order of magnitude slower over 3.0 nm Pt than over the other particle sizes. At 360 °C the isomerization reactions were more selective than the other reaction pathways over 3.0 nm Pt, which also yielded relatively less benzene.

Modern battery materials can contain many elements with substantial site disorder, and their configurational state has been shown to be critical for their performance. The intercalation voltage profile is a critical parameter to evaluate the performance of energy storage. The application of commonly used cluster expansion techniques to model the intercalation thermodynamics of such systems ab initio is challenged by the combinatorial increase in configurational degrees of freedom as the number of species grows. Such challenges necessitate the efficient generation of lattice models without overfitting and proper sampling of the configurational space under the requirement of charge balance in ionic systems. In this work, we introduce a combined approach that addresses these challenges by (1) constructing a robust cluster expansion Hamiltonian using the sparse regression technique, including -norm regularization and structural hierarchy; and (2) implementing semigrand-canonical Monte Carlo to sample charge-balanced ionic configurations using the table-exchange method and an ensemble average approach. These techniques are applied to a disordered rocksalt oxyfluoride (LMNOF) that is part of a family of promising earth-abundant cathode materials. The simulated voltage profile is found to be in good agreement with experimental data and particularly provides a clear demonstration of the and oxygen contributions to the redox potential as a function of content.

SUMMARY A (001) surface of molybdenum, covered by one monolayer of sulphur was prepared in UHV and characterized by LEED, Auger and XPS. This surface was found to be stable in air for periods of several days. STM images of the surface, obtained in air in the topographic and local barrier height modes, revealed the atomic arrangement of sulphur atoms in domains with 1×2 and 2×1 periodicities. Boundaries between domains, adsorbate and substrate defect structures and crystallites formed during the initial oxidation of the Mo substrate were observed.

Abstract Our understanding of galaxy properties and evolution is contingent on knowing the initial mass function (IMF), and yet to date the IMF is constrained only to local galaxies. Individual stars are now becoming routinely detected at cosmological distances, where luminous stars such as supergiants in background galaxies strongly lensed by galaxy clusters are temporarily further magnified by huge factors (up to 10 4 ) by intracluster stars, thus being detected as transients. The detection rate of these events depends on the abundance of luminous stars in the background galaxy and is thus sensitive to the IMF and the star formation history (SFH), especially for the blue supergiants detected as transients in the rest-frame ultraviolet/optical filters. As a proof of concept, we use simple SFH and IMF models constrained by spectral energy distributions (SEDs) to see how well we can predict the Hubble Space Telescope and James Webb Space Telescope transient detection rate in a lensed arc dubbed “Spock” ( z = 1.0054). We find that demanding a simultaneous fit of the SED and the transient detection rate places constraints on the IMF, independent of the assumed simple SFH model. We conclude that our likelihood analysis indicates that the data definitively prefers the “Spock” galaxy to have a Salpeter IMF ( α = 2.35) rather than a top-heavy IMF ( α = 1)—which is thought to be the case in the early universe—with no clear excess of supergiants above the standard IMF.

Abstract The relative importance of separation by distance and by environment to population genetic diversity can be conveniently tested in river networks, where these two drivers are often independently distributed over space. To evaluate the importance of dispersal and environmental conditions in shaping microbial population structures, we performed genome‐resolved metagenomic analyses of benthic Microcoleus ‐dominated cyanobacterial mats collected in the Eel and Russian River networks (California, USA). The 64 Microcoleus genomes were clustered into three species that shared >96.5% average nucleotide identity (ANI). Most mats were dominated by one strain, but minor alleles within mats were often shared, even over large spatial distances (>300 km). Within the most common Microcoleus species, the ANI between the dominant strains within mats decreased with increasing spatial separation. However, over shorter spatial distances (tens of kilometres), mats from different subwatersheds had lower ANI than mats from the same subwatershed, suggesting that at shorter spatial distances environmental differences between subwatersheds in factors like canopy cover, conductivity, and mean annual temperature decreases ANI. Since mats in smaller creeks had similar levels of nucleotide diversity ( π ) as mats in larger downstream subwatersheds, within‐mat genetic diversity does not appear to depend on the downstream accumulation of upstream‐derived strains. The four‐gamete test and sequence length bias suggest recombination occurs between almost all strains within each species, even between populations separated by large distances or living in different habitats. Overall, our results show that, despite some isolation by distance and environmental conditions, sufficient gene‐flow occurs among cyanobacterial strains to prevent either driver from producing distinctive population structures across the watershed.

We present extensive u'g'r'i'BVRIYJHKs photometry and optical spectroscopy of SN 2005hk. These data reveal that SN 2005hk was nearly identical in its observed properties to SN 2002cx, which has been called ``the most peculiar known type Ia supernova.'' Both supernovae exhibited high ionization SN 1991T-like pre-maximum spectra, yet low peak luminosities like SN 1991bg. The spectra reveal that SN 2005hk, like SN 2002cx, exhibited expansion velocities that were roughly half those of typical type Ia supernovae. The R and I light curves of both supernovae were also peculiar in not displaying the secondary maximum observed for normal type Ia supernovae. Our YJH photometry of SN 2005hk reveals the same peculiarity in the near-infrared. By combining our optical and near-infrared photometry of SN 2005hk with published ultraviolet light curves obtained with the Swift satellite, we are able to construct a bolometric light curve from ~10 days before to ~60 days after B maximum. The shape and unusually low peak luminosity of this light curve, plus the low expansion velocities and absence of a secondary maximum at red and near-infrared wavelengths, are all in reasonable agreement with model calculations of a 3D deflagration which produces ~0.25 M_sun of 56Ni.