Probing the structure and dynamics of molecular clusters using rotational wavepackets

The chemical and physical properties of molecular clusters can heavily depend on their size, which makes them very attractive for the design of new materials with tailored properties. Deriving the structure and dynamics of clusters is therefore of major interest in science. Weakly bound clusters can be studied using conventional spectroscopic techniques, but the number of lines observed is often too small for a comprehensive structural analysis. Impulsive alignment generates rotational wavepackets, which provides simultaneous information on structure and dynamics, as has been demonstrated successfully for isolated molecules. Here, we apply this technique for the firsttime to clusters comprising of a molecule and a single helium atom. By forcing the population of high rotational levels in intense laser fields we demonstrate the generation of rich rotational line spectra for this system, establishing the highly delocalised structure and the coherence of rotational wavepacket propagation. Our findings enable studies of clusters of different sizes and complexity as well as incipient superfluidity effects using wavepacket methods.Comment: 5 pages, 6 figure

Ramifications of Optical Pumping on the Interpretation of Time-Resolved Photoemission Experiments on Graphene

In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In particular, we find a time- and laser fluence-dependent spectral shift and broadening of the acquired spectra, and unambiguously show the presence of a double pump excitation. The dynamics of these effects is slower than the electron dynamics in the graphene sample, thereby permitting us to deconvolve the signals in the time domain. Our results demonstrate that complex pump-related processes should always be considered in the experimental setup and data analysis.Comment: 9 pages, 4 figure

Geochemical and Strontium Isotope Characterization of Produced Waters from Marcellus Shale Natural Gas Extraction

Extraction of natural gas by hydraulic fracturing of the Middle Devonian Marcellus Shale, a major gas-bearing unit in the Appalachian Basin, results in significant quantities of produced water containing high total dissolved solids (TDS). We carried out a strontium (Sr) isotope investigation to determine the utility of Sr isotopes in identifying and quantifying the interaction of Marcellus Formation produced waters with other waters in the Appalachian Basin in the event of an accidental release, and to provide information about the source of the dissolved solids. Strontium isotopic ratios of Marcellus produced waters collected over a geographic range of ∼375 km from southwestern to northeastern Pennsylvania define a relatively narrow set of values (εSr SW = +13.8 to +41.6, where εSr SW is the deviation of the 87Sr/86Sr ratio from that of seawater in parts per 104); this isotopic range falls above that of Middle Devonian seawater, and is distinct from most western Pennsylvania acid mine drainage and Upper Devonian Venango Group oil and gas brines. The uniformity of the isotope ratios suggests a basin-wide source of dissolved solids with a component that is more radiogenic than seawater. Mixing models indicate that Sr isotope ratios can be used to sensitively differentiate between Marcellus Formation produced water and other potential sources of TDS into ground or surface waters

Interpretating observations of ion cyclotron emission from Large Helical Device plasmas with beam-injected ion populations

Ion cyclotron emission (ICE) is detected from all large toroidal magnetically confined fusion (MCF) plasmas. It is a form of spontaneous suprathermal radiation, whose spectral peak frequencies correspond to sequential cyclotron harmonics of energetic ion species, evaluated at the emission location. We first present an account of the worldwide experimental ICE database, highlighting the phenomenological importance of the value of the ratio of energetic ion velocity v<sub>energetic</sub> to the local Alfvén speed V<sub>A</sub>. We then focus on ICE measurements from heliotron-stellarator hydrogen plasmas, heated by energetic proton neutral beam injection (NBI) in the Large Helical Device, for which v<sub>energetic</sub>/V<sub>A</sub> takes values both larger (super-Alfvénic) and smaller (sub-Alfvénic) than unity. The collective relaxation of the NBI proton population, together with the thermal plasma, is studied using a particle-in-cell (PIC) code. This evolves the Maxwell-Lorentz system of equations for hundreds of millions of kinetic gyro-orbit-resolved ions and fluid electrons, self-consistently with the electric and magnetic fields. For LHD-relevant parameter sets, the spatiotemporal Fourier transforms of the fields yield, in the nonlinear saturated regime, good computational proxies for the observed ICE spectra in both the super-and sub-Alfvénic regimes for NBI protons. At early times in the PIC treatment, the computed growth rates correspond to analytical linear growth rates of the magnetoacoustic cyclotron instability (MCI), which was previously identified to underly ICE from tokamak plasmas. The spatially localised PIC treatment does not include toroidal effects or geometry. Its success in simulating ICE spectra from tokamak and, here, heliotron-stellarator plasmas suggests that the plasma parameters and ion energetic distribution at the emission location suffice to determine the ICE phenomenology. The capability to span the super-Alfvénic and sub-Alfvénic energetic ion regimes is a generic challenge in interpreting MCF plasma physics, and it is encouraging that this first principles computational treatment of ICE has now achieved this

The relationship between reductions in knee loading and immediate pain response whilst wearing lateral wedged insoles in knee osteoarthritis.

Studies of lateral wedge insoles (LWIs) in medial knee osteoarthritis (OA) have shown reductions in the average external knee adduction moment (EKAM) but no lessening of knee pain. Some treated patients actually experience increases in the EKAM which could explain the overall absence of pain response. We examined whether, in patients with painful medial OA, reductions in the EKAM were associated with lessening of knee pain. Each patient underwent gait analysis whilst walking in a control shoe and two LWI’s. We evaluated the relationship between change in EKAM and change in knee pain using Spearman Rank Correlation coefficients and tested whether dichotomising patients into biomechanical responders (decreased EKAM) and non-responders (increased EKAM) would identify those with reductions in knee pain. In 70 patients studied, the EKAM was reduced in both LWIs vs. control shoe (-5.21% and -6.29% for typical and supported wedges, respectively). The change in EKAM using LWIs was not significantly associated with the direction of knee pain change. Further, 54% were biomechanical responders, but these persons did not have more knee pain reduction than non-responders. Whilst LWIs reduce EKAM, there is no clearcut relationship between change in medial load when wearing LWIs and corresponding change in knee pain

Shotgun metagenomic analysis of microbial communities from the Loxahatchee nature preserve in the Florida Everglades.

BackgroundCurrently, much is unknown about the taxonomic diversity and the mechanisms of methane metabolism in the Florida Everglades ecosystem. The Loxahatchee National Wildlife Refuge is a section of the Florida Everglades that is almost entirely unstudied in regard to taxonomic profiling. This short report analyzes the metagenome of soil samples from this Refuge to investigate the predominant taxa, as well as the abundance of genes involved in environmentally significant metabolic pathways related to methane production (nitrogen fixation and dissimilatory sulfite reduction).MethodsShotgun metagenomic sequencing using the Illumina platform was performed on 17 soil samples from four different sites within the Loxahatchee National Wildlife Refuge, and underwent quality control, assembly, and annotation. The soil from each sample was tested for water content and concentrations of organic carbon and nitrogen.ResultsThe three most common phyla of bacteria for every site were Actinobacteria, Acidobacteria, and Proteobacteria; however, there was variation in relative phylum composition. The most common phylum of Archaea was Euryarchaeota for all sites. Alpha and beta diversity analyses indicated significant congruity in taxonomic diversity in most samples from Sites 1, 3, and 4 and negligible congruity between Site 2 and the other sites. Shotgun metagenomic sequencing revealed the presence of biogeochemical biomarkers of particular interest (e.g., mrcA, nifH, and dsrB) within the samples. The normalized abundances of mcrA, nifH, and dsrB exhibited a positive correlation with nitrogen concentration and water content, and a negative correlation with organic carbon concentration.ConclusionThis Everglades soil metagenomic study allowed examination of wetlands biological processes and showed expected correlations between measured organic constituents and prokaryotic gene frequency. Additionally, the taxonomic profile generated gives a basis for the diversity of prokaryotic microbial life throughout the Everglades

Molecular Gas in the z=1.2 Ultraluminous Merger GOODS J123634.53+621241.3

We report the detection of CO(2-1) emission from the z=1.2 ultraluminous infrared galaxy (ULIRG) GOODS J123634.53+621241.3 (also known as the sub-millimeter galaxy GN26). These observations represent the first discovery of high-redshift CO emission using the new Combined Array for Research in Millimeter-Wave Astronomy (CARMA). Of all high-redshift (z>1) galaxies within the GOODS-North field, this source has the largest far-infrared (FIR) flux observed in the Spitzer 70um and 160um bands. The CO redshift confirms the optical identification of the source, and the bright CO(2-1) line suggests the presence of a large molecular gas reservoir of about 7x10^10 M(sun). The infrared-to-CO luminosity ratio of L(IR)/L'(CO) = 80+/-30 L(sun) (K Km/s pc^2)^-1 is slightly smaller than the average ratio found in local ULIRGs and high-redshift sub-millimeter galaxies. The short star-formation time scale of about 70 Myr is consistent with a starburst associated with the merger event and is much shorter than the time scales for spiral galaxies and estimates made for high-redshift galaxies selected on the basis of their B-z and z-K colors.Comment: Accepted for publication in ApJ Letter