Showing papers by "Paul Scherrer Institute published in 2007"

Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes

Abstract: Organic aerosol (OA) data acquired by the Aerosol Mass Spectrometer (AMS) in 37 field campaigns were deconvolved into hydrocarbon-like OA (HOA) and several types of oxygenated OA (OOA) components. HOA has been linked to primary combustion emissions (mainly from fossil fuel) and other primary sources such as meat cooking. OOA is ubiquitous in various atmospheric environments, on average accounting for 64%, 83% and 95% of the total OA in urban, urban downwind, and rural/remote sites, respectively. A case study analysis of a rural site shows that the OOA concentration is much greater than the advected HOA, indicating that HOA oxidation is not an important source of OOA, and that OOA increases are mainly due to SOA. Most global models lack an explicit representation of SOA which may lead to significant biases in the magnitude, spatial and temporal distributions of OA, and in aerosol hygroscopic properties.

Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer

Abstract: The application of mass spectrometric techniques to the realtime measurement and characterization of aerosols represents a significant advance in the field of atmospheric science. This review focuses on the aerosol mass spectrometer (AMS), an instrument designed and developed at Aerodyne Research, Inc. (ARI) that is the most widely used thermal vaporization AMS. The AMS uses aerodynamic lens inlet technology together with thermal vaporization and electron-impact mass spectrometry to measure the real-time non-refractory (NR) chemical speciation and mass loading as a function of particle size of fine aerosol particles with aerodynamic diameters between similar to 50 and 1,000 nm. The original AMS utilizes a quadrupole mass spectrometer (Q) with electron impact (EI) ionization and produces ensemble average data of particle properties. Later versions employ time-of-flight (ToF) mass spectrometers and can produce full mass spectral data for single particles. This manuscript presents a detailed discussion of the strengths and limitations of the AMS measurement approach and reviews how the measurements are used to characterize particle properties. Results from selected laboratory experiments and field measurement campaigns are also presented to highlight the different applications of this instrument. Recent instrumental developments, such as the incorporation of softer ionization techniques (vacuum ultraviolet (VUV) photo-ionization, Li(+) ion, and electron attachment) and high-resolution ToF mass spectrometers, that yield more detailed information about the organic aerosol component are also described. (c) 2007 Wiley Periodicals, Inc.

Operation of a free-electron laser from the extreme ultraviolet to the water window

Abstract: We report results on the performance of a free-electron laser operating at a wavelength of 13.7 nm where unprecedented peak and average powers for a coherent extreme-ultraviolet radiation source have been measured. In the saturation regime, the peak energy approached 170 J for individual pulses, and the average energy per pulse reached 70 J. The pulse duration was in the region of 10 fs, and peak powers of 10 GW were achieved. At a pulse repetition frequency of 700 pulses per second, the average extreme-ultraviolet power reached 20 mW. The output beam also contained a significant contribution from odd harmonics of approximately 0.6% and 0.03% for the 3rd (4.6 nm) and the 5th (2.75 nm) harmonics, respectively. At 2.75 nm the 5th harmonic of the radiation reaches deep into the water window, a wavelength range that is crucially important for the investigation of biological samples.

CMS physics technical design report, volume II: Physics performance

Abstract: CMS is a general purpose experiment, designed to study the physics of pp collisions at 14 TeV at the Large Hadron Collider (LHC). It currently involves more than 2000 physicists from more than 150 institutes and 37 countries. The LHC will provide extraordinary opportunities for particle physics based on its unprecedented collision energy and luminosity when it begins operation in 2007. The principal aim of this report is to present the strategy of CMS to explore the rich physics programme offered by the LHC. This volume demonstrates the physics capability of the CMS experiment. The prime goals of CMS are to explore physics at the TeV scale and to study the mechanism of electroweak symmetry breaking--through the discovery of the Higgs particle or otherwise. To carry out this task, CMS must be prepared to search for new particles, such as the Higgs boson or supersymmetric partners of the Standard Model particles, from the start-up of the LHC since new physics at the TeV scale may manifest itself with modest data samples of the order of a few fb−1 or less. The analysis tools that have been developed are applied to study in great detail and with all the methodology of performing an analysis on CMS data specific benchmark processes upon which to gauge the performance of CMS. These processes cover several Higgs boson decay channels, the production and decay of new particles such as Z' and supersymmetric particles, Bs production and processes in heavy ion collisions. The simulation of these benchmark processes includes subtle effects such as possible detector miscalibration and misalignment. Besides these benchmark processes, the physics reach of CMS is studied for a large number of signatures arising in the Standard Model and also in theories beyond the Standard Model for integrated luminosities ranging from 1 fb−1 to 30 fb−1. The Standard Model processes include QCD, B-physics, diffraction, detailed studies of the top quark properties, and electroweak physics topics such as the W and Z0 boson properties. The production and decay of the Higgs particle is studied for many observable decays, and the precision with which the Higgs boson properties can be derived is determined. About ten different supersymmetry benchmark points are analysed using full simulation. The CMS discovery reach is evaluated in the SUSY parameter space covering a large variety of decay signatures. Furthermore, the discovery reach for a plethora of alternative models for new physics is explored, notably extra dimensions, new vector boson high mass states, little Higgs models, technicolour and others. Methods to discriminate between models have been investigated. This report is organized as follows. Chapter 1, the Introduction, describes the context of this document. Chapters 2-6 describe examples of full analyses, with photons, electrons, muons, jets, missing ET, B-mesons and τ's, and for quarkonia in heavy ion collisions. Chapters 7-15 describe the physics reach for Standard Model processes, Higgs discovery and searches for new physics beyond the Standard Model

Hard-X-Ray Lensless Imaging of Extended Objects

Abstract: We demonstrate a hard-x-ray microscope that does not use a lens and is not limited to a small field of view or an object of finite size. The method does not suffer any of the physical constraints, convergence problems, or defocus ambiguities that often arise in conventional phase-retrieval diffractive imaging techniques. Calculation times are about a thousand times shorter than in current iterative algorithms. We need no a priori knowledge about the object, which can be a transmission function with both modulus and phase components. The technique has revolutionary implications for x-ray imaging of all classes of specimen.

The Higgs Boson Masses and Mixings of the Complex MSSM in the Feynman-Diagrammatic Approach

Abstract: New results for the complete one-loop contributions to the masses and mixing effects in the Higgs sector are obtained for the MSSM with complex parameters using the Feynman-diagrammatic approach. The full dependence on all relevant complex phases is taken into account, and all the imaginary parts appearing in the calculation are treated in a consistent way. The renormalization is discussed in detail, and a hybrid on-shell/ scheme is adopted. We also derive the wave function normalization factors needed in processes with external Higgs bosons and discuss effective couplings incorporating leading higher-order effects. The complete one-loop corrections, supplemented by the available two-loop corrections in the Feynman-diagrammatic approach for the MSSM with real parameters and a resummation of the leading (s)bottom corrections for complex parameters, are implemented into the public Fortran code FeynHiggs 2.5. In our numerical analysis the full results for the Higgs-boson masses and couplings are compared with various approximations, and -violating effects in the mixing of the heavy Higgs bosons are analyzed in detail. We find sizable deviations in comparison with the approximations often made in the literature.

Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra

Abstract: Submicron ambient aerosol was characterized in summer 2005 at an urban background site in Zurich, Switzer- land, during a three-week measurement campaign Highly time-resolved samples of non-refractory aerosol components were analyzed with an Aerodyne aerosol mass spectrometer (AMS) Positive matrix factorization (PMF) was used for the first time for aerosol mass spectra to identify the main com- ponents of the total organic aerosol and their sources The PMF retrieved factors were compared to measured reference mass spectra and were correlated with tracer species of the aerosol and gas phase measurements from collocated instru- ments Six factors were found to explain virtually all vari- ance in the data and could be assigned either to sources or to aerosol components such as oxygenated organic aerosol (OOA) Our analysis suggests that at the measurement site only a small (<10%) fraction of organic PM1 originates from freshly emitted fossil fuel combustion Other primary sources identified to be of similar or even higher importance are charbroiling (10-15%) and wood burning ( 10%) The fraction of all identified primary sources is considered as pri- mary organic aerosol (POA) This interpretation is supported by calculated ratios of the modelled POA and measured pri- mary pollutants such as elemental carbon (EC), NOx, and CO, which are in good agreement to literature values A high fraction (60-69%) of the measured organic aerosol mass is OOA which is interpreted mostly as secondary organic aerosol (SOA) This oxygenated organic aerosol can be sepa- rated into a highly aged fraction, OOA I, (40-50%) with low volatility and a mass spectrum similar to fulvic acid, and a more volatile and probably less processed fraction, OOA II (on average 20%) This is the first publication of a multiple component analysis technique to AMS organic spectral data and also the first report of the OOA II component

An overview of snow photochemistry: evidence, mechanisms and impacts

Abstract: It has been shown that sunlit snow and ice plays an important role in processing atmospheric species. Photochemical production of a variety of chemicals has recently been reported to occur in snow/ice and the release of these photochemically generated species may significantly impact the chemistry of the overlying atmosphere. Nitrogen oxide and oxidant precursor fluxes have been measured in a number of snow covered environments, where in some cases the emissions significantly impact the overlying boundary layer. For example, photochemical ozone production (such as that occurring in polluted mid-latitudes) of 3–4 ppbv/day has been observed at South Pole, due to high OH and NO levels present in a relatively shallow boundary layer. Field and laboratory experiments have determined that the origin of the observed NOx flux is the photochemistry of nitrate within the snowpack, however some details of the mechanism have not yet been elucidated. A variety of low molecular weight organic compounds have been shown to be emitted from sunlit snowpacks, the source of which has been proposed to be either direct or indirect photo-oxidation of natural organic materials present in the snow. Although myriad studies have observed active processing of species within irradiated snowpacks, the fundamental chemistry occurring remains poorly understood. Here we consider the nature of snow at a fundamental, physical level; photochemical processes within snow and the caveats needed for comparison to atmospheric photochemistry; our current understanding of nitrogen, oxidant, halogen and organic photochemistry within snow; the current limitations faced by the field and implications for the future.

Role of Oxygen Vacancies in Cr‐Doped SrTiO3 for Resistance‐Change Memory

Abstract: A high density of oxygen vacancies has been found in an experiment to determine the path of electrical conduction in Cr-doped SrTiO3 memory cells. The Cr acts as a seed for the localization of oxygen vacancies, leading to a statistically homogeneous distribution of charge carriers within the path. This warrants a controllable doping profile and improved device scaling down to the nanometer scale. The combination of laterally resolved micro-X-ray absorption spectroscopy and thermal imaging concludes that the resistance switching in Cr-doped SrTiO3 originates from an oxygen-vacancy drift to/from the electrode that was used as anode during the conditioning process. The experiments shows that this oxygen vacancy concept is crucial for the entire class of transition-metal-oxide-based bipolar resistance-change memory.

MICADAS: A new compact radiocarbon AMS system

Abstract: A novel tabletop AMS system with overall dimensions of only 2.5 × 3 m 2 has been built and tested. The mini radiocarbon dating System (MICADAS) is based on a vacuum insulated acceleration unit that uses a commercially available 200 kV power supply to generate acceleration fields in a tandem configuration. At the high-energy end, ions in charge state 1 + are selected and interfering molecules of mass 14 amu are destroyed in multiple collisions. The new system is now fully operational. It is the prototype of a new generation of radiocarbon spectrometers which fulfill the requirements for radiocarbon dating applications as well as for the less demanding 14 C/ 12 C isotopic ratio measurements as needed, e.g. in biomedical applications. A detailed description of the system is given and results of performance tests are discussed.

Identification of the mass spectral signature of organic aerosols from wood burning emissions.

Abstract: Throughout the winter months, the village of Roveredo, Switzerland, frequently experiences strong temperature inversions that contribute to elevated levels of particulate matter. Wood is used as fuel for 75% of the domestic heating installations in Roveredo, which makes it a suitable location to study wood burning emissions in the atmosphere in winter. An Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) was used to characterize the composition of the submicrometer, non-refractory aerosol particles at this location during two field campaigns in March and December 2005. Wood burning was found to be a major source of aerosols at this location in winter. Organics dominated the composition of the aerosols from this source, contributing up to 85% of the total AMS measured mass during the afternoon and evening hours. Carbonaceous particle analysis showed that organic carbon composed up to 86% of the total carbon mass collected at evening times. Results from 14C isotope determination revealed that up to 94% ...

Multiscale modeling of crowdion and vacancy defects in body-centered-cubic transition metals

Abstract: We investigate the structure and mobility of single self-interstitial atom and vacancy defects in body-centered-cubic transition metals forming groups 5B (vanadium, niobium, and tantalum) and 6B (chromium, molybdenum, and tungsten) of the Periodic Table. Density-functional calculations show that in all these metals the axially symmetric self-interstitial atom configuration has the lowest formation energy. In chromium, the difference between the energies of the and the self-interstitial configurations is very small, making the two structures almost degenerate. Local densities of states for the atoms forming the core of crowdion configurations exhibit systematic widening of the "local" d band and an upward shift of the antibonding peak. Using the information provided by electronic structure calculations, we derive a family of Finnis-Sinclair-type interatomic potentials for vanadium, niobium, tantalum, molybdenum, and tungsten. Using these potentials, we investigate the thermally activated migration of self-interstitial atom defects in tungsten. We rationalize the results of simulations using analytical solutions of the multistring Frenkel-Kontorova model describing nonlinear elastic interactions between a defect and phonon excitations. We find that the discreteness of the crystal lattice plays a dominant part in the picture of mobility of defects. We are also able to explain the origin of the non-Arrhenius diffusion of crowdions and to show that at elevated temperatures the diffusion coefficient varies linearly as a function of absolute temperature.

The XMM-Newton extended survey of the Taurus molecular cloud (XEST)

Abstract: The Taurus Molecular Cloud (TMC) is the nearest large star-forming region, prototypical for the distributed mode of low-mass star formation. Pre-main sequence stars are luminous X-ray sources, probably mostly owing to magnetic energy release. Aims. The XMM-Newton Extended Survey of the Taurus Molecular Cloud (EST) presented in this paper surveys the most populated =5 square degrees of the TMC, using the XMM-Newton X-ray observatory to study the thermal structure, variability, and long-term evolution of hot plasma, to investigate the magnetic dynamo, and to search for new potential members of the association. Many targets are also studied in the optical, and high-resolution X-ray grating spectroscopy has been obtained for selected bright sources. Methods. The X-ray spectra have been coherently analyzed with two different thermal models (2-component thermal model, and a continuous emission measure distribution model). We present overall correlations with fundamental stellar parameters that were derived from the previous literature. A few detections from Chandra observations have been added. Results. The present overview paper introduces the project and provides the basic results from the X-ray analysis of all sources detected in the XEST survey. Comprehensive tables summarize the stellar properties of all targets surveyed. The survey goes deeper than previous X-ray surveys of Taurus by about an order of magnitude and for the first time systematically accesses very faint and strongly absorbed TMC objects. We find a detection rate of 85% and 98% for classical and weak-line T Tau stars (CTTS resp. WTTS), and identify about half of the surveyed protostars and brown dwarfs. Overall, 136 out of 169 surveyed stellar systems are detected. We describe an X-ray luminosity vs. mass correlation, discuss the distribution of X-ray-to-bolometric luminosity ratios, and show evidence for lower X-ray luminosities in CTTS compared to WTTS. Detailed analysis (e.g., variability, rotation-activity relations, influence of accretion on X-rays) will be discussed in a series of accompanying papers.

Structural Basis for the Conducting Interface between LaAlO 3 and SrTiO 3

Abstract: The complete atomic structure of a five-monolayer film of ${\mathrm{LaAlO}}_{3}$ on ${\mathrm{SrTiO}}_{3}$ has been determined for the first time by surface x-ray diffraction in conjunction with the coherent Bragg rod analysis phase-retrieval method and further structural refinement. Cationic mixing at the interface results in dilatory distortions and the formation of metallic ${\mathrm{La}}_{1\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{TiO}}_{3}$. By invoking electrostatic potential minimization, the ratio of ${\mathrm{Ti}}^{4+}/{\mathrm{Ti}}^{3+}$ across the interface was determined, from which the lattice dilation could be quantitatively explained using ionic radii considerations. The correctness of this model is supported by density functional theory calculations. Thus, the formation of a quasi-two-dimensional electron gas in this system is explained, based on structural considerations.

Ancient Biomolecules from Deep Ice Cores Reveal a Forested Southern Greenland

Abstract: It is difficult to obtain fossil data from the 10% of Earth's terrestrial surface that is covered by thick glaciers and ice sheets, and hence, knowledge of the paleoenvironments of these regions has remained limited. We show that DNA and amino acids from buried organisms can be recovered from the basal sections of deep ice cores, enabling reconstructions of past flora and fauna. We show that high-altitude southern Greenland, currently lying below more than 2 kilometers of ice, was inhabited by a diverse array of conifer trees and insects within the past million years. The results provide direct evidence in support of a forested southern Greenland and suggest that many deep ice cores may contain genetic records of paleoenvironments in their basal sections.

Hard X-Ray Phase Tomography with Low-Brilliance Sources

Abstract: We report on a method for tomographic phase contrast imaging of centimeter sized objects. As opposed to existing techniques, our approach can be used with low-brilliance, lab based x-ray sources and thus is of interest for a wide range of applications in medicine, biology, and nondestructive testing. The work is based on the recent development of a hard x-ray grating interferometer, which has been demonstrated to yield differential phase contrast projection images. Here we particularly focus on how this method can be used for tomographic reconstructions using filtered back projection algorithms to yield quantitative volumetric information of both the real and imaginary part of the samples's refractive index.

CMS physics technical design report: Addendum on high density QCD with heavy ions

Abstract: This report presents the capabilities of the CMS experiment to explore the rich heavy-ion physics programme offered by the CERN Large Hadron Collider (LHC). The collisions of lead nuclei at energies , will probe quark and gluon matter at unprecedented values of energy density. The prime goal of this research is to study the fundamental theory of the strong interaction ? Quantum Chromodynamics (QCD) ? in extreme conditions of temperature, density and parton momentum fraction (low-x).This report covers in detail the potential of CMS to carry out a series of representative Pb-Pb measurements. These include bulk observables, (charged hadron multiplicity, low pT inclusive hadron identified spectra and elliptic flow) which provide information on the collective properties of the system, as well as perturbative probes such as quarkonia, heavy-quarks, jets and high pT hadrons which yield tomographic information of the hottest and densest phases of the reaction.

4D MR imaging of respiratory organ motion and its variability

Abstract: This paper describes a method for 4D imaging, which is used to study respiratory organ motion, a key problem in various treatments. Whilst the commonly used imaging methods rely on simplified breathing patterns to acquire one breathing cycle, the proposed method was developed to study irregularities in organ motion during free breathing over tens of minutes. The method does not assume a constant breathing depth or even strict periodicity and does not depend on an external respiratory signal. Time-resolved 3D image sequences were reconstructed by retrospective stacking of dynamic 2D images using internal image-based sorting. The generic method is demonstrated for the liver and for the lung. Quantitative evaluations of the volume consistency show the advantages over one-dimensional measurements for image sorting. Dense deformation fields describing the respiratory motion were estimated from the reconstructed volumes using non-rigid 3D registration. All obtained motion fields showed variations in the range of minutes such as drifts and deformations, which changed both the exhalation position of the liver and the breathing pattern. The obtained motion data are used in proton therapy planning to evaluate dose delivery methodologies with respect to their motion sensitivity. Besides this application, the new possibilities of studying respiratory motion are valuable for other applications such as the evaluation of gating techniques with respect to residual motion.

Evidence for an excitonic insulator phase in 1T-TiSe2.

Abstract: We present a new high-resolution angle-resolved photoemission study of 1T-TiSe2 in both its room-temperature, normal phase and its low-temperature, charge-density wave phase. At low temperature the photoemission spectra are strongly modified, with large band renormalizations at high-symmetry points of the Brillouin zone and a very large transfer of spectral weight to backfolded bands. A calculation of the theoretical spectral function for an excitonic insulator phase reproduces the experimental features with very good agreement. This gives strong evidence in favor of the excitonic insulator scenario as a driving force for the charge-density wave transition in 1T-TiSe2.

Electron fractionalization in two-dimensional graphenelike structures.

Abstract: Electron fractionalization is intimately related to topology. In one-dimensional systems, fractionally charged states exist at domain walls between degenerate vacua. In two-dimensional systems, fractionalization exists in quantum Hall fluids, where time-reversal symmetry is broken by a large external magnetic field. Recently, there has been a tremendous effort in the search for examples of fractionalization in two-dimensional systems with time-reversal symmetry. In this Letter, we show that fractionally charged topological excitations exist on graphenelike structures, where quasiparticles are described by two flavors of Dirac fermions and time-reversal symmetry is respected. The topological zero modes are mathematically similar to fractional vortices in p-wave superconductors. They correspond to a twist in the phase in the mass of the Dirac fermions, akin to cosmic strings in particle physics.

Dijet cross sections and parton densities in diffractive DIS at HERA

Abstract: Differential dijet cross sections in diffractive deep-inelastic scattering are measured with the H1 detector at HERA using an integrated luminosity of 51.5 pb−1. The selected events are of the type ep → eXY , where the system X contains at least two jets and is well separated in rapidity from the low mass proton dissociation system Y . The dijet data are compared with QCD predictions at next-to-leading order based on diffractive parton distribution functions previously extracted from measurements of inclusive diffractive deepinelastic scattering. The prediction describes the dijet data well at low and intermediate zIP (the fraction of the momentum of the diffractive exchange carried by the parton entering the hard interaction) where the gluon density is well determined from the inclusive diffractive data, supporting QCD factorisation. A new set of diffractive parton distribution functions is obtained through a simultaneous fit to the diffractive inclusive and dijet cross sections. This allows for a precise determination of both the diffractive quark and gluon distributions in the range 0.05 < zIP < 0.9. In particular, the precision on the gluon density at high momentum fractions is improved compared to previous extractions.

Water-use strategies in two co-occurring Mediterranean evergreen oaks: surviving the summer drought.

Abstract: In the Mediterranean evergreen oak woodlands of southern Portugal, the main tree species are Quercus ilex ssp. rotundifolia Lam. (holm oak) and Quercus suber L. (cork oak). We studied a savannah-type woodland where these species coexist, with the aim of better understanding the mechanisms of tree adaptation to seasonal drought. In both species, seasonal variations in transpiration and predawn leaf water potential showed a maximum in spring followed by a decline through the rainless summer and a recovery with autumn rainfall. Although the observed decrease in predawn leaf water potential in summer indicates soil water depletion, trees maintained transpiration rates above 0.7 mm day(-1) during the summer drought. By that time, more than 70% of the transpired water was being taken from groundwater sources. The daily fluctuations in soil water content suggest that some root uptake of groundwater was mediated through the upper soil layers by hydraulic lift. During the dry season, Q. ilex maintained higher predawn leaf water potentials, canopy conductances and transpiration rates than Q. suber. The higher water status of Q. ilex was likely associated with their deeper root systems compared with Q. suber. Whole-tree hydraulic conductance and minimum midday leaf water potential were lower in Q. ilex, indicating that Q. ilex was more tolerant to drought than Q. suber. Overall, Q. ilex seemed to have more effective drought avoidance and drought tolerance mechanisms than Q. suber.

Strong and electroweak corrections to the production of a Higgs boson+2 jets via weak interactions at the Large Hadron Collider.

Abstract: Radiative corrections of strong and electroweak interactions are presented at next-to-leading order for the production of a Higgs boson plus two hard jets via weak interactions at the CERN Large Hadron Collider. The calculation includes all weak-boson fusion and quark-antiquark annihilation diagrams as well as the corresponding interferences. The electroweak corrections, which are discussed here for the first time, reduce the cross sections by 5% and thus are of the same order of magnitude as the QCD corrections.

Quantum magnetism in the paratacamite family: towards an ideal kagomé lattice.

Abstract: We report muon spin rotation measurements on the $S=1/2$ (${\mathrm{Cu}}^{2+}$) paratacamite ${\mathrm{Zn}}_{x}{\mathrm{Cu}}_{4\ensuremath{-}x}(\mathrm{OH}{)}_{6}{\mathrm{Cl}}_{2}$ family. Despite a Weiss temperature of $\ensuremath{\sim}\ensuremath{-}300\text{ }\text{ }\mathrm{K}$, the $x=1$ compound is found to have no transition to a magnetic frozen state down to 50 mK as theoretically expected for the kagom\'e Heisenberg antiferromagnet. We find that the limit between a dynamical and a partly frozen ground state occurs around $x=0.5$. For $x=1$, we discuss the relevance to a singlet picture.

Thermodynamic stability and structure of copper oxide surfaces: A first-principles investigation

Abstract: To obtain insight into the structure and surface stoichiometry of copper-based catalysts in commercially important chemical reactions such as the oxygen-assisted water-gas shift reaction, we perform density-functional theory calculations to investigate the relative stability of low-index copper oxide surfaces. By employing the technique of ``ab initio atomistic thermodynamics,'' we identify low-energy surface structures that are most stable under realistic catalytic conditions are found to exhibit a metallic character. Three surfaces are shown to have notably lower surface free energies compared to the others considered and could be catalytically relevant; in particular, under oxygen-rich conditions, they are the ${\mathrm{Cu}}_{2}\mathrm{O}(110):\mathrm{Cu}\mathrm{O}$ surface, which is terminated with both Cu and O surface atoms, and the ${\mathrm{Cu}}_{2}\mathrm{O}(111)\text{\ensuremath{-}}{\mathrm{Cu}}_{\mathrm{CUS}}$ surface, which contains a surface (coordinatively unsaturated) Cu vacancy, while for the oxygen-lean conditions, the ${\mathrm{Cu}}_{2}\mathrm{O}(111)$ surface with a surface interstitial Cu atom is found to be energetically most favorable, highlighting the importance of defects at the surface.

Observations of 1,1‐difluoroethane (HFC‐152a) at AGAGE and SOGE monitoring stations in 1994–2004 and derived global and regional emission estimates

Abstract: [1] Ground-based in situ measurements of 1,1-difluoroethane (HFC-152a, CH3CHF2) which is regulated under the Kyoto Protocol are reported under the auspices of the AGAGE (Advanced Global Atmospheric Gases Experiment) and SOGE (System of Observation of halogenated Greenhouse gases in Europe) programs. Observations of HFC-152a at five locations (four European and one Australian) over a 10 year period were recorded. The annual average growth rate of HFC-152a in the midlatitude Northern Hemisphere has risen from 0.11 ppt/yr to 0.6 ppt/yr from 1994 to 2004. The Southern Hemisphere annual average growth rate has risen from 0.09 ppt/yr to 0.4 ppt/yr from 1998 to 2004. The 2004 average mixing ratio for HFC-152a was 5.0 ppt and 1.8 ppt in the Northern and Southern hemispheres, respectively. The annual cycle observed for this species in both hemispheres is approximately consistent with measured annual cycles at the same locations in other gases which are destroyed by OH. Yearly global emissions of HFC-152a from 1994 to 2004 are derived using the global mean HFC-152a observations and a 12-box 2-D model. The global emission of HFC-152a has risen from 7 Kt/yr to 28 Kt/yr from 1995 to 2004. On the basis of observations of above-baseline elevations in the HFC-152a record and a consumption model, regional emission estimates for Europe and Australia are calculated, indicating accelerating emissions from Europe since 2000. The overall European emission in 2004 ranges from 1.5 to 4.0 Kt/year, 5–15% of global emissions for 1,1-difluoroethane, while the Australian contribution is negligible at 5–10 tonnes/year, <0.05% of global emissions.

Chemical characterization of element 112

Abstract: Element 112 was discovered at the Heavy Ion Research Laboratory in Darmstadt, Germany in 1996 A decade on, and some of its chemical properties have now been determined Irradiation of plutonium-242 with intense calcium-48 beams for three weeks produced two atoms of element 112 (not yet officially named, but commonly called ununbium), and that's enough to do some chemistry on if you are quick Chemically ununbium behaves as a typical element of the group 12 in the periodic table (which it shares with Zn, Cd and Hg) It is very volatile and forms a metallic bond with a gold surface An experiment has scrutinized two atoms of element 112, finding that it is very volatile and forms a metallic bond with a gold surface These characteristics establish element 112 as a typical element of group 12 The heaviest elements to have been chemically characterized are seaborgium1 (element 106), bohrium2 (element 107) and hassium3 (element 108) All three behave according to their respective positions in groups 6, 7 and 8 of the periodic table, which arranges elements according to their outermost electrons and hence their chemical properties However, the chemical characterization results are not trivial: relativistic effects on the electronic structure of the heaviest elements can strongly influence chemical properties4,5,6 The next heavy element targeted for chemical characterization is element 112; its closed-shell electronic structure with a filled outer s orbital suggests that it may be particularly susceptible to strong deviations from the chemical property trends expected within group 12 Indeed, first experiments concluded that element 112 does not behave like its lighter homologue mercury7,8,9 However, the production and identification methods10,11 used cast doubt on the validity of this result Here we report a more reliable chemical characterization of element 112, involving the production of two atoms of 283112 through the alpha decay of the short-lived 287114 (which itself forms in the nuclear fusion reaction12 of 48Ca with 242Pu) and the adsorption of the two atoms on a gold surface By directly comparing the adsorption characteristics of 283112 to that of mercury and the noble gas radon, we find that element 112 is very volatile and, unlike radon, reveals a metallic interaction with the gold surface These adsorption characteristics establish element 112 as a typical element of group 12, and its successful production unambiguously establishes the approach to the island of stability of superheavy elements through 48Ca-induced nuclear fusion reactions with actinides