A comparative study of experimental and meteoritic metal-sulfide assemblages

Sulfide formation via a gas-solid reaction between iron-nickel metal and H_2/H_2S gas mixtures was studied experimentally. This reaction produces distinctive chemical fractionations in both metal and sulfide that can help identify pristine nebular sulfide condensates in meteorites. The resulting sulfide morphology consists of a troilite scale divided into two distinct layers : an inner layer containing small, randomly oriented crystals and an outer layer consisting of large, columnar crystals. A thin band of metal surrounding the unreacted metal core and small metal blebs located in the inner sulfide layer are significantly enriched in nickel relative to the starting metal composition. The stoichiometry of the sulfide is nearly ideal {(Fe+Ni+Co)/S=1} at the metal-sulfide interface but the sulfur content increases with distance from the metal. A significant amount of nickel is present in the sulfide layer and increases in concentration across the sulfide layer. The nickel concentration gradient results from diffusion of nickel ions in the sulfide being faster than that of iron ions. Microprobe analyses on metal-sulfide assemblages in the LL3 unequilibrated ordinary chondrite Allan Hills-764 (ALH-764) do not show these chemical fractionations. Instead, textural and chemical evidence suggests that these meteoritic sulfides were altered during a post accretion heating event

Validation of water vapour transport in the tropical tropopause region in coupled Chemistry Climate Models

International audienceIn this study backward trajectories from the tropical lower stratosphere were calculated for the Northern Hemisphere (NH) winters 1995?1996, 1997?1998 (El Niño) and 1998?1999 (La Niña) and summers 1996, 1997 and 1999 using both ERA-40 reanalysis data of the European Centre for Medium-Range Weather Forecast (ECMWF) and coupled chemistry climate model (CCM) data. The calculated trajectories were analyzed to determine the distribution of points where individual air masses encounter the minimum temperature and thus minimum water vapour mixing ratio during their ascent through the tropical tropopause layer (TTL) into the stratosphere. The geographical distribution of these dehydration points and the local conditions there determine the overall water vapour entry into the stratosphere. Results of two CCMs are presented: the ECHAM4.L39(DLR)/CHEM (hereafter: E39/C) from the German Aerospace Center (DLR) and the Freie Universität Berlin Climate Middle Atmosphere Model with interactive chemistry (hereafter: FUB-CMAM-CHEM). In the FUB-CMAM-CHEM model the minimum temperatures are overestimated by about 7 K in Northern Hemisphere (NH) winter as well as in NH summer, resulting in too high water vapour entry values compared to ERA-40. However, the geographical distribution of dehydration points is fairly reproduced for NH winter 1995?1996 and 1998?1999 and in all boreal summers. The distribution of dehydration points suggests an influence of the Indian monsoon upon the water vapour transport. The E39/C model displays a temperature bias of about +3 K. Hence, the minimum water vapour mixing ratios are higher relative to ERA-40. The geographical distribution of dehydration points is satisfactory in NH winter 1995?1996 and 1997?1998 with respect to ERA-40. The distribution is not reproduced for the NH winter 1998?1999 (La Niña event) compared to ERA-40. There is excessive mass flux through warm regions e.g. Africa, leading to excessive water vapour flux in the NH winter and summer. The possible influence of the Indian monsoon on the transport is not seen in the boreal summer. Further, the residence times of air parcels in the TTL were derived from the trajectory calculations. The analysis of the residence times reveals that in both CCMs residence times in the TTL are underestimated compared to ERA-40 and the seasonal variation is hardly present

Is it feasible to estimate radiosonde biases from interlaced measurements?

Upper-air measurements of essential climate variables (ECVs), such as temperature, are crucial for climate monitoring and climate change detection. Because of the internal variability of the climate system, many decades of measurements are typically required to robustly detect any trend in the climate data record. It is imperative for the records to be temporally homogeneous over many decades to confidently estimate any trend. Historically, records of upper-air measurements were primarily made for short-term weather forecasts and as such are seldom suitable for studying long-term climate change as they lack the required continuity and homogeneity. Recognizing this, the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) has been established to provide reference-quality measurements of climate variables, such as temperature, pressure, and humidity, together with well-characterized and traceable estimates of the measurement uncertainty. To ensure that GRUAN data products are suitable to detect climate change, a scientifically robust instrument replacement strategy must always be adopted whenever there is a change in instrumentation. By fully characterizing any systematic differences between the old and new measurement system a temporally homogeneous data series can be created. One strategy is to operate both the old and new instruments in tandem for some overlap period to characterize any inter-instrument biases. However, this strategy can be prohibitively expensive at measurement sites operated by national weather services or research institutes. An alternative strategy that has been proposed is to alternate between the old and new instruments, so-called interlacing, and then statistically derive the systematic biases between the two instruments. Here we investigate the feasibility of such an approach specifically for radiosondes, i.e. flying the old and new instruments on alternating days. Synthetic data sets are used to explore the applicability of this statistical approach to radiosonde change management

The kinetics and mechanism of iron sulfide formation in the solar nebula

We summarize an experimental study of the kinetics and mechanism of FeS formation by the reaction of H_2S-H_2 gas mixtures with iron metal. Characterization of the reacted samples by optical microscopy, X-ray diffraction, electron microprobe analyses, and gravimetric analyses provided detailed information on the Fe/S ratio, microstructure and morphology, and formation kinetics of the iron sulfide layers. The Fe/S ratios of the iron sulfide layers varied from Fe_S to FeS with temperature and gas composition, in agreement with models of gas-solid equilibrium. The morphology, microstructure, and growth orientation of the sulfide layers also varied with temperature and gas composition. Typically, sulfide layer growth proceeded by the development of a compact, uniformly oriented scale which later cracked when it could no longer plastically deform. Further reaction led to the growth of a finer grained, randomly oriented, highly porous inner layer between the metal and original sulfide scale. Initially sulfide layers grew linearly with time with the kinetics controlled by chemical reactions at the gas-solid interface. However, upon reaching a critical thickness, diffusion through the sulfide scale became the rate limiting step and layer growth followed parabolic kinetics. The linear and parabolic rate constants for iron sulfide growth were determined and then used to constrain FeS formation in the solar nebula. FeS formation is rapid compared to estimated nebular lifetimes of 1-10 million years. Our results also imply that the variations in the sulfur content of chondritic material are due to removal of metal grains from contact with the gas (e. g., by accretion into larger bodies) at temperatures above 400K, where complete sulfur condensation occurs, rather than by kinetic inhibition of gas-solid equilibrium between H_2S gas and iron metal grains

Towards understanding the variability in biospheric CO2 fluxes:Using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO2

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at five selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world

Fog type classification using a modified Richardson number for Christchurch, New Zealand

Situated on a coastal plain between the Southern Alps and Banks Peninsula, Christchurch, New Zealand, experiences around 49 fog days every year. Given its complex topography, accurate fog forecasting is difficult at Christchurch International Airport (CHA). Climatological analysis of local fog events is an important first step to gain insight into the processes involved in the fog lifecycle. In this study, fog events were identified using 12 years of meteorological observations from an automatic weather station situated at CHA. A novel fog type classification method was developed using the modified Richardson number (MRi). The MRi fog type classification method assesses the local dynamic stability of a 1.25 m shallow layer of near-surface air. Here, the MRi is used as a quantitative index to classify advection fog, advection–radiation fog, and radiation fog. Vertical gradients of air temperature and wind speed were derived for prefog and fog periods, and a number of criteria were applied to the MRi for the fog type classification. The fog type classification results were examined in correspondence with the derived fog intensity, duration, diurnal and seasonal variability of frequency of occurrences, and synoptic and local wind flows. In agreement with other fog studies across the world, fog occurs most frequently during local winter and spring. Radiation fog is the predominant type of fog identified at CHA, and its formation and development usually coincide with the local drainage northwesterlies. This study is the first to use long-term observational data to investigate the fog climatology and typology at CHA in detail. The fog climatological characteristics presented in this study will serve as the basis of future fog studies in Christchurch. The presented MRi fog type classification method can potentially be used in fog characteristic studies worldwide

An updated version of a gap-free monthly mean zonal mean ozone database

An updated and improved version of a global, vertically resolved, monthly mean zonal mean ozone database has been calculated – hereafter referred to as the BSVertOzone (Bodeker Scientific Vertical Ozone) database. Like its predecessor, it combines measurements from several satellite-based instruments and ozone profile measurements from the global ozonesonde network. Monthly mean zonal mean ozone concentrations in mixing ratio and number density are provided in 5° latitude bins, spanning 70 altitude levels (1 to 70km), or 70 pressure levels that are approximately 1km apart (878.4 to 0.046hPa). Different data sets or “tiers” are provided: Tier 0 is based only on the available measurements and therefore does not completely cover the whole globe or the full vertical range uniformly; the Tier 0.5 monthly mean zonal means are calculated as a filled version of the Tier 0 database where missing monthly mean zonal mean values are estimated from correlations against a total column ozone (TCO) database. The Tier 0.5 data set includes the full range of measurement variability and is created as an intermediate step for the calculation of the Tier 1 data where a least squares regression model is used to attribute variability to various known forcing factors for ozone. Regression model fit coefficients are expanded in Fourier series and Legendre polynomials (to account for seasonality and latitudinal structure, respectively). Four different combinations of contributions from selected regression model basis functions result in four different Tier 1 data sets that can be used for comparisons with chemistry–climate model (CCM) simulations that do not exhibit the same unforced variability as reality (unless they are nudged towards reanalyses). Compared to previous versions of the database, this update includes additional satellite data sources and ozonesonde measurements to extend the database period to 2016. Additional improvements over the previous version of the database include the following: (i) adjustments of measurements to account for biases and drifts between different data sources (using a chemistry-transport model, CTM, simulation as a transfer standard), (ii) a more objective way to determine the optimum number of Fourier and Legendre expansions for the basis function fit coefficients, and (iii) the derivation of methodological and measurement uncertainties on each database value are traced through all data modification steps. Comparisons with the ozone database from SWOOSH (Stratospheric Water and OzOne Satellite Homogenized data set) show good agreement in many regions of the globe. Minor differences are caused by different bias adjustment procedures for the two databases. However, compared to SWOOSH, BSVertOzone additionally covers the troposphere. Version 1.0 of BSVertOzone is publicly available at https://doi.org/http://doi.org/10.5281/zenodo.1217184

Longitudinal double spin asymmetries in single hadron quasi-real photoproduction at high pTp_T

We measured the longitudinal double spin asymmetries $A_{LL}$ for single hadron muo-production off protons and deuterons at photon virtuality $Q^2$ < 1(GeV/$\it c$)$^2$ for transverse hadron momenta $p_T$ in the range 0.7 GeV/$\it c$ to 4 GeV/$\it c$ . They were determined using COMPASS data taken with a polarised muon beam of 160 GeV/$\it c$ or 200 GeV/$\it c$ impinging on polarised $\mathrm{{}^6LiD}$ or $\mathrm{NH_3}$ targets. The experimental asymmetries are compared to next-to-leading order pQCD calculations, and are sensitive to the gluon polarisation $\Delta G$ inside the nucleon in the range of the nucleon momentum fraction carried by gluons $0.05 < x_g < 0.2$

Interplay among transversity induced asymmetries in hadron leptoproduction

In the fragmentation of a transversely polarized quark several left-right asymmetries are possible for the hadrons in the jet. When only one unpolarized hadron is selected, it exhibits an azimuthal modulation known as Collins effect. When a pair of oppositely charged hadrons is observed, three asymmetries can be considered, a di-hadron asymmetry and two single hadron asymmetries. In lepton deep inelastic scattering on transversely polarized nucleons all these asymmetries are coupled with the transversity distribution. From the high statistics COMPASS data on oppositely charged hadron-pair production we have investigated for the first time the dependence of these three asymmetries on the difference of the azimuthal angles of the two hadrons. The similarity of transversity induced single and di-hadron asymmetries is discussed. A new analysis of the data allows to establish quantitative relationships among them, providing for the first time strong experimental indication that the underlying fragmentation mechanisms are all driven by a common physical process.Comment: 6 figure

Interplay among transversity induced asymmetries in hadron leptoproduction

In the fragmentation of a transversely polarized quark several left-right asymmetries are possible for the hadrons in the jet. When only one unpolarized hadron is selected, it exhibits an azimuthal modulation known as Collins effect. When a pair of oppositely charged hadrons is observed, three asymmetries can be considered, a di-hadron asymmetry and two single hadron asymmetries. In lepton deep inelastic scattering on transversely polarized nucleons all these asymmetries are coupled with the transversity distribution. From the high statistics COMPASS data on oppositely charged hadron-pair production we have investigated for the first time the dependence of these three asymmetries on the difference of the azimuthal angles of the two hadrons. The similarity of transversity induced single and di-hadron asymmetries is discussed. A new analysis of the data allows to establish quantitative relationships among them, providing for the first time strong experimental indication that the underlying fragmentation mechanisms are all driven by a common physical process.Comment: 6 figure