Measuring Hg Isotopes in Bio-Geo-Environmental Reference Materials   总被引：1，自引：0，他引：1  

Nicolas Estrade  Jean Carignan  Jeroen E. Sonke  Olivier F.X. Donard 《Geostandards and Geoanalytical Research》2010,34(1):79-93

With the emergence of new analytical techniques and the expansion of scientific fields explored by using mercury isotopes, the community needs reference materials (RM) to validate and assure the accuracy of the results. The present work investigates (1) the characterisation of secondary RM in order to validate analytical systems, (2) the effects of two complex matrices on isotopic determination using stannous chloride cold vapour generation coupled to MC-ICP-MS (CV-MC-ICP-MS), (3) the effects of multiple digestion techniques for total Hg extraction and (4) the characterisation of nine geo-bio-environmental RM. Two secondary mono-elemental RMs analysed using two different analytical setups yielded isotopic compositions on δ²⁰²Hg of −3.54 ± 0.27‰ (CRPG-F65A, 2SD, n = 38) and +2.59 ± 0.19‰ (CRPG-RL24H, 2SD, n = 30) relative to the CRM NIST SRM 3133. These two RMs cover the whole range of Hg isotopic fractionation in natural samples and are made available to the scientific community. Complex fly ash and hydroxysulfate green rust matrices were synthesised, spiked with NIST SRM 3133, then digested and finally analysed versus the mono-elemental NIST SRM 3133 to show potential effect of these complex matrices during CV-MC-ICP-MS. Three digestions techniques, including traditional acid digestion, microwave digestion and high pressure-high temperature digestion, were applied to the lichen RM BCR-482 in order to compare advantages and drawbacks of these methods. Finally, the isotopic compositions of nine RMs including soils (NIST SRM 2711; GXR-2; GSS-4), sediment (GSD-10), jasperoid (GXR-1), ore deposit (GXR-3), fly ashes (BCR-176; BCR-176R) and lichen (BCR-482) are reported. These selected materials have δ²⁰²Hg values ranging from −1.75‰ to +0.11‰. Some RMs also presented mass-independent fractionation with Δ¹⁹⁹Hg and Δ²⁰¹Hg of up to −0.6‰.  相似文献   

Oxygen and iron isotope constraints on near-surface fractionation effects and the composition of lunar mare basalt source regions     

Yang Liu  Michael J. Spicuzza  James M.D. Day  Nicolas Dauphas 《Geochimica et cosmochimica acta》2010,74(21):6249-6262

Oxygen and iron isotope analyses of low-Ti and high-Ti mare basalts are presented to constrain their petrogenesis and to assess stable isotope variations within lunar mantle sources. An internally-consistent dataset of oxygen isotope compositions of mare basalts encompasses five types of low-Ti basalts from the Apollo 12 and 15 missions and eight types of high-Ti basalts from the Apollo 11 and 17 missions. High-precision whole-rock δ¹⁸O values (referenced to VSMOW) of low-Ti and high-Ti basalts correlate with major-element compositions (Mg#, TiO₂, Al₂O₃). The observed oxygen isotope variations within low-Ti and high-Ti basalts are consistent with crystal fractionation and match the results of mass-balance models assuming equilibrium crystallization. Whole-rock δ⁵⁶Fe values (referenced to IRMM-014) of high-Ti and low-Ti basalts range from 0.134‰ to 0.217‰ and 0.038‰ to 0.104‰, respectively. Iron isotope compositions of both low-Ti and high-Ti basalts do not correlate with indices of crystal fractionation, possibly owing to small mineral-melt iron fractionation factors anticipated under lunar reducing conditions.The δ¹⁸O and δ⁵⁶Fe values of low-Ti and the least differentiated high-Ti mare basalts are negatively correlated, which reflects their different mantle source characteristics (e.g., the presence or absence of ilmenite). The average δ⁵⁶Fe values of low-Ti basalts (0.073 ± 0.018‰, n = 8) and high-Ti basalts (0.191 ± 0.020‰, n = 7) may directly record that of their parent mantle sources. Oxygen isotope compositions of mantle sources of low-Ti and high-Ti basalts are calculated using existing models of lunar magma ocean crystallization and mixing, the estimated equilibrium mantle olivine δ¹⁸O value, and equilibrium oxygen-fractionation between olivine and other mineral phases. The differences between the calculated whole-rock δ¹⁸O values for source regions, 5.57‰ for low-Ti and 5.30‰ for high-Ti mare basalt mantle source regions, are solely a function of the assumed source mineralogy. The oxygen and iron isotope compositions of lunar upper mantle can be approximated using these mantle source values. The δ¹⁸O and δ⁵⁶Fe values of the lunar upper mantle are estimated to be 5.5 ± 0.2‰ (2σ) and 0.085 ± 0.040‰ (2σ), respectively. The oxygen isotope composition of lunar upper mantle is identical to the current estimate of Earth’s upper mantle (5.5 ± 0.2‰), and the iron isotope composition of the lunar upper mantle overlaps within uncertainty of estimates for the terrestrial upper mantle (0.044 ± 0.030‰).  相似文献   

Springtime changes in snow chemistry lead to new insights into mercury methylation in the Arctic     

Catherine Larose  Aurélien Dommergue  Martine De Angelis  Bernard Averty  Nicolas Soumis  Christophe Ferrari 《Geochimica et cosmochimica acta》2010,74(22):6263-6275

Seasonal snow is an active media and an important climate factor that governs nutrient transfer in Arctic ecosystems. Since the snow stores and transforms nutrients and contaminants, it is of crucial importance to gain a better understanding of the dynamics of contaminant cycling within the snowpack and its subsequent release to catchments via meltwater. Over the course of a two-month field study in the spring of 2008, we collected snow and meltwater samples from a seasonal snowpack in Ny-Ålesund, Norway (78°56′N, 11°52′E), which were analyzed for major inorganic ions and some organic acids, as well as total, dissolved, bioavailable mercury (THg, DHg, BioHg, respectively) and monomethylmercury (MMHg) species. We observe a seasonal gradient for ion concentrations, with surface samples becoming less concentrated as the season progressed. A significant negative correlation between BioHg and MMHg was observed in the snowpack. MMHg was positively and significantly correlated to methanesulfonate concentrations. Based on these results, we propose a new model for aerobic methylation of mercury involving species in the dimethylsulfoniopropionate cycle.  相似文献   

The Herschel PACS photometer calibration     

Markus Nielbock  Thomas Müller  Ulrich Klaas  Bruno Altieri  Zoltán Balog  Nicolas Billot  Hendrik Linz  Koryo Okumura  Miguel Sánchez-Portal  Marc Sauvage 《Experimental Astronomy》2013,36(3):631-660

We present a flux calibration scheme for the PACS chopped point-source photometry observing mode based on the photometry of five stellar standard sources. This mode was used for science observations only early in the mission. Later, it was only used for pointing and flux calibration measurements. Its calibration turns this type of observation into fully validated data products in the Herschel Science Archive. Systematic differences in calibration with regard to the principal photometer observation mode, the scan map, are derived and amount to 5 ? 6 %. An empirical method to calibrate out an apparent response drift during the first 300 Operational Days is presented. The relative photometric calibration accuracy (repeatability) is as good as 1 % in the blue and green band and up to 5 % in the red band. Like for the scan map mode, inconsistencies among the stellar calibration models become visible and amount to 2 % for the five standard stars used. The absolute calibration accuracy is therefore mainly limited by the model uncertainty, which is 5 % for all three bands.  相似文献   

Tall building performance‐based seismic design using SCEC broadband platform site‐specific ground motion simulations     

Kuanshi Zhong  Ting Lin  Gregory G. Deierlein  Robert W. Graves  Fabio Silva  Nicolas Luco 《地震工程与结构动力学》2021,50(1):81-98

The scarcity of strong ground motion records presents a challenge for making reliable performance assessments of tall buildings whose seismic design is controlled by large‐magnitude and close‐distance earthquakes. This challenge can be addressed using broadband ground‐motion simulation methods to generate records with site‐specific characteristics of large‐magnitude events. In this paper, simulated site‐specific earthquake seismograms, developed through a related project that was organized through the Southern California Earthquake Center (SCEC) Ground Motion Simulation Validation (GMSV) Technical Activity Group, are used for nonlinear response history analyses of two archetype tall buildings for sites in San Francisco, Los Angeles, and San Bernardino. The SCEC GMSV team created the seismograms using the Broadband Platform (BBP) simulations for five site‐specific earthquake scenarios. The two buildings are evaluated using nonlinear dynamic analyses under comparable record suites selected from the simulated BBP catalog and recorded motions from the NGA‐West database. The collapse risks and structural response demands (maximum story drift ratio, peak floor acceleration, and maximum story shear) under the BBP and NGA suites are compared. In general, this study finds that use of the BBP simulations resolves concerns about estimation biases in structural response analysis which are caused by ground motion scaling, unrealistic spectral shapes, and overconservative spectral variations. While there are remaining concerns that strong coherence in some kinematic fault rupture models may lead to an overestimation of velocity pulse effects in the BBP simulations, the simulations are shown to generally yield realistic pulse‐like features of near‐fault ground motion records.  相似文献   

Determination of physical properties of the Asteroid (41) Daphne from interferometric observations in the thermal infrared     

Alexis Matter  Marco Delbo  Nicolas Crouzet  Paolo Tanga 《Icarus》2011,215(1):47-56

We describe interferometric observations of the Asteroid (41) Daphne in the thermal infrared obtained with the Mid-Infrared Interferometric Instrument (MIDI) and the Auxiliary Telescopes (ATs) of the European Southern Observatory (ESO) Very Large Telescope Interferometer (VLTI). We derived the size and the surface thermal properties of (41) Daphne by means of a thermophysical model (TPM), which is used for the interpretation of interferometric data for the first time. From our TPM analysis, we derived a volume equivalent diameter for (41) Daphne of 189 km, using a non-convex 3-D shape model derived from optical lightcurves and adaptive optics images (B. Carry, private communication). On the other hand, when using the convex shape of Kaasalainen et al. (Kaasalainen, M., Mottola, S., Fulchignoni, M. [2002]. Icarus 159, 369-395) in our TPM analysis, the resulting volume equivalent diameter of (41) Daphne is between 194 and 209 km, depending on the surface roughness. The shape of the asteroid is used as an a priori information in our TPM analysis. No attempt is made to adjust the shape to the data. Only the size of the asteroid and its thermal parameters such as, albedo, thermal inertia and roughness are adjusted to the data. We estimated our model systematic uncertainty to be of 4% and of 7% on the determination of the asteroid volume equivalent diameter depending on whether the non-convex or the convex shape is used, respectively. In terms of thermal properties, we derived a value of the surface thermal inertia smaller than 50 J m⁻² s^−0.5 K⁻¹ and preferably in the range between 0 and ∼30 J m⁻² s^−0.5 K⁻¹. Our TPM analysis also shows that Daphne has a moderate macroscopic surface roughness.  相似文献   

Consistency and fidelity of Indonesian-throughflow total volume transport estimated by 14 ocean data assimilation products     

Tong Lee  Toshiyuki Awaji  Magdalena Balmaseda  Nicolas Ferry  Yosuke Fujii  Ichiro Fukumori  Benjamin Giese  Patrick Heimbach  Armin Köhl  Simona Masina  Elisabeth Remy  Anthony Rosati  Michael Schodlok  Detlef Stammer  Anthony Weaver 《Dynamics of Atmospheres and Oceans》2010

Monthly averaged total volume transport of the Indonesian throughflow (ITF) estimated by 14 global ocean data assimilation (ODA) products that are decade to multi-decade long are compared among themselves and with observations from the INSTANT Program (2004–2006). The main goals of the comparisons are to examine the consistency and evaluate the skill of different ODA products in simulating ITF transport. The ensemble averaged, time-mean value of ODA estimates is 13.6 Sv (1 Sv = 10⁶ m³/s) for the common 1993–2001 period and 13.9 Sv for the 2004–2006 INSTANT Program period. These values are close to the 15-Sv estimate derived from INSTANT observations. All but one ODA time-mean estimate fall within the range of uncertainty of the INSTANT estimate. In terms of temporal variability, the scatter among different ODA estimates averaged over time is 1.7 Sv, which is substantially smaller than the magnitude of the temporal variability simulated by the ODA systems. Therefore, the overall “signal-to-noise” ratio for the ensemble estimates is larger than one. The best consistency among the products occurs on seasonal-to-interannual time scales, with generally stronger (weaker) ITF during boreal summer (winter) and during La Nina (El Nino) events. The scatter among different products for seasonal-to-interannual time scales is approximately 1 Sv. Despite the good consistency, systematic difference is found between most ODA products and the INSTANT observations. All but the highest-resolution (18 km) ODA product show a dominant annual cycle while the INSTANT estimate and the 18-km product exhibit a strong semi-annual signal. The coarse resolution is an important factor that limits the level of agreement between ODA and INSTANT estimates. Decadal signals with periods of 10–15 years are seen. The most conspicuous and consistent decadal change is a relatively sharp increase in ITF transport during 1993–2000 associated with the strengthening tropical Pacific trade wind. Most products do not show a weakening ITF after the mid-1970s’ associated with the weakened Pacific trade wind. The scatter of ODA estimates is smaller after than before 1980, reflecting the impact of the enhanced observations after the 1980s. To assess the representativeness of using the average over a three-year period (e.g., the span of the INSTANT Program) to describe longer-term mean, we investigate the temporal variations of the three-year low-pass ODA estimates. The average variation is about 3.6 Sv, which is largely due to the increase of ITF transport from 1993 to 2000. However, the three-year average during the 2004–2006 INSTANT Program period is within 0.5 Sv of the long-term mean for the past few decades.  相似文献   

Air Flow Structure Over Short-gravity Breaking Water Waves     

Nicolas Reul  Hubert Branger  Jean-Paul Giovanangeli 《Boundary-Layer Meteorology》2008,126(3):477-505

Despite its importance for momentum and mass transfer across the air–sea interface, the dynamics of airflow over breaking waves is largely unknown. To fill this gap, velocity and vorticity distributions above short-gravity breaking waves have been measured in a wind-wave tank. A Digital Particle Image velocimetry technique (DPIV) was developed to accomplish these measurements above single breaking waves, propagating in mechanically-generated wave groups and forced by the wind. By varying the wind speed and initial characteristics of the groups, the airflow structure was captured over waves at different stages of the breaking process, and breaking with various intensities. The instantaneous airflow that separates from a sharp breaking crest is very similar to that occurring over a backward facing step. The separation bubble is however strongly unsteady: the steeper the wave crest and the larger the Reynolds number based on the crest-height, the higher the separated layer and the farther downwind the reattachment point. Instantaneous flow topology displays specific features of three-dimensional separation patterns. The tangential stress above the wave profile does not exhibit spikes at reattachment but grows progressively downwind from zero at reattachment to a value at the next crest approximately that found at the upwind breaking crest. Static pressure measurements revealed that large pressure falls are generated by vortices in the separated layer, as found in separated flows over solids. This study may provide useful data for theoretical and numerical modelling of the flow and associated phenomena.  相似文献   

Uncertainty, learning and ambiguity in economic models on climate policy: some classical results and new directions     

Andreas Lange  Nicolas Treich 《Climatic change》2008,89(1-2):7-21

We present how uncertainty and learning are classically studied in economic models. Specifically, we study a standard expected utility model with two sequential decisions, and consider two particular cases of this model to illustrate how uncertainty and learning may affect climate policy. While uncertainty has generally a negative effect on welfare, learning has always a positive, and thus opposite, effect. The effects of both uncertainty and learning on decisions are less clear. Neither uncertainty nor learning can be used as a general argument to increase or reduce emissions today without studying the specific intertemporal costs and benefits. Considering limits in applying the expected utility framework to climate change problems, we then consider a more recent framework with ambiguity-aversion which accounts for situations of imprecise or multiple probability distributions. We discuss both the impact of ambiguity-aversion on decisions and difficulties in applying such a non-expected utility framework to a dynamic context.  相似文献   

Benthic microbial mats: a possible major component of organic matter accumulation in the Lower Aptian oceanic anoxic event     

Georges Gorin  Nicolas Fiet  Muriel Pacton 《地学学报》2009,21(1):21-27

Oceanic anoxic events (OAEs) throughout the Cretaceous were periods of high organic carbon burial leading to drawdown of atmospheric carbon dioxide and lowering of bottom-water oxygen concentration, thereby enhancing the preservation of organic matter (OM). Two dynamic depositional models have been proposed for these events in the Tethyan domain: one is based on strong thermohaline stratification and low surface productivity, the other on high surface productivity with intensified deep-water circulation. Here, we propose another explanation for the concentration of OM, derived essentially from microscopical observations (scanning electron microscope and transmission electron microscope) in the organic-richest interval of an Early Aptian OAE in central Italy (OAE1a or Selli level, 116 Ma). This high-resolution microscopical study of OM highlights benthic microbial mats as the possible source of organic-rich samples where amorphous OM is the major organic constituent. These mats could be more common in OAE black shales than previously thought.  相似文献