The Global Distribution of Secondary Particulate Matter in a 3-D Lagrangian Chemistry Transport Model     

R. G. Derwent  W. J. Collins  M. E. Jenkin  C. E. Johnson  D. S. Stevenson 《Journal of Atmospheric Chemistry》2003,44(1):57-95

A global 3-D Lagrangian chemistry-transport model STOCHEM is used to describe the tropospheric distributions of four components of the secondary atmospheric aerosol: nitrate, sulphate, ammonium and organic compounds. The model describes the detailed chemistry of the formation of the acid precursors from the oxidation of SO₂, DMS, NO_x, NH₃ and terpenes and their uptake into the aerosol. Model results are compared in some detail with the available surface observations. Comparisons are made between the global budgets and burdens found in other modelling studies. The global distributions of the total mass of secondary aerosols have been estimated for the pre-industrial, present day and 2030 emissions and large changes have been estimated in the mass fractions of the different secondary aerosol components.  相似文献   

Reactive Nitrogen Compounds at Spitsbergen in the Norwegian Arctic     

S. Solberg  T. Krognes  F. Stordal  OØ Hov  H. J. Beine  D. A. Jaffe  K. C. Clemitshaw  S. A. Penkett 《Journal of Atmospheric Chemistry》1997,28(1-3):209-225

Simultaneousindependent measurements of NO_y and NO_x(NO_x= NO + NO₂) by high-sensitivitychemiluminescence systems and of PAN (peroxyacetylnitrate) and PPN (peroxypropionyl nitrate) by GC-ECDwere made at Spitsbergen in the Norwegian Arcticduring the first half year of 1994. The average mixingratio of the sum of PAN and PPN (denoted PANs)increased from around 150 pptv in early winter to amaximum of around 500 pptv in late March, whereasepisodic peak values reached 800 pptv. This occurredsimultaneously with a maximum in ozone which increasedto 45–50 ppbv in March–April. The average NO_xmixing ratio was 27 pptv and did not show any cyclethrough the period. The NO_y mixing ratio showeda maximum in late March, while the difference betweenNO_y and PAN decreased during spring. This is anindication of the dominance of PAN in the NO_ybudget in the Arctic, but possible changes in theefficiency of the NO_y converter could alsocontribute to this. Although most PAN in theArctic is believed to be due to long range transport,the observations indicate local loss and formationrates of up to 1–2 pptv h^-1 in April–May.Measurements of carbonyl compounds suggest thatacetaldehyde was the dominant, local precursor ofPAN.Now at 1.  相似文献   

Ultra-high-temperature metamorphism and multistage decompressional evolution of sapphirine granulites from the Palni Hill Ranges, southern India   总被引：12，自引：0，他引：12  

M. RAITH  S. KARMAKAR  & M. BROWN 《Journal of Metamorphic Geology》1997,15(3):379-399

Sapphirine granulites from a new locality in the Palni Hill Ranges, southern India, occur in a small enclave of migmatitic, highly magnesian metapelites (mg=85–72) within massive enderbitic orthogneiss. They show a variety of multiphase reaction textures that partially overprint a coarse-grained high-pressure assemblage of Bt+Opx+Ky+Grt+Pl+Qtz. The sequence of reactions as deduced from the corona and symplectite assemblages, together with petrogenetic grid considerations, records a clockwise P–T evolution with four distinct stages. (1) Equilibration of the initial high-P assemblage in deep overthickened crust (12 kbar/800–900 °C) was followed by a stage of near-isobaric heating, presumably as a consequence of input of extra heat provided by the voluminous enderbitic intrusives. During heating, kyanite was converted to sillimanite, and biotite was involved in a series of vapour-phase-absent melting reactions, which resulted in the ultra-high-temperature assemblage Opx+Crd+Kfs+Spr±Sil, Grt, Qtz, Bt, coexisting with melt (equilibration at c. 950–1000° C/11–10 kbar). (2) Subsequently, as a result of decompression of the order of 4 kbar at ultra-high temperature, a sequence of symplectite assemblages (Opx+Sil+Spr/Spr+Crd→Opx+Spr+Crd→Opx+Crd→Opx+Crd+Spl/Crd+Spl) developed at the expense of garnet, orthopyroxene and sillimanite. This stage of near-isothermal decompression implies rapid ascent of the granulites into mid-crustal levels, possibly due to extensional collapse and erosion of the overthickened crust. (3) Development of late biotite through back-reaction of melt with residual garnet indicates a stage of near-isobaric cooling to c. 875 °C at 7–8 kbar, i.e. relaxation of the rapidly ascended crust to the stable geotherm. (4) A second period of near-isothermal exhumation up to c. 6–5 kbar/850 °C is indicated by the partial breakdown of late biotite through volatile phase-absent melting reactions. Available isotope data suggest that the early part of the evolutionary history (stages 1–3) is presumably coeval with the early Proterozoic metamorphism in the extended granulite terrane of the Nilgiri, Biligirirangan and Shevaroy Hills to the north, while the exhumation of the granulites from mid-crustal levels (stage 4) occurred only during the Pan-African thermotectonic event, which led to the accretion of the Kerala Khondalite Belt to the south.  相似文献   

Rapid Variscan exhumation and the role of magma in core complex formation: southern Brittany metamorphic belt, France   总被引：6，自引：0，他引：6  

MICHAEL BROWN  R. DAVID DALLMEYER 《Journal of Metamorphic Geology》1996,14(3):361-379

ABSTRACT The high-grade migmatitic core to the southern Brittany metamorphic belt has mineralogical and textural features that suggest high-temperature decompression. The chronology of this decompression and subsequent cooling history have been constrained with ⁴⁰Ar/³⁹ Ar ages determined for multigrain concentrates of hornblende and muscovite prepared from amphibolite and late-orogenic granite sheets within the migmatitic core, and from amphibolite of the structurally overlying unit. Three hornblende concentrates yield plateau isotope correlation ages of c. 303–298 Ma. Two muscovite concentrates record well-defined plateau ages of c. 306–305 Ma. These ages are geologically significant and date the last cooling through temperatures required for intracrystalline retention of radiogenic argon. The concordancy of the hornblende and muscovite ages suggest rapid post-metamorphic cooling. Extant geochronology and the new ⁴⁰Ar/³⁹Ar data suggest a minimum time-integrated average cooling rate between c. 725 °C and c. 125 °C of c. 14 ± 4°C Ma^-1, although below 600 °C the data permit an infinitely fast rate of cooling. Mineral assemblages and reaction textures in diatexite migmatites suggest c. 4 kbar decompression at 800–750 °C. This must have pre-dated the rapid cooling. Emplacement of two-mica granites into the metamorphic belt occurred between 345 and 300 Ma. The youngest plutons were emplaced synkinematically along shallow-dipping normal faults interpreted to be reactivated Eo-Variscan thrusts. A penetrative, west-plunging stretching lineation developed in these granites suggests that extension was orogen-parallel. Extension was probably related to regional uplift and gravitational collapse of thermally weakened crust during constrictional (escape) tectonics in this narrow part of the Variscan orogen. This followed slab breakoff during the terminal stages of convergence between Gondwana and Laurasia; detachment may have been consequent upon a change in kinematics leading to dextral displacement within the orogen. Dextral ductile strike-slip displacement was concentrated in granites emplaced synkinematically along the South Armorican Shear Zone. Rapid cooling is interpreted to have resulted from tectonic unroofing with emplacement of granite along decollement surfaces. The high-grade migmatitic core of the southern Brittany metamorphic belt represents a type of metamorphic core complex formed during orogen-parallel extensional unroofing and regional-scale ductile flow.  相似文献   

Nature of the crust in Maine,USA: evidence from the Sebago batholith   总被引：7，自引：0，他引：7  

P. B. Tomascak  Eirik J. Krogstad  Richard J. Walker 《Contributions to Mineralogy and Petrology》1996,125(1):45-59

 Neodymium and lead isotope and elemental data are presented for the Sebago batholith (293±2 Ma), the largest exposed granite in New England. The batholith is lithologically homogeneous, yet internally heterogeneous with respect to rare earth elements (REE) and Nd isotopic composition. Two-mica granites in the southern/central portion of the batholith (group 1) are characterized by REE patterns with uniform shapes [Ce_N/Yb_N (chondrite normalized) = 9.4–19 and Eu/Eu* (Eu anomaly) = 0.27–0.42] and ɛ _Nd(t) = −3.1 to −2.1. Peripheral two-mica granites (group 2), spatially associated with stromatic and schlieric migmatites, have a wider range of total REE contents and patterns with variable shapes (Ce_N/Yb_N = 6.1–67, Eu/Eu* = 0.20–0.46) and ɛ _Nd(t) = −5.6 to −2.8. The heterogeneous REE character of the group 2 granites records the effects of magmatic differentiation that involved monazite. Coarse-grained leucogranites and aplites have kinked REE patterns and low total REE, but have Nd isotope systematics similar to group 2 granites with ɛ _Nd(t) = −5.5 to −4.7. Rare biotite granites have steep REE patterns (Ce_N/Yb_N = 51–61, Eu/Eu* = 0.32–0.84) and ɛ _Nd(t) = −4.6 to −3.8. The two-mica granites have a restricted range in initial Pb isotopic composition (²⁰⁶Pb/²⁰⁴Pb = 18.41–18.75; ²⁰⁷Pb/²⁰⁴Pb = 15.60–15.68; ²⁰⁸Pb/²⁰⁴Pb = 38.21–38.55), requiring and old, high U/Pb (but not Th/U) source component. The Nd isotope data are consistent with magma derivation from two sources: Avalon-like crust (ɛ _Nd>−3), and Central Maine Belt metasedimentary rocks (ɛ _Nd<−4), without material input from the mantle. The variations in isotope systematics and REE patterns are inconsistent with models of disequilibrium melting which involved monazite. Received: 8 December 1995 / Accepted: 29 April 1996  相似文献   

Nd and Sr isotopic constraints on the origin of igneous rocks resulting from the opening of the Japan Sea, southwestern Japan     

Y. Terakado  T. Fujitani  R. J. Walker 《Contributions to Mineralogy and Petrology》1997,129(1):75-86

Strontium and Nd isotopic compositions and trace element abundances were determined for Cretaceous to late Cenozoic igneous rocks from the Japan Sea side of Southwest Japan in order to investigate the effect of the opening of the Japan Sea on igneous activity. The ⁸⁷Sr/⁸⁶Sr ratios for both high and low silica rocks decrease with decreasing age since the middle Miocene, when the opening occurred. Similarly, ¹⁴³Nd/¹⁴⁴Nd values for these rocks increase with decreasing age, and are negatively correlated with ⁸⁷Sr/⁸⁶Sr ratios. A two-component mixing process can best account for these isotopic and chemical characteristics. One end-member is likely the subcontinental lithospheric mantle (SCLM) and its derivative mafic to intermediate materials which had ɛ_Nd values of around +3. The other endmember consists of mafic to intermediate rocks with low ɛ_Nd values (e.g., −8), probably located in the lower crust. The mantle upwelling associated with the opening of the Japan Sea did not supply typical MORB or MORB-source materials to the crust, but did provide the heat that caused the melting of lithospheric mantle and lower crust. Received: 29 August 1996 / Accepted: 6 May 1997  相似文献   

The making of Stars 'R' Us!     

Serena Viti  Wendy Brown  Martin McCoustra  Helen Fraser  Nigel Mason  Robert Massey 《Astronomy& Geophysics》2004,45(6):6.22-6.24

The team behind a successful project to broaden the understanding of astrochemistry – Serena Viti, Wendy Brown, Martin McCoustra, Helen Fraser, Nigel Mason and Robert Massey – recount how they went about it and what benefits resulted.  相似文献   

Soft X-ray spectroscopic studies of the reaction of fractured pyrite surfaces with Cr(VI)-containing aqueous solutions     

Colin S. Doyle  Tom Kendelewicz  Gordon E. Brown Jr 《Geochimica et cosmochimica acta》2004,68(21):4287-4299

We have used synchrotron-based soft X-ray core-level photoemission and adsorption spectroscopies to study the reaction of aqueous sodium chromate solutions with freshly fractured pyrite surfaces. Pyrite surfaces were reacted with 50 μM sodium chromate solution at pH 7 for reaction times between 1 min and 37 hr. Additional experiments were performed at pH 2 and pH 4 with 50 μM sodium chromate solutions and at pH 7 with 5 mM solutions. At chromate concentrations of 50 μM, all chromium present on the pyrite surface was in the form of Cr(III), while at 5 mM, both Cr(III) and Cr(VI) were present at the pyrite surface. Minor quantities of oxidized sulfur species (sulfate, sulfite, and zero-valent sulfur) were identified as reaction products on the pyrite surface. The amount of oxidized sulfur species observed on the surface was greater when pyrite was reacted with 5 mM Cr(VI) solutions because the rate of chromium deposition exceeded the rate of dissolution of pyrite oxidation products, effectively trapping Cr(VI) and oxidized sulfur species in an overlayer of iron(III)-containing Cr(III)-hydroxide. This work shows that pyrite, an extremely cheap and readily available waste material, may be suitable for the removal of hexavalent chromium from acidic to circumneutral waste streams. The reduced chromium ultimately forms a coating on the pyrite surface, which passivates the pyrite surface towards further oxidation.  相似文献   

Experimental partitioning of Tc, Mo, Ru, and Re between solid and liquid during crystallization in Fe-Ni-S     

C Lazar  R.J Walker 《Geochimica et cosmochimica acta》2004,68(3):643-651

Technetium isotopes ⁹⁷Tc, ⁹⁸Tc and ⁹⁹Tc decay to ⁹⁷Mo, ⁹⁸Ru and ⁹⁹Ru, with half-lives of 2.6 My, 4.1 My, and 0.21 My respectively. If there were early solar system processes that resulted in significant fractionation of Tc from the daughter elements, decay of extant Tc could have led to the creation of Mo and Ru isotopic heterogeneities. To assess the potential of metallic core crystallization to fractionate these elements, we examine the partitioning behavior of Tc relative to Re, Mo and Ru in the Fe-Ni-S system between solid metal and liquid metal alloy. The experimental evidence shows that Tc behaves more like the modestly compatible siderophile element Ru than the more highly compatible siderophile element Re, and that Tc is substantially more compatible than Mo. We also demonstrate a pressure effect in the partitioning of Mo during the crystallization of Fe-Ni-S melts. For a sulfur concentration in the liquid fraction of the core of 10 wt% (16.3 at%), the Jones and Malvin (1990) parameter is −ln(1-2 × 1.09 × 0.163) ≅ 0.44, which yields: D(Re) ≅ 4.1; D(Ru) ≅ 2.3; D(Tc) ≅ 1.7; D(Mo)_Lo-P ≅ 1.0;.and D(Mo)_Hi-P ≅ 0.5. Our results suggest that detectable Tc-induced isotopic anomalies (≥0.1 ε unit) in Ru and Mo could only be produced by unrealistically extreme degrees of crystallization of metal during asteroidal core fractionation, regardless of the time scales and initial Tc abundances involved.  相似文献   

Denitrification capacity in a subterranean estuary below a Rhode Island fringing salt marsh     

Kelly Addy  Arthur Gold  Barbara Nowicki  James McKenna  Mark Stolt  Peter Groffman 《Estuaries and Coasts》2005,28(6):896-908

Coastal waters are severely threatened by nitrogen (N) loading from direct groundwater discharge. The subterranean estuary, the mixing zone of fresh groundwater and sea water in a coastal aquifer, has a high potential to remove substantial N. A network of piezometers was used to characterize the denitrification capacity and groundwater flow paths in the subterranean estuary below a Rhode Island fringing salt marsh.¹⁵N-enriched nitrate was injected into the subterranean estuary (in situ push-pull method) to evaluate the denitrification capacity of the saturated zone at multiple depths (125–300 cm) below different zones (upland-marsh transition zone, high marsh, and low marsh). From the upland to low marsh, the water table became shallower, groundwater dissolved oxygen decreased, and groundwater pH, soil organic carbon, and total root biomass increased. As groundwater approached the high and low marsh, the hydraulic gradient increased and deep groundwater upwelled. In the warm season (groundwater temperature >12 °C), elevated groundwater denitrification capacity within each zone was observed. The warm season low marsh groundwater denitrification capacity was significantly higher than all other zones and depths. In the cool season (groundwater temperature <10.5 °C), elevated groundwater denitrification capacity was only found in the low marsh. Additions of dissolved organic carbon did not alter groundwater denitrification capacity suggesting that an alternative electron donor, possibly transported by tidal inundation from the root zone, may be limiting. Combining flow paths with denitrification capacity and saturated porewater residence time, we estimated that as much as 29–60 mg N could be removed from 11 of water flowing through the subterranean estuary below the low marsh, arguing for the significance of subterranean estuaries in annual watershed scale N budgets.  相似文献