Regime dependent changes in global precipitation   总被引：1，自引：1，他引：0  

Richard P. Allan 《Climate Dynamics》2012,39(3-4):827-840

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Molecular modelling of rare earth element complexation in subduction zone fluids     

Jelle van Sijl  Neil L. Allan  Wim van Westrenen 《Geochimica et cosmochimica acta》2009,73(13):3934-3947

Complexation of (trace) elements in fluids plays a critical role in determining element mobility in subduction zones, but to date, the atomic-scale processes controlling elemental solubilities are poorly understood. As a first step towards computer simulation of element complexation in subduction zone fluids, a thermodynamic cycle was developed to investigate the hydration environment and energetics of lanthanide complexes using density functional theory. The first solvation shell is explicitly defined and the remaining part of the aqueous fluid is modelled using a polarisable continuum model, which allows extrapolation to a broad pressure and temperature range.We illustrate our method by comparing solvation of lanthanide series elements in H₂O in the presence of fluoride or chloride for conditions relevant to subduction zones. The energetics of lanthanide- and lanthanide-fluoride/chloride hydration complexes were determined computationally. Calculated hydration free energies for trivalent lanthanides with explicit eight- and nine-fold coordinated first hydration shells show good agreement with literature data at room pressure and temperature. The hydration free energy is more negative for smaller complexes (heavy lanthanides) relative to larger complexes (light lanthanides), with the difference between La and Lu in water amounting to 361 kJ mol⁻¹. The hydration free energy of all lanthanide ions becomes less negative with increasing pressure (p) and temperature (T) up to 2.5 GPa and 1000 K (typical conditions in the upper part of subducting slabs). The free energy difference between light- and heavy-lanthanides remains essentially unchanged at elevated (p, T) conditions. There are minor geometrical differences in local hydration environment between light lanthanide-chloride (La-Nd) and heavy lanthanide-chloride (Pm-Lu) hydrated complexes, without a distinguishable energy difference. Complexation with fluoride is energetically more favourable than with chloride by 206 ± 4 kJ mol⁻¹ across the entire lanthanide series. The association of fluoride-water and chloride-water fragments with lanthanide-water complexes is energetically more favourable for aqueous lanthanide complexes surrounded by fewer first hydration shell water molecules.The methods developed in this study, in conjunction with simulation of the energetics of trace element incorporation into minerals, open the possibility to use molecular modelling to constrain elemental behaviour in subduction zones.  相似文献   

Electronic environments in carrollite, CuCo₂S₄, determined by soft X-ray photoelectron and absorption spectroscopy     

Alan N. Buckley  William M. Skinner  Allan Pring 《Geochimica et cosmochimica acta》2009,73(15):4452-4467

Fracture surfaces of a natural carrollite specimen have been characterised by synchrotron and conventional X-ray photoelectron spectroscopy and near-edge X-ray absorption spectroscopy. For the synchrotron X-ray measurements, the mineral surfaces were prepared under clean ultra high vacuum and were unoxidised. The characterisation was undertaken primarily to establish unequivocally the oxidation state of the Cu in the mineral, but also to obtain information on the electronic environments of the Co and S, and on the surface species. Experimental and simulated Cu L_2,3-edge absorption spectra confirmed an oxidation state of Cu^I, while Co 2p photoelectron and Co L_2,3 absorption spectra were largely consistent with the Co^III established previously by nuclear magnetic resonance spectroscopy. S 2p photoelectron spectra provided no evidence for S to be present in the bulk in more than one state, and were consistent with an oxidation state slightly less negative than S^-II. Therefore it was concluded that carrollite can be best represented by Cu^ICo^III₂(S₄)^-VII. The Cu^I oxidation state is in agreement with that expected for Cu tetrahedrally coordinated by S, but is in disagreement with the Cu^II deduced previously from some magnetic, magnetic resonance and Cu L-edge X-ray absorption spectroscopic measurements. A significant concentration of S species with core electron binding energies both lower and higher than the bulk value were formed at fracture surfaces, and these entities were assigned to monomeric and oligomeric surface S species. The density of Cu d states calculated for carrollite differed from that previously reported but was consistent with the observed Cu L₃ X-ray absorption spectrum. The initial oxidation of carrollite in air under ambient conditions was confirmed to be congruent, unlike the incongruent reaction undergone by a number of non-thiospinel sulfide minerals.  相似文献   

Towards molecular-level understanding of geochemical processes in mineral exploration     

Joël Brugger  Allan Pring  Frank Reith  Barbara Etschmann  Weihua Liu 《Journal of Geochemical Exploration》2009

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Properties of hot stars in the Wolf--Rayet galaxy NGC 5253 from ISO-SWS spectroscopy     

Paul A. Crowther  S. C. Beck  Allan J. Willis  Peter S. Conti  Patrick W. Morris  Ralph S. Sutherland 《Monthly notices of the Royal Astronomical Society》1999,304(3):654-668

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Cosmic-ray positrons: are there primary sources?     

Stphane Coutu  Steven W. Barwick  James J. Beatty  Amit Bhattacharyya  Chuck R. Bower  Christopher J. Chaput  Georgia A. de Nolfo  Michael A. DuVernois  Allan Labrador  Shawn P. McKee  Dietrich Müller  James A. Musser  Scott L. Nutter  Eric Schneider  Simon P. Swordy  Gregory Tarl  Andrew D. Tomasch  Eric Torbet 《Astroparticle Physics》1999,11(4):208-435

Galactic cosmic rays consist of primary and secondary particles. Primary cosmic rays are thought to be energized by first order Fermi acceleration processes at supernova shock fronts within our Galaxy. The cosmic rays that eventually reach the Earth from this source are mainly protons and atomic nuclei, but also include electrons. Secondary cosmic rays are created in collisions of primary particles with the diffuse interstellar gas. They are relatively rare but carry important information on the Galactic propagation of the primary particles. The secondary component includes a small fraction of antimatter particles, positrons and antiprotons. In addition, positrons and antiprotons may also come from unusual sources and possibly provide insight into new physics. For instance, the annihilation of heavy supersymmetric dark matter particles within the Galactic halo could lead to positrons or antiprotons with distinctive energy signatures. With the High-Energy Antimatter Telescope (HEAT) balloon-borne instrument, we have measured the abundances of positrons and electrons at energies between 1 and 50 GeV. The data suggest that indeed a small additional antimatter component may be present that cannot be explained by a purely secondary production mechanism. Here we describe the signature of the effect and discuss its possible origin.  相似文献   

A spatially resolved 'inside-out' outburst of IP Pegasi     

N. A. Webb  T. Naylor  Z. Ioannou  W. J. Worraker  J. Stull  A. Allan  R. Fried  N. D. James  D. Strange 《Monthly notices of the Royal Astronomical Society》1999,310(2):407-413

We present a comprehensive photometric data set taken over the entire outburst of the eclipsing dwarf nova IP Peg in 1997 September/October. Analysis of the light curves taken over the long rise to the peak-of-outburst shows conclusively that the outburst started near the centre of the disc and moved outwards. This is the first data set that spatially resolves such an outburst. The data set is consistent with the idea that long rise times are indicative of such 'inside-out' outbursts. We show how the thickness and the radius of the disc, along with the mass transfer rate, change over the whole outburst. In addition, we show evidence of the secondary and the irradiation thereof. We discuss the possibility of spiral shocks in the disc; however, we find no conclusive evidence of their existence in this data set.  相似文献   

Molecular biomarker evidence of origins and transport of organic matter in sediments of the Pearl River estuary and adjacent South China Sea   总被引：3，自引：0，他引：3  

Jianfang Hu  Ping&#x;an Peng  Allan R. Chivas 《Applied Geochemistry》2009,24(9):1666-1676

Surface sediments from the subtropical Pearl River estuary and adjacent South China Sea were investigated by molecular organic geochemical methods to determine the composition, distribution and origin of extractable lipids (n-alkanes, n-alkanols and sterols). The absolute and organic C normalized concentrations of total alkane, n-alkanol, and sterol ranged from 0.16 to 2.67 μg g⁻¹ and 0.9 to 12.3 μg g⁻¹ OC, 24.4 to 427.3 ng g⁻¹ and 63.2 to 1966.7 ng g⁻¹ OC, and 9.0 to 493.5 ng g⁻¹ and 58.4 to 1042.4 ng g⁻¹ OC, respectively. The spatial distributions of these biomarkers indicated that terrestrial-derived molecular biomarkers such as long-chain n-alkanes, n-alkanols and plant-derived sterols were higher at the river mouth and along the coastline, suggesting that a higher proportion of terrestrial particulate organic matter was deposited there. Relatively lower amounts of marine-derived biomarkers such as short-chain n-alkanes, algal sterols at the river mouth reflected the lower primary productivity due to high turbidity. The spatial patterns of these biomarkers were partially related to the estuarine processes and conditions, evidencing an increased terrestrial signal from the Pearl River mouth to the inner estuary, and enhanced marine conditions further offshore.  相似文献   

Energetic Constraints on Precipitation Under Climate Change     

Paul A. O’Gorman  Richard P. Allan  Michael P. Byrne  Michael Previdi 《Surveys in Geophysics》2012,33(3-4):585-608

Energetic constraints on precipitation are useful for understanding the response of the hydrological cycle to ongoing climate change, its response to possible geoengineering schemes, and the limits on precipitation in very warm climates of the past. Much recent progress has been made in quantifying the different forcings and feedbacks on precipitation and in understanding how the transient responses of precipitation and temperature might differ qualitatively. Here, we introduce the basic ideas and review recent progress. We also examine the extent to which energetic constraints on precipitation may be viewed as radiative constraints and the extent to which they are confirmed by available observations. Challenges remain, including the need to better demonstrate the link between energetics and precipitation in observations and to better understand energetic constraints on precipitation at sub-global length scales.  相似文献   

Spatial and temporal variation of organic carbon in the northern South China Sea revealed by sedimentary records   总被引：2，自引：0，他引：2  

Jianfang Hu  Xuesong Sun  Ping'an Peng  Gan Zhang  Allan R. Chivas 《Quaternary International》2009,206(1-2):46

Three sediment cores were taken from the Pearl River estuary and adjacent northern South China Sea (SCS). These sediment cores span the time interval 1900–2000 AD. The stratigraphy of the concentration, the ratio of total organic carbon (TOC) to total nitrogen (TN) and stable isotope (δ¹³C_org) of organic carbon (OC) from three high-resolution sediment cores were analyzed. The stratigraphic profiles of OC concentration, TOC/TN ratios and δ¹³C_org for the near past 100 yrs indicate that terrestrial organic matter decreases from 68.3% to 27.4% of the TOC in the Pearl River estuary, while Dapeng Bay (offshore east of Hong Kong) apparently had throughout little terrestrial organic matter input. The highest deposited OC occurs at the Humen River mouth and the OC concentrations are higher in the outer estuary than in the inner shelf of the northern SCS. The deposited OC at the River mouth increased with time, which could be caused by the high precipitation of land-derived organic matter and the high input of terrestrial organic matter, which is likely related to the rapid urbanization and industrial development in the Pearl River Delta since the 1970s. The OC concentrations did not exhibit an obvious increase with time in most areas of the Pear River estuary and adjacent inner shelf of the SCS, but the algal-derived OC concentration inferred from the δ¹³C_org values increased with time especially from 1980 to 2000 in the outer Pearl River estuary and Dapeng Bay. This increase is presumably caused by enhanced primary marine productivity supported by higher anthropogenic nutrient inputs.  相似文献