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Sökning: WFRF:(Brühwiler Paul)

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1.
  • Blunden, Jessica, et al. (författare)
  • State of the Climate in 2012
  • 2013
  • Ingår i: Bulletin of The American Meteorological Society - (BAMS). - 0003-0007 .- 1520-0477. ; 94:8, s. S1-S258
  • Tidskriftsartikel (refereegranskat)abstract
    • For the first time in serveral years, the El Nino-Southern Oscillation did not dominate regional climate conditions around the globe. A weak La Ni a dissipated to ENSOneutral conditions by spring, and while El Nino appeared to be emerging during summer, this phase never fully developed as sea surface temperatures in the eastern conditions. Nevertheless, other large-scale climate patterns and extreme weather events impacted various regions during the year. A negative phase of the Arctic Oscillation from mid-January to early February contributed to frigid conditions in parts of northern Africa, eastern Europe, and western Asia. A lack of rain during the 2012 wet season led to the worst drought in at least the past three decades for northeastern Brazil. Central North America also experienced one of its most severe droughts on record. The Caribbean observed a very wet dry season and it was the Sahel's wettest rainy season in 50 years. Overall, the 2012 average temperature across global land and ocean surfaces ranked among the 10 warmest years on record. The global land surface temperature alone was also among the 10 warmest on record. In the upper atmosphere, the average stratospheric temperature was record or near-record cold, depending on the dataset. After a 30-year warming trend from 1970 to 1999 for global sea surface temperatures, the period 2000-12 had little further trend. This may be linked to the prevalence of La Ni a-like conditions during the 21st century. Heat content in the upper 700 m of the ocean remained near record high levels in 2012. Net increases from 2011 to 2012 were observed at 700-m to 2000-m depth and even in the abyssal ocean below. Following sharp decreases in to the effects of La Ni a, sea levels rebounded to reach records highs in 2012. The increased hydrological cycle seen in recent years continued, with more evaporation in drier locations and more precipitation in rainy areas. In a pattern that has held since 2004, salty areas of the ocean surfaces and subsurfaces were anomalously salty on average, while fresher areas were anomalously fresh. Global tropical cyclone activity during 2012 was near average, with a total of 84 storms compared with the 1981-2010 average of 89. Similar to 2010 and 2011, the North Atlantic was the only hurricane basin that experienced above-normal activity. In this basin, Sandy brought devastation to Cuba and parts of the eastern North American seaboard. All other basins experienced either near-or below-normal tropical cyclone activity. Only three tropical cyclones reached Category 5 intensity-all in Bopha became the only storm in the historical record to produce winds greater than 130 kt south of 7 N. It was also the costliest storm to affect the Philippines and killed more than 1000 residents. Minimum Arctic sea ice extent in September and Northern Hemisphere snow cover extent in June both reached new record lows. June snow cover extent is now declining at a faster rate (-17.6% per decade) than September sea ice extent (-13.0% per decade). Permafrost temperatures reached record high values in northernmost Alaska. A new melt extent record occurred on 11-12 July on the Greenland ice sheet; 97% of the ice sheet showed some form of melt, four times greater than the average melt for this time of year. The climate in Antarctica was relatively stable overall. The largest maximum sea ice extent since records begain in 1978 was observed in September 2012. In the stratosphere, warm air led to the second smallest ozone hole in the past two decades. Even so, the springtime ozone layer above Antarctica likely will not return to its early 1980s state until about 2060. Following a slight decline associated with the global 2 emissions from fossil fuel combustion and cement production reached a record 9.5 +/- 0.5 Pg C in 2011 and a new record of 9.7 +/- 0.5 Pg C is estimated for 2012. Atmospheric CO2 concentrations increased by 2.1 ppm in 2012, to 392.6 ppm. In spring 2012, 2 concentration exceeded 400 ppm at 7 of the 13 Arctic observation sites. Globally, other greenhouse gases including methane and nitrous oxide also continued to rise in concentration and the combined effect now represents a 32% increase in radiative forcing over a 1990 baseline. Concentrations of most ozone depleting substances continued to fall.
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2.
  • Saunois, Marielle, et al. (författare)
  • The Global Methane Budget 2000–2017
  • 2020
  • Ingår i: Earth System Science Data. - : Copernicus GmbH. - 1866-3516 .- 1866-3508. ; 12:3, s. 1561-1623
  • Tidskriftsartikel (refereegranskat)abstract
    • Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations).For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4 yr−1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr−1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30∘ N) compared to mid-latitudes (∼ 30 %, 30–60∘ N) and high northern latitudes (∼ 4 %, 60–90∘ N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters.Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4 yr−1 by 8 Tg CH4 yr−1, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning.The data presented here can be downloaded from https://doi.org/10.18160/GCP-CH4-2019 (Saunois et al., 2020) and from the Global Carbon Project.
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3.
  • Bruhwiler, Lori, et al. (författare)
  • The Arctic Carbon Cycle and Its Response to Changing Climate
  • 2021
  • Ingår i: Current Climate Change Reports. - : Springer Science and Business Media LLC. - 2198-6061. ; 7:1, s. 14-34
  • Forskningsöversikt (refereegranskat)abstract
    • Purpose of Review: The Arctic has experienced the most rapid change in climate of anywhere on Earth, and these changes are certain to drive changes in the carbon budget of the Arctic as vegetation changes, soils warm, fires become more frequent, and wetlands evolve as permafrost thaws. In this study, we review the extensive evidence for Arctic climate change and effects on the carbon cycle. In addition, we re-evaluate some of the observational evidence for changing Arctic carbon budgets. Recent Findings: Observations suggest a more active CO2 cycle in high northern latitude ecosystems. Evidence points to increased uptake by boreal forests and Arctic ecosystems, as well as increasing respiration, especially in autumn. However, there is currently no strong evidence of increased CH4 emissions. Summary: Long-term observations using both bottom-up (e.g., flux) and top-down (atmospheric abundance) approaches are essential for understanding changing carbon cycle budgets. Consideration of atmospheric transport is critical for interpretation of top-down observations of atmospheric carbon.
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5.
  • Kjeldgaard, Lisbeth, et al. (författare)
  • Intramolecular vibronic dynamics in molecular solids: C60
  • 2005
  • Ingår i: Physical Review B (Condensed Matter and Materials Physics). - 1098-0121. ; 72:20
  • Tidskriftsartikel (refereegranskat)abstract
    • Vibronic coupling in solid C60 has been investigated with a combination of resonant photoemission spectroscopy (RPES) and resonant inelastic x-ray scattering (RIXS). Excitation as a function of energy within the lowest unoccupied molecular orbital resonance yielded strong oscillations in intensity and dispersion in RPES, and a strong inelastic component in RIXS. Reconciling these two observations establishes that vibronic coupling in this core hole excitation leads to predominantly inelastic scattering and localization of the excited vibrations on the molecule on a femtosecond time scale. The coupling extends throughout the widths of the frontier valence bands.
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6.
  • Käämbre, Tanel, et al. (författare)
  • Bulk electronic structure of K3C60 as revealed by soft x-rays
  • 2007
  • Ingår i: Physical Review B. Condensed Matter and Materials Physics. - 1098-0121 .- 1550-235X. ; 75:19, s. 195432-
  • Tidskriftsartikel (refereegranskat)abstract
    • We present C 1s x- ray absorption, x- ray emission, and resonant inelastic x- ray scattering (RIXS ) spectra of single- phase crystalline K3C60. The comparison to valence- band photoelectron spectra from the same sample facilitates identification of the contribution from surface and bulk electronic states in the latter. Bulk- sensitive techniques show that the valence bands of K3C60 and pure C-60 are characterized by spectral features of similar width, in agreement with the predictions of band- structure calculations. Symmetry selectivity in the RIXS process allows us to assign peaks in the C 1s absorption spectrum, demonstrating a close correspondence with pure C-60 also in the conduction band. The symmetry selectivity is as pronounced in K3C60 as in pure C-60, indicating that the local C-60 symmetry is not appreciably affected by the K doping, either in the ground state or intermediate state, on the time scale of 6 fs.
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7.
  • Macovez, R., et al. (författare)
  • Electronic surface reconstruction and correlation in the fcc and dimer phases of RbC60
  • 2007
  • Ingår i: Physical Review B. Condensed Matter and Materials Physics. - 1098-0121 .- 1550-235X. ; 75:19, s. 195424-
  • Tidskriftsartikel (refereegranskat)abstract
    • A combined photoemission and x-ray absorption study of a RbC60 crystalline film is presented. We find evidence for an electronic charge reconstruction of the film surface in both the fcc and the dimer phases of RbC60. We confirm the previous conclusion on less crystalline films that the dimer phase is insulating. Several observations, such as the presence of molecular features in the photoemission spectra, indicate that at least partial electron localization occurs in the high-temperature fcc phase. In the fcc phase, the surface consists in a half-charge C60(111) plane and appears weakly metallic, as found for the bulk. In the dimer phase, the charge reconstruction simply implies the presence of neutral C60 in the surface layer. The identification of neutral molecules in the surface layer drastically improves the agreement between calculations of the electronic density of states and photoelectron spectra in both phases.
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8.
  • Macovez, Roberto, et al. (författare)
  • Reversible Phase Transformation and Doubly Charged Anions at the Surface of Simple Cubic RbC60
  • 2008
  • Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 101:23, s. 236403-
  • Tidskriftsartikel (refereegranskat)abstract
    • The simple cubic phase of a RbC60 thin film has been studied using photoelectron spectroscopy. The simple cubic-to-dimer transition is found to be reversible at the film surface. A sharp Fermi edge is observed and a lower limit of 0.5 eV is found for the surface Hubbard U, pointing to a strongly correlated metallic character of thin-film simple cubic RbC60. A molecular charge state is identified in the valence band and core-level photoemission spectra which arises from C-60(2-) anions and contributes to the spectral intensity at the Fermi level.
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9.
  • Rudolf, P, et al. (författare)
  • Studies of fullerenes by the excitation, emission, and scattering of electrons
  • 1999
  • Ingår i: Journal of Electron Spectroscopy and Related Phenomena. - 0368-2048 .- 1873-2526. ; 100:1-3, s. 409-433
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper presents an overview of how electron spectroscopies have contributed to advances in fullerene research. In particular, we illustrate the vital role these techniques have played in improving our understanding of the importance of strong electronic correlation and of electron-phonon coupling in these materials, in the derivation of electron hopping rates, in providing a direct determination of charge transfer and hybridisation in both fullerene salts and adsorbed fullerenes and in determining the optical gap of these systems. We discuss systems of increasing complexity, starting with C60 in the gas phase and in the solid state, and moving on to C60 salts and to C60 adsorbed on surfaces. Finally we look at both higher fullerenes and fullerenes with a heteroatom either on or inside the cage.
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10.
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