The impact of air pollutant and methane emission controls on tropospheric ozone and radiative forcing: CTM calculations for the period 1990-2030

To explore the relationship between tropospheric ozone and radiative forcing with changing emissions, we compiled two sets of global scenarios for the emissions of the ozone precursors methane (CH₄), carbon monoxide (CO), non-methane volatile organic compounds (NMVOC) and nitrogen oxides (NO_x) up to the year 2030 and implemented them in two global Chemistry Transport Models. The 'Current Legislation' (CLE) scenario reflects the current perspectives of individual countries on future economic development and takes the anticipated effects of presently decided emission control legislation in the individual countries into account. In addition, we developed a 'Maximum technically Feasible Reduction' (MFR) scenario that outlines the scope for emission reductions offered by full implementation of the presently available emission control technologies, while maintaining the projected levels of anthropogenic activities. Whereas the resulting projections of methane emissions lie within the range suggested by other greenhouse gas projections, the recent pollution control legislation of many Asian countries, requiring introduction of catalytic converters for vehicles, leads to significantly lower growth in emissions of the air pollutants NO_x, NMVOC and CO than was suggested by the widely used and more pessimistic IPCC (Intergovernmental Panel on Climate Change) SRES (Special Report on Emission Scenarios) scenarios (Nakicenovic et al., 2000), which made Business-as-Usual assumptions regarding emission control technology. With the TM3 and STOCHEM models we performed several long-term integrations (1990-2030) to assess global, hemispheric and regional changes in CH₄, CO, hydroxyl radicals, ozone and the radiative climate forcings resulting from these two emission scenarios. Both models reproduce broadly the observed trends in CO, and CH₄ concentrations from 1990 to 2002. <P style='line-height: 20px;'> For the 'current legislation' case, both models indicate an increase of the annual average ozone levels in the Northern Hemisphere by 5ppbv, and up to 15ppbv over the Indian sub-continent, comparing the 2020s (2020-2030) with the 1990s (1990-2000). The corresponding higher ozone and methane burdens in the atmosphere increase radiative forcing by approximately 0.2 Wm^-2. Full application of today's emissions control technologies, however, would bring down ozone below the levels experienced in the 1990s and would reduce the radiative forcing of ozone and methane to approximately -0.1 Wm^-2. This can be compared to the 0.14-0.47 Wm^-2 increase of methane and ozone radiative forcings associated with the SRES scenarios. While methane reductions lead to lower ozone burdens and to less radiative forcing, further reductions of the air pollutants NO_x and NMVOC result in lower ozone, but at the same time increase the lifetime of methane. Control of methane emissions appears an efficient option to reduce tropospheric ozone as well as radiative forcing

Influence of future air pollution mitigation strategies on total aerosol radiative forcing

We apply different aerosol and aerosol precursor emission scenarios reflecting possible future control strategies for air pollution in the ECHAM5-HAM model, and simulate the resulting effect on the Earth's radiation budget. We use two opposing future mitigation strategies for the year 2030: one in which emission reduction legislation decided in countries throughout the world are effectively implemented (current legislation; CLE 2030) and one in which all technical options for emission reductions are being implemented independent of their cost (maximum feasible reduction; MFR 2030). We consider the direct, semi-direct and indirect radiative effects of aerosols. The total anthropogenic aerosol radiative forcing defined as the difference in the top-of-the-atmosphere radiation between 2000 and pre-industrial times amounts to -2.00 W/m2. In the future this negative global annual mean aerosol radiative forcing will only slightly change (+0.02 W/m2) under the "current legislation" scenario. Regionally, the effects are much larger: e.g. over Eastern Europe radiative forcing would increase by +1.50 W/m2 because of successful aerosol reduction policies, whereas over South Asia it would decrease by -1.10 W/m2 because of further growth of emissions. A "maximum feasible reduction" of aerosols and their precursors would lead to an increase of the global annual mean aerosol radiative forcing by +1.13 W/m2. Hence, in the latter case, the present day negative anthropogenic aerosol forcing could be more than halved by 2030 because of aerosol reduction policies and climate change thereafter will be to a larger extent be controlled by greenhouse gas emissions. We combined these two opposing future mitigation strategies for a number of experiments focusing on different sectors and regions. In addition, we performed sensitivity studies to estimate the importance of future changes in oxidant concentrations and the importance of the aerosol microphysical coupling within the range of expected future changes. For changes in oxidant concentrations caused by future air pollution mitigation, we do not find a significant effect for the global annual mean radiative aerosol forcing. In the extreme case of only abating SO2 or carbonaceous emissions to a maximum feasible extent, we find deviations from additivity for the radiative forcing over anthropogenic source regions up to 10% compared to an experiment abating both at the same time

Physical aerosol properties and their relation to air mass origin at Monte Cimone (Italy) during the first MINATROC campaign

Aerosol physical properties were measured at the Monte Cimone Observatory (Italy) from 1 June till 6 July 2000. The measurement site is located in the transition zone between the continental boundary layer and the free troposphere (FT), at the border between the Mediterranean area and Central Europe, and is exposed to a variety of air masses. Sub-&mu;m number size distributions, aerosol hygroscopicity near 90% RH, refractory size distribution at 270&deg;C and equivalent black carbon mass were continuously measured. Number size distributions and hygroscopic properties indicate that the site is exposed to aged continental air masses, however during daytime it is also affected by upslope winds. The mixing of this transported polluted boundary layer air masses with relatively clean FT air leads to frequent nucleation events around local noon. <P style='line-height: 20px;'> Night-time size distributions, including fine and coarse fractions for each air mass episode, have been parameterized by a 3-modal lognormal distribution. Number and volume concentrations in the sub-&mu;m modes are strongly affected by the air mass origin, with highest levels in NW-European air masses, versus very clean, free tropospheric air coming from the N-European sector. During a brief but distinct dust episode, the coarse mode is clearly enhanced. <P style='line-height: 20px;'> The observed hygroscopic behavior of the aerosol is consistent with the chemical composition described by Putaud et al.&nbsp;(2004), but no closure between known chemical composition and measured hygroscopicity could be made because the hygroscopic properties of the water-soluble organic matter (WSOM) are not known. The data suggest that WSOM is slightly-to-moderately hygroscopic (hygroscopic growth factor GF at 90% relative humidity between 1.05 and 1.51), and that this property may well depend on the air mass origin and history. <P style='line-height: 20px;'> External mixing of aerosol particles is observed in all air masses through the occurrence of two hygroscopicity modes (average GF of 1.22 and 1.37, respectively). However, the presence of 'less' hygroscopic particles has mostly such a low occurrence rate that the average growth factor distribution for each air mass sector actually appears as a single mode. This is not the case for the dust episode, where the external mixing between less hygroscopic and more hygroscopic particles is very prominent, and indicating clearly the occurrence of a dust accumulation mode, extending down to 50 nm particles, along with an anthropogenic pollution mode. <P style='line-height: 20px;'> The presented physical measurements finally allow us to provide a partitioning of the sub-&mu;m aerosol in four non-overlapping fractions (soluble/volatile, non-soluble/volatile, refractory/non-black carbon, black carbon) which can be associated with separate groups of chemical compounds determined with chemical-analytical techniques (ions, non-water soluble organic matter, dust, elemental carbon). All air masses except the free-tropospheric N-European and Dust episodes show a similar composition within the uncertainty of the data (53%, 37%, 5% and 5% respectively for the four defined fractions). Compared to these sectors, the dust episode shows a clearly enhanced refractory-non-BC fraction (17%), attributed to dust in the accumulation mode, whereas for the very clean N-EUR sector, the total refractory fraction is 25%, of which 13% non-BC and 12% BC

A GCM study of future climate response to aerosol pollution reductions

We use the global atmospheric GCM aerosol model ECHAM5-HAM to asses possible impacts of future air pollution mitigation strategies on climate. Air quality control strategies focus on the reduction of aerosol emissions. Here we investigate the extreme case of a maximum feasible end-of-pipe abatement of aerosols in the near term future (2030) in combination with increasing greenhouse gas (GHG) concentrations. The temperature response of increasing GHG concentrations and reduced aerosol emissions leads to a global annual mean equilibrium temperature response of 2.18 K. When aerosols are maximally abated only in the Industry and Powerplant sector, while other sectors stay with currently enforced regulations, the temperature response is 1.89 K. A maximum feasible abatement applied in the Domestic and Transport sector, while other sectors remain with the current legislation, leads to a temperature response of 1.39 K. Increasing GHG concentrations alone lead to a temperature response of 1.20 K. We also simulate 2–5% increases in global mean precipitation among all scenarios considered, and the hydrological sensitivity is found to be significantly higher for aerosols than for GHGs. Our study, thus highlights the huge potential impact of future air pollution mitigation strategies on climate and supports the need for urgent GHG emission reductions. GHG and aerosol forcings are not independent as both affect and are influenced by changes in the hydrological cycle. However, within the given range of changes in aerosol emissions and GHG concentrations considered in this study, the climate response towards increasing GHG concentrations and decreasing aerosols emissions is additive

A sentence completion procedure as an alternative to the Autobiographical Memory Test for assessing overgeneral memory in non-clinical populations

Overgeneral memory (OGM) has been proposed as a vulnerability factor for depression (Williams et al., 2007) or depressive reactivity to stressful life-events (e.g., Gibbs & Rude, 2004). Traditionally, a cue word procedure known as the Autobiographical Memory Test (AMT; Williams & Broadbent, 1986) is used to assess OGM. Although frequently and validly used in clinical populations, there is evidence suggesting that the AMT is insufficiently sensitive to measure OGM in non-clinical groups. Study 1 evaluated the usefulness of a sentence completion method to assess OGM in non-clinical groups, as an alternative to the AMT. Participants were 197 students who completed the AMT, the Sentence Completion for Events from the Past Test (SCEPT), a depression measure, and visual analogue scales assessing ruminative thinking. Results showed that the mean proportion of overgeneral responses was markedly higher for the SCEPT than for the standard AMT. Also, overgeneral responding on the SCEPT was positively associated to depression scores and depressive rumination scores, whereas overgeneral responding on the AMT was not. Results suggest that the SCEPT, relative to the AMT, is a more sensitive instrument to measure OGM, at least in non-clinical populations. Study 2 further showed that this enhanced sensitivity is most likely due to the omission of the instruction to be specific rather than to the SCEPT's sentence completion format (as opposed to free recall to cue words)

Imaging dielectric relaxation in nanostructured polymers by frequency modulation electrostatic force microscopy

We have developed a method for imaging the temperature-frequency dependence of the dynamics of nanostructured polymer films with spatial resolution. This method provides images with dielectric compositional contrast well decoupled from topography. Using frequency-modulation electrostatic-force-microscopy, we probe the local frequency-dependent (0.1–100 Hz) dielectric response through measurement of the amplitude and phase of the force gradient in response to an oscillating applied electric field. When the phase is imaged at fixed frequency, it reveals the spatial variation in dielectric losses, i.e., the spatial variation in molecular/dipolar dynamics, with 40 nm lateral resolution. This is demonstrated by using as a model system; a phase separated polystyrene/polyvinyl-acetate (PVAc) blend. We show that nanoscale dynamic domains of PVAc are clearly identifiable in phase images as those which light-up in a band of temperature, reflecting the variations in the molecular/dipolar dynamics approaching the glass transition temperature of PVAc

Observations of aerosols in the free troposphere and marine boundary layer of the subtropical Northeast Atlantic: discussion of processes determining their size distribution

During July 1994, submicron aerosol size distributions were measured at two sites on Tenerife, Canary Islands. One station was located in the free troposphere (FT), the other in the marine boundary layer (MBL). Transport toward these two sites was strongly decoupled: the FT was first affected by dust and sulfate-laden air masses advecting from North Africa and later by clean air masses originating over the North Atlantic, whereas the MBL was always subject to the northeasterly trade wind circulation. In the FT the submicron aerosol distribution was predominantly monomodal with a geometric mean diameter of 120 nm and 55 nm during dusty and clean conditions, respectively. The relatively small diameter during the clean conditions indicates that the aerosol originated in the upper troposphere rather than over continental areas or in the lower stratosphere. During dusty conditions the physical and chemical properties of the submicron aerosol suggest that it has an anthropogenic origin over southern Europe and that it remains largely externally mixed with the supermicron mineral dust particles during its transport over North Africa to Tenerife. Apart from synoptic variations, a strong diurnal variation in the aerosol size distribution is observed at the FT site, characterized by a strong daytime mode of ultrafine particles. This is interpreted as being the result of photoinduced nucleation in the upslope winds, which are perturbed by anthropogenic and biogenic emissions on the island. No evidence was found for nucleation occurring in the undisturbed FT. The MBL site was not strongly affected by European pollution during the period of the measurements. The MBL aerosol size distribution was bimodal, but the relative concentration of Aitken and accumulation mode varied strongly. The accumulation mode can be related to cloud processing of the Aitken mode but also to pollution aerosol which was advected within the MBL or entrained from the FT. No bursts of nucleation were observed within the MBL

Spin precession in anisotropic media

We generalize the diffusive model for spin injection and detection in nonlocal spin structures to account for spin precession under an applied magnetic field in an anisotropic medium, for which the spin lifetime is not unique and depends on the spin orientation.We demonstrate that the spin precession (Hanle) line shape is strongly dependent on the degree of anisotropy and on the orientation of the magnetic field. In particular, we show that the anisotropy of the spin lifetime can be extracted from the measured spin signal, after dephasing in an oblique magnetic field, by using an analytical formula with a single fitting parameter. Alternatively, after identifying the fingerprints associated with the anisotropy, we propose a simple scaling of the Hanle line shapes at specific magnetic field orientations that results in a universal curve only in the isotropic case. The deviation from the universal curve can be used as a complementary means of quantifying the anisotropy by direct comparison with the solution of our generalized model. Finally, we applied our model to graphene devices and find that the spin relaxation for graphene on silicon oxide is isotropic within our experimental resolution