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In this study we use the ERA-Interim reanalysis data set from the European Centre for Medium-Range Weather Forecasts (ECMWF) and a refined version of a previously developed Lagrangian methodology to compile a global 33 yr climatology of stratosphere–troposphere exchange (STE) from 1979 to 2011. Fluxes of mass and ozone are calculated across the tropopause, pressure surfaces in the troposphere, and the top of the planetary boundary layer (PBL). This climatology provides a state-of-the-art quantification of the geographical distribution of STE and the preferred transport pathways, as well as insight into the temporal evolution of STE during the last 33 yr. <br><br> We confirm the distinct zonal and seasonal asymmetry found in previous studies using comparable methods. The subset of "deep STE", where stratospheric air reaches the PBL within 4 days or vice versa, shows especially strong geographical and seasonal variations. The global hotspots for deep STE are found along the west coast of North America and over the Tibetan Plateau, especially in boreal winter and spring. An analysis of the time series reveals significant positive trends of the net downward mass flux and of deep STE in both directions, which are particularly large over North America. <br><br> The downward ozone flux across the tropopause is dominated by the seasonal cycle of ozone concentrations at the tropopause and peaks in summer, when the mass flux is nearly at its minimum. For the subset of deep STE events, the situation is reversed and the downward ozone flux into the PBL is dominated by the mass flux and peaks in early spring. Thus surface ozone concentration along the west coast of North America and around the Tibetan Plateau are likely to be influenced by deep stratospheric intrusions. <br><br> We discuss the sensitivity of our results on the choice of the control surface representing the tropopause, the horizontal and vertical resolution of the trajectory starting grid, and the minimum residence time τ used to filter out transient STE trajectories.
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In this study the sensitivity of the model performance of the chemistry transport model (CTM) LOTOS-EUROS to the description of the temporal variability of emissions was investigated. Currently the temporal release of anthropogenic emissions is described by European average diurnal, weekly and seasonal time profiles per sector. These default time profiles largely neglect the variation of emission strength with activity patterns, region, species, emission process and meteorology. The three sources dealt with in this study are combustion in energy and transformation industries (SNAP1), nonindustrial combustion (SNAP2) and road transport (SNAP7). First of all, the impact of neglecting the temporal emission profiles for these SNAP categories on simulated concentrations was explored. In a second step, we constructed more detailed emission time profiles for the three categories and quantified their impact on the model performance both separately as well as combined. The performance in comparison to observations for Germany was quantified for the pollutants NO<sub>2</sub>, SO<sub>2</sub> and PM<sub>10</sub> and compared to a simulation using the default LOTOS-EUROS emission time profiles. The LOTOS-EUROS simulations were performed for the year 2006 with a temporal resolution of 1 h and a horizontal resolution of approximately 25 × 25km<sup>2</sup>. <br><br> In general the largest impact on the model performance was found when neglecting the default time profiles for the three categories. The daily average correlation coefficient for instance decreased by 0.04 (NO<sub>2</sub>), 0.11 (SO<sub>2</sub>) and 0.01 (PM<sub>10</sub>) at German urban background stations compared to the default simulation. A systematic increase in the correlation coefficient is found when using the new time profiles. The size of the increase depends on the source category, component and station. Using national profiles for road transport showed important improvements in the explained variability over the weekdays as well as the diurnal cycle for NO<sub>2</sub>. The largest impact of the SNAP1 and 2 profiles were found for SO<sub>2</sub>. When using all new time profiles simultaneously in one simulation, the daily average correlation coefficient increased by 0.05 (NO<sub>2</sub>), 0.07 (SO<sub>2</sub>) and 0.03 (PM<sub>10</sub>) at urban background stations in Germany. This exercise showed that to improve the performance of a CTM, a better representation of the distribution of anthropogenic emission in time is recommendable. This can be done by developing a dynamical emission model that takes into account regional specific factors and meteorology.
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Two complementary case studies are conducted to analyse convective system properties in the region where strong cloud-top lidar backscatter anomalies are observed as reported by Platt et al. (2011). These anomalies were reported for the first time using in situ microphysical measurements in an isolated continental convective cloud over Germany during the CIRCLE2 experiment (Gayet et al., 2012). In this case, in situ observations quasi-collocated with CALIPSO (Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observation), CloudSat and Meteosat-9/SEVIRI observations confirm that regions of backscatter anomalies represent the most active and dense convective cloud parts with likely the strongest core updrafts and unusually high values of the particle concentration, extinction and ice water content (IWC), with the occurrence of small ice crystal sizes. Similar spaceborne observations of a maritime mesoscale cloud system (MCS) located off the Brazilian coast between 0° and 3° N latitude on 20 June 2008 are then analysed. Near cloud-top backscatter anomalies are evidenced in a region which corresponds to the coldest temperatures with maximum cloud top altitudes derived from collocated CALIPSO/IIR and Meteosat-9/SEVIRI infrared brightness temperatures. The interpretation of CALIOP (Cloud Aerosol Lidar with Orthogonal Polarization) data highlights significant differences in microphysical properties from those observed in the continental isolated convective cloud. Indeed, SEVIRI (Spinning Enhanced Visible and InfraRed Imager) retrievals in the visible spectrum confirm much smaller ice particles near the top of the isolated continental convective cloud, i.e. effective radius (<i>R</i><sub>eff</sub>) ~ 15 μm as opposed to 22–27 μm in the whole MCS area. Cloud profiling observations at 94 GHz from CloudSat are then used to describe the properties of the most active cloud regions at and below cloud top. The cloud ice-water content and effective radius retrieved with the CloudSat 2B-IWC and DARDAR (raDAR/liDAR) inversion techniques, show that at usual cruise altitudes of commercial aircraft (FL 350 or ~ 10 700 m level), high IWC (i.e. up to 2 to 4 g m<sup>−3</sup>) could be identified according to specific IWC–<i>Z</i> (<i>Z</i> being the reflectivity factor) relationships. These values correspond to a maximum reflectivity factor of +18 dBZ (at 94 GHz). Near-top cloud properties also indicate signatures of microphysical characteristics according to the cloud-stage evolution as revealed by SEVIRI images to identify the development of new cells within the MCS cluster. It is argued that the availability of real-time information (on the kilometre-scale) about cloud top IR brightness temperature decreases with respect to the cloud environment would help identify MCS cloud areas with potentially high ice water content and small particle sizes against which onboard meteorological radars may not be able to provide timely warning.
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A model of carbonaceous aerosols has been implemented in the TwO-Moment Aerosol Sectional (TOMAS) microphysics module in the GEOS-Chem chemical transport model (CTM), a model driven by assimilated meteorology. Inclusion of carbonaceous emissions alongside pre-existing treatments of sulfate and sea-salt aerosols increases the number of emitted primary aerosol particles by a factor of 2.5 and raises annual-average global cloud condensation nuclei at 0.2% supersaturation (CCN(0.2%)) concentrations by a factor of two. Compared to the prior model without carbonaceous aerosols, this development improves the model prediction of condensation nuclei with dry diameter larger than 10 nm (CN10) number concentrations significantly from −45% to −7% bias when compared to long-term observations. Inclusion of carbonaceous particles also largely eliminates a tendency for the model to underpredict higher cloud condensation nuclei (CCN) concentrations. Similar to other carbonaceous models, the model underpredicts organic carbon (OC) and elemental carbon (EC) mass concentrations by a factor of 2 when compared to EMEP and IMPROVE observations. Because primary organic aerosol (POA) and secondary organic aerosol (SOA) affect aerosol number size distributions via different microphysical processes, we assess the sensitivity of CCN production, for a fixed source of organic aerosol (OA) mass, to the assumed POA–SOA split in the model. For a fixed OA budget, we found that CCN(0.2%) decreases nearly everywhere as the model changes from a world dominated by POA emissions to one dominated by SOA condensation. POA is about twice as effective per unit mass at CCN production compared to SOA. Changing from a 100% POA scenario to a 100% SOA scenario, CCN(0.2%) concentrations in the lowest model layer decrease by about 20%. In any scenario, carbonaceous aerosols contribute significantly to global CCN. The SOA–POA split has a significant effect on global CCN, and the microphysical implications of POA emissions versus SOA condensation appear to be at least as important as differences in chemical composition as expressed by the hygroscopicity of OA. These findings stress the need to better understand carbonaceous aerosols loadings, the global SOA budget, microphysical pathways of OA formation (emissions versus condensation) as well as chemical composition to improve climate modeling.
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Bromine plays an important role in ozone chemistry in both the troposphere and stratosphere. When measured by mass, bromoform (CHBr<sub>3</sub>) is thought to be the largest organic source of bromine to the atmosphere. While seaweed and phytoplankton are known to be dominant sources, the size and the geographical distribution of CHBr<sub>3</sub> emissions remains uncertain. Particularly little is known about emissions from the Maritime Continent, which have usually been assumed to be large, and which appear to be especially likely to reach the stratosphere. In this study we aim to reduce this uncertainty by combining the first multi-annual set of CHBr<sub>3</sub> measurements from this region, and an inversion process, to investigate systematically the distribution and magnitude of CHBr<sub>3</sub> emissions. The novelty of our approach lies in the application of the inversion method to CHBr<sub>3</sub>. We find that local measurements of a short-lived gas like CHBr<sub>3</sub> can be used to constrain emissions from only a relatively small, sub-regional domain. We then obtain detailed estimates of CHBr<sub>3</sub> emissions within this area, which appear to be relatively insensitive to the assumptions inherent in the inversion process. We extrapolate this information to produce estimated emissions for the entire tropics (defined as 20° S–20° N) of 225 Gg CHBr<sub>3</sub> yr<sup>−1</sup>. The ocean in the area we base our extrapolations upon is typically somewhat shallower, and more biologically productive, than the tropical average. Despite this, our tropical estimate is lower than most other recent studies, and suggests that CHBr<sub>3</sub> emissions in the coastline-rich Maritime Continent may not be stronger than emissions in other parts of the tropics.
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We evaluate how regional characteristics of population and background pollution might impact the selection of optimal air quality model resolution when calculating the human health impacts of changes to air quality. Using an approach consistent with air quality policy evaluation, we use a regional chemical transport model (CAMx) and a health benefit mapping program (BenMAP) to calculate the human health impacts associated with changes in ozone and fine particulate matter resulting from an emission reduction scenario. We evaluate this same scenario at 36, 12 and 4 km resolution for nine regions in the eastern US representing varied characteristics. We find that the human health benefits associated with changes in ozone concentrations are sensitive to resolution. This finding is especially strong in urban areas where we estimate that benefits calculated using coarse resolution results are on average two times greater than benefits calculated using finer scale results. In three urban areas we analyzed, results calculated using 36 km resolution modeling fell outside the uncertainty range of results calculated using finer scale modeling. In rural areas the influence of resolution is less pronounced with only an 8% increase in the estimated health impacts when using 36 km resolution over finer scales. In contrast, health benefits associated with changes in PM<sub>2.5</sub> concentrations were not sensitive to resolution and did not follow a pattern based on any regional characteristics evaluated. The largest difference between the health impacts estimated using 36 km modeling results and either 12 or 4 km results was at most ±10% in any region. Several regions showed increases in estimated benefits as resolution increased (opposite the impact seen with ozone modeling), while some regions showed decreases in estimated benefits as resolution increased. In both cases, the dominant contribution was from secondary PM. Additionally, we found that the health impacts calculated using several individual concentration–response functions varied by a larger amount than the impacts calculated using results modeled at different resolutions. Given that changes in PM<sub>2.5</sub> dominate the human health impacts, and given the uncertainty associated with human health response to changes in air pollution, we conclude that, when estimating the human health benefits associated with decreases in ozone and PM<sub>2.5</sub> together, the benefits calculated at 36 km resolution agree, within errors, with the benefits calculated using fine (12 km or finer) resolution modeling when using the current methodology for assessing policy decisions.
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Over the 21st century, changes in CO<sub>2</sub> levels, climate and land use are expected to alter the global distribution of vegetation, leading to changes in trace gas emissions from plants, including, importantly, the emissions of isoprene. This, combined with changes in anthropogenic emissions, has the potential to impact tropospheric ozone levels, which above a certain level are harmful to animals and vegetation. In this study we use a biogenic emissions model following the empirical parameterisation of the MEGAN model, with vegetation distributions calculated by the Sheffield Dynamic Global Vegetation Model (SDGVM) to explore a range of potential future (2095) changes in isoprene emissions caused by changes in climate (including natural land use changes), land use, and the inhibition of isoprene emissions by CO<sub>2</sub>. From the present-day (2000) value of 467 Tg C yr<sup>−1</sup>, we find that the combined impact of these factors could cause a net decrease in isoprene emissions of 259 Tg C yr<sup>−1</sup> (55%) with individual contributions of +78 Tg C yr<sup>−1</sup> (climate change), −190 Tg C yr<sup>−1</sup> (land use) and −147 Tg C yr<sup>−1</sup> (CO<sub>2</sub> inhibition). Using these isoprene emissions and changes in anthropogenic emissions, a series of integrations is conducted with the UM-UKCA chemistry-climate model with the aim of examining changes in ozone over the 21st century. Globally, all combined future changes cause a decrease in the tropospheric ozone burden of 27 Tg (7%) from 379 Tg in the present-day. At the surface, decreases in ozone of 6–10 ppb are calculated over the oceans and developed northern hemispheric regions, due to reduced NO<sub>x</sub> transport by PAN and reductions in NO<sub>x</sub> emissions in these areas respectively. Increases of 4–6 ppb are calculated in the continental tropics due to cropland expansion in these regions, increased CO<sub>2</sub> inhibition of isoprene emissions, and higher temperatures due to climate change. These effects outweigh the decreases in tropical ozone caused by increased tropical isoprene emissions with climate change. Our land use change scenario consists of cropland expansion, which is most pronounced in the tropics. The tropics are also where land use change causes the greatest increases in ozone. As such there is potential for increased crop exposure to harmful levels of ozone. However, we find that these ozone increases are still not large enough to raise ozone to such damaging levels.
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The recent 23–30 January and 7–11 March 2012 solar proton event (SPE) periods were substantial and caused significant impacts on the middle atmosphere. These were the two largest SPE periods of solar cycle 24 so far. The highly energetic solar protons produced considerable ionization of the neutral atmosphere as well as HO<sub>x</sub> (H, OH, HO<sub>2</sub>) and NO<sub>x</sub> (N, NO, NO<sub>2</sub>). We compute a NO<sub>x</sub> production of 1.9 and 2.1 Gigamoles due to these SPE periods in January and March 2012, respectively, which places these SPE periods among the 12 largest in the past 50 yr. Aura Microwave Limb Sounder (MLS) observations of the peroxy radical, HO<sub>2</sub>, show significant enhancements of > 0.9 ppbv in the northern polar mesosphere as a result of these SPE periods. Both MLS measurements and Goddard Space Flight Center (GSFC) two-dimensional (2-D) model predictions indicated middle mesospheric ozone decreases of > 20% for several days in the northern polar region with maximum depletions > 60% over 1–2 days as a result of the HO<sub>x</sub> produced in both the January and March 2012 SPE periods. The SCISAT-1 Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE) and the Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instruments measured NO and NO<sub>2</sub> (~ NO<sub>x</sub>), which indicated enhancements of over 20 ppbv in most of the northern polar mesosphere for several days as a result of these SPE periods. The GSFC 2-D model and the Global Modeling Initiative three-dimensional chemistry and transport model were used to predict the medium-term (~ months) influence and showed that the polar middle atmospheric ozone was most affected by these solar events in the Southern Hemisphere due to the increased downward motion in the fall and early winter. The downward transport moved the SPE-produced NO<sub>y</sub> to lower altitudes and led to predicted modest destruction of ozone (5–13%) in the upper stratosphere days to weeks after the March 2012 event. Polar total ozone reductions were predicted to be a maximum of 1.5% in 2012 due to these SPEs.
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Recent ground networks and satellite remote-sensing observations have provided useful data related to spatial and vertical distributions of mineral dust particles in the atmosphere. However, measurements of temporal variations and spatial distributions of mineral dust deposition fluxes are limited in terms of their duration, location, and processes of deposition. To ascertain temporal variations and spatial distributions of mineral dust deposition using wet and dry processes, weekly deposition samples were obtained at Sapporo, Toyama, Nagoya, Tottori, Fukuoka, and Cape Hedo (Okinawa) in Japan during October 2008–December 2010 using automatic wet and dry separating samplers. Mineral dust weights in water-insoluble residue were estimated from Fe contents measured using an X-ray fluorescence analyser. Wet and dry deposition fluxes of mineral dusts were both high in spring and low in summer, showing similar seasonal variations to frequency of aeolian dust events (Kosa) in Japan. For wet deposition, highest and lowest annual dust fluxes were found at Toyama (9.6 g m<sup>−2</sup> yr<sup>−1</sup>) and at Cape Hedo (1.7 g m<sup>−2</sup> yr<sup>−1</sup>) as average values in 2009 and 2010. Higher wet deposition fluxes were observed at Toyama and Tottori, where frequent precipitation (> 60% days per month) was observed during dusty seasons. For dry deposition among Toyama, Tottori, Fukuoka, and Cape Hedo, the highest and lowest annual dust fluxes were found respectively at Fukuoka (5.2 g m<sup>−2</sup> yr<sup>−1</sup>) and at Cape Hedo (2.0 g m<sup>−2</sup> yr<sup>−1</sup>) as average values in 2009 and 2010. The average ratio of wet and dry deposition fluxes was the highest at Toyama (3.3) and the lowest at Hedo (0.82), showing a larger contribution of the dry process at western sites, probably because of the distance from desert source regions and because of the effectiveness of the wet process in the dusty season. <br><br> Size distributions of refractory dust particles were obtained using four-stage filtration: > 20, > 10, > 5, and > 1 μm diameter. Weight fractions of the sum of > 20 μm and 10–20 μm (giant fraction) were higher than 50% for most of the event samples. Irrespective of the deposition type, the giant dust fractions generally decreased with increasing distance from the source area, suggesting the selective depletion of larger giant particles during atmospheric transport. Based on temporal variations of PM<sub>c</sub> (2.5 < <i>D</i> < 10 μm), ground-based lidar, backward air trajectories, and vertical profiles of potential temperatures, transport processes of dust particles are discussed for events with high-deposition and low-deposition flux with high PM<sub>c</sub>. Low dry dust depositions with high PM<sub>c</sub> concentrations were observed under stronger (5 K km<sup>−1</sup>) stratification of potential temperature with thinner and lower (< 2 km) dust distributions because the PM<sub>c</sub> fraction of dust particles only survived after depletion of giant dust particles by rapid gravitational settling at the time they reach Japan. In contrast, transport through a thicker (> 2 km) dust layer with weak vertical gradient of potential temperature carry more giant dust particles to Japan. Because giant dust particles are an important mass fraction of dust accumulation, especially in the North Pacific, which is known as a high-nutrient, low-chlorophyll (HNLC) region, the transport height and fraction of giant dust particles are important factors for studying dust budgets in the atmosphere and their role in biogeochemical cycles.
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