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Stratospheric ozone profile measurements from the Stratospheric Aerosol and Gas Experiment~(SAGE) II satellite instrument (1984–2005) are combined with those from the Optical Spectrograph and InfraRed Imager System (OSIRIS) instrument on the Odin satellite (2001–Present) to quantify interannual variability and decadal trends in stratospheric ozone between 60° S and 60° N. These data are merged into a multi-instrument, long-term stratospheric ozone record (1984–present) by analyzing the measurements during the overlap period of 2002–2005 when both satellite instruments were operational. The variability in the deseasonalized time series is fit using multiple linear regression with predictor basis functions including the quasi-biennial oscillation, El Niño–Southern Oscillation index, solar activity proxy, and the pressure at the tropical tropopause, in addition to two linear trends (one before and one after 1997), from which the decadal trends in ozone are derived. From 1984 to 1997, there are statistically significant negative trends of 5–10% per decade throughout the stratosphere between approximately 30 and 50 km. From 1997 to present, a statistically significant recovery of 3–8% per decade has taken place throughout most of the stratosphere with the notable exception between 40° S and 40° N below approximately 22 km where the negative trend continues. The recovery is not significant between 25 and 35 km altitudes when accounting for a conservative estimate of instrument drift.
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We use nighttime measurements from the Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, together with a Lagrangian trajectory model, to study the initial dispersion of volcanic aerosol from the eruption of Mt. Nabro (Ethiopia/Eritrea) in June 2011. The Nabro eruption reached the upper troposphere and lower stratosphere (UTLS) directly, and the plume was initially entrained by the flow surrounding the Asian anticyclone, which prevails in the UTLS from the Mediterranean Sea to East Asia during boreal summer. CALIPSO detected aerosol layers, with optical properties consistent with sulfate, in the lower stratosphere above the monsoon convective region in South and Southeast Asia within 10 days of the eruption. We show that quasi-isentropic differential advection in the vertically sheared flow surrounding the Asian anticyclone explains many of these stratospheric aerosol layers. We use Meteosat-7 data to examine the possible role of deep convection in the Asian monsoon in transporting volcanic material to the lower stratosphere during this time, but find no evidence that convection played a direct role, in contrast with claims made in earlier studies. On longer timescales, we use CALIPSO data to illustrate diabatic ascent of the Nabro aerosol in the lower stratosphere at rates of ~ 10 K per month for the first two months after the eruption, falling to ~ 3 K per month after the Asian anticyclone dissipates. Maps of stratospheric aerosol optical depth (AOD) show local peaks of ~ 0.04–0.06 in July in the region of the Asian anticyclone; we find associated estimates of radiative forcing small, ~ 5–10% of those reported for the eruption of Mt. Pinatubo in 1991. Additionally, we find no clear response in outgoing shortwave (SW) flux due to the presence of Nabro aerosol viewed in the context of SW flux variability as measured by CERES (Clouds and Earth Radiant Energy System).
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During the 1950s and 1960s, when intensive investigations on atmospheric moist convection were launched, two possibilities were identified for the basic element of moist convection: bubble and plume. The present paper reviews the investigations of this period, and suggests how the mass-flux convection parameterization formulation emerged from these early investigations. The choice of the steady-plume model as a key ingredient of the mass-flux formulation is especially carefully discussed. Some historical lessons are suggested, especially in the light of the current trend of more emphasis on the bubble dynamics as elucidated by high-resolution numerical modeling and laboratory experiments.
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Aerosol optical properties were measured by the DOE/ARM (US Department of Energy Atmospheric Radiation Measurements) Program Mobile Facility during the Two-Column Aerosol Project (TCAP) campaign deployed at Cape Cod, Massachusetts, for a 1-year period (from summer 2012 to summer 2013). Measured optical properties included aerosol light-absorption coefficient (σ<sub>ap</sub>) at low relative humidity (RH) and aerosol light-scattering coefficient (σ<sub>sp</sub>) at low and at RH values varying from 30 to 85%, approximately. Calculated variables included the single scattering albedo (SSA), the scattering Ångström exponent (SAE) and the scattering enhancement factor (<i>f</i>(RH)). Over the period of measurement, <i>f</i>(RH = 80%) had a mean value of 1.9 ± 0.3 and 1.8 ± 0.4 in the PM<sub>10</sub> and PM<sub>1</sub> fractions, respectively. Higher <i>f</i>(RH = 80%) values were observed for wind directions from 0 to 180° (marine sector) together with high SSA and low SAE values. The wind sector from 225 to 315° was identified as an anthropogenically influenced sector, and it was characterized by smaller, darker and less hygroscopic aerosols. For the marine sector, <i>f</i>(RH = 80%) was 2.2 compared with a value of 1.8 obtained for the anthropogenically influenced sector. The air-mass backward trajectory analysis agreed well with the wind sector analysis. It shows low cluster to cluster variability except for air masses coming from the Atlantic Ocean that showed higher hygroscopicity. Knowledge of the effect of RH on aerosol optical properties is of great importance for climate forcing calculations and for comparison of in situ measurements with satellite and remote sensing retrievals. In this sense, predictive capability of <i>f</i>(RH) for use in climate models would be enhanced if other aerosol parameters could be used as proxies to estimate hygroscopic growth. Toward this goal, we propose an exponential equation that successfully estimates aerosol hygroscopicity as a function of SSA at Cape Cod. Further work is needed to determine if the equation obtained is valid in other environments.
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The study presents a long-term statistical trend analysis of total ozone data sets obtained from various satellites. A multi-variate linear regression was applied to annual mean zonal mean data using various natural and anthropogenic explanatory variables that represent dynamical and chemical processes which modify global ozone distributions in a changing climate. The study investigated the magnitude and zonal distribution of the different atmospheric chemical and dynamical factors contributing to long-term total ozone changes. The regression model included the equivalent effective stratospheric chlorine (EESC), the 11-year solar cycle, the quasi-biennial oscillation (QBO), stratospheric aerosol loading describing the effects from major volcanic eruptions, the El Niño–Southern Oscillation (ENSO), the Arctic and Antarctic oscillation (AO/AAO), and accumulated eddy heat flux (EHF), the latter representing changes due to the Brewer–Dobson circulation. The total ozone column data set used here comprises the Solar Backscater Ultraviolet SBUV/SBUV-2 merged ozone data set (MOD) V8.6, the merged data set of the Solar Backscaterr Ultraviolet, the Total Ozone Mapping Spectrometer and the Ozone Monitoring Instrument SBUV/TOMS/OMI (1979–2012) MOD V8.0 and the merged data set of the Global Ozone Monitoring Experiment, the Scanning Imaging Absorption spectroMeter for Atmospheric ChartograpHY and the Global Ozone Monitoring Experiment 2 GOME/SCIAMACHY/GOME-2 (GSG) (1995–2012). The trend analysis was performed for twenty-six 5° wide latitude bands from 65° S to 65° N, and the analysis explained most of the ozone variability to within 70 to 90%. The results show that QBO dominates the ozone variability in the tropics (±7 DU) while at higher latitudes, the dynamical indices, AO/AAO and eddy heat flux, have substantial influence on total ozone variations by up to ±10 DU. The contribution from volcanic aerosols is only prominent during the major eruption periods (El Chichón and Mt. Pinatubo), and together with the ENSO signal, is more evident in the Northern Hemisphere. The signature of the solar cycle covers all latitudes and contributes about 10 DU from solar maximum to solar minimum. EESC is found to be a main contributor to the long-term ozone decline and the trend changes after the end of the 1990s. From the EESC fits, statistically significant upward trends after 1997 were found in the extratropics, which points at the slowing of ozone decline and the onset of ozone recovery. The EESC based trends are compared with the trends obtained from the statistical piecewise linear trend (PWLT) model (known as hockey stick) with a turnaround in 1997 to examine the differences between both approaches. In case of the SBUV merged V8.6 data the EESC and PWLT trends before and after 1997 are in good agreement (within 2 σ), however, the positive post-1997 linear trends from the PWLT regression are not significant within 2 σ. <br><br> A sensitivity study is carried out by comparing the regression results, using SBUV/SBUV-2 MOD V8.6 merged time series (1979–2012) and a merged data set combining SBUV/SBUV-2 (1979–June 1995) and GOME/SCIAMACHY/GOME-2 ("GSG") WFDOAS (Weighting Function DOAS) (July 1995–2012) as well as SBUV/TOMS/OMI MOD V8.0 (1979–2012) in the regression analysis in order to investigate the uncertainty in the long-term trends due to different ozone data sets and data versions. Replacing the late SBUV/SBUV-2 merged data record with GSG data (unscaled and adjusted) leads to very similar results demonstrating the high consistency between satellite data sets. However, the comparison of the new SBUV/SBUV-2 MOD V8.6 with the MOD V8.0 and MOD8.6/GSG data showed somewhat smaller sensitivities with regard to several proxies as well as the linear EESC trends. On the other hand, the PWLT trends after 1997 show some differences, however, within the 2 σ error bars the PWLT trends agree with each other for all three data sets.
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We systematically evaluate the black carbon (BC) simulations for 2006 over the Tibetan Plateau by a global 3-D chemical transport model (CTM) (GEOS-Chem) driven by GEOS-5 assimilated meteorological fields, using in situ measurements of BC in surface air, BC in snow, and BC absorption aerosol optical depth (AAOD). Using improved anthropogenic BC emission inventories for Asia that account for rapid technology renewal and energy consumption growth (Zhang et al., 2009; Lu et al., 2011) and improved global biomass burning emission inventories that account for small fires (van der Werf et al., 2010; Randerson et al., 2012), we find that model results of both BC in surface air and in snow are statistically in good agreement with observations (biases < 15%) away from urban centers. Model results capture the seasonal variations of the surface BC concentrations at rural sites in the Indo-Gangetic Plain, but the observed elevated values in winter are absent. Modeled surface-BC concentrations are within a factor of 2 of the observations at remote sites. Part of the discrepancy is explained by the deficiencies of the meteorological fields over the complex Tibetan terrain. We find that BC concentrations in snow computed from modeled BC deposition and GEOS-5 precipitation are spatiotemporally consistent with observations (<i>r</i> = 0.85). The computed BC concentrations in snow are a factor of 2–4 higher than the observations at several Himalayan sites because of excessive BC deposition. The BC concentrations in snow are biased low by a factor of 2 in the central plateau, which we attribute to the absence of snow aging in the CTM and strong local emissions unaccounted for in the emission inventories. Modeled BC AAOD is more than a factor of 2 lower than observations at most sites, particularly to the northwest of the plateau and along the southern slopes of the Himalayas in winter and spring, which is attributable in large part to underestimated emissions and the assumption of external mixing of BC aerosols in the model. We find that assuming a 50% increase of BC absorption associated with internal mixing reduces the bias in modeled BC AAOD by 57% in the Indo-Gangetic Plain and the northeastern plateau and to the northeast of the plateau, and by 16% along the southern slopes of the Himalayas and to the northwest of the plateau. Both surface BC concentration and AAOD are strongly sensitive to anthropogenic emissions (from China and India), while BC concentration in snow is especially responsive to the treatment of BC aerosol aging. We find that a finer model resolution (0.5° × 0.667° nested over Asia) reduces the bias in modeled surface-BC concentration from 15 to 2%. The large range and non-homogeneity of discrepancies between model results and observations of BC across the Tibetan Plateau undoubtedly undermine current assessments of the climatic and hydrological impact of BC in the region and thus warrant imperative needs for more extensive measurements of BC, including its concentration in surface air and snow, AAOD, vertical profile and deposition.
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Aromatic hydrocarbons are associated with direct adverse human health effects and can have negative impacts on ecosystems due to their toxicity, as well as indirect negative effects through the formation of tropospheric ozone and secondary organic aerosol, which affect human health, crop production and regional climate. Measurements of aromatic hydrocarbons were conducted at the Welgegund measurement station (South Africa), which is considered to be a regionally representative background site. However, the site is occasionally impacted by plumes from major anthropogenic source regions in the interior of South Africa, which include the western Bushveld Igneous Complex (e.g. platinum, base metal and ferrochrome smelters), the eastern Bushveld Igneous Complex (platinum and ferrochrome smelters), the Johannesburg–Pretoria metropolitan conurbation (> 10 million people), the Vaal Triangle (e.g. petrochemical and pyrometallurgical industries), the Mpumalanga Highveld (e.g. coal-fired power plants and petrochemical industry) and also a region of anticyclonic recirculation of air mass over the interior of South Africa. The aromatic hydrocarbon measurements were conducted with an automated sampler on Tenax-TA and Carbopack-B adsorbent tubes with heated inlet for 1 year. Samples were collected twice a week for 2 h during daytime and 2 h during night-time. A thermal desorption unit, connected to a gas chromatograph and a mass selective detector was used for sample preparation and analysis. Results indicated that the monthly median (mean) total aromatic hydrocarbon concentrations ranged between 0.01 (0.011) and 3.1 (3.2) ppb. Benzene levels did not exceed the local air quality standard limit, i.e. annual mean of 1.6 ppb. Toluene was the most abundant compound, with an annual median (mean) concentration of 0.63 (0.89) ppb. No statistically significant differences in the concentrations measured during daytime and night-time were found, and no distinct seasonal patterns were observed. Air mass back trajectory analysis indicated that the lack of seasonal cycles could be attributed to patterns determining the origin of the air masses sampled. Aromatic hydrocarbon concentrations were in general significantly higher in air masses that passed over anthropogenically impacted regions. Inter-compound correlations and ratios gave some indications of the possible sources of the different aromatic hydrocarbons in the source regions defined in the paper. The highest contribution of aromatic hydrocarbon concentrations to ozone formation potential was also observed in plumes passing over anthropogenically impacted regions.
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This study evaluates a deployment strategy of a heavily instrumented mobile lab for characterizing multipollutant spatial patterns based upon a limited number of measurement days spread over different seasons. The measurements obtained through this deployment strategy are used to gain insight into average pollutant levels between routine monitoring sites and in relation to emission sources in the region, as well as to assess correlations between pollutant patterns to better understand the nature of urban air pollutant mixtures. A wide range of locations were part of the deployment in order to characterize the distribution of chronic exposures potentially allowing development of exposure models. Comparison of the mobile lab averages to the available adjacent air quality monitoring network stations to evaluate their representativeness showed that they were in reasonable agreement with the annual averages at the monitoring sites, thus providing some evidence that, through the deployment approach, the mobile lab is able to capture the main features of the average spatial patterns. The differences between mobile lab and network averages varied by pollutant with the best agreement for NO<sub>2</sub> with a percentage difference of 20%. Sharp differences in the average spatial distribution were found to exist between different pollutants on multiple scales, particularly on the sub-urban scale, i.e., the neighborhood to street scales. For example, NO<sub>2</sub> was observed to be 210–265% higher by the main highway in the study region compared to the nearby urban background monitoring site, while black carbon was higher by 180–200% and particle number concentration was 300% higher. The repeated measurements of near-roadway gradients showed that the rate of change differed by pollutant with elevated concentrations detected up to 600–700 m away for some pollutants. These results demonstrate that through systematic deployment mobile laboratory measurements can be used to characterize average or typical concentration patterns, thus providing data to assess monitoring site representativeness, spatial relationships between pollutants, and chronic multipollutant exposure patterns useful for evaluating and developing exposure models for outdoor concentrations in an urban environment.
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The effects of absorbing aerosols on the atmospheric radiation budget and dynamics over the eastern Mediterranean region are studied using satellites and ground-based observations, and radiative transfer model calculations, under summer conditions. Climatology of aerosol optical depth (AOD), single scattering albedo (SSA) and size parameters were analyzed using multi-year (1999–2012) observations from Moderate Resolution Imaging Spectroradiometer (MODIS), Multi-angle Imaging SpectroRadiometer (MISR) and AErosol RObotic NETwork (AERONET). Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP)-derived aerosol vertical distributions and their classifications are used to calculate the AOD of four dominant aerosol types: dust, polluted dust, polluted continental, and marine aerosol over the region. The seasonal mean (June–August 2010) AODs are 0.22 ± 0.02, 0.11 ± 0.04, 0.10 ± 0.04 and 0.06 ± 0.01 for polluted dust, polluted continental, dust and marine aerosol, respectively. Changes in the atmospheric temperature profile as a function of absorbing aerosol loading were derived for the same period using observations from the AIRS satellite. We inferred heating rates in the aerosol layer of ~1.7 ± 0.8 K day<sup>−1</sup> between 925 and 850 hPa, which is attributed to aerosol absorption of incoming solar radiation. Radiative transfer model (RTM) calculations show significant atmospheric warming for dominant absorbing aerosol over the region. A maximum atmospheric forcing of +16.7 ± 7.9 Wm<sup>−2</sup> is calculated in the case of polluted dust, followed by dust (+9.4 ± 4.9 Wm<sup>−2</sup>) and polluted continental (+6.4 ± 4.5 Wm<sup>−2</sup>). RTM-derived heating rate profiles for dominant absorbing aerosol show warming of 0.1–0.9 K day<sup>−1</sup> in the aerosol layer (< 3.0 km altitudes), which primarily depend on AODs of the different aerosol types. Diabatic heating due to absorbing aerosol stabilizes the lower atmosphere, which could significantly reduce the atmospheric ventilation. These conditions can enhance the "pollution pool" over the eastern Mediterranean.
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Mineral dust interacts with incoming/outgoing electromagnetic radiation in the atmosphere. This interaction depends on the microphysical properties of the dust particles, including size, mineral composition, external morphology, and internal structure. Ideally all of these properties should be accounted for in the remote sensing of dust, the modeling of single-scattering properties, and radiative effect assessment. There have been many reports on the microphysical characterizations of mineral dust, but no investigations of the internal structures of individual dust particles. We explored the interiors of Asian dust particles using the combined application of focused ion beam thin-slice preparation and high-resolution transmission electron microscopy. The results showed that individual dust particles consisted of numerous mineral grains, which were organized into several types of internal structure: single and polycrystalline cores of quartz, feldspars, calcite, and amphibole often with oriented clay coatings; individual clay agglomerates of nano-thin clay platelets showing preferred to random orientations common with coarser mineral inclusions; and platy coarse phyllosilicates (muscovite, biotite, and chlorite). Micron to submicron pores were scattered throughout the interior of particles. Clays in the coatings and agglomerates were dominated by nano-thin platelets of the clay minerals of illite–smectite series including illite, smectite, and their mixed layers with subordinate kaolinite and clay-sized chlorite. Submicron iron oxide grains, dominantly goethite, were distributed throughout the clay agglomerates and coatings. Unlike the common assumptions and simplifications, we found that the analyzed dust particles were irregularly shaped with birefringent, polycrystalline, and polymineralic heterogeneous compositions. Accounting for this structural and mineralogical makeup may improve the remote sensing retrieval of dust and the evaluation of radiation effects, but will also require sophisticated single-scattering modeling. In particular, the observed internal structures of dust particles such as clay coatings, preferred orientation, embedded grains in clays, and pores, have the potential to considerably impact on the light scattering by dust particles. The distribution and size of structural components with contrasting dielectric properties, such as iron oxides, should also be explicitly accounted for.
