Aerosol Burden Research Articles

Impacts of emission reductions on aerosol radiative effects

Abstract. The global aerosol–climate model ECHAM-HAMMOZ was used to investigate changes in the aerosol burden and aerosol radiative effects in the coming decades. Four different emissions scenarios were applied for 2030 (two of them applied also for 2020) and the results were compared against the reference year 2005. Two of the scenarios are based on current legislation reductions: one shows the maximum potential of reductions that can be achieved by technical measures, and the other is targeted to short-lived climate forcers (SLCFs). We have analyzed the results in terms of global means and additionally focused on eight subregions. Based on our results, aerosol burdens show an overall decreasing trend as they basically follow the changes in primary and precursor emissions. However, in some locations, such as India, the burdens could increase significantly. The declining emissions have an impact on the clear-sky direct aerosol effect (DRE), i.e. the cooling effect. The DRE could decrease globally 0.06–0.4 W m−2 by 2030 with some regional increases, for example, over India (up to 0.84 W m−2). The global changes in the DRE depend on the scenario and are smallest in the targeted SLCF simulation. The aerosol indirect radiative effect could decline 0.25–0.82 W m−2 by 2030. This decrease takes place mostly over the oceans, whereas the DRE changes are greatest over the continents. Our results show that targeted emission reduction measures can be a much better choice for the climate than overall high reductions globally. Our simulations also suggest that more than half of the near-future forcing change is due to the radiative effects associated with aerosol–cloud interactions.

Altitude‐resolved shortwave and longwave radiative effects of desert dust in the Mediterranean during the GAMARF campaign: Indications of a net daily cooling in the dust layer

AbstractDesert dust interacts with shortwave (SW) and longwave (LW) radiation, influencing the Earth radiation budget and the atmospheric vertical structure. Uncertainties on the dust role are large in the LW spectral range, where few measurements are available and the dust optical properties are not well constrained. The first airborne measurements of LW irradiance vertical profiles over the Mediterranean were carried out during the Ground‐based and Airborne Measurements of Aerosol Radiative Forcing (GAMARF) campaign, which took place in spring 2008 at the island of Lampedusa. The experiment was aimed at estimating the vertical profiles of the SW and LW aerosol direct radiative forcing (ADRF) and heating rates (AHR), taking advantage of vertically resolved measurements of irradiances, meteorological parameters, and aerosol microphysical and optical properties. Two cases, characterized respectively by the presence of a homogeneous dust layer (3 May, with aerosol optical depth, AOD, at 500 nm of 0.59) and by a low aerosol burden (5 May, with AOD of 0.14), are discussed. A radiative transfer model was initialized with the measured vertical profiles and with different aerosol properties, derived from measurements or from the literature. The simulation of the irradiance vertical profiles, in particular, provides the opportunity to constrain model‐derived estimates of the AHR. The measured SW and LW irradiances were reproduced when the model was initialized with the measured aerosol size distributions and refractive indices. For the dust case, the instantaneous (solar zenith angle, SZA, of 55.1°) LW‐to‐SW ADRF ratio was 23% at the surface and 11% at the top of the atmosphere (TOA), with a more significant LW contribution on a daily basis (52% at the surface and 26% at TOA), indicating a relevant reduction of the SW radiative effects. The AHR profiles followed the aerosol extinction profile, with comparable peaks in the SW (0.72 ± 0.11 K d−1) and in the LW (−0.52 ± 0.12 K d−1) for the considered SZA. On a daily basis, the absolute value of the heating rate was larger in the LW than in the SW, producing a net cooling effect at specific levels. These are quite unexpected results, emphasizing the important role of LW radiation.

Direct night-time ejection of particle-phase reduced biogenic sulfur compounds from the ocean to the atmosphere.

The influence of oceanic biological activity on sea spray aerosol composition, clouds, and climate remains poorly understood. The emission of organic material and gaseous dimethyl sulfide (DMS) from the ocean represents well-documented biogenic processes that influence particle chemistry in marine environments. However, the direct emission of particle-phase biogenic sulfur from the ocean remains largely unexplored. Here we present measurements of ocean-derived particles containing reduced sulfur, detected as elemental sulfur ions (e.g., (32)S(+), (64)S2(+)), in seven different marine environments using real-time, single particle mass spectrometry; these particles have not been detected outside of the marine environment. These reduced sulfur compounds were associated with primary marine particle types and wind speeds typically between 5 and 10 m/s suggesting that these particles themselves are a primary emission. In studies with measurements of seawater properties, chlorophyll-a and atmospheric DMS concentrations were typically elevated in these same locations suggesting a biogenic source for these sulfur-containing particles. Interestingly, these sulfur-containing particles only appeared at night, likely due to rapid photochemical destruction during the daytime, and comprised up to ∼67% of the aerosol number fraction, particularly in the supermicrometer size range. These sulfur-containing particles were detected along the California coast, across the Pacific Ocean, and in the southern Indian Ocean suggesting that these particles represent a globally significant biogenic contribution to the marine aerosol burden.

Evaluation of the global aerosol microphysical ModelE2-TOMAS model against satellite and ground-based observations

Abstract. The TwO-Moment Aerosol Sectional (TOMAS) microphysics model has been integrated into the state-of-the-art general circulation model, GISS ModelE2. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the ModelE2-TOMAS model is compared to the default aerosol model in ModelE2, which is a one-moment aerosol (OMA) model (i.e. no aerosol microphysics). Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement (mostly within a factor of 2) with observations of sulfur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as ModelE2-OMA) cannot capture the observed vertical distribution of sulfur dioxide over the Pacific Ocean, possibly due to overly strong convective transport and overpredicted precipitation. The ModelE2-TOMAS model simulates observed aerosol number concentrations and cloud condensation nuclei concentrations roughly within a factor of 2. Anthropogenic aerosol burdens in ModelE2-OMA differ from ModelE2-TOMAS by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. We observed larger differences for naturally emitted aerosols such as sea salt and mineral dust, as those emission rates are quite different due to different upper size cutoff assumptions.

Characterization of primary and secondary wood combustion products generated under different burner loads

Abstract. Residential wood burning contributes to the total atmospheric aerosol burden; however, large uncertainties remain in the magnitude and characteristics of wood burning products. Primary emissions are influenced by a variety of parameters, including appliance type, burner wood load and wood type. In addition to directly emitted particles, previous laboratory studies have shown that oxidation of gas-phase emissions produces compounds with sufficiently low volatility to readily partition to the particles, forming considerable quantities of secondary organic aerosol (SOA). However, relatively little is known about wood burning SOA, and the effects of burn parameters on SOA formation and composition are yet to be determined. There is clearly a need for further study of primary and secondary wood combustion aerosols to advance our knowledge of atmospheric aerosols and their impacts on health, air quality and climate. For the first time, smog chamber experiments were conducted to investigate the effects of wood loading on both primary and secondary wood combustion products. Products were characterized using a range of particle- and gas-phase instrumentation, including an aerosol mass spectrometer (AMS). A novel approach for polycyclic aromatic hydrocarbon (PAH) quantification from AMS data was developed and results were compared to those from GC-MS analysis of filter samples. Similar total particle mass emission factors were observed under high and average wood loadings; however, high fuel loadings were found to generate significantly higher contributions of PAHs to the total organic aerosol (OA) mass compared to average loadings. PAHs contributed 15 ± 4% (mean ±2 sample standard deviations) to the total OA mass in high-load experiments, compared to 4 ± 1% in average-load experiments. With aging, total OA concentrations increased by a factor of 3 ± 1 for high load experiments compared to 1.6 ± 0.4 for average-load experiments. In the AMS, an increase in PAH and aromatic signature ions at lower m / z values, likely fragments from larger functionalized PAHs, was observed with aging. Filter samples also showed an increase in functionalized PAHs in the particles with aging, particularly oxidized naphthalene species. As PAHs and their oxidation products are known to have deleterious effects on health, this is a noteworthy finding to aid in the mitigation of negative wood burning impacts by improving burner operation protocols.

A new Geoengineering Model Intercomparison Project (GeoMIP) experiment designed for climate and chemistry models

Abstract. A new Geoengineering Model Intercomparison Project (GeoMIP) experiment "G4 specified stratospheric aerosols" (short name: G4SSA) is proposed to investigate the impact of stratospheric aerosol geoengineering on atmosphere, chemistry, dynamics, climate, and the environment. In contrast to the earlier G4 GeoMIP experiment, which requires an emission of sulfur dioxide (SO2) into the model, a prescribed aerosol forcing file is provided to the community, to be consistently applied to future model experiments between 2020 and 2100. This stratospheric aerosol distribution, with a total burden of about 2 Tg S has been derived using the ECHAM5-HAM microphysical model, based on a continuous annual tropical emission of 8 Tg SO2 yr−1. A ramp-up of geoengineering in 2020 and a ramp-down in 2070 over a period of 2 years are included in the distribution, while a background aerosol burden should be used for the last 3 decades of the experiment. The performance of this experiment using climate and chemistry models in a multi-model comparison framework will allow us to better understand the impact of geoengineering and its abrupt termination after 50 years in a changing environment. The zonal and monthly mean stratospheric aerosol input data set is available at https://www2.acd.ucar.edu/gcm/geomip-g4-specified-stratospheric-aerosol-data-set.

Global atmospheric sulfur budget under volcanically quiescent conditions: Aerosol‐chemistry‐climate model predictions and validation

AbstractThe global atmospheric sulfur budget and its emission dependence have been investigated using the coupled aerosol‐chemistry‐climate model SOCOL‐AER. The aerosol module comprises gaseous and aqueous sulfur chemistry and comprehensive microphysics. The particle distribution is resolved by 40 size bins spanning radii from 0.39 nm to 3.2 μm, including size‐dependent particle composition. Aerosol radiative properties required by the climate model are calculated online from the aerosol module. The model successfully reproduces main features of stratospheric aerosols under nonvolcanic conditions, including aerosol extinctions compared to Stratospheric Aerosol and Gas Experiment II (SAGE II) and Halogen Occultation Experiment, and size distributions compared to in situ measurements. The calculated stratospheric aerosol burden is 109 Gg of sulfur, matching the SAGE II‐based estimate (112 Gg). In terms of fluxes through the tropopause, the stratospheric aerosol layer is due to about 43% primary tropospheric aerosol, 28% SO2, 23% carbonyl sulfide (OCS), 4% H2S, and 2% dimethyl sulfide (DMS). Turning off emissions of the short‐lived species SO2, H2S, and DMS shows that OCS alone still establishes about 56% of the original stratospheric aerosol burden. Further sensitivity simulations reveal that anticipated increases in anthropogenic SO2 emissions in China and India have a larger influence on stratospheric aerosols than the same increase in Western Europe or the U.S., due to deep convection in the western Pacific region. However, even a doubling of Chinese and Indian emissions is predicted to increase the stratospheric background aerosol burden only by 9%. In contrast, small to moderate volcanic eruptions, such as that of Nabro in 2011, may easily double the stratospheric aerosol loading.

Injection of mineral dust into the free troposphere during fire events observed with polarization lidar at Limassol, Cyprus

Abstract. Four-year observations (2010–2014) with EARLINET polarization lidar and AERONET sun/sky photometer at Limassol (34.7° N, 33° E), Cyprus, were used to study the soil dust content in lofted fire smoke plumes advected from Turkey. This first systematic attempt to characterize less than 3-day-old smoke plumes in terms of particle linear depolarization ratio (PDR), measured with lidar, contributes to the more general effort to properly describe the life cycle of free-tropospheric smoke–dust mixtures from the emission event to phases of long-range transport (> 4 days after emission). We found significant PDR differences with values from 9 to 18% in lofted aerosol layers when Turkish fires contributed to the aerosol burden and of 3–13 % when Turkish fires were absent. High Ångström exponents of 1.4–2.2 during all these events with lofted smoke layers, occurring between 1 and 3 km height, suggest the absence of a pronounced particle coarse mode. When plotted vs. travel time (spatial distance between Limassol and last fire area), PDR decreased strongly from initial values around 16–18% (1 day travel) to 4–8% after 4 days of travel caused by deposition processes. This behavior was found to be in close agreement with findings described in the literature. Computation of particle extinction coefficient and mass concentrations, derived from the lidar observations, separately for fine-mode dust, coarse-mode dust, and non-dust aerosol components show extinction-related dust fractions on the order of 10% (for PDR =4%, travel times > 4 days) and 50% (PDR =15%, 1 day travel time) and respective mass-related dust fractions of 25% (PDR =4%) to 80% (PDR =15%). Biomass burning should therefore be considered as another source of free tropospheric soil dust.

Non-sulfate sulfur in fine aerosols across the United States: Insight for organosulfate prevalence

We investigated the discrepancies in long-term sulfur measurements from 2000 to 2012 by two separate speciation methods, X-ray fluorescence (XRF) spectroscopy and ion chromatography (IC) across the United States (334 sites). Overall, there was a good correlation between sulfur measurements by XRF spectroscopy and IC (R ≥ 0.90 for most of the sites). However, the inorganic sulfate measured by ion chromatography was not sufficient to account for all the sulfur measured by XRF spectroscopy at many of the sites. Discrepancies were observed with the high ratios of sulfur measured by XRF spectroscopy to that by IC. Such high ratios also exhibited seasonal variation, and differed across land use types; significant differences occurred at locations classified as forest, agriculture, and mobile, but not in locations classified as commercial, desert, industrial, and residential. On average, the excess, or non-sulfate, sulfur (unmeasured organic sulfur or other inorganic species of sulfur) was variable and observed as high as ∼13% of organic carbon and ∼2% of PM2.5. The contribution of such assumed organosulfur was larger in the eastern region than other geographical locations in the United States. Besides the temporal and spatial trends, the additional sulfur was found to be related to other factors such as aerosol acidity and emission sources. The results suggest that these unmeasured sulfur species could have significant contribution to aerosol burden, and the understanding of these could help to control PM2.5 levels and to assess other effects of sulfur aerosols.

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

Abstract. We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41° N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere.

Systematic satellite observations of the impact of aerosols from passive volcanic degassing on local cloud properties

Abstract. The impact of volcanic emissions, especially from passive degassing and minor explosions, is a source of uncertainty in estimations of aerosol indirect effects. Observations of the impact of volcanic aerosol on clouds contribute to our understanding of both present-day atmospheric properties and of the pre-industrial baseline necessary to assess aerosol radiative forcing. We present systematic measurements over several years at multiple active and inactive volcanic islands in regions of low present-day aerosol burden. The time-averaged indirect aerosol effects within 200 km downwind of island volcanoes are observed using Moderate Resolution Imaging Spectroradiometer (MODIS, 2002–2013) and Advanced Along-Track Scanning Radiometer (AATSR, 2002–2008) data. Retrievals of aerosol and cloud properties at Kīlauea (Hawai'i), Yasur (Vanuatu) and Piton de la Fournaise (la Réunion) are rotated about the volcanic vent to be parallel to wind direction, so that upwind and downwind retrievals can be compared. The emissions from all three volcanoes – including those from passive degassing, Strombolian activity and minor explosions – lead to measurably increased aerosol optical depth downwind of the active vent. Average cloud droplet effective radius is lower downwind of the volcano in all cases, with the peak difference ranging from 2–8 μm at the different volcanoes in different seasons. Estimations of the difference in Top of Atmosphere upward Short Wave flux upwind and downwind of the active volcanoes from NASA's Clouds and the Earth's Radiant Energy System (CERES) suggest a downwind elevation of between 10 and 45 Wm−2 at distances of 150–400 km from the volcano, with much greater local (< 80 km) effects. Comparison of these observations with cloud properties at isolated islands without degassing or erupting volcanoes suggests that these patterns are not purely orographic in origin. Our observations of unpolluted, isolated marine settings may capture processes similar to those in the pre-industrial marine atmosphere.

Reflective ‘cool’ roofs under aerosol-burdened skies: radiative benefits across selected Indian cities

The use of reflective surfaces offers one low-cost solution for reducing solar loading to urban environments and the Earth that should be considered as part of sustainable urban design. Here, we characterize the radiative benefits, i.e. the additional shortwave radiation leaving the atmosphere, from the installation of highly reflective ‘cool’ roofs in urban areas in India that face relatively large local aerosol burdens. We use a previously tested column radiative transfer model to estimate the energy per unit area reflected to space from increasing the surface albedo at six cities within India. The model is used to characterize radiative transfer each day over five years (2008–2012) based on mid-day satellite retrievals of MODIS aerosol depth, cloud water path, and average surface albedo and MERRA atmospheric profiles of temperature and composition. Compared against ten months of field observations in two cities, the model derived incoming surface shortwave radiation estimates relative to observations show small biases (0.5% and −2.6%, at Pantnagar and Nainital, respectively). Despite the high levels of local aerosols we found cool roofs provided significant radiative benefits at all locations. Averaged over the five year period we found that increasing the albedo of 1 m2 of roof area by 0.5 would reflect to space 0.9–1.2 kWh daily from 08:30–15:30 LST, depending on location. This is equivalent to a constant forcing of 37–50 W m−2 (equivalent to reducing CO2 emissions by 74 to 101 kg CO2 m−2 roof area). Last, we identify a co-benefit of improving air quality, in that removing aerosols from the atmosphere could increase the radiative benefits from cool roofs by 23–74%, with the largest potential increase found at Delhi and the smallest change found at Nainital.

Can satellite-derived aerosol optical depth quantify the surface aerosol radiative forcing?

Aerosols play an important role in the climate of the Earth through aerosol radiative forcing (ARF). Nowadays, aerosol particles are detected, quantified and monitored by remote sensing techniques using low Earth orbit (LEO) and geostationary (GEO) satellites. In the present article, the use of satellite-derived AOD (aerosol optical depth) products is investigated in order to quantify on a daily basis the ARF at the surface level (SARF). By daily basis we mean that an average SARF value is computed every day based upon the available AOD satellite measurements for each station. In the first part of the study, the performance of four state-of-art different AOD products (MODIS-DT, MODIS-DB, MISR, and SEVIRI) is assessed through comparison against ground-based AOD measurements from 24 AERONET stations located in Europe and Africa during a 6-month period. While all AOD products are found to be comparable in terms of measured value (RMSE of 0.1 for low and average AOD values), a higher number of AOD estimates is made available by GEO satellites due to their enhanced frequency of scan. Experiments show a general lower agreement of AOD estimates over the African sites (RMSE of 0.2), which show the highest aerosol concentrations along with the occurrence of dust aerosols, coarse particles, and bright surfaces. In the second part of this study, the lessons learned about the confidence in aerosol burden derived from satellites are used to estimate SARF under clear sky conditions. While the use of AOD products issued from GEO observations like SEVIRI brings improvement in the SARF estimates with regard to LEO-based AOD products, the resulting absolute bias (13W/m2 in average when AERONET AOD is used as reference) is judged to be still high in comparison with the average values of SARF found in this study (from −25W/m2 to −43W/m2) and also in the literature (from −10W/m2 to −47W/m2).

Observational evidence of fire-driven reduction of cloud fraction in tropical Africa

Anthopogenic savanna fires in sub-Saharan Africa emit smoke that affects cloudiness in the region. We measured the cloud response to fire aerosols using aerosol data from the Multi-angle Imaging SpectroRadiometer (MISR) and cloud fraction data from the morning and afternoon overpasses of the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument. Considering the same cloud scene from the morning and afternoon satellite observations allowed us to observe the temporal relationship between clouds and aerosols. Level 2 data from 35 individual scenes during the fire season (December) between 2006 and 2010 were analyzed to quantify changes in MODIS cloud fraction from morning (10:30 A.M. local time) to afternoon (1:30 P.M. local time) in the presence of different morning aerosol burdens (from MISR). We controlled for the local meteorology by analyzing scenes from November, when fire activity and aerosol optical depth were low but cloud fraction and meteorological variables (boundary layer height, pressure, total column water vapor, temperature, and convective available potential energy) were similar to those of the fire season. High-fire-driven aerosol optical depth (AOD) was associated with reduced cloud fraction in both the raw and meteorologically normalized data. Fire aerosols reduced the relative cloud fraction in all sky conditions, but the effects were progressively larger in high-AOD conditions. These results may provide observational evidence of the semidirect cloud decimation effect in tropical regions and suggest a positive feedback loop between anthropogenic burning and cloudiness—where more aerosols lead to decreased clouds, increased surface exposure and drying, more fire, and thus more aerosols—which is consistent with previous studies linking smoke aerosols to reduced cloudiness and vice versa.

Contrasting the direct radiative effect and direct radiative forcing of aerosols

Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.

Investigating the coupling between phytoplankton biomass, aerosol optical depth and sea-ice cover in the Greenland Sea

We investigate the relationship between satellite-derived time series for microalgal biomass, measured using remotely sensed chlorophyll-a (CHL: mgm−3), aerosol optical depth (AOD) and sea ice cover (ICE) in the Greenland Sea (10° W–10° E, 65–80° N) over the decadal period 2003–2012. Zonal averages for all variables were computed in 5-degree latitude bands. Unlike other regions of the Arctic Ocean, the marginal ice zone in the Greenland Sea is confined to north of 75° N. The CHL time series is characterized by high interannual variability, especially in the northern marginal sea ice zone (MIZ) where variability in sea ice extent is a likely factor. The ten-year climatology shows that CHL increases from March, reaching a seasonal peak in May in the southern sector and in June in the northern sectors. The climatological peak of AOD is achieved in April in all latitude bands, about a month before the peak in CHL. This suggests that the Arctic aerosol burden is strongly affected by continental sources in early spring.Interestingly, a summer increase in AOD (which succeeds the CHL maximum) is seen in some years. Sea ice extent in early spring is less than 40% in the northern sector in all years. There is considerable interannual variability in both the onset of melt and the extent of sea ice loss during summer, with the minimum summer sea ice extent decreasing to almost zero in five of the years. Cross-correlation analyses of the three times series identify a statistically significant relation between CHL and AOD in six of the years in the southern sector, but no correlation between CHL and ICE was found in the northern sector. There is, however, a significant correlation between AOD and ICE time series in the northern sector in four years. High AOD values registered in early spring are most likely of anthropogenic origin, however, peaks later in summer coincident with the phytoplankton bloom and high emissions of biogenic aerosol precursors such as dimethylsulfide and other primary aerosols of marine origin, suggest the summer atmospheric aerosol burden is likely influenced by biogenic emissions.

Modifications of the quasi‐biennial oscillation by a geoengineering perturbation of the stratospheric aerosol layer

AbstractThis paper examines the impact of geoengineering via stratospheric sulfate aerosol on the quasi‐biennial oscillation (QBO) using the NASA Goddard Earth Observing System version 5 Chemistry Climate Model. We performed four 30 year simulations with a continuous injection of sulfur dioxide on the equator at 0° longitude. The four simulations differ by the amount of sulfur dioxide injected (5 Tg/yr and 2.5 Tg/yr) and the altitude of the injection (16 km–25 km and 22 km–25 km). We find that such an injection dramatically alters the quasi‐biennial oscillation, prolonging the phase of easterly shear with respect to the control simulation. This is caused by the increased aerosol heating and associated warming in the tropical lower stratosphere and higher residual vertical velocity. In the case of maximum perturbation, i.e., highest stratospheric aerosol burden, the lower tropical stratosphere is locked into a permanent westerly QBO phase.

Assessment of the effect of air pollution controls on trends in shortwave radiation over the United States from 1995 through 2010 from multiple observation networks

Abstract. Long-term data sets of all-sky and clear-sky downwelling shortwave (SW) radiation, cloud cover fraction, and aerosol optical depth (AOD) were analyzed together with surface concentrations from several networks (e.g., Surface Radiation Budget Network (SURFRAD), Clean Air Status and Trend Network (CASTNET), Interagency Monitoring of Protection Visual Environments (IMPROVE) and Atmospheric Radiation Measurement (ARM)) in the United States (US). Seven states with varying climatology were selected to better understand the effects of aerosols and clouds on SW radiation. This analysis aims to assess the effects of reductions in anthropogenic aerosol burden resulting from substantial reductions in emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx) over the past 16 yr across the US, based on trends in SW radiation. The SO2 and NOx emission data show decreasing trends from 1995 to 2010, which indirectly validates the effects of the Clean Air Act (CAA) in the US. Meanwhile, the total column AOD and surface total PM2.5 observations also show decreasing trends in the eastern US but slightly increasing trends in the western US. Moreover, measured surface concentrations of several other pollutants (i.e., SO2, SO4 and NOx) have similar behavior to AOD and total PM2.5. Analysis of the observed data shows strong increasing trends in all-sky downwelling SW radiation with decreasing trends in cloud cover. However, since observations of both all-sky direct and diffuse SW radiation show increasing trends, there may be other factors contributing to the radiation trends in addition to the decreasing trends in overall cloud cover. To investigate the role of direct radiative effects of aerosols, clear-sky downwelling radiation is analyzed so that cloud effects are eliminated. However, similar increasing trends in clear-sky total and diffuse SW radiation are observed. While significantly decreasing trends in AOD and surface PM2.5 concentrations along with increasing SW radiation (both all-sky and clear-sky) in the eastern US during 1995–2010 imply the occurrence of direct aerosol mediated "brightening", the increasing trends of both all-sky and clear-sky diffuse SW radiation contradicts this conclusion since diffuse radiation would be expected to decrease as aerosols direct effects decrease and cloud cover decreases. After investigating several confounding factors, the increasing trend in clear-sky diffuse SW may be due to more high-level cirrus from increasing air traffic over the US. The clear-sky radiation observations in the western US also show indications of "brightening" even though the AOD, PM2.5 and surface concentration do not vary drastically. This outcome was not unexpected because the CAA controls were mainly aimed at reducing air pollutant emissions in the eastern US and air pollutant levels in the western US were much lower at the onset. This suggests other factors affect the "brightening" especially in the western US.

The role of low volatile organics on secondary organic aerosol formation

Abstract. Large-scale atmospheric models, which typically describe secondary organic aerosol (SOA) formation based on chamber experiments, tend to systematically underestimate observed organic aerosol burdens. Since SOA constitutes a significant fraction of atmospheric aerosol, this discrepancy translates into an underestimation of SOA contribution to radiative forcing of atmospheric aerosol. Here we show that the underestimation of SOA yields can be partly explained by wall losses of SOA forming compounds during chamber experiments. We present a chamber experiment where α-pinene and ozone are injected into a Teflon chamber. When these two compounds react, we observe rapid formation and growth of new particles. Theoretical analysis of this formation and growth event indicates rapid formation of oxidized volatile organic compounds (OVOC) of very low volatility in the chamber. If these oxidized organic compounds form in the gas phase, their wall losses will have significant implications on their partitioning between the gas and particle phase. Although these OVOCs of very low volatility contribute to the growth of new particles, their mass will almost completely be depleted to the chamber walls during the experiment, while the depletion of OVOCs of higher volatilities is less efficient. According to our model simulations, the volatilities of OVOC contributing to the new particle formation event can be of the order of 10−5 μg m−3.

Seasonal variations of anhydrosugars in PM2.5 in the Pearl River Delta Region, China

Anhydrosugars including levoglucosan and mannosan are the most effective organic tracers for biomass burning aerosol in the atmosphere. In this study, to investigate the contribution of biomass burning emissions to the aerosol burden in the Pearl River Delta (PRD) region, China, 24-hour integrated PM2.5 samples were collected simultaneously at four locations, (i) Guangzhou (GZ), (ii) Zhaoqing (ZQ) in Guangdong province, (iii) Hok Tsui (HT) and (iv) Hong Kong Polytechnic University (PU) in Hong Kong, in four seasons between 2006 and 2007. Levoglucosan and mannosan, together with water-soluble inorganic ions and water-soluble organic carbon (WSOC), were determined to elucidate the seasonal and spatial variations in biomass burning contributions. The concentrations of levoglucosan and mannosan were on average 82.4±123 and 5.8±8.6 ng m−3, respectively. The WSOC concentrations ranged from 0.2 to 9.4 µg m−3, with an average of 2.1±1.6 µg m−3. The relative contributions of biomass burning emissions to OC were 33% in QZ, 12% in GZ, 4% at PU and 5% at HT, respectively, estimated by the measured levoglucosan to organic carbon ratio (LG/OC) relative to literature-derived LG/OC values. The contributions from biomass burning emissions were in general 1.7–2.8 times higher in winter than those in other seasons. Further, it was inferred from diagnostic tracer ratios that a significant fraction of biomass burning emissions was derived from burning of hard wood and likely also from field burning of agricultural residues, such as rice straw, in the PRD region. Our results highlight the contributions from biomass/biofuel burning activities on the regional aerosol budget in South China.