Enhancement Of Aerosol Optical Depth Research Articles

Optical Properties of Boundary Layer Aerosols From High Spectral Resolution Lidar Measurements in a Polluted Urban Environment (Seoul, Korea)

AbstractContinuous measurements of aerosol extinction coefficient (σext) from the High Spectral Resolution Lidar (HSRL) in Seoul from 2016 to 2018 were used to investigate the diurnal variation of the aerosol optical depth (AOD). Nighttime AOD displayed a larger mean and standard deviation (0.45 ± 0.47) than daytime (0.40 ± 0.29). Hygroscopic growth of aerosols under humid conditions was a key factor in the relative enhancement of nighttime AOD. Taking advantage of the HSRL's vertically resolved measurements, the contribution of aerosols within the boundary layer (BL) and free troposphere (FT) to AOD and its temporal variation were investigated. Unlike the diurnal AOD variation, AOD within the BL (AODBL) showed similar diurnal variations with the mixing layer height (MLH), displaying lower nighttime values with a peak around 14–15 local standard time. However, the low correlation between MLH and AODBL (R2 = 0.06) implied that MLH was not the sole deterministic factor of AODBL. A larger AOD of FT aerosols (AODFT) was observed during spring due to frequent elevated dust layers. Using mean σext within the BL and surface PM10 concentrations, the mass extinction efficiency (MEE) of aerosols in Seoul was estimated. The PM10 MEE showed a mean of 5.40 g m−2 and displayed significant variability by PM2.5 to PM10 ratio, season, and ambient relative humidity. The uncertainty of estimated surface PM10 concentrations was minimized when the seasonality and humidity factor in MEE were taken into account (the normalized mean bias decreased from 10.6%, using a single MEE value, to 6.2%).

The Role of Midlatitude Cyclones in the Emission, Transport, Production, and Removal of Aerosols in the Northern Hemisphere

AbstractWe examine the distribution of aerosol optical depth (AOD) across 27,707 northern hemisphere (NH) midlatitude cyclones for 2005–2018 using retrievals from the Moderate Resolution Spectroradiometer (MODIS) sensor on the Aqua satellite. Cyclone‐centered composites show AOD enhancements of 20%–45% relative to background conditions in the warm conveyor belt (WCB) airstream. Fine mode AOD accounts for 68% of this enhancement annually. Relative to background conditions, coarse mode AOD is enhanced by more than a factor of two near the center of the composite cyclone, co‐located with high surface wind speeds. Within the WCB, MODIS AOD maximizes in spring, with a secondary maximum in summer. Cyclone‐centered composites of AOD from the Modern Era Retrospective analysis for Research and Applications, version 2 Global Modeling Initiative (M2GMI) simulation reproduce the magnitude and seasonality of the MODIS AOD composites and enhancements. M2GMI simulations show that the AOD enhancement in the WCB is dominated by sulfate (37%) and organic aerosol (25%), with dust and sea salt each accounting for 15%. MODIS and M2GMI AOD are 60% larger in North Pacific WCBs compared to North Atlantic WCBs and show a strong relationship with anthropogenic pollution. We infer that NH midlatitude cyclones account for 355 Tg yr−1 of sea salt aerosol emissions annually, or 60% of the 30–80°N total. We find that deposition within WCBs is responsible for up to 35% of the total aerosol deposition over the NH ocean basins. Furthermore, the cloudy environment of WCBs leads to efficient secondary sulfate production.

Impacts of Aerosol Loading in the Hindu Kush Himalayan Region Based on MERRA-2 Reanalysis Data

The impacts of climate change have severely affected geosphere, biosphere and cryosphere ecosystems in the Hindu Kush Himalayan (HKH) region. The impact has been accelerating further during the last few decades due to rapid increase in anthropogenic activities such as modernization, industrialization and urbanization, along with energy demands. In view of this, the present work attempts to examine aerosol optical depth (AOD) over the HKH region using the long-term homogeneous MERRA-2 reanalysis data from January, 1980 to December, 2020. The AOD trends are examined statistically with student’s t-test (t). Due to a vast landmass, fragile topography and harsh climatic conditions, we categorized the HKH region into three sub-regions, namely, the northwestern and Karakoram (HKH1), the Central (HKH2) and the southeastern Himalaya and Tibetan Plateau (HKH3). Among the sub-regions, the significant enhancement of AOD is observed at several potential sites in the HKH2 region, namely, Pokhara, Nainital, Shimla and Dehradun by 55.75 × 10−4 ± 3.76 × 10−4, 53.15 × 10−4 ± 3.94 × 10−4, 51.53 × 10−4 ± 4.99 × 10−4 and 39.16 × 10−4 ± 4.08 × 10−4 AOD year−1 (550 nm), respectively, with correlation coefficients (Rs) of 0.86 to 0.93. However, at a sub-regional scale, HKH1, HKH2 and HKH3 exhibit 23.33 × 10−4 ± 2.28 × 10−4, 32.20 × 10−4 ± 2.58 × 10−4 and 9.48 × 10−4 ± 1.21 × 10−4 AOD year−1, respectively. The estimated trends are statistically significant (t > 7.0) with R from 0.81 to 0.91. Seasonally, the present study also shows strong positive AOD trends at several potential sites located in the HKH2 region, such as Pokhara, Nainital, Shimla and Dehradun, with minimum 19.81 × 10−4 ± 3.38 × 10−4 to maximum 72.95 × 10−4 ± 4.89 × 10−4 AOD year−1 with statistical significance. In addition, there are also increasing AOD trends at all the high-altitude background sites in all seasons.

Radiative Impacts of Aerosols During COVID-19 Lockdown Period Over the Indian Region

The COVID-19 lockdown restrictions influenced global atmospheric aerosols. We report aerosol variations over India using multiple remote sensing datasets [Moderate Resolution Imaging Spectroradiometer (MODIS), Ozone Monitoring Instrument (OMI), Cloud-Aerosol Lidar, and Infrared Pathfinder (CALIPSO)], and model reanalysis [Copernicus Atmosphere Monitoring Service (CAMS)] during the lockdown implemented during the COVID-19 pandemic outbreak period from March 25 to April 14, 2020. Our analysis shows that, during this period, MODIS and CALIPSO showed a 30–40% reduction in aerosol optical depth (AOD) over the Indo-Gangetic Plain (IGP) with respect to decadal climatology (2010–2019). The absorbing aerosol index and dust optical depth measurements also showed a notable reduction over the Indian region, highlighting less emission of anthropogenic dust and also a reduced dust transport from West Asia during the lockdown period. On the contrary, central India showed an ∼12% AOD enhancement. CALIPSO measurements revealed that this increase was due to transported biomass burning aerosols. Analysis of MODIS fire data product and CAMS fire fluxes (black carbon, SO2, organic carbon, and nitrates) showed intense fire activity all over India but densely clustered over central India. Thus, we show that the lockdown restrictions implemented at the government level have significantly improved the air quality over northern India but fires offset its effects over central India. The biomass-burning aerosols formed a layer near 2–4 km (AOD 0.08–0.1) that produced heating at 3–4 K/day and a consequent negative radiative forcing at the surface of ∼−65 W/m2 (±40 W/m2) over the central Indian region.

Long term trend in aerosol direct radiative effects over Indian Ocean region from multi- satellite observations

ABSTRACT Long-term (2000–2020) trend in aerosol optical depth (AOD) and the associated radiative effect over Indian Ocean region (Arabian Sea and Bay of Bengal) during winter time south Asian outflow is investigated using multi-satellite data. Analysis revealed a statistically significant increasing trend of ~0.01 year−1 over the study regions. This study revealed that aerosols are confined within 2 km from ocean surface, and the trend in columnar AOD is significantly modulated by aerosol loading at higher altitudes. Although there has been no significant change in aerosol direct radiative forcing efficiency, the significant enhancement in AOD over the study region has induced an increase in cooling at the top of the atmosphere by ~0.1 to 0.2 W m−2 year−1.

Investigating the aerosol optical depth variation during a persisting mass gathering event of Kumbh-2019 in India

The Kumbh mela is a huge public gathering event in Hindu tradition. During 2019 Kumbh which was organized at Prayagraj/Allahabad, India, large infrastructure was created to facilitate the visitors. To monitor impact of such gathering and infrastructure on the atmospheric composition, a road campaign was conducted from Nagpur (21.15 N, 79.03 E) to Prayagraj (25.42 N, 81.87 E) during 17–23 February 2019 with a hand-held microtop sun photometer as a primary instrument. Data revealed AOD variation to be higher by about 19% at the centre of the event. The derived angstrom exponent suggests that the mass gathering and large infrastructure may have raised the dust level in the ambient atmosphere which was reflected in the enhanced Aerosol optical depth values and size distribution.

Influence of cloud, fog, and high relative humidity during pollution transport events in South Korea: Aerosol properties and PM2.5 variability

Abstract This investigation examines aerosol dynamics during major fine mode aerosol transboundary pollution events in South Korea primarily during the KORUS-AQ campaign from May 1 – June 10, 2016, particularly when cloud fraction was high and/or fog was present to quantify the change in aerosol characteristics due to near-cloud or fog interaction. We analyze the new AERONET Version 3 data that have significant changes to cloud screening algorithms, allowing many more fine-mode observations in the near vicinity of clouds or fog. Case studies for detailed investigation include May 25–26, 2016 when cloud fraction was high over much of the peninsula, associated with a weak frontal passage and advection of pollution from China. These cloud-influenced Chinese transport dates also had the highest aerosol optical depth (AOD), surface PM2.5 concentrations and fine mode particle sizes of the entire campaign. Another likewise cloud/high relative humidity (RH) case is June 9 and 10, 2016 when fog was present over the Yellow Sea that appears to have affected aerosol properties well downwind over the Korean peninsula. In comparison we also investigated aerosol properties on air stagnation days with very low cloud cover and relatively low RH (May 17 & 18, 2016), when local Korean emissions dominated. Aerosol volume size distributions show marked differences between the transport days (with high RH and cloud influences) and the local pollution stagnation days, with total column-integrated particle fine mode volume being an order of magnitude greater on the pollution transport dates. The PM2.5 over central Seoul were significantly greater than for coastal sites on the transboundary transport days yet not on stagnation days, suggesting additional particle formation from gaseous urban emissions in cloud/fog droplets and/or in the high RH humidified aerosol environment. Many days had KORUS-AQ research aircraft flights that provided observations of aerosol absorption, particle chemistry and vertical profiles of extinction. AERONET retrievals and aircraft in situ measurements both showed high single scattering albedo (weak absorption) on the cloudy or cloud influenced days, plus aircraft profile in situ measurements showed large AOD enhancements (versus dried aerosol) at ambient relative humidity (RH) on the pollution transport days, consistent with the significantly larger fine mode particle radii and weak absorption.

Vertical characteristics of aerosol hygroscopicity and impacts on optical properties over the North China Plain during winter

Abstract. The water uptake of aerosol influences its optical depth and capacity for cloud formation, depending on the vertical profile of aerosol hygroscopicity because of different solar radiation received and supersaturation (SS) conditions at different atmospheric levels. Such information is lacking over the polluted East Asian region. This study presents aircraft-based in situ measured aerosol size distributions and chemical compositions by a series of flights over the Beijing area in wintertime. Under high relative humidity (hRH) conditions (surface RH > 60 %), a significant enhancement of aerosol hygroscopicity parameter (κ) in the planetary boundary layer (PBL) was observed to increase by 50 % from 0.20 up to 0.34 from the surface to the top of the PBL (vertical gradient of ∼0.13 km−1), along with the dry particle effective diameter (Deff) being increased by 71 % and activation ratio up to 0.23 (0.64) at SS =0.05 % (0.1 %). However, a lower vertical gradient of κ (0.05 km−1) and smaller Deff was exhibited under low RH (lRH, surface RH < 60 %). This suggests that the aqueous processes played an important role in promoting the enhancement of particle hygroscopicity in the PBL. The κ in the lower free troposphere (LFT) was relatively stable at 0.24±0.03 with a slight increase during regional transport. The enhancement of aerosol optical depth (AOD) due to water uptake ranged 1.0–1.22 for the PBL under lRH and LFT, but it reached as high as 6.4 in the PBL under hRH. About 80 % and 18 % of the AOD were contributed to by aerosol hygroscopic growth under hRH and lRH, respectively. These results emphasize the important evolution of aerosol water-uptake capacity in the PBL, especially under the high RH condition.

Impact of dust storm on phytoplankton bloom over the Arabian Sea: a case study during March 2012.

Dust storms affect the primary productivity of the ocean by providing necessary micronutrients to the surface layer. One such dust storm during March 2012 led to a substantial reduction in visibility and enhancement in aerosol optical depth (AOD) up to ~ 0.8 (AOD increased from 0.1 to 0.9) over the Arabian Sea. We explored the possible effects and mechanisms through which this particular dust storm could impact the ocean's primary productivity (phytoplankton concentration), using satellite-borne remote sensors and reanalysis model data (2003-2016). The climatological analyses revealed anomalous March 2012 in terms of dust deposition and enhancement in phytoplankton concentration in the month of March during 2003-2016 over this region. The studied dust storm accounts for increase in the daily average surface dust deposition rate from ~ 3 to ~53mgm-2day-1, which is followed by a significant enhancement in the chlorophyll-a (Chl_a) concentration (~ 2 to ~9mgm-3). We show strong association between a dust storm and an event of anomalously high biological production (with a 4-day forward lag) in the Arabian Sea. We suggest that the increase in biological production results from the superposition of two complementary processes (deposition of atmospheric nutrients and deepening of the mixed layer due to dust-induced sea surface temperature cooling) that enhance nutrient availability in the euphotic layer.

Analysis of long-range transboundary transport (LRTT) effect on Korean aerosol pollution during the KORUS-AQ campaign

We investigated the influence of long-range transboundary transport (LRTT) on the aerosol concentrations in the Korean peninsula using the ground- and satellite-based remote sensing with back-trajectory calculations during the Korea-United States Air Quality (KORUS-AQ) campaign. Specifically, aerosol optical depth (AOD) observations from a geostationary satellite can directly provide the progression and evolution of aerosol plume transport. During high pollution cases in western Korea, we found the AOD enhancement over the Yellow Sea and east-central China, at maximum >200% over the pathway of LRTT compared to the mean condition. Particularly, high AOD in the Shandong peninsula appears coincidentally with the high AOD over South Korea in a day, revealing the strong influence of the east-central Chinese emission. Back-trajectory patterns remarkably capture the movement of high AOD bands detected by the geostationary satellite monitoring. LRTT cases through the inside of boundary layer at east-central China usually contribute to the high AOD in Korea, while air-masses above the boundary layer in north China and Mongolia do not much relate to the Korean pollution, showing the importance for both the direction and height of the air-mass movement. Travel speed is another significant factor to describe the LRTT effect. Despite the large effect of LRTT to both urban and rural sites in Korea, sometimes urban sites are more affected by the domestic emission when the air-mass travels shorter than ∼250 km per day, notifying that the effect of Korean domestic emission cannot be negligible as well. Our findings reveal that usage of geostationary satellite observations enables us to better evaluate the influence of LRTT on the local air pollution.

Satellite-based view of the aerosol spatial and temporal variability in the Córdoba region (Argentina) using over ten years of high-resolution data

Space-based observations offer a unique opportunity to investigate the atmosphere and its changes over decadal time scales, particularly in regions lacking in situ and/or ground based observations. In this study, we investigate temporal and spatial variability of atmospheric particulate matter (aerosol) over the urban area of Córdoba (central Argentina) using over ten years (2003–2015) of high-resolution (1 km) satellite-based retrievals of aerosol optical depth (AOD). This fine resolution is achieved exploiting the capabilities of a recently developed inversion algorithm (Multiangle implementation of atmospheric correction, MAIAC) applied to the MODIS sensor datasets of the NASA-Terra and -Aqua platforms. Results of this investigation show a clear seasonality of AOD over the investigated area. This is found to be shaped by an intricate superposition of aerosol sources, acting over different spatial scales and affecting the region with different yearly cycles. During late winter and spring (August-October), local as well as near- and long-range transported biomass burning (BB) aerosols enhance the Córdoba aerosol load, and AOD levels reach their maximum values (>0.35 at 0.47 µm). The fine AOD spatial resolution allowed to disclose that, in this period, AOD maxima are found in the rural/agricultural area around the city, reaching up to the city boundaries pinpointing that fires of local and near-range origin play a major role in the AOD enhancement. A reverse spatial AOD gradient is found from December to March, the urban area showing AODs 40–80% higher than in the city surroundings. In fact, during summer, the columnar aerosol load over the Córdoba region is dominated by local (urban and industrial) sources, likely coupled to secondary processes driven by enhanced radiation and mixing effects within a deeper planetary boundary layer (PBL). With the support of modelled AOD data from the Modern-Era Retrospective Analysis for Research and Application (MERRA), we further investigated into the chemical nature of AOD. The results suggest that mineral dust is also an important aerosol component in Córdoba, with maximum impact from November to February. The use of a long-term dataset finally allowed a preliminary assessment of AOD trends over the Córdoba region. For those months in which local sources and secondary processes were found to dominate the AOD (December to March), we found a positive AOD trend in the Córdoba outskirts, mainly in the areas with maximum urbanization/population growth over the investigated decade. Conversely, a negative AOD trend (up to −0.1 per decade) is observed all over the rural area of Córdoba during the BB season, this being attributed to a decrease of fires both at the local and the continental scale.

Assessment of cloud-related fine-mode AOD enhancements based on AERONET SDA product

Abstract. AERONET (AErosol RObotic NETwork), which is a network of ground-based sun photometers, produces a data product called the aerosol spectral deconvolution algorithm (SDA) that utilizes spectral total aerosol optical depth (AOD) data to infer the component fine- and coarse-mode optical depths at 500 nm. Based on its assumptions, SDA identifies cloud optical depth as the coarse-mode AOD component and therefore effectively computes the fine-mode AOD also in mixed cloud–aerosol observations. Therefore, it can be argued that the more representative AOD for fine-mode fraction should be based on all direct sun measurements and not only on those cloud screened for clear-sky conditions, i.e., on those from level 1 (L1) instead of level 2 (L2) in AERONET. The objective of our study was to assess, including all the available AERONET sites, how the fine-mode AOD is enhanced in cloudy conditions, contrasting SDA L1 and L2 in our analysis. Assuming that the cloud screening correctly separates the cloudy and clear-sky conditions, then the increases in fine-mode AOD can be due to various cloud-related processes, mainly by the strong hygroscopic growth of particles in the vicinity of clouds and in-cloud processing leading to growth of accumulation mode particles. We estimated these cloud-related enhancements in fine-mode AOD seasonally and found, for instance, that in June–August season the average over all the AERONET sites was 0.011, when total fine-mode AOD from L2 data was 0.154; therefore, the relative enhancement was 7 %. The enhancements were largest, both absolutely and relatively, in East Asia; for example, in June–August season the absolute and relative differences in fine-mode AOD, between L1 and L2 measurements, were 0.022 and 10 %, respectively. Corresponding values in North America and Europe were about 0.01 and 6–7 %. In some highly polluted areas, the enhancement is greater than these regional averages, e.g., in Beijing region and in June–July–August (JJA) season the corresponding absolute values were about 0.1. It is difficult to separate the fine-mode AOD enhancements due to in-cloud processing and hygroscopic growth, but we attempted to get some understanding by conducting a similar analysis for SDA-based fine-mode Ångström exponent (AE) patterns. Moreover, we exploited a cloud parcel model, in order to understand in detail the relative role of different processes. We found that in marine conditions, were aerosol concentration are low and cloud scavenging is efficient, the AE changes in opposite direction than in the more polluted conditions, were hygroscopic growth of particles leads to a negative AE change.

Probing into the aging dynamics of biomass burning aerosol by using satellite measurements of aerosol optical depth and carbon monoxide

Abstract. Carbonaceous aerosol released into the atmosphere from open biomass burning (BB) is known to undergo considerable chemical and physical transformations (aging). However, there is substantial controversy about the nature and observable effects of these transformations. A shortage of consistent observational evidence on BB aerosol aging processes under different environmental conditions and at various temporal scales hinders development of their adequate representations in chemistry transport models (CTMs). In this study, we obtain insights into the BB aerosol dynamics by using available satellite measurements of aerosol optical depth (AOD) and carbon monoxide (CO). The basic concept of our method is to consider AOD as a function of the BB aerosol photochemical age (that is, the time period characterizing the exposure of BB aerosol emissions to atmospheric oxidation reactions) predicted by means of model tracers. We evaluate the AOD enhancement ratio (ER) defined as the ratio of optical depth of actual BB aerosol with respect to that of a modeled aerosol tracer that is assumed to originate from the same fires as the real BB aerosol but that is not affected by any aging processes. To limit possible effects of model transport errors, the AOD measurements are normalized to CO column amounts that are also retrieved from satellite measurements. The method is applied to the analysis of the meso- and synoptic-scale evolution of aerosol in smoke plumes from major wildfires that occurred in Siberia in summer 2012. AOD and CO retrievals from MODIS and IASI measurements, respectively, are used in combination with simulations performed with the CHIMERE CTM. The analysis indicates that aging processes strongly affected the evolution of BB aerosol in the situation considered, especially in dense plumes (with spatial average PM2. 5 concentration exceeding 100 µg m−3). For such plumes, the ER is found to increase almost 2-fold on the scale of ∼ 10 h of daytime aerosol evolution (after a few first hours of the evolution that are not resolved in our analysis). The robustness of this finding is corroborated by sensitivity tests and Monte Carlo experiments. Furthermore, a simulation using the volatility basis set framework suggests that a large part of the increase in the ER can be explained by atmospheric processing of semi-volatile organic compounds. Our results are consistent with findings of a number of earlier studies reporting considerable underestimation of AOD by CTMs in which BB aerosol aging processes have either been disregarded or simulated in a highly simplified way. In general, this study demonstrates the feasibility of using satellite measurements of AOD in biomass burning plumes in combination with aerosol tracer simulations for the investigation of BB aerosol evolution and validation of BB aerosol aging schemes in atmospheric models.

Taklimakan Desert nocturnal low-level jet: climatology and dust activity

Abstract. While nocturnal low-level jets (NLLJs) occur frequently in many parts of the world, the occurrence and other detailed characteristics of NLLJs over the Taklimakan Desert (TD) are not well known. This paper presents a climatology of NLLJs and coincident dust over the TD by analyzing multi-year ERA-Interim reanalysis and satellite observations. It is found that the ERA-Interim dataset can capture the NLLJs' features well by comparison with radiosonde data from two surface sites. The NLLJs occur in more than 60 % of nights, which are primarily easterly to east-northeasterly. They typically appear at 100 to 400 m above the surface with a speed of 4 to 10 m s−1. Most NLLJs are located above the nocturnal inversion during the warm season, while they are embedded in the inversion layer during the cold season. NLLJs above the inversion have a strong annual cycle with a maximum frequency in August. We also quantify the convective boundary layer (CBL) height and construct an index to measure the magnitude of the momentum in the CBL. We find that the magnitude of momentum in the lower atmosphere from the top of the surface layer to the top of mixed layer is larger for NLLJ cases than for non-NLLJ cases, and in the warm season the downward momentum transfer process is more intense and rapid. The winds below the NLLJ core to the desert surface gain strength in summer and autumn, and these summer and autumn winds are coincident with an enhancement of aerosol optical depth. This indicates that the NLLJ is an important mechanism for dust activity and transport during the warm season over the Taklimakan.

In situ vertical profiles of aerosol extinction, mass, and composition over the southeast United States during SENEX and SEAC<sup>4</sup>RS: observations of a modest aerosol enhancement aloft

Abstract. Vertical profiles of submicron aerosol from in situ aircraft-based measurements were used to construct aggregate profiles of chemical, microphysical, and optical properties. These vertical profiles were collected over the southeastern United States (SEUS) during the summer of 2013 as part of two separate field studies: the Southeast Nexus (SENEX) study and the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS). Shallow cumulus convection was observed during many profiles. These conditions enhance vertical transport of trace gases and aerosol and create a cloudy transition layer on top of the sub-cloud mixed layer. The trace gas and aerosol concentrations in the transition layer were modeled as a mixture with contributions from the mixed layer below and the free troposphere above. The amount of vertical mixing, or entrainment of air from the free troposphere, was quantified using the observed mixing ratio of carbon monoxide (CO). Although the median aerosol mass, extinction, and volume decreased with altitude in the transition layer, they were ~10 % larger than expected from vertical mixing alone. This enhancement was likely due to secondary aerosol formation in the transition layer. Although the transition layer enhancements of the particulate sulfate and organic aerosol (OA) were both similar in magnitude, only the enhancement of sulfate was statistically significant. The column integrated extinction, or aerosol optical depth (AOD), was calculated for each individual profile, and the transition layer enhancement of extinction typically contributed less than 10 % to the total AOD. Our measurements and analysis were motivated by two recent studies that have hypothesized an enhanced layer of secondary aerosol aloft to explain the summertime enhancement of AOD (2–3 times greater than winter) over the southeastern United States. The first study attributes the layer aloft to secondary organic aerosol (SOA) while the second study speculates that the layer aloft could be SOA or secondary particulate sulfate. In contrast to these hypotheses, the modest enhancement we observed in the transition layer was not dominated by OA and was not a large fraction of the summertime AOD.

A theoretical study of the effect of subsurface oceanic bubbles on the enhanced aerosol optical depth band over the southern oceans as detected from MODIS and MISR

Abstract. Submerged oceanic bubbles, which have a much longer life span than whitecaps or bubble rafts, have been hypothesized to increase the water-leaving radiance and thus affect satellite-based estimates of water-leaving radiance to non-trivial levels. This study explores this effect further to determine whether such bubbles are of sufficient magnitude to impact satellite aerosol optical depth (AOD) retrievals through perturbation of the lower boundary conditions. There has been significant discussion in the community regarding the high positive biases in retrieved AODs in many remote ocean regions. In this study, for the first time, the effects of oceanic bubbles on satellite retrievals of AOD are studied by using a linked Second Simulation of a Satellite Signal in the Solar Spectrum (6S) atmospheric and HydroLight oceanic radiative transfer models. The results suggest an insignificant impact on AOD retrievals in regions with near-surface wind speeds of less than 12 m s−1. However, the impact of bubbles on aerosol retrievals could be on the order of 0.02–0.04 for higher wind conditions within the scope of our simulations (e.g., winds < 20 m −1. This bias is propagated to global scales using 1 year of Moderate Resolution Imaging Spectroradiometer (MODIS) and Advanced Microwave Scanning Radiometer EOS (AMSR-E) data to investigate the possible impacts of oceanic bubbles on an enhanced AOD belt observed over the high-latitude southern oceans (also called the enhanced southern oceans anomaly, or ESOA) by some passive satellite sensors. Ultimately, this study is supportive of the null hypothesis: submerged bubbles are not the major contributor to the ESOA feature. This said, as retrievals progress to higher and higher resolutions, such as from airborne platforms, the uniform bubble correction in clean marine conditions should probably be separately accounted for against individual bright whitecaps and bubble rafts.

Observations of rapid aerosol optical depth enhancements in the vicinity of polluted cumulus clouds

Abstract. During the July 2011 Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field experiment in Maryland, significant enhancements in Aerosol Robotic Network (AERONET) sun–sky radiometer measured aerosol optical depth (AOD) were observed in the immediate vicinity of non-precipitating cumulus clouds on some days. Both measured Ångström exponents and aerosol size distribution retrievals made before, during and after cumulus development often suggest little change in fine mode particle size; therefore, implying possible new particle formation in addition to cloud processing and humidification of existing particles. In addition to sun–sky radiometer measurements of large enhancements of fine mode AOD, lidar measurements made from both ground-based and aircraft-based instruments during the experiment also measured large increases in aerosol signal at altitudes associated with the presence of fair weather cumulus clouds. These data show modifications of the aerosol vertical profile as a result of the aerosol enhancements at and below cloud altitudes. The airborne lidar data were utilized to estimate the spatial extent of these aerosol enhancements, finding increased AOD, backscatter and extinction out to 2.5 km distance from the cloud edge. Furthermore, in situ measurements made from aircraft vertical profiles over an AERONET site during the experiment also showed large increases in aerosol scattering and aerosol volume after cloud formation as compared to before. The 15-year AERONET database of AOD measurements at the Goddard Space Flight Center (GSFC), Maryland site, was investigated in order to obtain a climatological perspective of this phenomenon of AOD enhancement. Analysis of the diurnal cycle of AOD in summer showed significant increases in AOD from morning to late afternoon, corresponding to the diurnal cycle of cumulus development.

Aerosol interactions with African/Atlantic climate dynamics

Mechanistic relationships exist between variability of dust in the oceanic Saharan air layer (OSAL) and transient changes in the dynamics of Western Africa and the tropical Atlantic Ocean. This study provides evidence of possible interactions between dust in the OSAL region and African easterly jet–African easterly wave (AEJ–AEW) system in the climatology of boreal summer, when easterly wave activity peaks. Synoptic-scale changes in instability and precipitation in the African/Atlantic intertropical convergence zone are correlated with enhanced aerosol optical depth (AOD) in the OSAL region in response to anomalous 3D overturning circulations and upstream/downstream thermal anomalies at above and below the mean-AEJ level. Upstream and downstream anomalies are referred to the daily thermal/dynamical changes over the West African monsoon region and the Eastern Atlantic Ocean, respectively. Our hypothesis is that AOD in the OSAL is positively correlated with the downstream AEWs and negatively correlated with the upstream waves from climatological perspective. The similarity between the 3D pattern of thermal/dynamical anomalies correlated with dust outbreaks and those of AEWs provides a mechanism for dust radiative heating in the atmosphere to reinforce AEW activity. We proposed that the interactions of OSAL dust with regional climate mainly occur through coupling of dust with the AEWs.

Investigation of CO, C<sub>2</sub>H<sub>6</sub> and aerosols in a boreal fire plume over eastern Canada during BORTAS 2011 using ground- and satellite-based observations and model simulations

Abstract. We present the results of total column measurements of CO, C2H6 and fine-mode aerosol optical depth (AOD) during the "Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites" (BORTAS-B) campaign over eastern Canada. Ground-based observations, using Fourier transform spectrometers (FTSs) and sun photometers, were carried out in July and August 2011. These measurements were taken in Halifax, Nova Scotia, which is an ideal location to monitor the outflow of boreal fires from North America, and also in Toronto, Ontario. Measurements of fine-mode AOD enhancements were highly correlated with enhancements in coincident trace gas (CO and C2H6) observations between 19 and 21 July 2011, which is typical for a smoke plume event. In this paper, we focus on the identification of the origin and the transport of this smoke plume. We use back trajectories calculated by the Canadian Meteorological Centre as well as FLEXPART forward trajectories to demonstrate that the enhanced CO, C2H6 and fine-mode AOD seen near Halifax and Toronto originated from forest fires in northwestern Ontario that occurred between 17 and 19 July 2011. In addition, total column measurements of CO from the satellite-borne Infrared Atmospheric Sounding Interferometer (IASI) have been used to trace the smoke plume and to confirm the origin of the CO enhancement. Furthermore, the enhancement ratio – that is, in this case equivalent to the emission ratio (ERC2H6/CO) – was estimated from these ground-based observations. These C2H6 emission results from boreal fires in northwestern Ontario agree well with C2H6 emission measurements from other boreal regions, and are relatively high compared to fires from other geographical regions. The ground-based CO and C2H6 observations were compared with outputs from the 3-D global chemical transport model GEOS-Chem, using the Fire Locating And Modeling of Burning Emissions (FLAMBE) inventory. Agreement within the stated measurement uncertainty (~3% for CO and ~8% for C2H6) was found for the magnitude of the enhancement of the CO and C2H6 total columns between the measured and modelled results. However, there is a small shift in time (of approximately 6 h) of arrival of the plume over Halifax between the results.

Multi-year observations of the spatial and vertical distribution of aerosols and the genesis of abnormal variations in aerosol loading over the Arabian Sea during Asian summer monsoon season

Intense aerosol plumes engulf a vast region of the Arabian Sea during the Asian summer monsoon season (ASM: June–September). The largest value of aerosol optical depth (AOD) at 550nm in this region generally occurs in July when the mean AOD attains its annual peak value of >0.8. However, the AOD over this region is abnormally large during the ASM in some years, especially during the June–July period. Long term satellite observations using MODIS reveal that the largest AOD during the 11-year period of March 2000–February 2011 occurred in June 2008 with a regional mean AOD of 1.1, which was ~97% larger than that of the corresponding long term mean value in June and ~49% larger than that in July. The availability of CALIPSO data since June 2006 provides a unique opportunity to quantify the role of continental aerosols transported from the West Asian desert regions in the genesis of the above abnormality over the Arabian Sea. We examine the spatial and vertical distributions of aerosols over the Arabian Sea and adjoining continents using multi-year data from MODIS and CALIPSO and explore the genesis of the above abnormal enhancement in AOD. The observed anomalies in AOD are substantially larger than that can be attributed to changes in wind-generated sea salt aerosols. The CALIPSO observations show that the anomalous enhancement in aerosol loading over the Arabian Sea during June 2008 was primarily caused by an enhancement in aerosol abundance in the altitude range of ~1–4km with a distinctly large volume depolarization ratio of >0.25, clearly indicating the dominance of highly non-spherical mineral dust. Although the aerosol loading over the Arabian Sea during the ASM is observed to be mainly caused by the mineral dust transported from the West Asian Deserts at northwest of the Arabian Sea, the abnormal enhancement in the observed AOD during June 2008 was primarily caused by a distinct increase in dust storms over the northern continents and subsequent transport into the Arabian Sea.