Aerosol Trends Research Articles

Performance of multi-decadal ocean simulations in the Adriatic Sea

A performance study of seven regional ocean configurations based on NEMO has been carried out for the Adriatic Sea over a common period (1980–2012). Assessed models differ in resolution, model physics, atmospheric forcing (forced vs. coupled models) and river discharges imposed within the Adriatic Sea. Models have been evaluated on the long-term temperature and salinity measurements in all of the Adriatic sub-basins, in particular within dense water collectors (Jabuka Pit and South Adriatic Pit) and dense water formation sites (northern and southern Adriatic). Adriatic-wide salinity content is mostly linked to the proper introduction of the overall water budget, rather than to the local river forcing. Forced models mostly overestimate temperature and salinity values. On average, coupled models better reproduce the thermohaline properties and processes, in particular the Adriatic-Ionian Bimodal Oscillating System (BiOS) reversals and its decadal variability. Wintertime heat losses are playing major role in defining the Adriatic Deep Water (ADW) transport rates in coupled models, while in forced models preconditioning in salinity is the most important factor. Further on, increase of resolution of the atmospheric forcing results in more realistic ocean behaviour, including dense water formation (DWF) in the complex coastal northern Adriatic. However, all models have large temperature biases and lower deep stratification at the dense water collector sites, indicating overall underrepresentation of the Adriatic DWF. Consequently, mixed-layer depth in the southern Adriatic is overestimated, reaching the bottom during some years. Ocean model resolution and river forcing seem to play a second-order role in defining the overall Adriatic-Ionian thermohaline properties, while inclusion of aerosol trend only slightly modified the BiOS reproduction.

Evidence for Elevation-Dependent Warming in the St. Elias Mountains, Yukon, Canada

AbstractThe climate of high midlatitude mountains appears to be warming faster than the global average, but evidence for such elevation-dependent warming (EDW) at higher latitudes is presently scarce. Here, we use a comprehensive network of remote meteorological stations, proximal radiosonde measurements, downscaled temperature reanalysis, ice cores, and climate indices to investigate the manifestation and possible drivers of EDW in the St. Elias Mountains in subarctic Yukon, Canada. Linear trend analysis of comprehensively validated annual downscaled North American Regional Reanalysis (NARR) gridded surface air temperatures for the years 1979–2016 indicates a warming rate of 0.028°C a−1 between 5500 and 6000 m above mean sea level (MSL), which is ~1.6 times larger than the global-average warming rate between 1970 and 2015. The warming rate between 5500 and 6000 m MSL was ~1.5 times greater than the rate at the 2000–2500 m MSL bin (0.019°C a−1), which is similar to the majority of warming rates estimated worldwide over similar elevation gradients. Accelerated warming since 1979, measured by radiosondes, indicates a maximum rate at 400 hPa (~7010 m MSL). EDW in the St. Elias region therefore appears to be driven by recent warming of the free troposphere. MODIS satellite data show no evidence for an enhanced snow albedo feedback above 2500 m MSL, and declining trends in sulfate aerosols deposited in high-elevation ice cores suggest a modest increase in radiative forcing at these elevations. In contrast, increasing trends in water vapor mixing ratio at the 500-hPa level measured by radiosonde suggest that a longwave radiation vapor feedback is contributing to EDW.

Impact of Biomass Burning in South and Southeast Asia on Background Aerosol in Southwest China

ABSTRACT Biomass burning (BB) in Southeast Asia is particularly pronounced during the dry season. However, the complex topography and long-range transport inherent to Southeast Asia have limited local research on pollution resulting from BB. In this study, the monthly variation in aerosol optical properties at six sites in Southeast Asia (Chiang Mai, Mukdahan, Bac-Lieu, Penang, Singapore, and Bandung) and the fire-point distribution have been analyzed in detail. The Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model was used to simulate the 72-hour back-trajectory from the Shangri-La atmospheric background station in Yunnan Province, China. Our results showed that BB was more common on the Indochinese Peninsula from March to May, whereas it was more common on the Malay Archipelago from August to October due to the latitudinal difference and crop harvest season. Significant BB activity on the Indochinese Peninsula in March resulted in a high surge in extinction (AODt440nm = 1.32 ± 0.69, AODf440nm = 1.24 ± 0.59) by particles with a smaller diameter (AE = 1.68 ± 0.13) in Chiang Mai. Mapping the long-range transport of BB aerosols reveals that Shangri-La’s pollution was primarily affected by emissions from northern-central India (accounting for 45.2%), and Bangladesh and northern Myanmar (accounting for 38.7%), which indicates that the aerosol pollution on the Yunnan-Guizhou Plateau in springtime could have originated on the southern periphery of the Tibetan Plateau. The results also indicate that BB emission in Southeast Asia had a limited impact on pollution in Southwest China but a relatively large effect on local areas. This study is the first to analyze the trend of aerosols produced from BB in Southeast Asia via ground-based observation, which deepens our understanding of the potential effects of BB aerosols transported long-range from outside Southwest China.

Investigation of various aerosols over different locations in South Africa using satellite, model simulations and LIDAR

Decadal studies (2004–2014) of various aerosols were carried out over South Africa (SA) using various satellite data and model simulations. The aerosols investigated included black carbon (BC), sulphate, dust and marine aerosols. BC aerosols were observed to be dominant in the northeastern parts of SA while sulphate aerosols were dominant in eastern parts of the country. Seasonal studies revealed that BC aerosols were more dominant in the eastern parts of SA during spring and less dominant in autumn. Sulphate also showed dominance in the eastern parts of SA during summer and less dominance in winter. The high sulphate concentration in summer is a result of an increase in relative humidity which favours the production of sulphates. Air masses from the north and northeastern parts of the subcontinent were responsible for the transport of BC resulting from biomass burning into SA. The Goddard Chemistry Aerosol Radiation and Transport model indicated that there was no significant change in the sulphate aerosol trends from 2004 to 2007. The highest sulphate aerosol levels were observed in the summer whilst the lowest sulphate aerosol levels were observed in winter. The Council for Scientific and Industrial Research (CSIR) Light Detection and Ranging (LIDAR) was used to carry out measurements in Lephalale during July 10–18, 2014. Aerosol extinction co‐efficient profiles were retrieved by the CSIR mobile LIDAR and were compared to aerosol extinction co‐efficient profiles retrieved from the Cloud‐Aerosol LIDAR and Infrared Pathfinder Satellite Observations (CALIPSO). The aerosol extinction co‐efficients of 0.26 and 0.17/km on July 14 and 16, 2014, respectively could be identified as dust aerosols.

Factors controlling the long-term (2009–2015) trend of PM2.5 and black carbon aerosols at eastern Himalaya, India

A first-ever long-term (2009–2015) study on the fine particulate matter (PM2.5) and black carbon (BC) aerosol were conducted over Himalaya in order to investigate the characteristics, temporal variations and the important factors regulating the long-term trend. The study was conducted over a high altitude station, Darjeeling (27°01′N, 88°15′E, 2200 m asl) representing a typical high altitude urban atmosphere at eastern Himalaya in India. The average concentrations of PM2.5 and BC over a period of seven years were 25.2 ± 5.6 μg m−3 (ranging between 2.2 and 220.4 μg m−3) and 3.4 ± 0.7 μg m−3 (0.4 to 15.6 μg m−3) respectively. We observed decreasing trends in both PM2.5 (49% at a rate of 170 ng m−3 month−1) and BC (34% at the rate of 20 ng m−3 month−1) mass concentration over this region from 2009 to 2015. We extensively studied the impact of micrometeorological parameters on the long-term trend in PM2.5 and BC through the correlation analysis. The significant changes in boundary layer dynamics over this region played a major role in the decreasing trend of aerosols. The concentration weighted trajectory analysis revealed that the important contributory long-distant source regions for PM2.5 and BC over eastern Himalaya were Indo Gangetic Plane and Nepal. The contributions from these regions were found to be decreased significantly from 2009 to 2015. Investigations on the fire counts associated with the forest fire, and open burning activities through the satellite observations revealed that the decreasing trend in PM2.5 and BC over eastern Himalaya is well correlated to the decreasing trend in the fire counts over IGP and Nepal. We also explored that the changes and up gradation of the domestic fuel at the Indo Gangetic Plane regions in recent years not only improved the regional air quality but also affected the atmospheric environment over the eastern part of Himalaya.

Source Apportionments of Aerosols and Their Direct Radiative Forcing and Long‐Term Trends Over Continental United States

AbstractDue to U.S. air pollution regulations, aerosol and precursor emissions have decreased during recent decades, while changes in emissions in other regions of the world also influence U.S. aerosol trends through long‐range transport. We examine here the relative roles of these domestic and foreign emission changes on aerosol concentrations and direct radiative forcing at the top of the atmosphere over the continental United States. Long‐term (1980–2014) trends and aerosol source apportionment are quantified in this study using a global aerosol‐climate model equipped with an explicit aerosol source tagging technique. Due to U.S. emission control policies, the annual mean near‐surface concentration of particles, consisting of sulfate, black carbon, and primary organic aerosol, decreases by about −1.1 (±0.1)/−1.4 (±0.1) μg/m3 in western United States and −3.3 (±0.2)/−2.9 (±0.2) μg/m3 in eastern United States during 2010–2014, as compared to those in 1980–1984. Meanwhile, decreases in U.S. emissions lead to a warming of +0.48 (±0.03)/+0.46 (±0.03) W/m2 in western United States and +1.41 (±0.07)/+1.32 (±0.09) W/m2 in eastern United States through changes in aerosol direct radiative forcing. Increases in emissions from East Asia generally have a modest impact on U.S. air quality but mitigated the warming effect induced by reductions in U.S. emissions by 25% in western United States and 7% in eastern United States. As U.S. domestic aerosol and precursor emissions continue to decrease, foreign emissions may become increasingly important to radiative forcing over the United States.

Long-term (2001–2012) trends of carbonaceous aerosols from a remote island in the western North Pacific: an outflow region of Asian pollutants

Abstract. The present study reports on long-term trends of carbonaceous aerosols in total suspended particulate (TSP) samples collected at Chichijima in the western North Pacific during 2001–2012. Seasonal variations of elemental carbon (EC), organic carbon (OC), and water-soluble organic carbon (WSOC) concentrations showed maxima in winter to spring and minima in summer. These seasonal differences in the concentrations of carbonaceous aerosols were associated with the outflows of polluted air masses from East Asia, which are clearly distinguishable from pristine air masses from the central Pacific. The higher concentrations of carbonaceous aerosols during winter to spring are associated with long-range atmospheric transport of East Asian continental polluted air masses, whereas lower concentrations may be due to pristine air masses from the central Pacific in summer. The annual trends of OC ∕ EC (+0.46 % yr−1), WSOC (+0.18 % yr−1) and WSOC ∕ OC (+0.08 % yr−1) showed significant (p < 0.05) increases during the period of 2001–2012, suggesting that photochemical formation of WSOC and its contributions to secondary organic aerosols (SOAs) have increased over the western North Pacific via long-range atmospheric transport. We found a significant increase (+0.33 % yr−1) in nss-K+ ∕ EC ratios, demonstrating that concentrations of biomass-burning-derived carbonaceous aerosols have increased, while those of primary fossil-fuel-derived aerosols have decreased over the western North Pacific. Further, secondary biogenic emissions are also important over the western North Pacific as inferred from a significant increase (+0.14 % yr−1) in the concentrations of methanesulfonate (MSA−, a tracer for biogenic sources). This point was further supported by a moderate correlation (r = 0.40) between WSOC and MSA−. We also found a significant increase in OC ∕ TC (total carbon) and WSOC ∕ TC ratios, further suggesting that photochemical formation of WSOC and its contributions to SOAs have increased over the western North Pacific during 2001–2012 via long-range atmospheric transport from East Asia.

A study of 15-year aerosol optical thickness and direct shortwave aerosol radiative effect trends using MODIS, MISR, CALIOP and CERES

Abstract. By combining Collection 6 Moderate Resolution and Imaging Spectroradiometer (MODIS) and Version 22 Multi-angle Imaging Spectroradiometer (MISR) aerosol products with Cloud and Earth's Radiant Energy System (CERES) flux products, the aerosol optical thickness (AOT, at 0.55 µm) and shortwave (SW) aerosol radiative effect (SWARE) trends are studied over ocean for the near-full Terra (2000–2015) and Aqua (2002–2015) data records. Despite differences in sampling methods, regional SWARE and AOT trends are highly correlated with one another. Over global oceans, weak SWARE (cloud-free SW flux) and AOT trends of 0.5–0.6 W m−2 (−0.5 to −0.6 W m−2) and 0.002 AOT decade−1 are found using Terra data. Near-zero AOT and SWARE trends are also found for using Aqua data, regardless of the angular distribution models (ADMs) used. Regionally, positive AOT and cloud-free SW flux (negative SWARE) trends are found over the Bay of Bengal, the Arabian Sea, the Arabian/Persian Gulf and the Red Sea, while statistically significant negative trends are derived over the Mediterranean Sea and the eastern US coast. In addition, the global mean instantaneous SW aerosol direct forcing efficiencies are found to be ∼ −60 W m−2 AOT−1, with corresponding SWARE values of ∼ −7 W m−2 from both Aqua and Terra data, again regardless of CERES ADMs used. Regionally, SW aerosol direct forcing efficiency values of ∼ −40 W m−2 AOT−1 are found over the southwest coast of Africa where smoke aerosol particles dominate in summer. Larger (in magnitude) SW aerosol direct forcing efficiency values of −50 to −80 W m−2 AOT−1 are found over several other dust- and pollutant-aerosol-dominated regions. Lastly, the AOT and SWARE trends from this study are also intercompared with aerosol trends (such as active-based ones) from several previous studies. Findings suggest that a cohesive understanding of the changing aerosol skies can be achieved through the analysis of observations from both passive- and active-based analyses, as well as from both narrowband and broadband datasets.

Aerosol trends as a potential driver of regional climate in the central United States: evidence from observations

Abstract. In situ surface observations show that downward surface solar radiation (SWdn) over the central and southeastern United States (US) has increased by 0.58–1.0 Wm−2 a−1 over the 2000–2014 time frame, simultaneously with reductions in US aerosol optical depth (AOD) of 3.3–5.0 × 10−3 a−1. Establishing a link between these two trends, however, is challenging due to complex interactions between aerosols, clouds, and radiation. Here we investigate the clear-sky aerosol–radiation effects of decreasing US aerosols on SWdn and other surface variables by applying a one-dimensional radiative transfer to 2000–2014 measurements of AOD at two Surface Radiation Budget Network (SURFRAD) sites in the central and southeastern United States. Observations characterized as clear-sky may in fact include the effects of thin cirrus clouds, and we consider these effects by imposing satellite data from the Clouds and Earth's Radiant Energy System (CERES) into the radiative transfer model. The model predicts that 2000–2014 trends in aerosols may have driven clear-sky SWdn trends of +1.35 Wm−2 a−1 at Goodwin Creek, MS, and +0.93 Wm−2 a−1 at Bondville, IL. While these results are consistent in sign with observed trends, a cross-validated multivariate regression analysis shows that AOD reproduces 20–26 % of the seasonal (June–September, JJAS) variability in clear-sky direct and diffuse SWdn at Bondville, IL, but none of the JJAS variability at Goodwin Creek, MS. Using in situ soil and surface flux measurements from the Ameriflux network and Illinois Climate Network (ICN) together with assimilated meteorology from the North American Land Data Assimilation System (NLDAS), we find that sunnier summers tend to coincide with increased surface air temperature and soil moisture deficits in the central US. The 1990–2015 trends in the NLDAS SWdn over the central US are also of a similar magnitude to our modeled 2000–2014 clear-sky trends. Taken together, these results suggest that climate and regional hydrology in the central US are sensitive to the recent reductions in aerosol concentrations. Our work has implications for severely polluted regions outside the US, where improvements in air quality due to reductions in the aerosol burden could inadvertently pose an enhanced climate risk.

AEROCAN, the Canadian sub-network of AERONET: Aerosol monitoring and air quality applications

Previous studies have demonstrated the utility of AERONET (Aerosol Robotic Network) aerosol optical depth (AOD) data for monitoring the spatial variability of particulate matter (PM) in relatively polluted regions of the globe. AEROCAN, a Canadian sub-network of AERONET, was established 20 years ago and currently consists of twenty sites across the country. In this study, we examine whether the AEROCAN sunphotometer data provide evidence of anthropogenic contributions to ambient particulate matter concentrations in relatively clean Canadian locations. The similar weekly cycle of AOD and PM2.5 over Toronto provides insight into the impact of local pollution on observed AODs. High temporal correlations (up to r = 0.78) between daily mean AOD (or its fine-mode component) and PM2.5 are found at southern Ontario AEROCAN sites during May–August, implying that the variability in the aerosol load resides primarily in the boundary layer and that sunphotometers capture day-to-day PM2.5 variations at moderately polluted sites. The sensitivity of AEROCAN AOD data to anthropogenic surface-level aerosol enhancements is demonstrated using boundary-layer wind information for sites near sources of aerosol or its precursors. An advantage of AEROCAN relative to the Canadian in-situ National Air Pollution Surveillance (NAPS) network is the ability to detect free tropospheric aerosol enhancements, which can be large in the case of lofted forest fire smoke or desert dust. These aerosol plumes eventually descend to the surface, sometimes in populated areas, exacerbating air quality. In cases of large AOD (≥0.4), AEROCAN data are also useful in characterizing the aerosol type. The AEROCAN network includes three sites in the high Arctic, a region not sampled by the NAPS PM2.5 monitoring network. These polar sites show the importance of long-range transport and meteorology in the Arctic haze phenomenon. Also, AEROCAN sunphotometers are, by design and due to regular maintenance, the most valuable monitors available for long term aerosol trends. Using a variety of data analysis techniques and timescales, the usefulness of this ground-based remote-sensing sub-network for providing information relevant to air quality is demonstrated.

Opposite long-term trends in aerosols between low and high altitudes: a testimony to the aerosol–PBL feedback

Abstract. Interactions between absorbing aerosols and the planetary boundary layer (PBL) play an important role in affecting air pollution near the surface. In this study, a unique feature of the aerosol–PBL interaction is identified that has important implications in monitoring and combating air pollution. Opposite trends in aerosol loading between the lower and upper PBL are shown on a wide range of timescales and data acquired by various platforms: from a short-term field experiment to decadal satellite observations and multidecadal ground observations in China. A novel method is proposed to obtain the vertical profiles of aerosol loading from passive sensors by virtue of varying elevations. The analyses of visibility, aerosol optical depth, and extinction with different temporal scales exhibit the similar trend, i.e., increasing in the lower atmosphere but decreasing in the upper atmosphere. Integration of the reversal aerosol trend below and above the PBL resulted in a much less change in the column-integrated quantities. The surface cooling effect, together with the change in the heating rate induced by the absorbing aerosol, unevenly modifies the atmospheric temperature profile, causing a more stable atmosphere inside the PBL but a destabilized atmosphere above the PBL. Such a change in the atmospheric stability favors the accumulation of pollutants near the surface and the vertical diffusion of aerosol particles in the upper atmosphere, both of which are consistent with the observed reversal aerosol trends. These findings have multiple implications in understanding and combating air pollution, especially in many developing countries with high emissions of light-absorbing aerosols.

Towards a combined SAGE II and SCIAMACHY aerosol dataset and implications for stratospheric aerosol trend analysis over East Asia

AbstractScanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) limb observation data are used to retrieve stratospheric aerosol extinction profiles. The retrieved aerosol profiles are compared with Stratospheric Aerosol and Gas Experiment (SAGE) II aerosol data records. The comparisons are made over the period 2003–2004. The results show that the SCIAMACHY aerosol profile retrievals exhibit general agreement with the coincident SAGE II data records. In the 15–35 km altitude range, the percentage differences between the SCIAMACHY-retrieved and SAGE II–measured zonal mean aerosol extinction profiles are less than 20% for the 20–30°N and 30–40°N latitude zones, and less than 25% for the 40–50°N zone. The stratospheric aerosol optical depths in this altitude range calculated from SCIAMACHY retrievals are in good agreement with SAGE II measurements, with present differences less than 6% for the three latitude zones. The aerosol retrievals from SCIAMACHY observations are combined with ...

Natural and Anthropogenic Aerosol Trends from Satellite and Surface Observations and Model Simulations over the North Atlantic Ocean from 2002 to 2012

AbstractAerosols contribute to Earth’s radiative budget both directly and indirectly, and large uncertainties remain in quantifying aerosol effects on climate. Variability in aerosol distribution and properties, as might result from changing emissions and transport processes, must be characterized. In this study, variations in aerosol loading across the eastern seaboard of the United States and the North Atlantic Ocean during 2002 to 2012 are analyzed to examine the impacts of anthropogenic emission control measures using monthly mean data from MODIS, AERONET, and IMPROVE observations and Goddard Chemistry Aerosol Radiation and Transport (GOCART) model simulation. MODIS observes a statistically significant negative trend in aerosol optical depth (AOD) over the midlatitudes (−0.030 decade−1). Correlation analyses with surface AOD from AERONET sites in the upwind region combined with trend analysis from GOCART component AOD confirm that the observed decrease in the midlatitudes is chiefly associated with anthropogenic aerosols that exhibit significant negative trends from the eastern U.S. coast extending over the western North Atlantic. Additional analysis of IMPROVE surface PM2.5 observations demonstrates statistically significant negative trends in the anthropogenic components with decreasing mass concentrations over the eastern United States. Finally, a seasonal analysis of observational datasets is performed. The negative trend seen by MODIS is strongest during spring (MAM) and summer (JJA) months. This is supported by AERONET seasonal trends and is identified from IMPROVE seasonal trends as resulting from ammonium sulfate decreases during these seasons.

An 11-year global gridded aerosol optical thickness reanalysis (v1.0) for atmospheric and climate sciences

Abstract. While stand alone satellite and model aerosol products see wide utilization, there is a significant need in numerous atmospheric and climate applications for a fused product on a regular grid. Aerosol data assimilation is an operational reality at numerous centers, and like meteorological reanalyses, aerosol reanalyses will see significant use in the near future. Here we present a standardized 2003–2013 global 1 × 1° and 6-hourly modal aerosol optical thickness (AOT) reanalysis product. This data set can be applied to basic and applied Earth system science studies of significant aerosol events, aerosol impacts on numerical weather prediction, and electro-optical propagation and sensor performance, among other uses. This paper describes the science of how to develop and score an aerosol reanalysis product. This reanalysis utilizes a modified Navy Aerosol Analysis and Prediction System (NAAPS) at its core and assimilates quality controlled retrievals of AOT from the Moderate Resolution Imaging Spectroradiometer (MODIS) on Terra and Aqua and the Multi-angle Imaging SpectroRadiometer (MISR) on Terra. The aerosol source functions, including dust and smoke, were regionally tuned to obtain the best match between the model fine- and coarse-mode AOTs and the Aerosol Robotic Network (AERONET) AOTs. Other model processes, including deposition, were tuned to minimize the AOT difference between the model and satellite AOT. Aerosol wet deposition in the tropics is driven with satellite-retrieved precipitation, rather than the model field. The final reanalyzed fine- and coarse-mode AOT at 550 nm is shown to have good agreement with AERONET observations, with global mean root mean square error around 0.1 for both fine- and coarse-mode AOTs. This paper includes a discussion of issues particular to aerosol reanalyses that make them distinct from standard meteorological reanalyses, considerations for extending such a reanalysis outside of the NASA A-Train era, and examples of how the aerosol reanalysis can be applied or fused with other model or remote sensing products. Finally, the reanalysis is evaluated in comparison with other available studies of aerosol trends, and the implications of this comparison are discussed.

Discussion on linear long-term trends in aerosol and cloud properties over India and its surrounding waters

Spatial and seasonal variations in the linear long-term trend estimates of aerosol and cloud properties over Indian subcontinent and the surrounding oceanic regions of Bay of Bengal (BoB) and Arabian Sea (AS) are studied and discussed utilizing 12 complete years (2003–2014) of Moderate Resolution Imaging Spectroradiometer (MODIS) derived Aerosol and cloud products. Annual Aerosol Optical Depth (AOD) trends (in terms of AOD/year) are found to be positive (upward) over most of the study region with a spatial mean (median) value of ∼0.0065 (0.0064) and exhibited significant spatial and seasonal heterogeneity. Over Indian landmass AOD trends and their statistical significance decreased towards north along the Indo-Gangetic plains (IGP), for which the probable causes are discussed. Same kind of pattern in AOD trends has been observed as we move deeper into the oceanic regions of BoB and AS, away from Indian subcontinent. Observed trend patterns are discussed in light of the possible increase in emissions (over Indian landmass) and transported aerosol component, co-variation with trends in meteorological parameters and their possible feedbacks. Trend maps in seasonal AOD are shown to understand the aerosol build up over the study region under varying meteorological conditions. Seasonal AOD trend patterns resembled the synoptic scale wind circulation over the study region revealing that the upward trend in aerosol abundance over the adjoining oceanic regions of India is a result of effective transport of increasing emissions over India on to them. No significant trends in cloud properties (over the whole study region) are depicted in concert with that of aerosols, except over few pockets. The study also highlighted the role of large scale atmospheric processes in modulating the shape of the AOD time series over the regions with significant abundance of natural aerosol component (dust).

Modelled and observed changes in aerosols and surface solar radiation over Europe between 1960 and 2009

Abstract. Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry–climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry–climate model for the period 1960–2009 against extensive ground-based observations of sulfate aerosol mass (1978–2009), total suspended particle matter (SPM, 1978–1998), PM10 (1997–2009), aerosol optical depth (AOD, 2000–2009), aerosol size distributions (2008–2009) and surface solar radiation (SSR, 1960–2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = −0.4), SPM (NMBF = −0.9), PM10 (NMBF = −0.2), aerosol number concentrations (N30 NMBF = −0.85; N50 NMBF = −0.65; and N100 NMBF = −0.96) and AOD (NMBF = −0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of −68 % (−78 %), SPM of −42 % (−20 %), PM10 of −9 % (−8 %) and AOD of −11 % (−14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990–2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by > 3.0 W m−2 during the period 1970–2009 in response to changes in anthropogenic emissions and aerosol concentrations.

A 12-year observation of water-soluble ions in TSP aerosols collected at a remote marine location in the western North Pacific: an outflow region of Asian dust

Abstract. In order to characterize the long-term trend of remote marine aerosols, a 12-year observation was conducted for water-soluble ions in TSP (total suspended particulate) aerosols collected from 2001 to 2012 in the Asian outflow region at Chichijima Island in the western North Pacific. We found a clear difference in chemical composition between the continentally affected and marine background air masses over the observation site. Asian continental air masses are delivered from late autumn to spring, whereas marine air masses were dominated in summer. Concentrations of non-sea salt (nss-) SO42−, NO3−, NH4+, nss-K+ and nss-Ca2+ are high in winter and spring and low in summer. On the other hand, MSA− (methanesulfonate) exhibits higher concentrations during spring and winter, probably due to springtime dust bloom or due to the direct continental transport of MSA− to the observation site. We could not find any clear decadal trend for Na+, Cl−, Mg2+ and nss-Ca2+ in all seasons, although there exists a clear seasonal trend. However, concentrations of nss-SO42− continuously decreased from 2007 to 2012, probably due to the decreased SO2 emissions in East Asia especially in China. In contrast, nss-K+ and MSA− concentrations continuously increased from 2001 to 2012 during winter and spring seasons, demonstrating that biomass burning and/or terrestrial biological emissions in East Asia are being increasingly transported from the Asian continent to the western North Pacific. This study also demonstrates that Asian dusts can act as an important source of nutrients for phytoplankton and thus sea-to-air emission of dimethyl sulfide over the western North Pacific.

Satellite Observed Aerosol Optical Thickness and Trend around Megacities in the Coastal Zone

Nearly 30-year aerosol optical thickness (AOT) climate data record (CDR) derived from the operational satellite observations of National Ocean and Atmospheric Administration (NOAA) Advanced Very High Resolution Radiometer (AVHRR) is used to study the AOT trends over seventeen megacities in the coast zone (MCCZ). Linear trends are derived from monthly and seasonal mean AOT in the past three decades and used in the analysis. The results indicate the following: (1) AOT around a MCCZ in fast developing countries has relatively high value and a positive trend with a confidence level generally above 95%; (2) AOT around a MCCZ in industrialized countries has relatively low value and a negative trend with a confidence level generally above 95%; (3) AOT values and their trends show distinct seasonal variations in MCCZ, which can be explained somewhat by the seasonal variations of meteorological conditions. AOT trend is an effective index for examining the efficacy of air pollution control policies implemented for these megacities.

AERONET data investigation of the aerosol mixtures over Iasi area, One-year time scale overview

In order to analyze the troposphere dynamics under particular conditions in North-East region of Romania, various types of aerosols chemical compositions have been studied using complementary techniques. Thus, the seasonal trends of aerosols and its external influences have been studied using aerosol optical properties retrieved from Aerosol Robotic Network (AERONET). Complementary studies were taken into account by using several meteorological factors, computational models and meteorological data. Moreover, this paper presents optical properties analysis of different types of aerosols and the seasonal variability of them in one year of measurements. The major categories of aerosol types are evidenced, such as urban/industrial aerosol, biomass burning and mineral dust.

Long-term trends in aerosol and precipitation composition over the western North Atlantic Ocean at Bermuda

Abstract. Since the 1980s, emissions of SO2 and NOx (NO + NO2) from anthropogenic sources in the United States (US), Canada, and Europe have decreased significantly suggesting that the export of oxidized S and N compounds from surrounding continents to the atmosphere overlying the North Atlantic Ocean (NAO) has also decreased. The chemical compositions of aerosols and precipitation sampled daily on Bermuda (32.27° N, 64.87° W) from 1989 to 1997 and from 2006 to 2009 were evaluated to quantify the magnitudes, significance, and implications of associated tends in atmospheric composition. The chemical data were stratified based on FLEXPART (FLEXible PARTicle dispersion model) retroplumes into four discrete transport regimes: westerly flow from eastern North America (NEUS/SEUS); easterly trade-wind flow from northern Africa and the subtropical NAO (Africa); long, open-ocean, anticyclonic flow around the Bermuda High (Oceanic); and transitional flow from the relatively clean open ocean to the polluted eastern North America (North). Based on all data, annual average concentrations of non-sea-salt (nss) SO42– associated with aerosols and annual volume-weighted-average (VWA) concentrations in precipitation decreased significantly (by 22% and 49%, respectively) whereas annual VWA concentrations of NH4+ in precipitation increased significantly (by 70%). Corresponding trends in aerosol and precipitation NO3– and of aerosol NH4+ were insignificant. Nss SO42– in precipitation under NEUS/SEUS and Oceanic flow decreased significantly (61% each) whereas corresponding trends in particulate nss SO42– under both flow regimes were insignificant. Trends in precipitation composition were driven in part by decreasing emissions of SO2 over upwind continents and associated decreases in anthropogenic contributions to nss SO42– concentrations. Under NEUS/SEUS and Oceanic flow, the ratio of anthropogenic to biogenic contributions to nss SO42– in the column scavenged by precipitation were relatively greater than those in near surface aerosol, which implies that, for these flow regimes, precipitation is a better indicator of overall anthropogenic impacts on the lower troposphere. Particulate nss SO42– under African flow also decreased significantly (34%) whereas the corresponding decrease in nss SO42– associated with precipitation was insignificant. We infer that these trends were driven in part by reductions in the emissions and transport of oxidized S compounds from Europe. The lack of significant trends in NO3– associated with aerosols and precipitation under NEUS/SEUS flow is notable in light of the large decrease (37%) in NOx emissions in the US and Canada over the period of record. Rapid chemical processing of oxidized N in marine air contributed to this lack of correspondence. Decreasing ratios of nss SO42– to NH4+ and the significant decreasing trend in precipitation acidity (37%) indicate that the total amount of acidity in the multiphase gas–aerosol system in the western NAO troposphere decreased over the period of record. Decreasing aerosol acidities would have shifted the phase partitioning of total NH3 (NH3 + particulate NH4+ towards the gas phase thereby decreasing the atmospheric lifetime of total NH3 against wet plus dry deposition. The trend of increasing NH4+ in precipitation at Bermuda over the period of record suggests that NH3 emissions from surrounding continents also increased. Decreasing particulate nss SO42– in near-surface air under NEUS/SEUS flow over the period of record implies that the corresponding shortwave scattering and absorption by nss S and associated aerosols constituents also decreased. These changes in radiative transfer suggest a corresponding lower limit for net warming over the period in the range of 0.1–0.3 W m–2.