Aerosol Radiative Properties Research Articles

Aerosol above-cloud direct radiative effect and properties in the Namibian region during the AErosol, RadiatiOn, and CLOuds in southern Africa (AEROCLO-sA) field campaign – Multi-Viewing, Multi-Channel, Multi-Polarization (3MI) airborne simulator and sun photometer measurements

Abstract. We analyse the airborne measurements of above-cloud aerosols from the AErosol, RadiatiOn, and CLOuds in southern Africa (AEROCLO-sA) field campaign performed in Namibia during August and September 2017. The study aims to retrieve the aerosol above-cloud direct radiative effect (DRE) with well-defined uncertainties. To improve the retrieval of the aerosol and cloud properties, the airborne demonstrator of the Multi-Viewing, Multi-Channel, Multi-Polarization (3MI) satellite instrument, called the Observing System Including PolaRisation in the Solar Infrared Spectrum (OSIRIS), was deployed on-board the SAFIRE (Service des Avions Français Instrumentés pour la Rechercheen Environnement) Falcon 20 aircraft during 10 flights performed over land, over the ocean, and along the Namibian coast. The airborne instrument OSIRIS provides observations at high temporal and spatial resolutions for aerosol above clouds (AACs) and cloud properties. OSIRIS was supplemented with the Photomètre Léger Aéroporté pour la surveillance des Masses d'Air version 2 (PLASMA2). The combined airborne measurements allow, for the first time, the validation of AAC algorithms previously developed for satellite measurements. The variations in the aerosol properties are consistent with the different atmospheric circulation regimes observed during the deployment. Airborne observations typically show strong aerosol optical depth (AOD; up to 1.2 at 550 nm) of fine-mode particles from biomass burning (extinction Ångström exponent varying between 1.6 and 2.2), transported above bright stratocumulus decks (mean cloud top around 1 km above mean sea level), with cloud optical thickness (COT) up to 35 at 550 nm. The above-cloud visible AOD retrieved with OSIRIS agrees within 10 % of the PLASMA2 sun photometer measurements in the same environment. The single scattering albedo (SSA) is one of the most influential parameters on the AAC DRE calculation that remains largely uncertain in models. During the AEROCLO-sA campaign, the average SSA obtained by OSIRIS at 550 nm is 0.87, which is in agreement within 3 %, on average, with previous polarimetric-based satellite and airborne retrievals. The strong absorption of the biomass burning plumes in the visible range is generally consistent with the observations from the Aerosol Robotic Network (AERONET) ground-based sun photometers. This, however, shows a significant increase in the particles' absorption at 440 nm in northern Namibia and Angola, which indicates more absorbing organic species within the observed smoke plumes. Biomass burning aerosols are also vertically collocated, with significant amounts of water content up to the top of the plume at around 6 km height in our measurements. The detailed characterization of aerosol and cloud properties, water vapour, and their uncertainties obtained from OSIRIS and PLASMA2 measurements allows us to study their impacts on the AAC DRE. The high-absorbing load of AAC, combined with high cloud albedo, leads to unprecedented DRE estimates, which are higher than previous satellite-based estimates. The average AAC DRE calculated from the airborne measurements in the visible range is +85 W m−2 (standard deviation of 26 W m−2), with instantaneous values up to +190 W m−2 during intense events. These high DRE values, associated with their uncertainties, have to be considered as new upper cases in order to evaluate the ability of models to reproduce the radiative impact of the aerosols over the southeastern Atlantic region.

Impact of COVID-19 lockdown on aerosol optical and radiative properties over Indo-Gangetic Plain

Aerosol optical and radiative properties, measured with the ground based sun-sky radiometer (under AERONET), were explored at Kanpur in the central and Gandhi College (Ballia) in the Eastern Indo-Gangetic Plain (IGP) in Northern India during January to July 2019 (non-lockdown) and 2020 (lockdown). This year 2020 is marked an overall reduction of 15.79% and 3.39% in aerosol optical depth (AOD) than year 2019 at Kanpur and Gandhi College respectively. Lockdown 1 (23rd March to 14th April 2020) showed a reduction of 52.52% and 42.22% in AOD compared to pre-lockdown condition at Kanpur and Gandhi College respectively. Higher values of angstrom exponent measured at Eastern region (1.13 ± 0.17) than central region (0.97 ± 0.26) indicating the dominance of fine particles at Gandhi College. There was an overall reduction of 1.31% in single scattering albedo (SSA) at Kanpur while 4.34% reduction was observed at Gandhi College in year 2020 than 2019. The resultant atmospheric forcing and heating rate shows 11.86% reduction at Kanpur while 35.27% increase at Gandhi College during the lockdown period in 2020 compared to 2019. However, these values were found to decrease by 23.48% and 15.07% at Kanpur and Gandhi College respectively during the strict lockdown period compared to year 2019.

Optical Characteristics and Radiative Properties of Aerosols in Harbin, Heilongjiang Province during 2017

This study considers aerosol optical properties and direct radiative forcing over Harbin (126.63° E, 45.75° N), the highest latitude city in Northeast China, during 2017. Observations based on the CE-318 sun-photometer show that the annual mean values of the aerosol optical depth (AOD) at 500 nm and the Angstrom exponent (AE) at 440–870 nm over Harbin are respectively 0.26 ± 0.20 and 1.36 ± 0.26. Aerosol loading is the highest in the spring followed by winter, and the lowest loading is in autumn. AE440–870 is the highest in summer, second highest in winter, and lowest in autumn. The Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model is used to estimate the shortwave aerosol radiative forcing at the top of the atmosphere, on the Earth’s surface and in the atmosphere, and the annual mean values are −16.36 ± 18.42 Wm−2, −71.01 ± 27.37 Wm−2 and 54.65 ± 30.62 Wm−2, respectively, which indicate that aerosols cause climate effects of cooling the earth-atmosphere system, cooling the earth’s surface and heating the atmosphere. Four main aerosol types in Harbin are classified via AOD and AE. Specifically, clean continental, mixed type, biomass burning and urban industry, and desert dust aerosols accounted for 51%, 38%, 9%, and 2% of the total, respectively. Aerosol radiative forcing varies greatly in different seasons, and the aerosol load and type from different emission sources have an important influence on the seasonal variation of radiative forcing.

In situ optical and microphysical properties of tropospheric aerosols in the Canadian High Arctic from 2016 to 2019

Since aerosols are an integral part of the Arctic climate system, understanding aerosol radiative properties and the relation of these properties to each other is important for constraining aerosol radiative forcing effects in this remote region where measurements are sparse. In situ measurements of aerosol size distribution, aerosol light scattering and absorption were taken near Eureka (80.05oN, 86.42oW), on Ellesmere Island, in the Canadian High Arctic over three consecutive years to provide insights into radiative properties of Arctic aerosols.During periods of Arctic haze, we find that the single scattering albedo (SSA) at 405 nm is generally higher and more stable than that determined at 870 nm, with values ranging between 0.90–0.99 and 0.79–0.97, respectively. Events with elevated absorption coefficients (Babs) exhibit generally an absorption Ångström exponent (AAE) of around 1 suggesting that black carbon (BC) is the dominant absorbing aerosol for the measurement period. AAE values close to 2 occurring with scattering Ångström exponent (SAE) values near 0 and SAE values below 0 occasionally observed in December indicate a potential contribution from mineral dust aerosols in late fall and early winter. The apparent real and imaginary parts of the complex refractive index at 405 nm have been found to range between 1.6–1.9 and 0.002–0.02, respectively. The low imaginary component indicates very weak intrinsic absorption compared to BC-rich aerosols.Systematic variabilities between different aerosol optical and microphysical properties depend strongly on the given wavelength. SSA at 405 nm shows a strong inverse dependence with Babs, because Babs correlates positively with the imaginary component of the refractive index. On the other hand, SSA at 870 nm correlates with scattering coefficient (Bsca) and not with Babs due to a greater sensitivity to the ambient particle size distribution for 870 nm scattering. Smaller particles with higher SAE that are prevalent during less polluted periods only weakly scatter at 870 nm leading to lower SSA when Bsca is also low.Lastly, FLEXPART back-trajectories show that lower aerosol SSA and higher Babs correspond to air masses which are more influenced by Eurasian and Alaskan regions, including regions known to have important BC emissions. This work emphasizes the important variability in Arctic aerosol optical properties during winter and spring, which is likely due to changes in source regions.

How secondary inorganic aerosols from Delhi influence aerosol optical and radiative properties at a downwind sub-urban site over Indo-Gangetic Basin?

The particulate matters less than 10 μm sizes (PM10) were measured at a highly polluted urban environment of Delhi, and simultaneously at a downwind semi-urban site, Gual Pahari, in the north-west Indo-Gangetic Basin (IGB). The measurements were conducted during January–December 2008 to compare and contrast aerosol emissions, compositions and related optical and radiative properties for two different environments. While the total PM10 was about 30% lower at Gual Pahari as compared to Delhi, the total mass of water-soluble inorganic species (WSIs) was significantly enhanced (~23%) at Gual Pahari. Amongst WSIs, the major secondary inorganic species (SIs) were about 52% higher at Gual Pahari as compared to Delhi, with elevated levels in the post-monsoon/winter seasons. In contrast, the major crustal species were about 76% higher at Delhi as compared to Gual Pahari, with elevated levels in the summer/monsoon seasons. This indicates a strong inter-seasonal spatial variability in aerosol sources and compositions at these sites. Further, the simulations using aerosol optical model had resulted mean absorption coefficient (babs) and single scattering albedo (SSA) higher by about 50% and lower by about 18%, respectively, at Delhi (babs, 147 ± 63 M m−1 and SSA, 0.65 ± 0.12) as compared to Gual Pahari (babs, 73 ± 26 M m−1 and SSA, 0.79 ± 0.07). This reveals relative abundance of absorbing particles at Delhi compared to Gual Pahari. As a result, the estimated mean atmospheric forcing was 91 ± 23 W m−2 at Delhi, which was ~55% higher as compared to Gual Pahari. This is further corroborated with observed higher heating rate at Delhi (2.5 ± 0.7 K day−1) as compared to Gual Pahari (1.1 ± 0.4 K day−1). Our results highlight that diverse near-surface emissions together with atmospheric processing leads to strong inter-seasonal spatial heterogeneity in aerosol chemical, optical and radiative properties between the adjacent distinct sites. This has an important implication for a city-scale air pollution modeling.

Interferences with aerosol acidity quantification due to gas-phase ammonia uptake onto acidic sulfate filter samples

Abstract. Measurements of the mass concentration and chemical speciation of aerosols are important to investigate their chemical and physical processing from near emission sources to the most remote regions of the atmosphere. A common method to analyze aerosols is to collect them onto filters and analyze the filters offline; however, biases in some chemical components are possible due to changes in the accumulated particles during the handling of the samples. Any biases would impact the measured chemical composition, which in turn affects our understanding of numerous physicochemical processes and aerosol radiative properties. We show, using filters collected onboard the NASA DC-8 and NSF C-130 during six different aircraft campaigns, a consistent, substantial difference in ammonium mass concentration and ammonium-to-anion ratios when comparing the aerosols collected on filters versus an Aerodyne aerosol mass spectrometer (AMS). Another online measurement is consistent with the AMS in showing that the aerosol has lower ammonium-to-anion ratios than obtained by the filters. Using a gas uptake model with literature values for accommodation coefficients, we show that for ambient ammonia mixing ratios greater than 10 ppbv, the timescale for ammonia reacting with acidic aerosol on filter substrates is less than 30 s (typical filter handling time in the aircraft) for typical aerosol volume distributions. Measurements of gas-phase ammonia inside the cabin of the DC-8 show ammonia mixing ratios of 45±20 ppbv, consistent with mixing ratios observed in other indoor environments. This analysis enables guidelines for filter handling to reduce ammonia uptake. Finally, a more meaningful limit of detection for University of New Hampshire Soluble Acidic Gases and Aerosol (SAGA) filters collected during airborne campaigns is ∼0.2 µg sm−3 of ammonium, which is substantially higher than the limit of detection of ion chromatography. A similar analysis should be conducted for filters that collect inorganic aerosol and do not have ammonia scrubbers and/or are handled in the presence of human ammonia emissions.

Optical, Radiative and Chemical Characteristics of Aerosol in Changsha City, Central China

Industrial pollution has a significant effect on aerosol properties in Changsha City, a typical city of central China. Therefore, year-round measurements of aerosol optical, radiative and chemical properties from 2012 to 2014 at an urban site in Changsha were analyzed. During the observation period, the energy structure was continuously optimized, which was characterized by the reduction of coal combustion. The aerosol properties have obvious seasonal variations. The seasonal average aerosol optical depth (AOD) at 500 nm ranged from 0.49 to 1.00, single scattering albedo (SSA) ranged from 0.93 to 0.97, and aerosol radiative forcing at the top of the atmosphere (TOA) ranged from −24.0 to 3.8 W m−2. The chemical components also showed seasonal variations. Meanwhile, the scattering aerosol, such as organic carbon, SO42−, NO3−, and NH4+ showed a decrease, and elemental carbon increased. Compared with observation in winter 2012, AOD and TOA decreased by 0.14 and −1.49 W m−2 in winter 2014. The scattering components, SO42−, NO3− and NH4+, decreased by 12.8 μg m−3 (56.8%), 9.2 μg m−3 (48.8%) and 6.4 μg m−3 (45.2%), respectively. The atmospheric visibility and pollution diffusion conditions improved. The extinction and radiative forcing of aerosol were significantly controlled by the scattering aerosol. The results indicate that Changsha is an industrial city with strong scattering aerosol. The energy structure optimization had a marked effect on controlling pollution, especially in winter (strong scattering aerosol).

Aerosol optical properties and its type classification based on multiyear joint observation campaign in north China plain megalopolis

Since haze and other air pollution are frequently seen in the North China Plain (NCP), detail information on aerosol optical and radiative properties and its type classification is demanded for the study of regional environmental pollution. Here, a multiyear ground-based synchronous sun photometer observation at seven sites on North China Plain megalopolis from 2013 to 2018 was conducted. First, the annual and seasonal variation of these characteristics as well as the intercomparsion were analyzed. Then the potential relationships between these properties with meteorological factors and the aerosol type classification were discussed. The results show: Particle volume exhibited a decreasing trend from the urban downtown to suburban and the rural region. The annual average aerosol optical depth at 440 nm (AOD440) varied from ∼0.43 to 0.86 over the NCP. Annual average single-scattering albedo at 440 nm (SSA440) varied from ∼0.89 to 0.93, indicating a moderate to slight absorption capacity. Average absorption aerosol optical depth at 440 nm (AAOD440) varied from ∼0.07 to 0.10. The absorption Ångström exponent (AAE) (∼0.89–1.40) indicated the multi-types of absorptive matters originated form nature and anthropogenic emission. The discussion of aerosol composition showed a smaller particle size of aerosol from biomass burning and/or fossil foil consumption with enhanced aerosol scattering and enlarged light extinction. Aerosol classification indicated a large percentage of mixed absorbing aerosol (∼20%–49%), which showed increasing trend between relative humidity (RH) with aerosol scattering and dust was an important environmental pollutant compared to southern China.

Radiative characteristics of near-surface aerosols at a tropical site: An estimation based on concurrent measurements of their physico-chemical characteristics

This study is an attempt to estimate the radiative characteristics of aerosols, namely, the scattering coefficient (βsc), absorption coefficient (βab), extinction coefficient (βex), single scattering albedo (ω) and the phase function P(θ), on a seasonal basis, incorporating the concurrent measurements of aerosol mass loading, size distribution and chemical composition at the tropical coastal site, Thiruvananthapuram. The software package Optical Properties of Aerosols and Clouds (OPAC) has been made use for the estimation of the radiative parameters. This paper presents the seasonal features of aerosol chemical composition and their source characteristics also. Along with this, the association between size-resolved number density of aerosols and their chemical characteristics were also investigated through correlation analysis. The location is significantly influenced by human activities as seen from the dominance of the anthropogenic component which is highest in winter (22%) with comparable values in pre-monsoon and post-monsoon and minimum in monsoon (13%). The sea-salt contribution is found to peak in monsoon (~40%) and attain a minimum in winter. The source characterization using principal component analysis along with back-trajectory analysis showed the seasonally changing mixed aerosol sources over the region. Accordingly, the radiative properties of aerosols also exhibit significant seasonal variations. βsc varied from 0.04 to 0.14 km−1 and βab between 0.01 and 0.05 km−1 over a year. The single-scattering albedo exhibited significant seasonal differences being ~0.71 for winter and ~0.89 (0.55 μm) for monsoon season, indicating the presence of more absorbing aerosols in winter.

Observations of Aerosol, Cloud, Turbulence, and Radiation Properties at the Top of the Marine Boundary Layer over the Eastern North Atlantic Ocean: The ACORES Campaign

AbstractWe report on the Azores Stratocumulus Measurements of Radiation, Turbulence and Aerosols (ACORES) campaign, which took place around Graciosa and Pico Islands/Azores in July 2017. The main objective was to investigate the vertical distribution of aerosol particles, stratocumulus microphysical and radiative properties, and turbulence parameters in the eastern North Atlantic. The vertical exchange of mass, momentum, and energy between the free troposphere (FT) and the cloudy marine boundary layer (MBL) was explored over a range of scales from submeters to kilometers. To cover these spatial scales with appropriate measurements, helicopter-borne observations with unprecedented high resolution were realized using the Airborne Cloud Turbulence Observation System (ACTOS) and Spectral Modular Airborne Radiation Measurement System–Helicopter-Borne Observations (SMART-HELIOS) instrumental payloads. The helicopter-borne observations were combined with ground-based aerosol measurements collected at two continuously running field stations on Pico Mountain (2,225 m above sea level, in the FT), and at the Atmospheric Radiation Measurement (ARM) station on Graciosa (at sea level). First findings from the ACORES observations we are discussing in the paper are as follows: (i) we have observed a high variability of the turbulent cloud-top structure on horizontal scales below 100 m with local temperature gradients of up to 4 K over less than 1 m vertical distance, (ii) we have collected strictly collocated radiation measurements supporting the relevance of small-scale processes by revealing significant inhomogeneities in cloud-top brightness temperature to scales well below 100 m, and (iii) we have concluded that aerosol properties are completely different in the MBL and FT with often-complex stratification and frequently observed burst-like new particle formation.

Vertical distributions of the microscopic morphological characteristics and elemental composition of aerosols over India

Particle morphology and elemental compositions are among the crucial parameters of aerosols required for accurate understanding of the climatic effect of aerosols in the earth-atmosphere system; yet their vertical distributions and region specific properties are poorly characterised due to sparse in-situ measurements. This is the first study to classify and quantify the vertical distributions of the morphological characteristics and elemental composition of aerosols based on single particle as well as bulk chemical analysis over seven geographically diverse regions of northern and central parts of India during spring (April–May, 2013), carried out as a part of Regional Aerosol Warming Experiment (RAWEX). Significant regional distinctiveness in shapes (non-sphericity), sizes and elemental compositions of the airborne particles were conspicuous, having dominance of highly irregular granular aggregates over the north Indian sites. The non-spherical coarse mode particles dominated the lower free tropospheric regions (> 2 km) of the Indo-Gangetic Plains (IGP). These particles could be responsible for enhanced spring time aerosol absorption in the elevated region of the atmosphere. Elemental compositions of the single particle analysis indicate that the free tropospheric layer over the IGP and central India is enriched with Na and Ca compounds mixed with Fe or Al (soil particles), indicating long range transport of crustal aerosols. This finding is very well supported by the bulk particle analysis indicating abundance of Ca2+ in the free troposphere with low contribution of ssNa+. Particles with irregular rough surfaces having dominance of SiO2 were observed over all the study sites. The percentage share of spherical (either smooth or rough) particles to the total morphological characteristics of the particles was found to be highly subdued (< 10%). The present study thus critically assesses the relevant knowledge pertaining to the morphological features of aerosols over the IGP during spring for the accurate estimation of aerosol radiative properties. More such efforts are required in future to study the connections and dependencies between morphological and radiative properties of aerosols in different seasons.

Long-term (2008–2017) analysis of atmospheric composite aerosol and black carbon radiative forcing over a semi-arid region in southern India: Model results and ground measurement

To achieve an in-depth understanding of radiative forcing due to aerosols is a crucial challenge for climate change studies. The first-ever long-term measurement of direct shortwave composite and black carbon aerosol radiative properties over a semi-arid region, Anantapur, in southern India is presented. Long-term variations in Aerosol Optical Depth (AOD) and Black Carbon (BC) mass concentration from December 2007 to November 2017 are discussed with specific emphasis on intra-seasonal variation in aerosol optical properties, meteorology, transport pathways, and their implications for direct short wave radiative forcing over Anantapur. The intra-seasonal mean AOD showed strong seasonal dependence with the highest (0.47 ± 0.03) during summer and lowest (0.28 ± 0.03) during the monsoon. Meanwhile, the intra-seasonal mean (±σ) BC mass concentration was about 3.57 ± 0.45, 2.60 ± 0.58, 1.22 ± 0.18 and 2.24 ± 0.28 μg m−3 during winter, summer, monsoon and post-monsoon respectively. Furthermore, there is an obvious temporal variation in intra-seasonal BC mass concentration during the dry season (winter and summer). To be more specific, the intra-seasonal mean (±σ) BC mass concentration before 2012 (after 2012) during the dry season was about 3.37 ± 0.7 μg m−3 (2.80 ± 0.58 μg m−3), respectively. Concentration weighted trajectory analyses (CWT) revealed that the air masses originated from the continental and polluted environments located in the central and northern parts of India (except monsoon), in regulating BC mass concentration over measurement location. Further, Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) derived aerosol vertical extinction profiles (532 nm) showed that majority aerosols (>250 Mm−1) are confined within 2 km from the surface during winter while in summer particles are distributed throughout the profile (~6 km) with extinction coefficient varying between 200 and 250 Mm−1. The Santa Barbara Discrete Ordinate Radiative Transfer (SBDART) model estimated intra-seasonal mean direct shortwave composite aerosol radiative forcing (DARF) in the atmosphere (ATM) was about 31.13 ± 3.36, 34.82 ± 3.89, 17.10 ± 1.15, and 17.44 ± 1.81 Wm-2 during winter, summer, monsoon and post-monsoon, respectively. The positive signs of ATM forcing in all seasons indicate a warming of the atmosphere, and the corresponding heating rate was around a factor of two higher during the dry season (0.92 ± 0.12 Kday−1) than the wet season (monsoon and post-monsoon) (0.49 ± 0.04 Kday−1). The intra-seasonal mean BC forcing in ATM before 2012 (After 2012) during the dry season was about 24.14 ± 2.85Wm-2(20.09 ± 2.59Wm-2), respectively. The contribution of BC alone to the composite forcing during the study period over the station was ~68%. These findings would be helpful for regional climate studies and making air pollution control policy over the region.

Environmental impacts of fireworks on aerosol characteristics and radiative properties over a mega city, India

The study focusses to investigate the variations in aerosol characteristics, concentrations and radiative properties due to the burning of firecrackers during Diwali festival event followed with New year festival celebrations over a representative urban environment. A six day's long intensive in situ measurements of Black Carbon, Particulate Matter and Aerosol Optical Depth were collected to capture pre to post-Diwali and New Year festival celebrations marked with massive fireworks. We observed an increase of 286%, 89.5%, and 60.5%, in BC, PM10, and PM2.5 concentrations, respectively on festival night as compared to pre-event days. An increase in in situ measured AOD is comparable with concurrent satellite derived AOD. Angstrom exponent, α > 1.0 along with high turbidity coefficient; β estimated for the festival period clearly implies the abundance of fine-mode particles, probably the smoke aerosols loading from fireworks. The Mie-scattered return signals received by the ground based Raman LiDAR at 532 nm showed an increased concentration of ‘anthropogenic aerosols’, attributed to the increased crackers activity. Space based CALIPSO LiDAR observations also validate the presence of ‘polluted dust’ and ‘smoke’ types aerosols at the near surface to 5 km altitude over the study area. A sharp increase in gaseous air pollutants like SO2 and NOx concentrations exceeding the National Ambient Air Quality Standards is also observed. The COART model run simulations in SWIR region showed an increased ‘cooling’ at the surface (−125 Wm−2 to −185 Wm−2) as compared to ‘warming’ in the atmosphere during the event period. A maximum heating rate (1.9 Kday−1) due to total aerosol radiative forcing is also estimated. These investigations provide useful insights into the impact of burning firecrackers on urban air quality besides radiative impacts at a regional scale. Such celebration induced air pollution events may lead to severe health impacts; particularly respiratory and cardiovascular ailments in the resident population.

Year-round aerosol characteristics and radiative effects in the South Asian pollution outflow over a background site in the Maldives

Aerosol radiative properties using recently available high-quality columnar aerosol data collected at several AERONET sites in South Asia, with a focus on pollution outflow from continental South Asia observed over Hanimaadhoo in Maldives, a small island in northern Indian Ocean are quantified. The seasonal mean aerosol optical depth (AOD) over Hanimaadhoo is ≥ 0.3 (except ca. 0.2 during monsoon season), and single scattering albedo (SSA) is > 0.90 in all seasons. Fine mode aerosols contribute dominantly to AOD. SSA decreases as a function of wavelength due to influence of continental aerosols, except during the monsoon season when its spectral trend reverses due to increase in dust. Carbonaceous aerosols dominate (>90%) contribution to absorption AOD (AAOD). Black carbon (BC) and brown carbon (BrC) contribute >75% and <25%, respectively, to AAOD due to carbonaceous aerosols. The observed seasonal mean aerosol radiative forcing at the surface (ARFSFC), at the top of the atmosphere (ARFTOP) and in the atmosphere (ARFATM) is > −25 Wm-2, >−20 Wm-2 and ~+20 Wm-2, respectively. Aerosol loading and atmospheric heating have increased over this background site over the last decade. A regional-scale analysis of aerosol properties and radiative effects across and surrounding the Indo-Gangetic Plain (IGP) shows that AOD is ≥ 0.3 over entire region, and aerosols reduce seasonally 30–50 Wm-2 of solar radiation reaching the surface, contributing significantly to solar dimming effect. The atmospheric solar heating rate due to aerosols (HR) is ≥ 1 K day−1 across IGP. These high ARFs, ARFESFC and HR, and increasing trends have significant implications to climate and hydrological cycle over South Asia and beyond.

Multidecadal trend analysis of in situ aerosol radiative properties around the world

Abstract. In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes.

Differing precipitation response between solar radiation management and carbon dioxide removal due to fast and slow components

Abstract. Solar radiation management (SRM) and carbon dioxide removal (CDR) are geoengineering methods that have been proposed to mitigate global warming in the event of insufficient greenhouse gas emission reductions. Here, we have studied temperature and precipitation responses to CDR and SRM with the Representative Concentration Pathway 4.5 (RCP4.5) scenario using the MPI-ESM and CESM Earth system models (ESMs). The SRM scenarios were designed to meet one of the two different long-term climate targets: to keep either global mean (1) surface temperature or (2) precipitation at the 2010–2020 level via stratospheric sulfur injections. Stratospheric sulfur fields were simulated beforehand with an aerosol–climate model, with the same aerosol radiative properties used in both ESMs. In the CDR scenario, atmospheric CO2 concentrations were reduced to keep the global mean temperature at approximately the 2010–2020 level. Results show that applying SRM to offset 21st century climate warming in the RCP4.5 scenario leads to a 1.42 % (MPI-ESM) or 0.73 % (CESM) reduction in global mean precipitation, whereas CDR increases global precipitation by 0.5 % in both ESMs for 2080–2100 relative to 2010–2020. In all cases, the simulated global mean precipitation change can be represented as the sum of a slow temperature-dependent component and a fast temperature-independent component, which are quantified by a regression method. Based on this component analysis, the fast temperature-independent component of the changed atmospheric CO2 concentration explains the global mean precipitation change in both SRM and CDR scenarios. Based on the SRM simulations, a total of 163–199 Tg S (CESM) or 292–318 Tg S (MPI-ESM) of injected sulfur from 2020 to 2100 was required to offset global mean warming based on the RCP4.5 scenario. To prevent a global mean precipitation increase, only 95–114 Tg S was needed, and this was also enough to prevent global mean climate warming from exceeding 2∘ above preindustrial temperatures. The distinct effects of SRM in the two ESM simulations mainly reflected differing shortwave absorption responses to water vapour. Results also showed relatively large differences in the individual (fast versus slow) precipitation components between ESMs.

Physico-chemical characterization and sink mechanism of atmospheric aerosols over South-west India

The properties of the atmospheric aerosols depend on the source region and on the modifications that occur during their transport in the air. We have studied physical and chemical properties of aerosols along with their sink mechanism over two locations in southwest India, an urban site (Pune) and well-established climate observatory at Sinhagad (SINH), which represents rural and high altitude site. The ground-based measurements of aerosols, together with their radiative properties in this study have provided means to understand the observed variability and the impact on the aerosol radiative properties effectively over this region. The annual mean elemental carbon concentration (3.4 µg m− 3) at Pune was observed about three times higher compared to SINH (1.3 µg m− 3), indicating strong emissions of carbon-rich aerosols at the urban location. Aerosol optical properties were derived using the OPAC model which were used to compute the Aerosol radiative forcing (ARF) over both stations calculated using SBDART (Santa Barbara DISORT Atmospheric Radiative Transfer) model shows pronounced seasonal variations due to changes in aerosol optical depth and single scattering albedo at both locations. The year-round ARF was 4–5 times higher over Pune (31.4 ± 3.5 Wm− 2) compared to SINH (7.2 ± 1.1 Wm− 2). The atmospheric heating rate due to aerosols shows a similar pattern as ARF for these locations. The heating was higher in the wintertime, ~ 0.9–1.6 K day− 1 at Pune, and ~ 0.3–0.6 K day− 1 at SINH. The estimated scavenging ratio was found high for NO3− and Ca.2+. The wet deposition fluxes of Cl−, SO42−, Na+, Mg2+ were observed higher for SINH as compared to Pune, due to the high amount of rain received at SINH.

A La Niña‐Like Climate Response to South African Biomass Burning Aerosol in CESM Simulations

AbstractThe climate response to atmospheric aerosols, including their effects on dominant modes of climate variability like El Niño–Southern Oscillation (ENSO), remains highly uncertain. This is due to several sources of uncertainty, including aerosol emission, transport, removal, vertical distribution, and radiative properties. Here, we conduct coupled ocean‐atmosphere simulations with two versions of the Community Earth System Model (CESM) driven by semiempirical fine‐mode aerosol direct radiative effects without dust and sea salt. Aerosol atmospheric heating off the west coast of Africa—most of which is due to biomass burning—leads to a significant atmospheric dynamical response, including localized ascent and upper‐level divergence. Coupled Model Intercomparison Project version 6 (CMIP6) biomass burning simulations support this response. Moreover, CESM shows that the anomalous aerosol heating in the Atlantic triggers an atmospheric teleconnection to the tropical Pacific, including strengthening of the Walker circulation. The easterly trade winds accelerate, and through coupled ocean‐atmosphere processes and the Bjerknes feedback, a La Niña‐like response develops. Observations also support a relationship between south African biomass burning emissions and ENSO, with La Niña events preceding strong south African biomass burning in boreal fall. Our simulations suggest a possible two‐way feedback between ENSO and south African biomass burning, with La Niña promoting more biomass burning emissions, which may then strengthen the developing La Niña.

Long Term Analysis of Optical and Radiative Properties of Aerosols in the Amazon Basin

ABSTRACT The Amazon region is an excellent laboratory for analysis of natural aerosols in the wet season; however, in the dry season the biomass burning emissions highly influence it, which considerably alters the physical and chemical properties of the atmosphere. We analyzed long-term time series (2000–2017) of optical and radiative properties of aerosols during dry and rain seasons from nine AERONET stations located in the Amazon Basin (Western Brazil). Aerosols have been classified into two groups: organic carbon (OC) and elemental carbon (EC), which allowed quantification of their effects on the radiative forcing for these sites. It was possible to conclude that the optical depth values of aerosols (AOD 500 nm), which remained in a downward inclination beginning in 2010 to 2012, returned to rise since 2013. The analysis showed that the fraction of biogenic particles varied from approximately 38% to 67% at the site of Manaus EMBRAPA. However, for ATTO this fraction remained practically constant throughout the year, around 68% as the fraction of OC-EC went from approximately 16 to 27%. In that way, the study found that in the central Amazon region, in the dry season, the OC fraction generates instantaneous effects of up to –100 W m–2 in the radiative surface forcing (FR-Surface), while in the Cerrado region (Cuiaba) the instantaneous values reached up to –350 W m–2. The impact of the primary biogenic particles on the radiative flux resulted in a mean, approximately –20 W m–2 FR-Surface, representing 45% of the total effect caused by aerosols in the Amazon.

Anthropogenic and meteorological drivers of 1980–2016 trend in aerosol optical and radiative properties over the Yangtze River Basin

Since the reform and opening up, Yangtze River Basin (YRB) with rapid industrialization and urbanization has become the most important source of anthropogenic aerosol emissions. However, the drivers of long-term trends in aerosol optical and radiative properties have not yet been adequately clarified. In this study, the multiple linear regression (MLR) and geographically weighted regression (GWR) models were employed to quantitatively estimate the impact of anthropogenic emissions, land use cover changes, urban forms and meteorological conditions on aerosol optical depth (AOD) and direct radiative effect (ADRE). A trend analysis revealed that over-increasing trends in AOD and ADRE were curbed around 2010. In addition, there were remarkable regional differences with respect to the effects of anthropogenic and meteorological factors on aerosol trends. Anthropogenic emissions dominated the growth of AOD and ADRE in the middle and lower reaches of the YRB after 1980, but not in the source of the YRB. Besides, the expansion of built-up land (at a 5.79% rate of increase) during 1980–2010 mainly occurred in the YRD, CC, and SB, which thus accelerated the growth of AOD and ADRE. Furthermore, AOD-ADRE was positively related to the patch area (CA), patch number (NP), and patch edge density (ED), but negatively associated with the largest patch index (LPI). It indicated that a compact urban form could mitigate aerosol loadings by enhancing urban connectivity and reducing vehicle dependence. Finally, a rise in temperature was found to be one of the driving factors for AOD growth. However, the theoretical growth in AOD (0.00084 yr−1) in relation to temperature rise was far less than the actual growth (0.0065 yr−1).