Aerosol Direct Radiative Forcing Research Articles

Aerosol optical properties and radiative effect under different weather conditions in Harbin, China

The aerosol optical properties and radiative effect under different weather conditions in Harbin (126.63°E, 45.75°N) were analyzed based on ground-based Sun/Sky radiometric (CE-318) measurements during September 2016-April 2017. The means values of aerosol optical depth (AOD500) and Angstrom exponent (AE440–870) were 0.37 ± 0.27 and 1.08 ± 0.33, respectively. The mean AOD500 under four weather conditions are apparently higher in severe pollution (Se-Po) days (0.80 ± 0.31) and moderate pollution (Mo-Po) days (0.53 ± 0.25) but lower in slight pollution (Sl-Po) days (0.37 ± 0.26) and no pollution (No-Po) days (0.26 ± 0.20), while the mean values of AE440–870 maintain high, varying from 0.98 to 1.25. The higher AE440–870 indicated that the air quality in Harbin is mainly affected by aerosols originated from anthropogenic sources. The daily values of shortwave (0.25–4 μm) direct aerosol radiative forcing (DARF) at top/bottom of atmosphere (TOA/BOA) were estimated through Santa Barbara DISORT Atmosphere Radiative Transfer (SBDART) model. Further, the aerosol radiative forcing efficiency (ARFE), radiation flux (RF) and atmosphere heating rate (HR) in Harbin were also estimated by the SBDART model.

Influence of aerosol hygroscopicity and mixing state on aerosol optical properties in the Pearl River Delta region, China

Both the effects of aerosol hygroscopicity and mixing state on aerosol optical properties were analyzed using ground-based measurements and a Mie model in this study. The sized-resolved particle hygroscopic growth factor at RH = 90% (Gf(90%)) and the enhancement factor for the scattering coefficients (f(RH)sp) were measured by a self-constructed Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) and two nephelometers in parallel (PNEPs) respectively from 22nd February to 18th March 2014 in the Pearl River Delta, China. In addition, the particle number size distribution (PNSD) and BC mass concentration (MBC) were measured simultaneously.During the observation period, the f(RH)sp increased sharply along with increasing RH (40%–85%) and the value of f(80%)sp was 1.77 ± 0.18. The mean Gf(90%) for all particles are 1.44 (80 nm), 1.48 (110 nm), 1.52 (150 nm) and 1.55 (200 nm), and the mean Gf(90%) for more-hygroscopic particles are 1.58 (80 nm), 1.63 (110 nm), 1.66 (150 nm) and 1.67 (200 nm) respectively. Based on Gf, PNSD and MBC, the enhancement factor of the aerosol optical properties (extinction (f(RH)ep), scattering (f(RH)sp), backscattering (f(RH)hbsp), absorption (f(RH)absp), and hemispheric backscatter fraction (f(RH)hbsp)) were calculated under three aerosol mixing state assumptions. The results show that the calculated f(80%)sp values agreed well with the ones measured by PNEPs, illustrating that the Gf size distribution fittings are reasonable. The f(RH)ep, f(RH)sp and f(RH)hbsp increased along with increasing RH for three mixtures, while f(RH)HBF decreased. The f(RH)absp increased for the homogenously internal mixture, but remained stable for the external mixture. For the core-shell mixture, the f(RH)absp increased from RH = 0 to 75% and then decreased, due to a decrease of light entering the BC core. The enhancement factor of aerosol direct radiative forcing (f(RH)Fr) increased sharply as the RH elevated for the external mixing state. However, f(RH)Fr increased or decreased along with the elevated RH for the homogenously internal mixture and the core-shell mixture depending on initial value of the aerosol direct radiative forcing (∆Fr) in a dry condition.

The optical properties, physical properties and direct radiative forcing of urban columnar aerosols in the Yangtze River Delta, China

Abstract. The optical and physical properties as well as the direct radiative forcings (DRFs) of fractionated aerosols in the urban area of the western Yangtze River Delta (YRD) are investigated with measurements from a Cimel sun photometer combined with a radiation transfer model. Ground-based observations of aerosols have much higher temporal resolutions than satellite retrievals. An initial analysis reveals the characteristics of the optical properties of different types of fractionated aerosols in the western YRD. The total aerosols, mostly composed of scattering components (93.8 %), have mean optical depths of 0.65 at 550 nm and refractive index of 1.44 + 0.0084i at 440 nm. The fine aerosols are approximately four times more abundant and have very different compositions from coarse aerosols. The absorbing components account for only ∼ 4.6 % of fine aerosols and 15.5 % of coarse aerosols and have smaller sizes than the scattering aerosols within the same mode. Therefore, fine particles have stronger scattering than coarse ones, simultaneously reflecting the different size distributions between the absorbing and scattering aerosols. The relationships among the optical properties quantify the aerosol mixing and imply that approximately 15 and 27.5 % of the total occurrences result in dust- and black-carbon-dominating mixing aerosols, respectively, in the western YRD. Unlike the optical properties, the size distributions of aerosols in the western YRD are similar to those found at other sites over eastern China on a climatological scale, peaking at radii of 0.148 and 2.94 µm. However, further analysis reveals that the coarse-dominated particles can also lead to severe haze pollution over the YRD. Observation-based estimations indicate that both fine and coarse aerosols in the western YRD exert negative DRFs, and this is especially true for fine aerosols (−11.17 W m−2 at the top of atmosphere, TOA). A higher absorption fraction leads directly to the negative DRF being further offset for coarse aerosols (−0.33 W m−2) at the TOA. Similarly, the coarse-mode DRF contributes to only 13.3 % of the total scattering aerosols but > 33.7 % to the total absorbing aerosols. A sensitivity analysis states that aerosol DRFs are not highly sensitive to their profiles in clear-sky conditions. Most of the aerosol properties and DRFs have substantial seasonality in the western YRD. The results further reveal the contributions of each component of the different size particles to the total aerosol optical depths (AODs) and DRFs. Additionally, these results can be used to improve aerosol modelling performance and the modelling of aerosol effects in the eastern regions of China.

An Evaluation of the Shortwave Direct Aerosol Radiative Forcing Using CALIOP and MODIS Observations

AbstractIn this study, all‐sky ShortWave Direct Aerosol Radiative Forcing (SWDARF) at the top of atmosphere is estimated using the method of Oikawa et al. (2013) applied to two generations of Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Level 2 products, i.e., version 2 (V2) and version 3 (V3), and the Moderate Resolution Imaging Spectroradiometer (MODIS) cloud product. The estimated SWDARF in Oikawa et al. (2013) was based on CALIPSO V2 product, which contained significant errors in cloud clearing and low‐altitude aerosols. This error was corrected in V3, resulting in greatly improved and significantly different aerosol and cloud distributions. In clear‐sky conditions, the magnitude of aerosol optical thickness underestimation becomes smaller and SWDARF becomes more negative using the V3 product. In addition, above‐cloud aerosols, which cause positive SWDARF, are less frequently detected and below‐cloud aerosols are more frequently detected in the V3 product than in the V2 product, so that cloudy‐sky SWDARF becomes more negative using the V3 product. From these results, clear‐sky, cloudy‐sky, and all‐sky SWDARFs become more negative using the V3 product than the V2 product. The magnitude of negative SWDARF using the V3 product is more than twice as large as the V2 product under all‐sky conditions due to V3 improvements in the lidar retrieval algorithms. Considering the uncertainties of aerosol and cloud measurements, annual zonal averages of clear‐sky, cloudy‐sky, and all‐sky SWDARFs from 60°S to 60°N are estimated as −4.0 ± 0.2, −1.1 ± 0.3, and −2.1 ± 0.2 Wm−2 from the V3 product.

Aerosol optical properties and direct radiative forcing based on measurements from the China Aerosol Remote Sensing Network (CARSNET) in eastern China

Abstract. Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71–0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (∼ 0.40–0.60) than in January and February (0.71–0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ∼ 0.04–0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was −93 ± 44 to −79 ± 39 W m−2 at the Earth's surface and ∼ −40 W m−2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80∘) under cloud-free conditions. The fine mode composed a major contribution of the absorbing particles in the classification scheme based on SSA, fine-mode fraction and extinction Angström exponent. This study contributes to our understanding of aerosols and regional climate/air quality, and the results will be useful for validating satellite retrievals and for improving climate models and remote sensing algorithms.

Aerosol optical properties and radiative impacts in the Pearl River Delta region of China during the dry season

Aerosol optical properties and direct radiative effects on surface irradiance were examined using seven years (2006–2012) of Cimel sunphotometer data collected at Panyu—the main atmospheric composition monitoring station in the Pearl River Delta (PRD) region of China. During the dry season (October to February), mean values of the aerosol optical depth (AOD) at 550 nm, the Angstrom exponent, and the single scattering albedo at 440 nm (SSA) were 0.54, 1.33 and 0.87, respectively. About 90% of aerosols were dominated by fine-mode strongly absorbing particles. The size distribution was bimodal, with fine-mode particles dominating. The fine mode showed a peak at a radius of 0.12 μm in February and October (∼ 0.10 μm3μm-2). The mean diurnal shortwave direct radiative forcing at the surface, inside the atmosphere (FATM), and at the top of the atmosphere, was −33.4±7.0, 26.1±5.6 and −7.3±2.7Wm−2, respectively. The corresponding mean values of aerosol direct shortwave radiative forcing per AOD were −60.0 ± 7.8, 47.3 ± 8.3 and −12.8 ± 3.1 W m−2, respectively. Moreover, during the study period, FATM showed a significant decreasing trend (p < 0.01) and SSA increased from 0.87 in 2006 to 0.91 in 2012, suggesting a decreasing trend of absorbing particles being released into the atmosphere. Optical properties and radiative impacts of the absorbing particles can be used to improve the accuracy of inversion algorithms for satellite-based aerosol retrievals in the PRD region and to better constrain the climate effect of aerosols in climate models.

Optical, microphysical and radiative properties of aerosols over a tropical rural site in Kenya, East Africa: Source identification, modification and aerosol type discrimination

A better understanding of aerosol optical, microphysical and radiative properties is a crucial challenge for climate change studies. In the present study, column-integrated aerosol optical and radiative properties observed at a rural site, Mbita (0.42°S, 34.20 °E, and 1125 m above sea level) located in Kenya, East Africa (EA) are investigated using ground-based Aerosol Robotic Network (AERONET) data retrieved during January, 2007 to December, 2015. The annual mean aerosol optical depth (AOD500 nm), Ångström exponent (AE440–870 nm), fine mode fraction of AOD500 nm (FMF500 nm), and columnar water vapor (CWV, cm) were found to be 0.23 ± 0.08, 1.01 ± 0.16, 0.60 ± 0.07, and 2.72 ± 0.20, respectively. The aerosol optical properties exhibited a unimodal distribution with substantial seasonal heterogeneity in their peak values being low (high) during the local wet (dry) seasons. The observed data showed that Mbita and its environs are significantly influenced by various types of aerosols, with biomass burning and/or urban-industrial (BUI), mixed (MXD), and desert dust (DDT) aerosol types contributing to 37.72%, 32.81%, and 1.40%, respectively during the local dry season (JJA). The aerosol volume size distribution (VSD) exhibited bimodal lognormal structure with a geometric mean radius of 0.15 μm and 3.86–5.06 μm for fine- and coarse-mode aerosols, respectively. Further, analysis of single scattering albedo (SSA), asymmetry parameter (ASY) and refractive index (RI) revealed dominance of fine-mode absorbing aerosols during JJA. The averaged aerosol direct radiative forcing (ARF) retrieved from the AERONET showed a strong cooling effect at the bottom of the atmosphere (BOA) and significant warming within the atmosphere (ATM), representing the important role of aerosols played in this rural site of Kenya. Finally, the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model revealed that aerosols from distinct sources resulted in enhanced loading during JJA.

Satellite‐retrieved direct radiative forcing of aerosols over North‐East India and adjoining areas: climatology and impact assessment

In order to understand the climatic implications of atmospheric aerosols, top of atmosphere (TOA) shortwave (SW, 0.3–5 µm) fluxes and aerosol optical depth (AOD) at 550 nm retrieved simultaneously by clouds and the earth's radiant energy system (CERES) and moderate resolution imaging spectroradiometer (MODIS) instruments, respectively, are analysed over North-East India and its adjoining areas for the period July 2002–December 2013. The aerosol-free TOA flux obtained by establishing the linear regression between CERES SW TOA fluxes and MODIS AODs exhibits strong seasonality with peak values in monsoon and minimum in winter. Same seasonality is captured by the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model, but with difference in absolute values. SBDART code is used to extend instantaneous radiative forcing estimates into 24-h averages. AOD over the North East India region with complex terrain shows altitudinal variation with maximum value at the lowest elevation site Dhaka and minimum value at the high-altitude locations Shillong and Aizwal. In general, strong seasonality in AOD is observed with a peak in pre-monsoon (March–May) and dip in post-monsoon (October–November) at all the locations. The direct instantaneous TOA shortwave aerosol radiative forcing (SWARF) shows maximum values in pre-monsoon over all the locations except at Guwahati, Banmauk, Aizawl, and Shillong. The lowest value of instantaneous SWARF is observed in post-monsoon except at Banmauk and Shillong. Climatologically TOA diurnally averaged SWARF varies between −6.95 W m−2 in Aizawl to −20.39 W m−2 in Shillong. In general, the TOA SW forcing efficiency is highest in monsoon at all the locations. The radiative forcing efficiency is found to be less negative when surface reflectance increases.

제주 애월 대기오염집중측정소의 PM2.5 에어로졸 화학성분 자료를 이용한 광학특성 및 직접적 복사강제력 추정 연구

제주 애월 대기오염집중측정소의 PM2.5 에어로졸 화학성분 자료를 이용한 광학특성 및 직접적 복사강제력 추정 연구

Wintertime aerosol optical and radiative properties in the Kathmandu Valley during the SusKat-ABC field campaign

Abstract. Particulate air pollution in the Kathmandu Valley has reached severe levels that are mainly due to uncontrolled emissions and the location of the urban area in a bowl-shaped basin with associated local wind circulations. The AERONET measurements from December 2012 to August 2014 revealed a mean aerosol optical depth (AOD) of approximately 0.30 at 675 nm during winter, which is similar to that of the post-monsoon but half of that of the pre-monsoon AOD (0.63). The distinct seasonal variations are closely related to regional-scale monsoon circulations over South Asia and emissions in the Kathmandu Valley. During the SusKat-ABC campaign (December 2012–February 2013), a noticeable increase in both aerosol scattering (σs; 313 → 577 Mm−1 at 550 nm) and absorption (σa; 98 → 145 Mm−1 at 520 nm) coefficients occurred before and after 4 January 2013. This can be attributed to the increase in wood-burned fires due to a temperature drop and the start of firing at nearby brick kilns. The σs value in the Kathmandu Valley was a factor of 0.5 lower than that in polluted cities in India. The σa value in the Kathmandu Valley was approximately 2 times higher than that at severely polluted urban sites in India. The aerosol mass scattering efficiency of 2.6 m2 g−1 from PM10 measurements in the Kathmandu Valley is similar to that reported in urban areas. However, the aerosol mass absorption efficiency was determined to be 11 m2 g−1 from PM10 measurements, which is higher than that reported in the literature for pure soot particles (7.5 ± 1.2 m2 g−1). This might be due to the fact that most of the carbonaceous aerosols in the Kathmandu Valley were thought to be mostly externally mixed with other aerosols under dry conditions due to a short travel time from their sources. The σs and σa values and the equivalent black carbon (EBC) mass concentration reached up to 757 Mm−1, 224 Mm−1, and 29 µg m−3 at 08:00 LST (local standard time), respectively but decreased dramatically during the daytime (09:00–18:00 LST), to one-quarter of the morning average (06:00–09:00 LST) due to the development of valley winds and an atmospheric bounder layer. The σs and σa values and the EBC concentration remained almost constant during the night at the levels of 410 Mm−1, 130 Mm−1, and 17 µg m−3, respectively. The average aerosol direct radiative forcings over the intensive measurement period were estimated to be −6.9 ± 1.4 W m−2 (top of the atmosphere) and −20.8 ± 4.6 W m−2 (surface). Therefore, the high atmospheric forcing (i.e., 13.9 ± 3.6 W m−2) and forcing efficiency (74.8 ± 24.2 W m−2 τ−1) can be attributed to the high portion of light-absorbing aerosols in the Kathmandu Valley, as indicated by the high black carbon (or elemental carbon) to sulphate ratio (1.5 ± 1.1).

Ambient black carbon particulate matter in the coal region of Dhanbad, India

Light-absorbing, atmospheric particles have gained greater attention in recent years because of their direct and indirect impacts on regional and global climate. Atmospheric black carbon (BC) aerosol is a leading climate warming agent, yet uncertainties in the global direct aerosol radiative forcing remain large. Based on a year of aerosol absorption measurements at seven wavelengths, BC concentrations were investigated in Dhanbad, the coal capital of India. Coal is routinely burned for cooking and residential heat as well as in small industries. The mean daily concentrations of ultraviolet-absorbing black carbon measured at 370nm (UVBC) and black carbon measured at 880nm (BC) were 9.8±5.7 and 6.5±3.8μgm−3, respectively. The difference between UVBC and BC, Delta-C, is an indicator of biomass or residential coal burning and averaged 3.29±4.61μgm−3. An alternative approach uses the Ǻngstrom Exponent (AE) to estimate the biomass/coal and traffic BC concentrations. Biomass/coal burning contributed ~87% and high temperature, fossil-fuel combustion contributed ~13% to the annual average BC concentration. The post-monsoon seasonal mean UVBC values were 10.9μgm−3 and BC of 7.2μgm−3. Potential source contribution function analysis showed that in the post-monsoon season, air masses came from the central and northwestern Indo-Gangetic Plains where there is extensive agricultural burning. The mean winter UVBC and BC concentrations were 15.0 and 10.1μgm−3, respectively. These higher values were largely produced by local sources under poor dispersion conditions. The direct radiative forcing (DRF) due to UVBC and BC at the surface (SUR) and the top of the atmosphere (TOA) were calculated. The mean atmospheric heating rates due to UVBC and BC were estimated to be 1.40°Kday−1 and 1.18°Kday−1, respectively. This high heating rate may affect the monsoon circulation in this region.

Most probable mixing state of aerosols in Delhi NCR, northern India

Unknown mixing state is one of the major sources of uncertainty in estimating aerosol direct radiative forcing (DRF). Aerosol DRF in India is usually reported for external mixing and any deviation from this would lead to high bias and error. Limited information on aerosol composition hinders in resolving this issue in India. Here we use two years of aerosol chemical composition data measured at megacity Delhi to examine the most probable aerosol mixing state by comparing the simulated clear-sky downward surface flux with the measured flux. We consider external, internal, and four combinations of core-shell (black carbon, BC over dust; water-soluble, WS over dust; WS over water-insoluble, WINS and BC over WINS) mixing. Our analysis reveals that choice of external mixing (usually considered in satellite retrievals and climate models) seems reasonable in Delhi only in the pre-monsoon (Mar-Jun) season. During the winter (Dec-Feb) and monsoon (Jul-Sep) seasons, ‘WS coating over dust’ externally mixed with BC and WINS appears to be the most probable mixing state; while ‘WS coating over WINS’ externally mixed with BC and dust seems to be the most probable mixing state in the post-monsoon (Oct–Nov) season. Mean seasonal TOA (surface) aerosol DRF for the most probable mixing states are 4.4±3.9 (−25.9±3.9), −16.3±5.7 (−42.4±10.5), 13.6±11.4 (−76.6±16.6) and −5.4±7.7 (−80.0±7.2)Wm−2 respectively in the pre-monsoon, monsoon, post-monsoon and winter seasons. Our results highlight the importance of realistic mixing state treatment in estimating aerosol DRF to aid in policy making to combat climate change.

Study on Aerosol Properties Based on CALIPSO in Representative Regions over China

To assess the aerosol direct and indirect radiative forcing, this paper analyzed the seasonal aerosol optical properties and vertical distribution characteristics in eight representative regions over China by using CALIPSO Level 2 products. The seasonal aerosol optical properties were validated by the AERONET data. The results show that the Taklamakan Desert (TD) and Tibet Plateau (TP) have the greatest depolarization and color ratios (PDR and CR) while the Northeast Plain (NP), Sichuan Basin (SB), North China Plain (NCP) and Yangtze River Delta (YRD) have the smallest PDR and CR, the Loess Plateau (LP) has intermediate PDR and CR, and that the Pearl River Delta (PRD) has the same PDR and greater CR compared with the polluted regions. The dust is transported to the middle and upper troposphere in spring, the strong vertical convection activities in summer transport massive aerosols from the atmospheric boundary layer to the free troposphere, and the stable meteorological conditions in autumn and winter trap massive aerosols within the boundary layer. The ratio of the AOD within 1.5 km above the ground to the total AOD and the extinction lapse rate in winter are greater than those in other seasons and 48.25% and 0.13km-2, respectively. The extinction lapse rates in the planetary boundary layer for the heavier polluted regions are greater than those in the polluted regions.

Grid-cell aerosol direct shortwave radiative forcing calculated using the SBDART model with MODIS and AERONET observations: An application in winter and summer in eastern China

Taking winter and summer in eastern China as an example application, a grid-cell method of aerosol direct radiative forcing (ADRF) calculation is examined using the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model with inputs from MODIS and AERONET observations and reanalysis data. Results show that there are significant seasonal and regional differences in climatological mean aerosol optical parameters and ADRF. Higher aerosol optical depth (AOD) occurs in summer and two prominent high aerosol loading centers are observed. Higher single scattering albedo (SSA) in summer is likely associated with the weak absorbing secondary aerosols. SSA is higher in North China during summer but higher in South China during winter. Aerosols induce negative forcing at the top of the atmosphere (TOA) and surface during both winter and summer, which may be responsible for the decrease in temperature and the increase in relative humidity. Values of ADRF at the surface are four times stronger than those at the TOA. Both AOD and ADRF present strong interannual variations; however, their amplitudes are larger in summer. Moreover, patterns and trends of ADRF do not always correspond well to those of AOD. Differences in the spatial distributions of ADRF between strong and weak monsoon years are captured effectively. Generally, the present results justify that to calculate grid-cell ADRF at a large scale using the SBDART model with observational aerosol optical properties and reanalysis data is an effective approach.

Estimation of shortwave direct aerosol radiative forcing at four locations on the Indo-Gangetic plains: Model results and ground measurement

This study provides observational results of aerosol optical and radiative characteristics over four locations in IGP. Spectral variation of Aerosol Optical Depth (AOD), Single Scattering Albedo (SSA) and Asymmetry Parameter (AP) were analysed using AErosol RObotic NETwork (AERONET) data. The analysis revealed that coarse particles were dominant in summer and pre-monsoon, while fine particles were more pronounced in winter and post-monsoon. Furthermore, the spatio-temporal variations of Shortwave Direct Aerosol Radiative Forcing (SDARF) and Shortwave Direct Aerosol Radiative Forcing Efficiency (SDARFE) at the Top Of Atmosphere (TOA), SURface (SUR) and within ATMosphere (ATM) were calculated using SBDART model. The atmospheric Heating Rate (HR) associated with SDARFATM were also computed. It was observed that the monthly averaged SDARFTOA and SDARFSUR were found to be negative leading to positive SDARFATM during all the months over all sites. The increments in net atmospheric forcing lead to maximum HR in November–December and May. The seasonal analysis of SDARF revealed that SDARFTOA and SDARFSUR were negative during all seasons. The SW atmospheric absorption translates to highest atmospheric HR during summer over Karachi and during pre-monsoon over Lahore, Jaipur and Kanpur. Like SDARF, the monthly and seasonal variations of SDARFETOA and SDARFESUR were found to be negative, resulting in positive atmospheric forcing. Additionally, to compare the model estimated forcing against AERONET derived forcing, the regression analysis of AERONET-SBDART forcing were carried out. It was observed that SDARF at SUR and TOA showed relatively higher correlation over Lahore, moderate over Jaipur and Kanpur and lower over Karachi. Finally, the analysis of National Oceanic and Atmospheric Administration Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model revealed that air masses were arriving from multiple source locations.

Characteristics of columnar aerosol optical and microphysical properties retrieved from the sun photometer and its impact on radiative forcing over Skukuza (South Africa) during 1999-2010.

The detailed analysis of columnar optical and microphysical properties of aerosols obtained from the AErosol RObotic NETwork (AERONET) Cimel sun photometer operated at Skukuza (24.98° S, 31.60° E, 150m above sea level), South Africa was carried out using the level 2.0 direct sun and inversion products measured during 1999-2010. The observed aerosol optical depth (AOD) was generally low over the region, with high values noted in late winter (August) and mid-spring (September and October) seasons. The major aerosol types found during the study period were made of 3.74, 69.63, 9.34, 8.83, and 8.41% for polluted dust (PD), polluted continental (PC), non-absorbing (NA), slightly absorbing (SA), and moderately absorbing (MA) aerosols, respectively. Much attention was given to the aerosol fine- and coarse-modes deduced from the particle volume concentration, effective radius, and fine-mode volume fraction. The aerosol volume size distribution pattern was found to be bimodal with the fine-mode showing predominance relative to coarse-mode during the winter and spring seasons, owing to the onset of the biomass burning season. The mean values of total, fine-, and coarse-mode volume particle concentrations were 0.07±0.04, 0.03±0.03, and 0.04±0.02μm3μm-2, respectively, whereas the mean respective effective radii observed at Skukuza for the abovementioned modes were 0.35±0.17, 0.14±0.02, and 2.08±0.02μm. The averaged shortwave direct aerosol radiative forcing (ARF) observed within the atmosphere was found to be positive (absorption or heating effect), whereas the negative forcing in the surface and TOA depicted significant cooling effect due to more scattering type particles.

Importance of aerosol non-sphericity in estimating aerosol radiative forcing in Indo-Gangetic Basin

Aerosols are usually presumed spherical in shape while estimating the direct radiative forcing (DRF) using observations or in the models. In the Indo-Gangetic Basin (IGB), a regional aerosol hotspot where dust is a major aerosol species and has been observed to be non-spherical in shape, it is important to test the validity of this assumption. We address this issue using measured chemical composition at megacity Delhi, a representative site of the western IGB. Based on the observation, we choose three non-spherical shapes - spheroid, cylinder and chebyshev, and compute their optical properties. Non-spherical dust enhances aerosol extinction coefficient (βext) and single scattering albedo (SSA) at visible wavelengths by >0.05km−1 and >0.04 respectively, while it decreases asymmetry parameter (g) by ~0.1. Accounting non-sphericity leads top-of-the-atmosphere (TOA) dust DRF to more cooling due to enhanced backscattering and increases surface dimming due to enhanced βext. Outgoing shortwave flux at TOA increases by up to 3.3% for composite aerosols with non-spherical dust externally mixed with other spherical species. Our results show that while non-sphericity needs to be accounted for, choice of shape may not be important in estimating aerosol DRF in the IGB.

Diurnal and seasonal characteristics of the optical properties and direct radiative forcing of different aerosol components in Seoul megacity

The temporal variations (diurnal and seasonal) of the optical properties and direct aerosol radiative forcing (DARF) of different aerosol components (water-soluble, insoluble, black carbon (BC), and sea-salt) were analyzed using the hourly resolution data (PM2.5) measured at an urban site in Seoul, Korea during 2010, based on a modeling approach. In general, the water-soluble component was predominant over all other components (with a higher concentration) in terms of its impact on the optical properties (except for absorbing BC) and DARF. The annual mean aerosol optical depth (AOD, τ) at 500nm for the water-soluble component was 0.38±0.07 (0.06±0.01 for BC). The forcing at the surface (DARFSFC) and top of the atmosphere (DARFTOA), and in the atmosphere (DARFATM) for most aerosol components (except for BC) during the daytime were highest in spring and lowest in late fall or early winter. The maximum DARFSFC occurred in the morning during most seasons (except for the water-soluble components showing peaks in the afternoon or noon in summer, fall, or winter), while the maximum DARFTOA occurred in the morning during spring and/or winter and in the afternoon during summer and/or fall. The estimated DARFSFC and DARFATM of the water-soluble component were in the range of −49 to −84Wm−2 and +10 to +22Wm−2, respectively. The DARFSFC and DARFATM of BC were −26 to −39Wm−2 and +32 to +51Wm−2, respectively, showing highest in summer and lowest in spring, with morning peaks regardless of the season. This positive DARFATM of BC in this study area accounted for approximately 64% of the total atmospheric aerosol forcing due to strong radiative absorption, thus increasing atmospheric heating by 2.9±1.2Kday−1 (heating rate efficiency of 39K day−1τ−1) and then causing further atmospheric warming.

Aerosol characterization and radiative properties over Kavaratti, a remote island in southern Arabian Sea from the period of observations

Long-term measurements of spectral aerosol optical depth (AOD) using sun/sky radiometer for a period of five years (2009–2014) from the remote island location at Kavaratti (KVT; 10.56°N, 72.64°E) in the southern Arabian sea have been analysed. Climatologically, AODs decrease from October to reach maximum of ~0.6 (at 500nm) in March, followed by a sudden fall towards May. Significant modulations of intra-seasonal timescales over this general pattern are noticed due to the changes in the relative strength of distinctively different sources. The corresponding changes in aerosol inversion parameters reveal the presence of coarse-mode aerosols during spring and fine-mode absorbing aerosols in autumn and winter months. An overall dominance of a mixed type of aerosols (~41%) with maximum in winter (~53%) was found via the AOD500 vs. Ångström exponent (α440–870) relationship, while biomass-burning aerosols or thick urban/industrial plumes contribute to ~19%. Spectral dependence of Ångström exponent and aerosol absorbing properties were used to identify the aerosol types and its modification processes. Based on air mass back trajectory analysis, we revealed that the advection of aerosols from Indian subcontinent and western regions plays a major role in modifying the optical properties of aerosols over the observational site. The shortwave aerosol direct radiative forcing estimated via SBDART model ranges from −11.00Wm−2 to −7.38Wm−2, −21.51Wm−2 to −14.33Wm−2 and 3.17Wm−2 and 10.0Wm−2 at top of atmosphere, surface and within the atmosphere, respectively. This atmospheric forcing translates into heating rate of 0.62–1.04Kday−1. Furthermore, the vertical profiles of aerosols and heating rate exhibit significant increase in lower (during winter and autumn) and mid troposphere (during spring). This may cause serious climate implications over Kavaratti with further consequences on cloud microphysics and monsoon rainfall.

Contrasting influences of aerosols on cloud properties during deficient and abundant monsoon years

Direct aerosol radiative forcing facilitates the onset of Indian monsoon rainfall, based on synoptic scale fast responses acting over timescales of days to a month. Here, we examine relationships between aerosols and coincident clouds over the Indian subcontinent, using observational data from 2000 to 2009, from the core monsoon region. Season mean and daily timescales were considered. The correlation analyses of cloud properties with aerosol optical depth revealed that deficient monsoon years were characterized by more frequent and larger decreases in cloud drop size and ice water path, but increases in cloud top pressure, with increases in aerosol abundance. The opposite was observed during abundant monsoon years. The correlations of greater aerosol abundance, with smaller cloud drop size, lower evidence of ice processes and shallower cloud height, during deficient rainfall years, imply cloud inhibition; while those with larger cloud drop size, greater ice processes and a greater cloud vertical extent, during abundant rainfall years, suggest cloud invigoration. The study establishes that continental aerosols over India alter cloud properties in diametrically opposite ways during contrasting monsoon years. The mechanisms underlying these effects need further analysis.