Aerosol Direct Radiative Effect Research Articles

Clear-sky solar radiation changes over arid and semi-arid areas in China and their determining factors during 2001–2015

In the study, we investigated the clear-sky solar radiation at the surface and their determining factors over the arid and semi-arid (ASA) areas in China using the simulations by Mesoscale Atmospheric Global Irradiance Code (MAGIC) radiation code with satellite remote sensing aerosol data and reanalysis data as input. The coefficient of determination (R2) between ground-based measurements and simulations was 0.959, and the average relative error was 6.33%. Stations with an average relative error of less than 10% accounted for 100%, confirming the reliability of simulations. The distribution of clear-sky solar radiation showed low values in regions with high latitudes and low altitudes, and high ones in regions with low latitudes and high altitudes. The monthly average of water vapour radiative effects (WVRE) was higher than the monthly average of aerosol direct radiative effects (ADRE) for each month. WVRE were even more than six times that of ADRE in July, August, September, indicating that water vapour has stronger weakening of clear-sky solar radiation than aerosols. The annual trend indicated increases in clear-sky solar radiation in most part of ASA areas. Central Inner Mongolia (0.389 W m−2 year−1) has the significant increase. There was an interesting finding that the area where the clear-sky solar radiation decreased/increased has a good match with the area where ADRE enhanced/weakened. The R2 between clear-sky solar radiation trend and ADRE trend was 0.957, indicating that the ADRE trends were the determining factor of the clear-sky solar radiation trends. Central Inner Mongolia (0.345 Wm-2 year−1) has the significant weakening of ADRE.

Aerosol direct radiative effect over clouds from a synergy of Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer (MODIS) reflectances

Abstract. The retrieval of geophysical parameters is increasingly dependent on synergistic use of satellite instruments. More sophisticated parameters can be retrieved and the accuracy of retrievals can be increased when more information is combined. In this paper, a synergistic application of Ozone Monitoring Instrument (OMI), on the Aura platform, and Moderate Resolution Imaging Spectroradiometer (MODIS), on the Aqua platform, Level 1B reflectances is described, enabling the retrieval of the aerosol direct radiative effect (DRE) over clouds using the differential aerosol absorption (DAA) technique. This technique was first developed for reflectances from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) on the Environmental Satellite (Envisat), which had the unique capability of measuring contiguous radiances from the ultraviolet (UV) at 240 to 1750 nm in the shortwave-infrared (SWIR), at a moderate spectral resolution of 0.2 to 1.5 nm. However, the spatial resolution and global coverage of SCIAMACHY was limited, and Envisat stopped delivering data in 2012. In order to continue the DRE data retrieval, reflectances from OMI and MODIS, flying in formation, were combined from the UV to the SWIR. This resulted in reflectances at a limited but sufficient spectral resolution, available at the OMI pixel grid, which have a much higher spatial resolution and coverage than SCIAMACHY. The combined reflectance spectra allow the retrieval of cloud microphysical parameters in the SWIR, and the subsequent retrieval of aerosol DRE over cloud scenes using the DAA technique. For liquid cloud scenes in the south-east Atlantic region with cloud fraction (CF) >0.3, the area-averaged instantaneous aerosol DRE over clouds in June to August 2006 was 25 Wm−2 with a standard deviation of 30 Wm−2. The maximum area-averaged instantaneous DRE from OMI–MODIS in August 2006 was 75.6±13 Wm−2. The new aerosol DRE over-cloud dataset from OMI–MODIS is compared to the SCIAMACHY dataset for the period 2006 to 2009, showing a very high correlation. The OMI–MODIS DRE dataset over the Atlantic Ocean is highly correlated to above-cloud AOT measurements from OMI and MODIS. It is related to AOT measurements over Ascension Island in 2016, showing the transport of smoke all the way from its source region in Africa over the Atlantic to Ascension and beyond.

Spatial distribution of aerosol microphysical and optical properties and direct radiative effect from the China Aerosol Remote Sensing Network

Abstract. Multi-year observations of aerosol microphysical and optical properties, obtained through ground-based remote sensing at 50 China Aerosol Remote Sensing Network (CARSNET) sites, were used to characterize the aerosol climatology for representative remote, rural, and urban areas over China to assess effects on climate. The annual mean effective radii for total particles (ReffT) decreased from north to south and from rural to urban sites, and high total particle volumes were found at the urban sites. The aerosol optical depth at 440 nm (AOD440 nm) increased from remote and rural sites (0.12) to urban sites (0.79), and the extinction Ångström exponent (EAE440–870 nm) increased from 0.71 at the arid and semi-arid sites to 1.15 at the urban sites, presumably due to anthropogenic emissions. Single-scattering albedo (SSA440 nm) ranged from 0.88 to 0.92, indicating slightly to strongly absorbing aerosols. Absorption AOD440 nm values were 0.01 at the remote sites versus 0.07 at the urban sites. The average direct aerosol radiative effect (DARE) at the bottom of atmosphere increased from the sites in the remote areas (−24.40 W m−2) to the urban areas (−103.28 W m−2), indicating increased cooling at the latter. The DARE for the top of the atmosphere increased from −4.79 W m−2 at the remote sites to −30.05 W m−2 at the urban sites, indicating overall cooling effects for the Earth–atmosphere system. A classification method based on SSA440 nm, fine-mode fraction (FMF), and EAE440–870 nm showed that coarse-mode particles (mainly dust) were dominant at the rural sites near the northwestern deserts, while light-absorbing, fine-mode particles were important at most urban sites. This study will be important for understanding aerosol climate effects and regional environmental pollution, and the results will provide useful information for satellite validation and the improvement of climate modelling.

Investigating the regional difference of aerosol feedback effects over South Korea using the WRF-CMAQ two-way coupled modeling system

We study the regionally different impacts of aerosol direct radiative effects (DRE) by PM2.5 on the decrease in the solar radiation over South Korea (hereafter, Korea) for February 2015, using the WRF-CMAQ two-way modeling system. Two different numerical experiments were designed based on the on- and off-aerosol feedback option to evaluate the impact of aerosol DRE on the simulated meteorology and solar radiation. We find that the spatial pattern of the decrease in solar radiation does not agree with that of the PM2.5 concentrations. The largest decrease in solar radiation occurs around the southwest part of Korea (G1), where much lower PM2.5 concentrations appear, compared to other inland regions (G2). The investigation of the chemical species that constitute PM2.5 reveals that the G1 sites have a relatively higher fraction of sulfate (S/PM2.5) than the G2 sites. This finding reveals that the higher sulfate loading over Korea could lead to the larger aerosol DRE. The high sulfate loading, which mainly appeared in the southwest part of Korea, was identified as not only originating from national local emission sources, but also from the long-range transport (LRT) of sulfate and its precursors. Overall, the regionally different distributions of aerosol DRE, especially for solar radiation in Korea, can be attributed partly to the different contributions of the chemical species that constitute PM2.5, particularly sulfate.

Land Cover Regulates the Spatial Variability of Temperature Response to the Direct Radiative Effect of Aerosols

AbstractAerosol impact on the surface temperature varies between the shortwave and the longwave components of radiation, depends on the time of the day, and is modulated by underlying biophysical processes. We disentangle these complexities by isolating the direct surface shortwave and longwave radiative effects from a global reanalysis data product and calculating their spatially explicit climate sensitivities. Higher sensitivity is found for the longwave component and is driven by a combination of spatial variability of aerosol species and biophysical control of the underlying surface. The opposing shortwave and longwave effects reduce the global terrestrial mean diurnal temperature range by 0.47 K, with almost half the contribution in the regions of interest considered coming from aerosols of anthropogenic origin. We also find evidence of an increasing trend in the local climate sensitivity in the equatorial zone, possibly caused by deforestation. These surface processes can partially explain why the climate forcing efficacy of aerosols exceeds unity.

New Estimates of Aerosol Direct Radiative Effects and Forcing From A‐Train Satellite Observations

AbstractAerosol direct radiative effects are assessed using multi‐sensor observations from the A‐Train satellite constellation. By leveraging vertical cloud and aerosol information from CloudSat and CALIPSO, this study reports new global estimates of aerosol radiative effects and the component owing to anthropogenic aerosols. We estimate that the global mean aerosol direct radiative effect is −2.40 W/m2 with an error of ± 0.6 W/m2 owing to uncertainties in aerosol type classification and optical depth retrievals. Anthropogenic direct radiative forcing is assessed using new observation‐based aerosol radiative kernels. Anthropogenic aerosols are found to account for 21% of the global radiative effect, or −0.50 ± 0.3 W/m2, mainly from sulfate pollution (−0.54 W/m2) partially offset by absorption from smoke (0.03 W/m2). Uncertainty estimates effectively rule out the possibility that anthropogenic aerosols warm the planet, although strong positive forcing is observed locally where anthropogenic aerosols reside above clouds and bright surfaces.

Direct radiative effect of dust–pollution interactions

Abstract. The chemical ageing of aeolian dust, through interactions with air pollution, affects the optical and hygroscopic properties of the mineral particles and hence their atmospheric residence time and climate forcing. Conversely, the chemical composition of the dust particles and their role as coagulation partners impact the abundance of particulate air pollution. This results in a change in the aerosol direct radiative effect that we interpret as an anthropogenic radiative forcing associated with mineral dust–pollution interactions. Using the ECHAM/MESSy atmospheric chemistry climate model (EMAC), which combines the Modular Earth Submodel System (MESSy) with the European Centre Hamburg (ECHAM) climate model, including a detailed parametrisation of ageing processes and an emission scheme accounting for the chemical composition of desert soils, we study the direct radiative forcing globally and regionally, considering solar and terrestrial radiation. Our results indicate positive and negative forcings, depending on the region. The predominantly negative forcing at the top of the atmosphere over large parts of the dust belt, from West Africa to East Asia, attains a maximum of about −2 W m−2 south of the Sahel, in contrast to a positive forcing over India. Globally averaged, these forcings partially counterbalance, resulting in a net negative forcing of −0.05 W m−2, which nevertheless represents a considerable fraction (40 %) of the total dust forcing.

Estimations of global shortwave direct aerosol radiative effects above opaque water clouds using a combination of A-Train satellite sensors

Abstract. All-sky direct aerosol radiative effects (DARE) play a significant yet still uncertain role in climate. This is partly due to poorly quantified radiative properties of aerosol above clouds (AAC). We compute global estimates of shortwave top-of-atmosphere DARE over opaque water clouds (OWCs), DAREOWC, using observation-based aerosol and cloud radiative properties from a combination of A-Train satellite sensors and a radiative transfer model. There are three major differences between our DAREOWC calculations and previous studies: (1) we use the depolarization ratio method (DR) on CALIOP (Cloud–Aerosol Lidar with Orthogonal Polarization) Level 1 measurements to compute the AAC frequencies of occurrence and the AAC aerosol optical depths (AODs), thus introducing fewer uncertainties compared to using the CALIOP standard product; (2) we apply our calculations globally, instead of focusing exclusively on regional AAC “hotspots” such as the southeast Atlantic; and (3) instead of the traditional look-up table approach, we use a combination of satellite-based sensors to obtain AAC intensive radiative properties. Our results agree with previous findings on the dominant locations of AAC (south and northeast Pacific, tropical and southeast Atlantic, northern Indian Ocean and northwest Pacific), the season of maximum occurrence and aerosol optical depths (a majority in the 0.01–0.02 range and that can exceed 0.2 at 532 nm) across the globe. We find positive averages of global seasonal DAREOWC between 0.13 and 0.26 W m−2 (i.e., a warming effect on climate). Regional seasonal DAREOWC values range from −0.06 W m−2 in the Indian Ocean offshore from western Australia (in March–April–May) to 2.87 W m−2 in the southeast Atlantic (in September–October–November). High positive values are usually paired with high aerosol optical depths (>0.1) and low single scattering albedos (<0.94), representative of, for example, biomass burning aerosols. Because we use different spatial domains, temporal periods, satellite sensors, detection methods and/or associated uncertainties, the DAREOWC estimates in this study are not directly comparable to previous peer-reviewed results. Despite these differences, we emphasize that the DAREOWC estimates derived in this study are generally higher than previously reported. The primary reasons for our higher estimates are (i) the possible underestimate of the number of dust-dominated AAC cases in our study; (ii) our use of Level 1 CALIOP products (instead of CALIOP Level 2 products in previous studies) for the detection and quantification of AAC aerosol optical depths, which leads to larger estimates of AOD above OWC; and (iii) our use of gridded 4∘×5∘ seasonal means of aerosol and cloud properties in our DAREOWC calculations instead of simultaneously derived aerosol and cloud properties from a combination of A-Train satellite sensors. Each of these areas is explored in depth with detailed discussions that explain both the rationale for our specific approach and the subsequent ramifications for our DARE calculations.

Global vertically resolved aerosol direct radiation effect from three years of CALIOP data using the FORTH radiation transfer model

We use global aerosol optical depth data from CALIOP with a radiation transfer model to investigate the aerosol direct radiative effect (DRE) and its sensitivity to the aerosol vertical resolution. Our study spans three years (2007–2009) and uses cloud data from ISCCP D2 to take into account cloud-aerosol radiative interactions on a monthly 2.5° × 2.5° resolution. The three-year global average all-sky aerosol DRE at the surface, in the atmosphere, and at the top of atmosphere (TOA) was calculated to be −4.23, 2.40, and −1.83 Wm−2, respectively. As expected, local DREs and atmospheric heating rates are shown to vary significantly. The largest magnitudes of the DREs are observed in regions with heavy aerosol load consisting of both natural and anthropogenic particles, such as desert dust, biomass burning and urban/industrial pollution. At TOA the aerosol effect is generally of negative sign, though a planetary heating effect is found in regions characterized by both absorbing aerosol and large surface albedo, such as deserts. Clouds scatter and absorb solar radiation, which generally decreases the aerosol cooling at the surface and the aerosol warming in the atmosphere. However, the latter effect is attenuated due to the enhancement of radiation absorption by the above-cloud aerosols. As a result, clouds decrease the aerosol TOA (planetary) cooling, and sometimes even cause aerosol warming (e.g. over the tropical South Atlantic). The cloud effect on the aerosol DRE depends strongly on the aerosol optical properties and the aerosol load fraction above low clouds. Comparing the effect of the observed aerosol vertical profile against an exponentially decreasing profile, we find a small sensitivity for the surface DRE, but larger for the atmospheric column and the top of the atmosphere. Under all-sky conditions, when continental aerosols are lifted higher in the atmosphere, the outgoing shortwave radiation at TOA decreases, due to the increase of UV and visible radiation absorption by particles while higher oceanic aerosols generally increase the outgoing shortwave radiation through more efficient backscatter and decrease of the NIR radiation absorption by atmospheric gases below aerosol particles.

Aerosol radiative effects from observations and modelling over the Yangtze River Basin, China from 2001 to 2015

In this study, a quantitative assessment of clear‐sky aerosol direct radiative effects (ADREs) at the surface over the Yangtze River Basin (YRB), China was conducted based on Mesoscale Atmospheric Global Irradiance Code (MAGIC) radiation code (direct method) and ground‐based measurements (indirect method). For the direct method, The ADRE at the surface was calculated using MAGIC radiation code with Moderate Resolution Imaging Spectroradiometer (MODIS) and interim ECMWF Re‐Analysis (ERA‐INTERIM) integrated water vapour as input. Results showed that the multi‐year average ADRE ranged from −39.29 to −1.95 W/m2 with mean values of −18.19 ± 1.44 W/m2. High ADRE (larger than −34 W/m2) occurred in Sichuan Basin, Central Hubei Province and Yangtze River Delta. The seasonal ADRE was high in spring (−23.05 ± 13.48 W/m2) and low in winter (−14.24 ± 8.51 W/m2). Generally, an increasing trend (0.27 W/m2 per year) of ADRE was found from 2001 to 2010 and a decreasing trend (−0.72 W/m2 per year) from 2011 to 2015. The water vapour radiative effect (WVRE) was calculated using MAGIC radiation code and the multi‐year average value was −52.59 ± 1.45 W/m2, which indicated the attenuation of clear‐sky radiation in YRB due to water vapour was stronger than the aerosols. However, the trends of water vapour effects were 0.03 W/m2 per year during 2001–2010 and −0.37 W/m2 per year during 2011–2015, which were much smaller than the trends of ADRE. For the indirect method, the clear‐sky ADRE at sites was calculated using the solar radiation observations. The variations of annual average ADRE obtained by above methods gave good match. An obvious increasing trend (−0.71 W/m2 per year) of aerosol radiative cooling effect was found in Central Hubei Province from 2001 to 2010 and an obvious decreasing trend (3.23 W/m2 per year) in Sichuan Basin from 2011 to 2015. The determination coefficient (R2) between ADRE trends and clear‐sky solar radiation trends is 0.874, indicating that the trends of clear‐sky solar radiation were mainly determined by the trends of ADRE.

Climatological study for understanding the aerosol radiative effects at southwest Atlantic coast of Europe

In order to describe the means, variability and trends of the aerosol radiative effects on the southwest Atlantic coast of Europe, 11 years of aerosol light scattering (σsp) and 4 years of aerosol light absorption (σap) are analyzed. A 2006–2016 trend analysis of σsp for D < 10 μm indicates statistically significant trends for March, May–June and September–November, with a decreasing trend ranging from −1.5 to −2.8 Mm−1/year. In the 2009–2016 period, the decreasing trend is only observed for the months of June and September. For scattering Ångström exponent (SAE) there is an increasing trend during June with a rate of 0.059/year and a decreasing trend during October with −0.060/year. The trends observed may be caused by a reduction of Saharan dust aerosol or a drop in particle loading in anthropogenic influenced air masses. The relationship between SAE and absorption Ångström exponent is used to assess the aerosol typing. Based on this typing, the sub-micron particles are dominated by black carbon, mixed black and brown carbon or marine with anthropogenic influences, while the super-micrometer particles are desert dust and sea spray aerosol. The mean and standard deviation of the dry aerosol direct radiative effect at the top of the atmosphere (DRETOA) are −4.7 ± 4.2 W m−2. DRETOA for marine aerosol shows all observations more negative than −4 W m−2 and for anthropogenic aerosol type, DRETOA ranges from −5.0 to −13.0 W m−2. DRETOA of regional marine aerosol ranges from −3 to −7 W m−2, as it consists of a mixture of sea salt and anthropogenic aerosol. The variability in DRETOA is mainly dependent on AOD, given that variations in backscatter fraction and the single scattering albedo tend to counteract each other in the radiative forcing efficiency equation. The results shown here may help in interpretation of satellite retrieval products and provide context for model evaluation.

Aerosol Direct Radiative and Cloud Adjustment Effects on Surface Climate over Eastern China: Analyses of WRF Model Simulations

The WRF-simulated changes in clouds and climate due to the increased anthropogenic aerosols for the summers of 2002–08 (vs the 1970s) over eastern China were used to offline calculate the radiative forcings associated with aerosol–radiation (AR) and aerosol–cloud–radiation (ACR) interactions, which subsequently facilitated the interpretation of surface temperature changes. During this period, the increases of aerosol optical depth (ΔAOD) averaged over eastern China range from 0.18 in 2004 to 0.26 in 2007 as compared to corresponding cases in the 1970s, and the multiyear means (standard deviations) of AR and ACR forcings at the surface are −6.7 (0.58) and −3.5 (0.63) W m−2, respectively, indicating the importance of cloud changes in affecting both the aerosol climate forcing and its interannual variation. The simulated mean surface cooling is 0.35°C, dominated by AR and ACR with a positive (cooling) feedback associated with changes in meteorology (~10%), and two negative (warming) feedbacks associated with decreases in latent (~70%) and sensible (~20%) heat fluxes. More detailed spatial characteristics were analyzed using ensemble simulations for the year 2008. Three regions—Jing-Jin-Ji (ΔAOD ~ 0.63), Sichuan basin (ΔAOD ~ 0.31), and middle Yangtze River valley (ΔAOD ~ 0.26)—at different climate regimes were selected to investigate the relative roles of AR and ACR. While the AR forcing is closely related to ΔAOD values, the ACR forcing presents different regional characteristics owing to cloud changes. In addition, the surface heat flux feedbacks are also different between regions. The study thus illustrates that ACR forcing is useful as a diagnostic parameter to unravel the complexity of climate change to aerosol forcing over eastern China.

Suppression of aerosol-induced atmospheric warming by clouds in the Indo-Gangetic Basin, northern India

Aerosol direct radiative effect (DRE) in India is mostly reported for the clear sky conditions. Here, we quantify the modulation of aerosol DRE in the presence of clouds using 2 years (2007–2008) of measured aerosol chemical composition data at megacity Delhi in the Indo-Gangetic Basin. Mean (± 1σ) seasonal top-of-the-atmosphere (TOA) aerosol DRE for the most probable mixing states in the presence of water and ice clouds are 7.3 ± 4.3 and 3.7 ± 1.8 W m−2 in the pre-monsoon, − 0.3 ± 3.7 and − 2.1 ± 4.4 W m−2 in the monsoon, 18.9 ± 15.9 W m−2 in the post-monsoon (no ice cloud is present in this season) and 11.8 ± 6.2 and 6.9 W m−2 in the winter seasons, respectively. The corresponding values for surface DRE are − 20.7 ± 5.5 and − 17.9 ± 8.4 W m−2, − 20.8 ± 8.1 and − 18.0 ± 9.4 W m−2, − 70.9 ± 11.7 W m−2, and − 55.7 ± 1.4 and − 49.8 W m−2 in the four seasons, respectively. Solar radiation reflected by water clouds interacts with aerosol layer aloft, enhancing TOA warming, while ice clouds reflect back a fraction of radiation supposed to interact with the aerosol layer beneath, thereby reducing TOA warming. We observe a reduction in the surface aerosol DRE in the presence of clouds by a larger magnitude relative to the change in TOA DRE. The aerosol DRE in the presence of water and ice clouds leads to a net decrease in atmospheric heating by 7.6% and 28.7% in the pre-monsoon, 21.5% and 39.1% in the monsoon, 0.6% (no discernable ice clouds) in the post-monsoon, and 9.5% and 24.0% in the winter seasons, respectively, for the most probable mixing state cases. Our results imply that under cloudy-sky condition, the aerosol-induced atmospheric heating in India is overestimated if the aerosol mixing state deviates (e.g., core-shell mixing) from the usually assumed external mixing.

Impact of mineral dust on shortwave and longwave radiation: evaluation of different vertically resolved parameterizations in 1-D radiative transfer computations

Abstract. Aerosol radiative properties are investigated in southeastern Spain during a dust event on 16–17 June 2013 in the framework of the ChArMEx/ADRIMED (Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) campaign. Particle optical and microphysical properties from ground-based sun/sky photometer and lidar measurements, as well as in situ measurements on board the SAFIRE ATR 42 French research aircraft, are used to create a set of different levels of input parameterizations, which feed the 1-D radiative transfer model (RTM) GAME (Global Atmospheric ModEl). We consider three datasets: (1) a first parameterization based on the retrievals by an advanced aerosol inversion code (GRASP; Generalized Retrieval of Aerosol and Surface Properties) applied to combined photometer and lidar data, (2) a parameterization based on the photometer columnar optical properties and vertically resolved lidar retrievals with the two-component Klett–Fernald algorithm, and (3) a parameterization based on vertically resolved optical and microphysical aerosol properties measured in situ by the aircraft instrumentation. Once retrieved, the outputs of the RTM in terms of both shortwave and longwave radiative fluxes are compared against ground and in situ airborne measurements. In addition, the outputs of the model in terms of the aerosol direct radiative effect are discussed with respect to the different input parameterizations. Results show that calculated atmospheric radiative fluxes differ no more than 7 % from the measured ones. The three parameterization datasets produce a cooling effect due to mineral dust both at the surface and the top of the atmosphere. Aerosol radiative effects with differences of up to 10 W m−2 in the shortwave spectral range (mostly due to differences in the aerosol optical depth) and 2 W m−2 for the longwave spectral range (mainly due to differences in the aerosol optical depth but also to the coarse mode radius used to calculate the radiative properties) are obtained when comparing the three parameterizations. The study reveals the complexity of parameterizing 1-D RTMs as sizing and characterizing the optical properties of mineral dust is challenging. The use of advanced remote sensing data and processing, in combination with closure studies on the optical and microphysical properties from in situ aircraft measurements when available, is recommended.

Multiyear Ground‐Based Measurements of Aerosol Optical Properties and Direct Radiative Effect Over Different Surface Types in Northeastern China

AbstractAerosol microphysical and optical properties as well as aerosol direct radiative effect (ADRE) were measured at a few ground sites to investigate aerosol optical‐radiative characteristics in northeastern China. Bimodal size distributions showed a dominance of fine mode particles at Shenyang, a megacity, and more impacts from larger particles at Fushun and Dalian, industrial and coastal sites, respectively. High aerosol optical depths at 440 nm in July (0.67–1.25) were ascribed to hygroscopic effects or cloud processing. Single scattering albedos at 440 nm show strong to moderate absorption at the urban and industrial sites (0.84–0.86) and weaker absorption at the coastal and rural sites (0.92–0.94). The single scattering albedo wavelength dependence implied influences of dust at the urban, industrial, and coastal regions (shorter wavelengths) and biomass emissions at the rural site (longer wavelengths). Absorptive aerosol optical depths at the urban and industrial sites were ~2.5 and 3.7 times higher than at the coastal and rural sites. Large negative ADREs at the bottom of the atmosphere at the urban and industrial sites implied strong surface cooling and the larger ADREs at the top of the atmosphere at the coastal site indicated more cooling of the Earth‐atmosphere system. The main aerosol types at the urban and industrial sites were mixed absorbing particles, while weakly‐absorbing fine mode particles dominated the coastal and rural sites. This study provides new information on the aerosol distributions and potential regional climate effects of aerosols in northeastern China.

Size-resolved mixing state of black carbon in the Canadian high Arctic and implications for simulated direct radiative effect

Abstract. Transport of anthropogenic aerosol into the Arctic in the spring months has the potential to affect regional climate; however, modeling estimates of the aerosol direct radiative effect (DRE) are sensitive to uncertainties in the mixing state of black carbon (BC). A common approach in previous modeling studies is to assume an entirely external mixture (all primarily scattering species are in separate particles from BC) or internal mixture (all primarily scattering species are mixed in the same particles as BC). To provide constraints on the size-resolved mixing state of BC, we use airborne single-particle soot photometer (SP2) and ultrahigh-sensitivity aerosol spectrometer (UHSAS) measurements from the Alfred Wegener Institute (AWI) Polar 6 flights from the NETCARE/PAMARCMIP2015 campaign to estimate coating thickness as a function of refractory BC (rBC) core diameter and the fraction of particles containing rBC in the springtime Canadian high Arctic. For rBC core diameters in the range of 140 to 220 nm, we find average coating thicknesses of approximately 45 to 40 nm, respectively, resulting in ratios of total particle diameter to rBC core diameters ranging from 1.6 to 1.4. For total particle diameters ranging from 175 to 730 nm, rBC-containing particle number fractions range from 16 % to 3 %, respectively. We combine the observed mixing-state constraints with simulated size-resolved aerosol mass and number distributions from GEOS-Chem–TOMAS to estimate the DRE with observed bounds on mixing state as opposed to assuming an entirely external or internal mixture. We find that the pan-Arctic average springtime DRE ranges from −1.65 to −1.34 W m−2 when assuming entirely externally or internally mixed BC. This range in DRE is reduced by over a factor of 2 (−1.59 to −1.45 W m−2) when using the observed mixing-state constraints. The difference in DRE between the two observed mixing-state constraints is due to an underestimation of BC mass fraction in the springtime Arctic in GEOS-Chem–TOMAS compared to Polar 6 observations. Measurements of mixing state provide important constraints for model estimates of DRE.

A parameterization for the light scattering enhancement factor with aerosol chemical compositions

The light scattering enhancement factor f (RH), defined as the ratio of the light scattering coefficient (σSP) observed under an elevated relative humidity (RH) conditions to that under dry conditions, is a crucial parameter for estimating aerosol direct radiative effects and atmospheric visibility. In this paper, a new f (RH) parameterization scheme considering both the influence of aerosol chemical compositions and that of particle number size distribution (PNSD) is proposed based on in situ measurements in the North China Plain. The development of this parameterization scheme includes three steps. First, aerosol hygroscopicity parameter κ is parameterized with aerosol chemical compositions. Then, the ratio between f (RH) fitted parameter κsca (f(RH)=1+κscaRH100−RH) and κ is introduced to correlate f (RH) with κ. The ratio, influenced mostly by PNSD, is described as a function of scattering Ångström exponent (SAE) because the SAE can represent the predominant size of aerosol particles to some extent. Finally, f (RH) cycle is parameterized with κsca. Validation results show that a good consistency between the parameterized and measured f (RH = 80%) is achieved and the correlation coefficient is 0.80. This parameterization scheme between aerosol chemistry and f (RH) can be used in chemical transport models for reducing uncertainties in estimations of direct aerosol radiative forcing and air quality assessments.

What drives changes in aerosol properties over the Yangtze River Basin in past four decades？

Since the Reform and Opening up in China, aerosols increasingly affect the country's climate change and human health. However, remote sensing studies have been inconclusive as to long-term trends in Chinese aerosol emissions. The newly-released MERRA-2 product provides a long-term (1980 onward) aerosol reanalysis dataset, and thus is used in this study for identifying trends in aerosol optical depth (AOD) and aerosol direct radiative effect (ADRE) in clear sky over the Yangtze River Basin (YRB) based on the MK nonparametric method. Results reveal that there is a notable turning point in AOD trends around 2008, i.e., significantly increasing by 0.0201 year−1 before 2008 and then deceasing by −0.0185 year−1. The reason may be the decreases of S02, NOx and soot (dust) emissions from major cities in the YRB since 2006. Likewise, the cooling (warming) effects at the top of atmosphere (TOA), surface (SFC) and atmosphere (ATM) strongly increase by −0.3744 and −0.5652 (0.2935) wm−2 year−1 before 2008, and then significantly decrease by 0.2731 and 0.5868 (−0.3145) wm−2 year−1. Trend analyses confirm that changes in AOD dominate ADRE trends. Furthermore, AOD is significantly negatively (positively) associated with NDVI and precipitation (GDP and Population density) over most areas of the YRB. Besides, similar spatial trends with AOD are also identified in GDP and NDVI. This indicates that increases in GDP and decreases in NDVI caused by rapid urbanization partly lead to the growth of AOD over the middle and lower reaches of the YRB. However, changes in precipitation and Population density alone may not be the main factors for the increasing AOD.

RETRIEVAL OF AEROSOL OPTICAL PROPERTIES FROM GROUND-BASED REMOTE SENSING MEASUREMENTS: AEROSOL ASYMMETRY FACTOR AND SINGLE SCATTERING ALBEDO

Abstract. The Devaux-Vermeulen-Li method (DVL method) is a simple approach to retrieve aerosol optical parameters from the Sun-sky radiance measurements. This study inherited the previous works of retrieving aerosol single scattering albedo (SSA) and scattering phase function, the DVL method was modified to derive aerosol asymmetric factor (g). To assess the algorithm performance at various atmospheric aerosol conditions, retrievals from AERONET observations were implemented, and the results are compared with AERONET official products. The comparison shows that both the DVL SSA and g were well correlated with those of AERONET. The RMSD and the absolute value of MBD deviations between the SSAs are 0.025 and 0.015 respectively, well below the AERONET declared SSA uncertainty of 0.03 for all wavelengths. For asymmetry factor g, the RMSD deviations are smaller than 0.02 and the absolute values of MBDs smaller than 0.01 at 675, 870 and 1020 nm bands. Then, considering several factors probably affecting retrieval quality (i.e. the aerosol optical depth (AOD), the solar zenith angle, and the sky residual error, sphericity proportion and Ǻngström exponent), the deviations for SSA and g of these two algorithms were calculated at varying value intervals. Both the SSA and g deviations were found decrease with the AOD and the solar zenith angle, and increase with sky residual error. However, the deviations do not show clear sensitivity to the sphericity proportion and Ǻngström exponent. This indicated that the DVL algorithm is available for both large, non-spherical particles and spherical particles. The DVL results are suitable for the evaluation of aerosol direct radiative effects of different aerosol types.

Measurement-based climatology of aerosol direct radiative effect, its sensitivities, and uncertainties from a background southeast US site

Abstract. Aerosol optical properties measured at Appalachian State University's co-located NASA AERONET and NOAA ESRL aerosol network monitoring sites over a nearly four-year period (June 2012–Feb 2016) are used, along with satellite-based surface reflectance measurements, to study the seasonal variability of diurnally averaged clear sky aerosol direct radiative effect (DRE) and radiative efficiency (RE) at the top-of-atmosphere (TOA) and at the surface. Aerosol chemistry and loading at the Appalachian State site are likely representative of the background southeast US (SE US), home to high summertime aerosol loading and one of only a few regions not to have warmed during the 20th century. This study is the first multi-year ground truth DRE study in the SE US, using aerosol network data products that are often used to validate satellite-based aerosol retrievals. The study is also the first in the SE US to quantify DRE uncertainties and sensitivities to aerosol optical properties and surface reflectance, including their seasonal dependence.Median DRE for the study period is −2.9 W m−2 at the TOA and −6.1 W m−2 at the surface. Monthly median and monthly mean DRE at the TOA (surface) are −1 to −2 W m−2 (−2 to −3 W m−2) during winter months and −5 to −6 W m−2 (−10 W m−2) during summer months. The DRE cycles follow the annual cycle of aerosol optical depth (AOD), which is 9 to 10 times larger in summer than in winter. Aerosol RE is anti-correlated with DRE, with winter values 1.5 to 2 times more negative than summer values. Due to the large seasonal dependence of aerosol DRE and RE, we quantify the sensitivity of DRE to aerosol optical properties and surface reflectance, using a calendar day representative of each season (21 December for winter; 21 March for spring, 21 June for summer, and 21 September for fall). We use these sensitivities along with measurement uncertainties of aerosol optical properties and surface reflectance to calculate DRE uncertainties. We also estimate uncertainty in calculated diurnally-averaged DRE due to diurnal aerosol variability. Aerosol DRE at both the TOA and surface is most sensitive to changes in AOD, followed by single-scattering albedo (ω0). One exception is under the high summertime aerosol loading conditions (AOD ≥ 0.15 at 550 nm), when sensitivity of TOA DRE to ω0 is comparable to that of AOD. Aerosol DRE is less sensitive to changes in scattering asymmetry parameter (g) and surface reflectance (R). While DRE sensitivity to AOD varies by only ∼ 25 to 30 % with season, DRE sensitivity to ω0, g, and R largely follow the annual AOD cycle at APP, varying by factors of 8 to 15 with season. Since the measurement uncertainties of AOD, ω0, g, and R are comparable at Appalachian State, their relative contributions to DRE uncertainty are largely influenced by their (seasonally dependent) DRE sensitivity values, which suggests that the seasonal dependence of DRE uncertainty must be accounted for. Clear sky aerosol DRE uncertainty at the TOA (surface) due to measurement uncertainties ranges from 0.45 (0.75 W m−2) for December to 1.1 (1.6 W m−2) for June. Expressed as a fraction of DRE computed using monthly median aerosol optical properties and surface reflectance, the DRE uncertainties at TOA (surface) are 20 to 24 % (15 to 22 %) for March, June, and September and 49 (50 %) for DEC. The relatively low DRE uncertainties are largely due to the low uncertainty in AOD measured by AERONET. Use of satellite-based AOD measurements by MODIS in the DRE calculations increases DRE uncertainties by a factor of 2 to 5 and DRE uncertainties are dominated by AOD uncertainty for all seasons. Diurnal variability in AOD (and to a lesser extent g) contributes to uncertainties in DRE calculated using daily-averaged aerosol optical properties that are slightly larger (by ∼ 20 to 30 %) than DRE uncertainties due to measurement uncertainties during summer and fall, with comparable uncertainties during winter and spring.