Sky Radiometer Research Articles

Unveiling global land fine- and coarse-mode aerosol dynamics from 2005 to 2020 using enhanced satellite-based monthly inversion data

Accurate fine-mode and coarse-mode aerosol knowledge is crucial for understanding their impacts on the climate and Earth's ecosystems. However, current satellite-based Fine-Mode Aerosol Optical Depth (FAOD) and Coarse-Mode Aerosol Optical Depth (CAOD) methods have drawbacks including inaccuracies, low spatial coverage, and limited temporal duration. To overcome these issues, we developed new global-scale FAOD and CAOD from 2005 to 2020 using a novel deep learning model capable of the synergistic retrieval of two aerosol sizes. After validation with the aerosol robotic network (AERONET) and sky radiometer network (SKYNET), the new monthly FAOD and CAOD showed significant improvements in accuracy and spatial coverage. From 2005 to 2020, the new data showed that China had the greatest decrease in FAOD and CAOD. In contrast, India and South Latin America had a significant increase in FAOD versus North Africa in CAOD. FAOD in the regions of Argentina, Paraguay, and Uruguay in South America have shown an upward trend. The results reveal that FAOD and CAOD display distinct patterns of change in the same regions, particularly on the west coast of the United States where FAOD is increasing, while CAOD is decreasing. Aside from the year 2020 due to the global COVID-19 pandemic, the analysis showed that although China has seen at least an +85% increase in energy consumption and urban expansion in 2019 compared to 2005 due to the needs of development and construction, the implementation of China's air pollution control policies has led to a significant decrease in FAOD (−46%) and CAOD (−65%) after 2013. This research enriches our comprehension of global fine and coarse aerosol patterns, additional investigations are needed to determine the potential global implications of these changes.

Novel use of an adapted ultraviolet double monochromator for measurements of global and direct irradiance, ozone, and aerosol

Abstract. A novel ultraviolet spectrometer has been developed and tested over 10 years at Lauder, New Zealand. The system, UV2, makes alternating measurements of the global and direct UV irradiance and can therefore be used to measure ozone and aerosol optical depth. After an analysis of the stability of UV2, these measurements, along with UV irradiance, are compared to relevant observations made by an additional UV spectrometer (UV4), a Dobson spectrophotometer (no. 072), and two radiometers measuring aerosol optical depth – a Prede sky radiometer and a Middleton Solar radiometer (SP02). UV2 irradiance is shown to be lower than UV4 by between 2.5 % and 3.5 %, with a standard deviation of a similar magnitude. Total column ozone values are shown to agree with Dobson spectrophotometer values with a mean bias of 2.57 Dobson units (DU) and standard deviation of 1.15 DU when using the direct sun measurements. Aerosol optical depth at 400–412 and 500 nm agrees to within 0.015 and is comparable to the difference between the reference radiometers. Further work is needed, particularly in the radiometric calibration at longer wavelengths, in order to determine if this instrument can supersede or enhance measurements made by the Dobson spectrophotometer or the aerosol radiometers.

Screening Approach of the Langley Calibration Station for Sun Photometers in China

A sun photometer is a type of photometer that points at the sun, and it has been playing an increasingly important role in characterizing aerosols across the world. As long as the solar photometer is accurately calibrated, the optical thickness of the aerosol can be obtained from the measured value of this device. When the calibration of a single instrument is not accurate, the inversion quantity varies greatly. The calibration constant of the sun photometer changes during its use process; thus, calibrations are frequently needed in order to ensure the accuracy of the measured value. The calibration constant of the solar photometer is usually determined using the Langley method. Internationally, AERONET has two Langley calibration stations: the Mauna Loa observatory in the United States and the Izaña observatory in Spain. So far, the International Comparison and Calibration System has been established in Beijing, similar to AERONET at GSFC, but the Langley calibration system has not yet been established. Therefore, it is necessary to select a suitable calibration station in China. This paper studies the requirements of the calibration station using the Langley method. We used long-term records of satellite-derived measurements and survey data belonging to the aerosol optical thickness data of SNPP/VIIRS, CERES, MERRA-2, etc., in order to gain a better understanding of whether these stations are suitable for calibration. From the existing astronomical observation stations, meteorological stations, and the Sun–Sky Radiometer Observation Network (SONET) observation stations in China, the qualified stations were selected. According to the statistical data from the Ali observatory, the monthly average of clear sky is 20.21 days, and it is always greater than 15 days. The monthly average of aerosol is not more than 0.15 and is less than 0.3. We believe that the atmosphere above the Ali observatory is stable, and the results show that the Ali observatory has excellent weather conditions. This study can provide a selection of calibration sites for solar photometer calibrations in China that may need to be further characterized and evaluated, and at the same time provide a method to exclude unsuitable calibration sites.

Analysis of Aerosol Optical Depth and Forward Scattering in an Ultraviolet Band Based on Sky Radiometer Measurements

The sky-radiometer/sun-photometer is the most widely used instrument for obtaining aerosol optical depth (AOD) or aerosol optical properties worldwide. Due to the existence of field of view (FOV, 1°), the radiation received by the sky-radiometer includes the forward scattering in addition to direct solar irradiance. This leads to more diffuse light errors of retrieved AODs, especially for shorter wavelength and heavily polluted weather conditions. Using simulation data of three typical aerosol particles (dust, soot, water-soluble), we first verified the accuracy of the Monte Carlo method for calculating the forward scattering effect. Based on the sky-radiometer data collected in Xi’an (2015–2020) where heavy pollution weather is common, the relative errors and correction factors of the AOD were obtained under different conditions, including various short wavelengths (≤400 nm), solar zenith angles (SZAs) and AODs. Our analysis indicates the close dependence of AOD correction factors on wavelength, SZA, AOD and the optical properties of aerosol particles. The mean relative error in Xi’an increases with the decrease of wavelength (~16.1% at 315 nm) and decreases first and then increases with the increase of the SZA. The relative errors caused by forward scattering can exceed 10% when the AOD is greater than 1 and 25% when the AOD is larger than 2 in the ultraviolet (UV) band. The errors with a wavelength greater than 400 nm and an AOD below 1.0 can be within 5%, which can be ignored. The correlation coefficients of AODs before and after a correction from 315 nm to 400 nm are greater than 0.96, which basically increase with the increase of the wavelength. This indicates that the significance of the forward scattering effect in the Xi’an area with heavy pollution cannot be ignored for short wavelengths. However, such effect is negligible at the longer wavelengths and lower AODs (<1.0) of a sky-radiometer.

Evaluating the effects of columnar NO2on the accuracy of aerosol optical properties retrievals

Abstract. We aim to evaluate the NO2 absorption effect in aerosol columnar properties, namely the aerosol optical depth (AOD), Ångström exponent (AE), and single scattering albedo (SSA), derived from sun–sky radiometers in addition to the possible retrieval algorithm improvements by using more accurate characterization of NO2 optical depth from co-located or satellite-based real-time measurements. For this purpose, we employ multiannual (2017–2022) records of AOD, AE, and SSA collected by sun photometers at an urban and a suburban site in the Rome area (Italy) in the framework of both the Aerosol Robotic Network (AERONET) and SKYNET networks. The uncertainties introduced in the aerosol retrievals by the NO2 absorption are investigated using high-frequency observations of total NO2 derived from co-located Pandora spectroradiometer systems in addition to spaceborne NO2 products from the Tropospheric Monitoring Instrument (TROPOMI). For both AERONET and SKYNET, the standard network products were found to systematically overestimate AOD and AE. The average AOD bias found for Rome is relatively low for AERONET (∼ 0.002 at 440 nm and ∼ 0.003 at 380 nm) compared to the retrieval uncertainties but quite a bit higher for SKYNET (∼ 0.007). On average, an AE bias of ∼ 0.02 and ∼ 0.05 was estimated for AERONET and SKYNET, respectively. In general, the correction seems to be low for areas with low columnar NO2 concentrations, but it is still useful for low AODs (< 0.3), where the majority of observations are found, especially under high NO2 pollution events. For the cases of relatively high NO2 levels (> 0.7 DU), the mean AOD bias was found within the range 0.009–0.012 for AERONET, depending on wavelength and location, and about 0.018 for SKYNET. The analysis does not reveal any significant impact of the NO2 correction on the derived aerosol temporal trends for the very limited data sets used in this study. However, the effect is expected to become more evident for trends derived from larger data sets and in the case of an important NO2 trend. In addition, the comparisons of the NO2-modified ground-based AOD data with satellite retrievals from the Deep Blue (DB) algorithm of the NASA Moderate Resolution Imaging Spectroradiometer (MODIS) resulted in a slight improvement in the agreement of about 0.003 and 0.006 for AERONET and SKYNET, respectively. Finally, the uncertainty in assumptions on NO2 seems to have a non-negligible impact on the retrieved values of SSA at 440 nm leading to an average positive bias of about 0.02 (2 %) in both locations for high NO2 loadings (> 0.7 DU).

Evaluation of MODIS DT, DB, and MAIAC Aerosol Products over Different Land Cover Types in the Yangtze River Delta of China

The Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) has been widely used in atmospheric environment and climate change research. Based on data of the Aerosol Robotic Network and Sun–Sky Radiometer Observation Network in the Yangtze River Delta, the retrieval accuracies of MODIS C6.1 Dark Target (DT), Deep Blue (DB), and C6.0 Multi-angle Implementation of Atmospheric Correction (MAIAC) products under different land cover types, aerosol types, and observation geometries were analyzed. About 65.64% of MAIAC AOD is within the expected error (Within EE), which is significantly higher than 41.43% for DT and 56.98% for DB. The DT product accuracy varies most obviously with the seasons, and the Within EE in winter is more than three times that in spring. The DB and MAIAC products have low accuracy in summer but high in other seasons. The accuracy of the DT product gradually decreases with the increase in urban and water land-cover proportion. After being corrected by bias and mean relative error, the DT accuracy is significantly improved, and the Within EE increases by 24.12% and 32.33%, respectively. The observation geometries and aerosol types were also examined to investigate their effects on AOD retrieval.

Development and Classification of Japanese-Region-Specific Aerosol Models Based on 10-Year Sky Radiometer Observations

Development and Classification of Japanese-Region-Specific Aerosol Models Based on 10-Year Sky Radiometer Observations

Aerosol classification using fuzzy clustering over a tropical rural site

Exact knowledge on the types of aerosols present over a region is very important in the radiative forcing estimates. Several techniques are available to classify aerosols, which have their own pros and cons. In the present study, a soft clustering technique, Fuzzy C-Means (FCM) is employed to classify aerosols using multiple aerosol parameters over a rural site Gadanki (13.48oN, 79.18°E), India. The optical and microphysical properties of the aerosols (26 parameters) derived from long-term measurements of the Sky Radiometer (from April 2008 to October 2020) are utilized for cluster analysis. The three resultant clusters were found to be distinct and compact based on high intra-cluster similarity and low inter-cluster similarity. By comparing the clustering results of different subsets of data and testing the robustness of the FCM algorithm, we found that the correct classification percentage for each scenario was about 98.4%. Even by introducing a 10% random error for each of the aerosol microphysical properties used in the cluster analysis, around 94.5% of the records were found to retain the original clusters. Based on the aerosol properties of the clusters, the three clusters were identified as mixed mode moderately absorbing, mixed mode slightly absorbing, and coarse mode slightly absorbing type of aerosols. While comparing with the global aerosol models, these three aerosol types showed similarities with biomass burning, polluted marine, and polluted continental aerosol types. Significant seasonal variability of the identified aerosol types was observed, with biomass burning type dominating in the pre-monsoon season, polluted marine during the monsoon season, and polluted continental in a relatively higher percentage compared to the other two types in winter and post-monsoon seasons. An increasing trend in polluted marine aerosol type is noticed, whilst biomass burning and polluted continental showed decreasing trends. Furthermore, the existing knowledge on various aspects of aerosols over Gadanki ascertains that the identified aerosol types are reasonable, implying that the FCM clustering technique for aerosol classification is effective and it might be extend to other locations.

Quantitative evaluation of mixed biomass burning and anthropogenic aerosols over the Indochina Peninsula using MERRA-2 reanalysis products validated by sky radiometer and MAX-DOAS observations

In this study, we conducted the quantitative evaluation of aerosol optical properties in the Indochina Peninsula (ICP), which is significantly affected yearly by both biomass burning (BB) and anthropogenic aerosols, using Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) aerosol products. To perform spatiotemporal analysis with validated aerosol data, the MERRA-2 aerosol optical depth (AOD) and absorption AOD (AAOD) data were evaluated based on sky radiometer observations at the SKYNET Phimai site (15.18° N, 102.56° E). Furthermore, multi-axis differential optical absorption spectroscopy was conducted, providing additional data for the comparison of the aerosol extinction coefficient (AEC) vertical profile data. MERRA-2 AOD, AAOD, and AEC at altitudes below 1 km were underestimated in the dry season, with relative mean biases of 0.84, 0.54, and 0.48, respectively. These underestimations are attributed to insufficient BB emissions of light-absorbing aerosols near the surface. On the basis of these results, we investigated the factors that determined spatiotemporal variations in AOD over ICP from 2009 to 2020. We found that the seasonal variations in AOD were driven mainly by organic carbon (OC) and sulfate aerosols. OC AOD was dominant during the active BB period (from January to March), whereas sulfate AOD was high all year round, accounting for more than 25% of the total AOD. Sulfate AOD in the northeast ICP (NEIC) was approximately 74% of the total AOD in October, indicating the remarkable effect of sulfate aerosol transportation from southern China (SC). In the period of study, AOD decreased in NEIC and south ICP (SIC) by − 4.40% and − 3.00% year−1, respectively, corresponding to the decrease in sulfur dioxide concentrations in SC and NEIC. Thus, OC AOD was dominant during the active BB periods, whereas a significant amount of anthropogenic aerosols from SC contributed to the atmospheric environment over ICP throughout 2009–2020.

FY-4A/AGRI Aerosol Optical Depth Retrieval Capability Test and Validation Based on NNAeroG

The Advanced Geostationary Radiation Imager (AGRI) is one of the main imaging sensors on the Fengyun-4A (FY-4A) satellite. Due to the combination of high spatial and temporal resolution, the AGRI is suitable for continuously monitoring atmospheric aerosol. Existing studies only perform AOD retrieval on the dark target area of FY-4A/AGRI, and the full disk AOD retrieval is still under exploration. The Neural Network AEROsol Retrieval for Geostationary Satellite (NNAeroG) based on the Fully Connected Neural Network (FCNN) was used to retrieve FY-4A/AGRI full disk aerosol optical depth (AOD). The data from 111 ground-based Aerosol Robotic Network (AERONET) and Sun–Sky Radiometer Observation Network (SONET) sites were used to train the neural network, and the data from 28 other sites were used for independent validation. FY-4A/AGRI AOD data from 2017 to 2020 were validated over the full disk and three different surface types (vegetated areas, arid areas, and marine and coastal areas). For general validation, the AOD predicted by the application of NNAeroG to FY-4A/AGRI observations is consistent with the ground-based reference AOD data. The validation of the FY-4A/AGRI AOD versus the reference data set shows that the root-mean-square error (RMSE), mean absolute error (MAE), R squared (R2), and percentage of data with errors within the expected error ± (0.05 + 15%) (EE15) are 0.237, 0.145, 0.733, and 58.7%, respectively. The AOD retrieval accuracy over vegetated areas is high but there is potential for improvement of the results over arid areas and marine and coastal areas. AOD retrieval results of FY-4A/AGRI were compared under fine and coarse modes. The retrieved AOD has low accuracy in coarse mode but is better in coarse–fine mixed mode and fine mode. The current AOD products over the ocean of NNAeroG-FY4A/AGRI are not recommended. Further development of algorithms for marine areas is expected to improve the full disk AOD retrieval accuracy.

Quality assessment of Second-generation Global Imager (SGLI)-observed cloud properties using SKYNET surface observation data

Abstract. The Second-generation Global Imager (SGLI) onboard the Global Change Observation Mission – Climate (GCOM-C) satellite, launched on 23 December 2017, observes various geophysical parameters with the aim of better understanding the global climate system. As part of that aim, SGLI has great potential to unravel several uncertainties related to clouds by providing new cloud products along with several other atmospheric products related to cloud climatology, including aerosol products from polarization channels. However, very little is known about the quality of the SGLI cloud products. This study uses data about clouds and global irradiances observed from the Earth's surface using a sky radiometer and a pyranometer, respectively, to understand the quality of the two most fundamental cloud properties – cloud optical depth (COD) and cloud-particle effective radius (CER) – of both water and ice clouds. The SGLI-observed COD agrees well with values observed from the surface, although it agrees better for water clouds than for ice clouds, while the SGLI-observed CER exhibits poorer agreement than does the COD, with SGLI values being generally higher than the sky radiometer values. These comparisons between the SGLI and sky radiometer cloud properties are found to differ for different cloud types of both the water and ice cloud phases and different solar and satellite viewing angles by agreeing better for relatively uniform and flat cloud type and for relatively low solar zenith angle. Analyses of SGLI-observed reflectance functions and values calculated by assuming plane-parallel cloud layers suggest that SGLI-retrieved cloud properties can have biases in the solar and satellite viewing angles, similar to other satellite sensors including the Moderate Resolution Imaging Spectroradiometer (MODIS). Furthermore, it is found that the SGLI-observed cloud properties reproduce global irradiances quite satisfactorily for both water and ice clouds by resembling several important features of the COD comparison, such as better agreement for water clouds than for ice clouds and the tendency to underestimate (resp. overestimate) the COD in SGLI observations for optically thick (resp. thin) clouds.

Aerosol optical characteristics in the urban area of Rome, Italy, and their impact on the UV index

Abstract. The impact of the aerosol optical properties on the ultraviolet index (UVI) in the urban area of Rome is investigated in this study. In particular, the influence of aerosol optical depth (AOD) and single scattering albedo (SSA), estimated at the wavelength of 340 nm, and of the Ångström exponent, calculated in the range 340–500 nm, over a period of 11 years (2010–2020) in the months from March to September are analyzed. The UVI is monitored by a Brewer spectrophotometer, whereas measurements of the direct Sun and diffuse sky irradiances are performed by a co-located PREDE-POM sun–sky radiometer of the ESR/SKYNET network; the aerosol optical properties are obtained by the Skyrad MRIv2 retrieval. A novel method, based on physical principles and easily adaptable to other contexts, is developed to extrapolate the aerosol properties to the UV range during periods when only visible to near-infrared measurements are available. The retrievals from the sun–sky radiometer are consistent with the chemical characterization of urban PM10 (particulate matter 10 mm or less in diameter) samples collected during an intensive field campaign held in summer 2011 at the same site (URBan Sustainability Related to Observed and Monitored Aerosol – URBS ROMA). The PM macro components identified during the campaign are grouped in order to evaluate the contribution of the main macro sources (soil, sea, secondary inorganic, organics, and traffic) whose relative role is indeed expected to strongly affect the aerosol absorption capability. The surface forcing efficiency, calculated as the change in the UV index for a unit AOD variation, shows that AOD is the primary parameter affecting the surface irradiance under clear-sky conditions in Rome. SSA and the Ångström exponent are also identified as secondary influencing factors, i.e., the surface forcing efficiency is found to be greater for smaller zenith angles and for larger and more absorbent particles in the UV range (such as, e.g., mineral dust).

Influences of aerosols and thin cirrus clouds on GOSAT XCO2 and XCH4 using Total Carbon Column Observing Network, sky radiometer, and lidar data

ABSTRACT The column-averaged, dry air mole fractions of CO2 and CH4 (XCO2 and XCH4, respectively) were retrieved from short-wavelength infrared (SWIR) spectra observed by the Greenhouse gases Observing SATellite (GOSAT). Continuous measurements of SWIR spectra have been made via GOSAT since 2009, but there has been insufficient investigation of the effects of cirrus clouds and aerosols on the observations. In this work, we investigated the influences of aerosols and cirrus clouds on the differences between GOSAT observations and Total Carbon Column Observing Network (TCCON) data for XCO2 and XCH4 (ΔXCO2 and ΔXCH4) at three sites: Tsukuba and Saga in Japan, and Lauder in New Zealand. We used aerosol optical thickness (AOT), Angstrom exponents (AEs), and single scattering albedo (SSA), all obtained from sky radiometer observations, as well as vertical profiles of aerosols and thin cirrus clouds from lidar observations. Matchups were performed within ±0.1° latitude/longitude rectangular areas of each TCCON site, and within 30 min of the GOSAT overpass time. The results show a negative slope between ΔXCO2 and AOT at 500 nm determined from sky radiometer data at Tsukuba and Saga. The GOSAT XCO2 values tended to be lowered in the presence of cirrus clouds and dense boundary-layer aerosols. Moreover, a significant negative ΔXCO2 was observed at times of large AOTs that resulted from dust-like events. At Lauder, ΔXCO2 was negatively correlated with the AOT at 500 nm, although the AOT at this site was generally small. The mean ± standard deviation for ΔXCO2 and ΔXCH4 at Lauder are −0.80 ± 1.83 (ppm) and −5.27 ± 10.79 (ppb) with correlation coefficients r between GOSAT and TCCON of 0.94 and 0.83, respectively. Both ΔXCO2 and ΔXCH4 were significantly and negatively correlated with the AOT during Sep-Oct-Nov. In addition, stratospheric aerosols caused large negative biases of ΔXCO2 and ΔXCH4 at Lauder despite the small stratospheric aerosol optical depth at that site.

Evaluation of MERRA-2 Aerosol Optical and Component Properties over China Using SONET and PARASOL/GRASP Data

The Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) is widely used as an advanced model dataset for the understanding of global climate change. However, independent validation and comparison of MERRA-2 are both insufficient and always desired. Therefore, in this study, the quantitative evaluation of MERRA-2 aerosol products was conducted over China for Aerosol Optical Depth (AOD), Angstrom exponent (AE), absorbing AOD (AAOD) and chemical components (black carbon (BC) and dust (DU)) using Sun sky radiometer Observation NETwork (SONET) ground-based measurements and POLDER-3/PARASOL satellite products generated by the GRASP algorithm. The available MERRA-2 monthly dataset and PARASOL/GRASP monthly and seasonal products were intercompared over China. MERRA-2 AOD (550 nm) show general good agreement with SONET and PARASOL/GRASP. For example, the correlation coefficients are usually 0.6–0.85 with SONET and 0.75–0.85 with PARASOL/GRASP, the bias is usually −0.293 to +0.008 with SONET. For AE and AAOD, the agreement is still reasonable. MERRA-2 is found to overestimate fine mode AE and to display a general underestimation of aerosol absorption over China. In addition, MERRA-2 BC and DU mass concentrations show spatial and quantitative consistency with PARASOL/GRASP components climatological products. The relatively high columnar BC mass concentration is observed around 1.5–2 mg/m3 over the East China industrial region and high DU mass concentration is around 150 mg/m3 near Taklimakan desert. MERRA-2 shows slightly higher BC and lower DU concentration than PARASOL/GRASP over East China. The evaluations with in situ BC measurements near surface verify the overestimation (MAE = +0.44 µg/m2) of MERRA-2 and underestimation (MAE = −0.38 µg/m2) of PARASOL/GRASP. The analysis demonstrates multi-source datasets, such as ground-based, space-borne remote sensing, in situ measurements, model simulation as well as reanalysis data, complement each other and can be used to refine aerosol characterization.

Vertical profile of the clear-sky aerosol direct radiative effect in an Alpine valley, by the synergy of ground-based measurements and radiative transfer simulations

Atmospheric aerosols play an important role in Earth’s radiative balance, directly interacting with solar radiation or influencing cloud formation and properties. In order to assess their radiative impact, it is necessary to accurately characterise their optical properties, together with their spatial and vertical distribution. The information on aerosol vertical profile is often scarce, in particular in mountainous, complex terrains. This study presents the first attempt to evaluate the shortwave aerosol direct radiative effect in the Aosta Valley, a mountainous region in the Northwestern Italian Alps. Ground-based, remote sensing instruments (a sky radiometer and an Automated Lidar Ceilometer) are used to derive two descriptions of the aerosol properties and vertical distribution: a first, more accurate description, which includes the whole spectral information about the aerosol extinction coefficient, phase function and single scattering albedo; a second, more approximate one, which only relies on spectrally constant values of aerosol single scattering albedo and asymmetry factor. This information is used as input for radiative transfer simulations, which allow to estimate, in cloudless conditions, the shortwave aerosol direct radiative effect and the vertical profile of the instantaneous heating rates in the lower layers of the atmosphere. The simulations obtained with the two descriptions do not differ significantly: they highlight a strong surface dimming (between − 25 and − 50 W m− 2) due to the presence of aerosol, with a considerable radiative absorption inside the atmospheric column (around + 30 W m− 2), and an overall small cooling effect for the Earth-atmospheric system. The absorption of solar radiation within the atmospheric column due to aerosol leads to instantaneous heating rates up to 1.5 K day− 1 in the tropospheric layers below 6 km a.s.l. These results show that, in some conditions, the shortwave aerosol direct radiative effect can be considerable even in this Alpine environment, usually considered as relatively pristine (yearly average PM10 concentration about 20 μg m− 3).

Variabilities in PM2.5 and Black Carbon Surface Concentrations Reproduced by Aerosol Optical Properties Estimated by In-Situ Data, Ground Based Remote Sensing and Modeling

Because of the increased temporal and spatial resolutions of the sensors onboard recently launched satellites, satellite-based surface aerosol concentration, which is usually estimated from the aerosol optical depth (AOD), is expected to become a strategic tool for air quality studies in the future. By further exploring the relationships of aerosol concentrations and their optical properties using ground observations, the accuracies of these products can be improved. Here, we analyzed collocated observations of surface mass concentrations of fine particulate matter (PM2.5) and black carbon (BC), as well as columnar aerosol optical properties from a sky radiometer and aerosol extinction profiles obtained by multi-axis differential optical absorption spectroscopy (MAX-DOAS), during the 2019–2020 period. We focused the analyses on a daily scale, emphasizing the role of the ultraviolet (UV) spectral region. Generally, the correlation between the AOD of the fine fraction (i.e., fAOD) and the PM2.5 surface concentration was moderately strong, regardless of considerations of boundary layer humidity and altitude. In contrast, the fAOD of the partial column below 1 km, which was obtained by combining sky radiometer and MAX-DOAS retrievals, better reproduced the variability of the PM2.5 and resulted in a linear relationship. In the same manner, we demonstrated that the absorption AOD of the fine fraction (fAAOD) of the partial column was related to the variability of the BC concentration. Analogous analyses based on aerosol products from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) confirmed these findings and highlighted the importance of the shape of the aerosol profile. Overall, our results indicated a remarkable consistency among the retrieved datasets, and between the datasets and MERRA-2 products. These results confirmed the well-known sensitivity to aerosol absorption in the UV spectral region; they also highlighted the efficacy of combined MAX-DOAS and sky radiometer observations.

Light-absorption properties of brown carbon aerosols in the Asian outflow: Implications of a combination of filter and ground remote-sensing observations at Fukue Island, Japan

Brown carbon (BrC) aerosols have important warming effects on Earth's radiative forcing. However, information on the evolution of the light-absorption properties of BrC aerosols in the Asian outflow region is limited. In this study, we evaluated the light-absorption properties of BrC using in-situ filter measurements and sky radiometer observations of the ground-based remote sensing network SKYradiometer NETwork (SKYNET) made on Fukue Island, western Japan in 2018. The light-absorption coefficient of BrC obtained from filter measurements had a temporal trend similar to that of the ambient concentration of black carbon (BC), indicating that BrC and BC have common combustion sources. The absorption Angstrom exponent in the wavelength range of 340–870 nm derived from the SKYNET observations was 15% higher in spring (1.81 ± 0.30) than through the whole year (1.53 ± 0.50), suggesting that the Asian outflow carries light-absorbing aerosols to Fukue Island and the western North Pacific. After eliminating the contributions of BC, the absorption Angstrom exponent of BrC alone obtained from filter observations had a positive Spearman correlation (rs = 0.77, p < 0.1) with that derived from SKYNET observations but 33% higher values, indicating that the light-absorption properties of BrC were successfully captured using the two methods. Using the atmospheric transport model FLEXPART and fire hotspots obtained from the Visible Infrared Imaging Radiometer Suite product, we identified a high-BrC event related to an air mass originating from regions with consistent fossil fuel combustion and sporadic open biomass burning in central East China. The results of the study may help to clarify the dynamics and climatic effects of BrC aerosols in East Asia.

Optimal use of the Prede POM sky radiometer for aerosol, water vapor, and ozone retrievals

Abstract. The Prede POM sky radiometer is a filter radiometer deployed worldwide in the SKYNET international network. A new method, called Skyrad pack MRI version 2 (MRI v2), is presented here to retrieve aerosol properties (size distribution, real and imaginary parts of the refractive index, single-scattering albedo, asymmetry factor, lidar ratio, and linear depolarization ratio), water vapor, and ozone column concentrations from the sky radiometer measurements. MRI v2 overcomes two limitations of previous methods (Skyrad pack versions 4.2 and 5, MRI version 1). One is the use of all the wavelengths of 315, 340, 380, 400, 500, 675, 870, 940, 1020, 1627, and 2200 nm if available from the sky radiometers, for example, in POM-02 models. The previous methods cannot use the wavelengths of 315, 940, 1627, and 2200 nm. This enables us to provide improved estimates of the aerosol optical properties, covering almost all the wavelengths of solar radiation. The other is the use of measurements in the principal plane geometry in addition to the solar almucantar plane geometry that is used in the previous versions. Measurements in the principal plane are regularly performed; however, they are currently not exploited despite being useful in the case of small solar zenith angles when the scattering angle distribution for almucantars becomes too small to yield useful information. Moreover, in the inversion algorithm, MRI v2 optimizes the smoothness constraints of the spectral dependencies of the refractive index and size distribution, and it changes the contribution of the diffuse radiances to the cost function according to the aerosol optical depth. This overcomes issues with the estimation of the size distribution and single-scattering albedo in the Skyrad pack version 4.2. The scattering model used here allows for non-spherical particles, improving results for mineral dust and permitting evaluation of the depolarization ratio. An assessment of the retrieval uncertainties using synthetic measurements shows that the best performance is obtained when the aerosol optical depth is larger than 0.2 at 500 nm. Improvements over the Skyrad pack versions 4.2 and 5 are obtained for the retrieved size distribution, imaginary part of the refractive index, single-scattering albedo, and lidar ratio at Tsukuba, Japan, while yielding comparable retrievals of the aerosol optical depth, real part of the refractive index, and asymmetry factor. A radiative closure study using surface solar irradiances from the Baseline Surface Radiation Network and the parameters retrieved from MRI v2 showed consistency, with a positive bias of the simulated global irradiance of about +1 %. Furthermore, the MRI v2 retrievals of the refractive index, single-scattering albedo, asymmetry factor, and size distribution have been found to be in agreement with integrated profiles of aircraft in situ measurements of two Saharan dust events at the Cape Verde archipelago during the Sunphotometer Airborne Validation Experiment in Dust (SAVEX-D) 2015 field campaign.

Estimation of Aerosol Complex Refractive Index over a tropical atmosphere using a synergy of in-situ measurements

Aerosol complex refractive index (ACRI) is a key micro-physical parameter used for modeling their radiative effects. In this study, an approach is developed to estimate the ACRI using a combination of surface-based measurements (2008–2015) from the Aerodynamic Particle Sizer (APS), the integrating Nephelometer, and the Aethalometer over a tropical rural location in the southern peninsular India. Around 98% of the real part of the estimated ACRI varied in the range of 1.3–1.8 while 99% of the imaginary part was found to vary in the range of 0.01–0.2 at 550 nm. The estimated imaginary parts are found to be high during pre-monsoon season suggesting the dominance of the increased absorption type aerosols. This is in line with the high concentration of black carbon aerosol observed during the pre-monsoon. The spectral variation of estimated ACRI is also studied and finally the significance of refractive index of surface aerosols in columnar properties is analysed by using the columnar single scattering albedo (SSA) and aerosol optical depth (AOD) observations from Sky radiometer. During winter season, the contribution to the total columnar scattering and absorption are mainly from surface or below the atmospheric boundary layer aerosols, whereas in monsoon season 80–90% contribution is from aerosols above.

Aerosol Optical Properties Observed by Sky Radiometer During Haze Observation in Kyusyu and Okinawa Areas in Early August 2020

Aerosol Optical Properties Observed by Sky Radiometer During Haze Observation in Kyusyu and Okinawa Areas in Early August 2020