Aerosol Extinction Profiles Research Articles

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.

Evaluation of UV–visible MAX-DOAS aerosol profiling products by comparison with ceilometer, sun photometer, and in situ observations in Vienna, Austria

Abstract. Since May 2017 and August 2018, two ground-based MAX-DOAS (multi-axis differential optical absorption spectroscopy) instruments have been continuously recording daytime spectral UV–visible measurements in the northwest (University of Natural Resources and Life Sciences (BOKU) site) and south (Arsenal site), respectively, of the Vienna city center (Austria). In this study, vertical aerosol extinction (AE) profiles, aerosol optical depth (AOD), and near-surface AE are retrieved from MAX-DOAS measurements recorded on cloud-free days applying the Bremen Optimal estimation REtrieval for Aerosols and trace gaseS (BOREAS) algorithm. Measurements of atmospheric profiles of pressure and temperature obtained from routinely performed sonde ascents are used to calculate box-air-mass factors and weighting functions for different seasons. The performance of BOREAS was evaluated against co-located ceilometer, sun photometer, and in situ instrument observations covering all four seasons. The results show that the vertical AE profiles retrieved from the BOKU UV–visible MAX-DOAS observations are in very good agreement with data from the co-located ceilometer, reaching correlation coefficients (R) of 0.936–0.996 (UV) and 0.918–0.999 (visible) during the fall, winter, and spring seasons. Moreover, AE extracted using the lowest part of MAX-DOAS vertical profiles (up to 100 m above ground) is highly consistent with near-surface ceilometer AE (R>0.865 and linear regression slopes of 0.815–1.21) during the fall, winter, and spring seasons. A strong correlation is also found for the BOREAS-based AODs when compared to the AERONET ones. Notably, the highest correlation coefficients (R=0.953 and R=0.939 for UV and visible, respectively) were identified for the fall season. While high correlation coefficients are generally found for the fall, winter, and spring seasons, the results are less reliable for measurements taken during summer. For the first time, the spatial variability of AOD and near-surface AE over the urban environment of Vienna is assessed by analyzing the retrieved and evaluated BOREAS aerosol profiling products in terms of different azimuth angles of the two MAX-DOAS instruments and for different seasons. We found that the relative differences of averaged AOD between different azimuth angles are 7–13 %, depending on the season. Larger relative differences of up to 32 % are found for near-surface AE in the different azimuthal directions. This study revealed the strong capability of BOREAS to retrieve AE profiles, AOD, and near-surface AE over urban environments and demonstrated its use for identifying the spatial variability of aerosols in addition to the temporal variation.

Research of NO2 vertical profiles with look-up table method based on MAX-DOAS

Obtaining the vertical distribution profile of trace gas is of great significance for studying the diffusion procedure of air pollution. In this article, a look-up table method based on multi-axis differential optical absorption spectroscopy (MAXDOAS) technology is established for retrieving the tropospheric NO2 vertical distribution profiles. This method retrieves the aerosol extinction profiles with minimum cost function. Then, the aerosol extinction profiles and the atmospheric radiation transfer model (RTM) are employed to establish the look-up table for retrieving the NO2 vertical column densities (VCDs) and profiles. The measured NO2 differential slant column densities (DSCDs) are compared with the NO2 DSCDs simulated by the atmospheric RTM, and the NO2 VCDs, the weight factor of NO2 in the boundary layer, and the boundary layer height are obtained by the minimization process. The look-up table is established to retrieve NO2 VCDs based on MAX-DOAS measurements in Huaibei area, and the results are compared with the data from Copernicus Atmospheric Monitoring Service(CAMS) model. It isfound that there are nearly consistent and the correlation coefficient R2 is morethan 0.86. The results show that this technology provides a more convenient and accurate retrieval method for the stereoscopic monitoring ofatmospheric environment.

OMPS LP Version 2.0 multi-wavelength aerosol extinction coefficient retrieval algorithm

Abstract. The OMPS Limb Profiler (LP) instrument is designed to provide high-vertical-resolution ozone and aerosol profiles from measurements of the scattered solar radiation in the 290–1000 nm spectral range. It collected its first Earth limb measurement on 10 January 2012 and continues to provide daily global measurements of ozone and aerosol profiles from the cloud top up to 60 and 40 km, respectively. The relatively high vertical and spatial sampling allow detection and tracking of sporadic events when aerosol particles are injected into the stratosphere, such as volcanic eruptions or pyrocumulonimbus (PyroCb) events. In this paper we discuss the newly released Version 2.0 OMPS multi-wavelength aerosol extinction coefficient retrieval algorithm. The algorithm now produces aerosol extinction profiles at 510, 600, 674, 745, 869 and 997 nm wavelengths. The OMPS LP Version 2.0 data products are compared to the SAGE III/ISS, OSIRIS and CALIPSO missions and shown to be of good quality and suitable for scientific studies. The comparison shows significant improvements in the OMPS LP retrieval performance in the Southern Hemisphere (SH) and at lower altitudes. These improvements arise from use of the longer wavelengths, in contrast with the V1.0 and V1.5 OMPS aerosol retrieval algorithms, which used radiances only at 675 nm and therefore had limited sensitivity in those regions. In particular, the extinction coefficients at 745, 869 and 997 nm are shown to be the most accurate, with relative accuracies and precisions close to 10 % and 15 %, respectively, while the 675 nm relative accuracy and precision are on the order of 20 %. The 510 nm extinction coefficient is shown to have limited accuracy in the SH and is only recommended for use between 20–24 km and only in the Northern Hemisphere. The V2.0 retrieval algorithm has been applied to the complete set of OMPS LP measurements, and the new dataset is publicly available.

A global analysis of diurnal variability in dust and dust mixture using CATS observations

Abstract. The current study investigates the diurnal cycle of dust and dust mixture loading across the global tropics, subtropics, and mid-latitudes by analyzing aerosol extinction and typing profiles observed by the Cloud-Aerosol Transport System (CATS) lidar aboard the International Space Station. According to the comparison with ground-based and other satellite observations, CATS aerosol and dust and dust mixture loading observations exhibit reasonable quality but significant day–night inconsistency. To account for this day–night inconsistency in CATS data quality, the diurnal variability in dust and dust mixture characteristics is currently examined separately for daytime and nighttime periods. Based on an analysis of variance (ANOVA) analytical framework, pronounced diurnal variations in dust and dust mixture loading are generally uncovered during daytime periods and over terrestrial areas. The current study identifies statistically significant diurnal variability in dust and dust mixture loading over key dust sources, including the Bodélé Depression, the West African El Djouf, Rub' al-Khali desert, and western and southern North America, confirming the previous observation-based findings regarding the diurnal cycle of dust emission and underlying meteorological processes in these regions. Significant seasonal and diurnal variability in dust and dust mixture is identified over the Iraqi and Thar deserts. The identified significant diurnal cycles in dust mixture loading over the vegetated regions in the Amazon and tropical southern Africa are hypothesized to be driven by enhanced dust emission due to wildfires.

Retrieval and evaluation of tropospheric-aerosol extinction profiles using multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements over Athens, Greece

Abstract. In this study, we report on the retrieval of aerosol extinction profiles from ground-based scattered sunlight multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements, carried out at Athens, Greece. It is the first time that aerosol profiles are retrieved from MAX-DOAS measurements in Athens. The reported aerosol vertical distributions at 477 nm are derived from the oxygen dimer (O4) differential-slant-column-density observations at different elevation angles by applying the BRemen Optimal estimation REtrieval for Aerosol and trace gaseS (BOREAS) retrieval algorithm. Four case studies have been selected for validation purposes; the retrieved aerosol profiles and the corresponding aerosol optical depths (AODs) from the MAX-DOAS are compared with lidar extinction profiles and with sun-photometric measurements (Aerosol Robotic Network, AERONET, observations), respectively. Despite the different approach of each method regarding the retrieval of the aerosol information, the comparison with the lidar measurements at 532 nm reveals a very good agreement in terms of vertical distribution, with r>0.90 in all cases. The AODs from the MAX-DOAS and the sun photometer (the latter at 500 nm) show a satisfactory correlation (with 0.45 < r < 0.7 in three out of the four cases). The comparison indicates that the MAX-DOAS systematically underestimates the AOD in the cases of large particles (small Ångström exponent) and for measurements at small relative azimuthal angles between the viewing direction and the sun. Better agreement is achieved in the morning, at large relative azimuthal angles. Overall, the aerosol profiles retrieved from MAX-DOAS measurements are of good quality; thus, new perspectives are opened up for assessing urban aerosol pollution on a long-term basis in Athens from continuous and uninterrupted MAX-DOAS measurements.

First TROPOMI Retrieval of Aerosol Effective Height Using O₄ Absorption Band at 477 nm and Aerosol Classification

We retrieved aerosol effective height (AEH) values from TROPOspheric monitoring instrument (TROPOMI) measurements based on the O₄ absorption at 477 nm. As the first step in the AEH retrieval algorithm, TROPOMI carbon monoxide and aerosol index products were used for the first time to determine aerosol type. An online radiative transfer calculation method was introduced to the AEH retrieval process. The AEHs were retrieved over northeast Asia (various aerosol types), South Africa (biomass-burning smoke), and the Sahara Desert (dust). The retrieved AEHs were compared with AEHs derived using aerosol extinction profiles from ground and satellite-based lidar measurements. A preliminary evaluation based on comparison with lidar suggests reasonable performance, but shows that cloud masking is the main source of uncertainty. The errors associated with the online-based AEH retrieval algorithm were calculated using synthetic radiance. The total AEH retrieval errors were 0.91 km (0.4 le AOD < 1) and 0.30 km (2 le AOD < 3), highlighting the increased sensitivity of the AEH retrieval algorithm under high AOD conditions. This study demonstrates that the O₄ absorption band at 477 nm is applicable to aerosol height retrieval from TROPOMI with a high spatial resolution.

Aerosol vertical distribution and interactions with land/sea breezes over the eastern coast of the Red Sea from lidar data and high-resolution WRF-Chem simulations

Abstract. With advances in modeling approaches and the application of satellite and ground-based data in dust-related research, our understanding of the dust cycle has significantly improved in recent decades. However, two aspects of the dust cycle, namely the vertical profiles and diurnal cycles, are not yet adequately understood, mainly due to the sparsity of direct observations. Measurements of backscattering caused by atmospheric aerosols have been ongoing since 2014 at the King Abdullah University of Science and Technology (KAUST) campus using a micro-pulse lidar (MPL) with a high temporal resolution. KAUST is located on the eastern coast of the Red Sea and currently hosts the only operating lidar system in the Arabian Peninsula. We use the data from the MPL together with other collocated observations and high-resolution simulations (with 1.33 km grid spacing) from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to study the following three aspects of dust over the Red Sea coastal plains. Firstly, we compare the model-simulated surface winds, aerosol optical depth (AOD), and aerosol size distributions with observations and evaluate the model performance in representing a typical large-scale dust event over the study site. Secondly, we investigate the vertical profiles of aerosol extinction and concentration in terms of their seasonal and diurnal variability. Thirdly, we explore the interactions between dust aerosols and land/sea breezes, which are the most influential components of the local diurnal circulation in the region. The WRF-Chem model successfully reproduced the diurnal profile of surface wind speed, AOD, and dust size distributions over the study area compared to observations. The model also captured the onset, demise, and height of a large-scale dust event that occurred in 2015, as compared to the lidar data. The vertical profiles of aerosol extinction in different seasons were largely consistent between the MPL data and WRF-Chem simulations along with key observations and reanalyses used in this study. We found a substantial variation in the vertical profile of aerosols in different seasons and between daytime and nighttime, as revealed by the MPL data. The MPL data also identified a prominent dust layer at ∼5–7 km during the nighttime, which likely represents the long-range transported dust brought to the site by the easterly flow from remote inland deserts. The sea breeze circulation was much deeper (∼2 km) than the land breeze circulation (∼1 km), but both breeze systems prominently affected the distribution of dust aerosols over the study site. We observed that sea breezes push the dust aerosols upwards along the western slope of the Sarawat Mountains. These sea breezes eventually collide with the dust-laden northeasterly trade winds coming from nearby inland deserts, thus causing elevated dust maxima at a height of ∼1.5 km above sea level over the mountains. Moreover, the sea and land breezes intensify dust emissions from the coastal region during the daytime and nighttime, respectively. Our study, although focused on a particular region, has broader environmental implications as it highlights how aerosols and dust emissions from the coastal plains can affect the Red Sea climate and marine habitats.

Aerosol optical properties of haze episodes in eastern China based on remote-sensing observations and WRF-Chem simulations

The ability for remote-sensing sensors and global/regional models to describe aerosol optical properties (AOPs) is critical to reducing the uncertainty in aerosol radiative forcing associated with climate change, and improving model prediction accuracy. In this study, remote-sensing observations and WRF-Chem simulations were used to evaluate AOPs over Eastern China during a severe winter haze event, in terms of aerosol optical depth (AOD), Ångström exponent (AE) and aerosol extinction profiles (AEP). This study also characterizes whether the inclusion of aerosol radiative feedbacks (ARFs) may improve the ability of WRF-Chem to acquire AOPs during haze episodes. Three simulation scenarios were considered: the non-radiation feedback (NRF), aerosol direct effect (ADE), as well as combined ADE and aerosol indirect effect (ADE + AIE). The results indicate that the satellite AOD products could represent the spatiotemporal distribution characteristics of the haze event. The AOD retrieved by the MODIS C6.1 DB algorithm was highly consistent with ground-based observations. A comparison between simulations and observations demonstrated that WRF-Chem, including the ADE or ADE + AIE scheme, may improve AOPs simulation in heavily polluted areas. The most significant improvements occurred in the Sichuan basin (SB) and North China Plain (NCP) (AOD = 50–70%; AE = 10–20%). In particular, the ADE + AIE scheme was the most obvious for AOD improvement, followed by AE. The AEP was also qualitatively analyzed through simulations and observations, and the result showed that the model overestimates aerosol extinction coefficients in NCP. However, the model is still able to represent the entire AEP contour over East China. Similar to AOD and AE, the model can also improve AEP simulation by adding ADE or ADE + AIE scheme, especially in SB. In summary, it is found that the ability of WRF-Chem to simulate the AOPs was significantly enhanced, particularly for regions loading with heavy aerosol during haze events in Eastern China.

Shipborne lidar measurements showing the progression of the tropical reservoir of volcanic aerosol after the June 1991 Pinatubo eruption

Abstract. A key limitation of volcanic forcing datasets for the Pinatubo period is the large uncertainty that remains with respect to the extent of the optical depth of the Pinatubo aerosol cloud in the first year after the eruption, the saturation of the SAGE-II instrument restricting it to only be able to measure the upper part of the aerosol cloud in the tropics. Here we report the recovery of stratospheric aerosol measurements from two shipborne lidars, both of which measured the tropical reservoir of volcanic aerosol produced by the June 1991 Mount Pinatubo eruption. The lidars were on board two Soviet vessels, each ship crossing the Atlantic, their measurement datasets providing unique observational transects of the Pinatubo cloud across the tropics from Europe to the Caribbean (∼ 40 to 8∘ N) from July to September 1991 (the Professor Zubov ship) and from Europe to south of the Equator (∼ 40∘ N to 8∘ S) between January and February 1992 (the Professor Vize ship). Our philosophy with the data recovery is to follow the same algorithms and parameters that appear in the two peer-reviewed articles that presented these datasets in the same issue of GRL in 1993, and here we provide all 48 lidar soundings made from the Professor Zubov and 11 of the 20 conducted from the Professor Vize, ensuring we have reproduced the aerosol backscatter and extinction values in the figures of those two papers. These original approaches used thermodynamic properties from the CIRA-86 standard atmosphere to derive the molecular backscattering, vertically and temporally constant values applied for the aerosol backscatter-to-extinction ratio, and the correction factor of the aerosol backscatter wavelength dependence. We demonstrate this initial validation of the recovered stratospheric aerosol extinction profiles, providing full details of each dataset in this paper's Supplement S1, the original profiles of backscatter ratio, and the calculated profiles of aerosol backscatter and extinction. We anticipate these datasets will provide potentially important new observational case studies for modelling analyses, including a 1-week series of consecutive soundings (in September 1991) at the same location showing the progression of the entrainment of part of the Pinatubo plume into the upper troposphere and the formation of an associated cirrus cloud. The Zubov lidar dataset illustrates how the tropically confined Pinatubo aerosol cloud transformed from a highly heterogeneous vertical structure in August 1991, maximum aerosol extinction values around 19 km for the lower layer and 23–24 for the upper layer, to a more homogeneous and deeper reservoir of volcanic aerosol in September 1991. We encourage modelling groups to consider new analyses of the Pinatubo cloud, comparing the recovered datasets, with the potential to increase our understanding of the evolution of the Pinatubo aerosol cloud and its effects. Data described in this work are available at https://doi.org/10.1594/PANGAEA.912770 (Antuña-Marrero et al., 2020).

Accurate retrieval of aerosol lidar ratio by Raman-Mie lidar in Nanjing

The observational experiments on atmospheric aerosols based on the Raman-Mie scattering lidar were introduced. To provide a reference for the selection of the lidar ratio in Fernald method, we analyzed the change of lidar ratios at different altitudes over Nanjing in December. Furthermore, the variation of aerosol extinction and backscattering profiles during the observational experiments was also analyzed. The study shows that the experimental results were mostly influenced by the dust aerosol particles.

Stratospheric aerosol extinction profiles from SCIAMACHY solar occultation

Abstract. The Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument on Envisat provided, between August 2002 and April 2012, measurements of solar and Earthshine spectra from the UV to the shortwave infrared spectral region in multiple viewing geometries. We present a new approach to derive stratospheric aerosol extinction profiles from SCIAMACHY solar occultation measurements based on an onion-peeling method similar to the onion-peeling differential optical absorption spectroscopy (DOAS) retrieval, which has already been successfully used for the derivation of greenhouse gas profiles. Since the retrieval of aerosol extinction requires as input measured transmissions in absolute units, an improved radiometric calibration of the SCIAMACHY solar occultation measurements has been developed, which considers various instrumental and atmospheric effects specific to solar occultation. The aerosol extinction retrieval can in principle be applied to all wavelengths measured by SCIAMACHY. As a first application, we show results for 452, 525 and 750 nm. The SCIAMACHY solar occultation time series has been processed, covering a latitudinal range of about 50–70∘ N. Reasonable aerosol extinctions are derived between about 15 and 30 km with typically larger uncertainties at higher altitudes due to decreasing aerosol extinction. Comparisons with collocated Stratospheric Aerosol and Gas Experiment II (SAGE-II) and SCIAMACHY limb aerosol data products revealed good agreement with essentially no mean bias. However, dependent on altitude, differences of up to ±20 %–30% to SAGE-II at 452 and 525 nm are observed. Similar results are obtained from comparisons with SAGE-III. SCIAMACHY solar occultation data at 750 nm have been compared with corresponding SAGE-III, Optical Spectrograph and InfraRed Imager System (OSIRIS) and SCIAMACHY limb results. The agreement with SCIAMACHY limb data at 750 nm is within 5 %–20 % between 17 and 27 km. SAGE-III and OSIRIS show at this wavelength and altitude range on average about 40 % and 25 % smaller values, with some additional 10 %–20 % modulation with altitude. The altitude variations in the differences are mainly caused by systematic vertical oscillations in the SCIAMACHY occultation data of up to 30 % below about 25 km. These oscillations decrease to amplitudes below 10 % with increasing number of collocations and are no longer visible in monthly anomalies. Major volcanic eruptions as well as occurrences of polar stratospheric clouds (PSCs) can be identified in the time series of aerosol extinction data and related anomalies. The influence of the quasi-biennial oscillation (QBO) is visible above 25 km.

Measuring the Vertical Profiles of Aerosol Extinction in the Lower Troposphere by MAX-DOAS at a Rural Site in the North China Plain

Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were performed during the summer (13 June–20 August) of 2014 at a rural site in North China Plain. The vertical profiles of aerosol extinction (AE) in the lower troposphere were retrieved to analyze the temporal variations of AE profiles, near-surface AE, and aerosol optical depth (AOD). The average AOD and near-surface AE over the period of study were 0.51 ± 0.26 and 0.33 ± 0.18 km−1 during the effective observation period, respectively. High AE events and elevated AE layers were identified based on the time series of hourly AE profiles, near-surface AEs and AODs. It is found that in addition to the planetary boundary layer height (PBLH) and relative humidity (RH), the variations in the wind field have large impacts on the near-surface AE, AOD, and AE profile. Among 16 wind sectors, higher AOD or AE occur mostly in the directions of the cities upstream. The diurnal variations of the AE profiles, AODs and near-surface AEs are significant and influenced mainly by the source emissions, PBLH, and RH. The AE profile shape from MAX-DOAS measurement is generally in agreement with that from light detection and ranging (lidar) observations, although the AE absolute levels are different. Overall, ground-based MAX-DOAS can serve as a supplement to measure the AE vertical profiles in the lower troposphere.

Comparison of V4 and V3 CALIOP (L3) aerosol products: A global perspective

Gridded satellite products provide (computationally less-intense) opportunities to compare and contrast parameters from different versions/sensors. In the present study, Level-3 (L3) Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol products from the most recent release (version 4, V4) are compared with its earlier version (version 3, V3) products. The various improvements in V4 are detailed and the resultant changes in aerosol optical depth (AOD) and aerosol vertical extinction profiles for various aerosol species (total aerosol, dust, polluted dust, smoke) over various regions are discussed. Broadly, V4 global AOD is higher than the V3 AOD (except for polluted dust). Significant differences in V4 and V3 AODs are observed over Africa, East Asia, Atlantic Ocean, Arabian Sea, Bay of Bengal and South America. Seasonal-wise global mean percentage difference in V4 and V3 total-AODs (with respect to V4 AODs) ranged between 9% and 15%. The change in the spatial distribution of polluted dust over oceanic regions is one of the significant differences between V4 and V3. V4 total-AODs are closer to Moderate Resolution Imaging Spectroradiometer (MODIS) AODs than V3 total-AODs are. The shape of the aerosol extinction profiles also differed between V4 and V3. The altitudinal differences in the V4 and V3 extinction values varied spatio-temporally.

A Method for Retrieving Stratospheric Aerosol Extinction and Particle Size from Ground-Based Rayleigh-Mie-Raman Lidar Observations

We report on the retrieval of stratospheric aerosol particle size and extinction coefficient profiles from multi-color backscatter measurements with the Rayleigh–Mie–Raman lidar operated at the Arctic Lidar Observatory for Middle Atmosphere Research (ALOMAR) in northern Norway. The retrievals are based on a two-step approach. In a first step, the median radius of an assumed monomodal log-normal particle size distribution with fixed width is retrieved based on a color index formed from the measured backscatter ratios at the wavelengths of 1064 nm and 532 nm. An intrinsic ambiguity of the retrieved aerosol size information is discussed. In a second step, this particle size information is used to convert the measured lidar backscatter ratio to aerosol extinction coefficients. The retrieval is currently based on monthly-averaged lidar measurements and the results for March 2013 are discussed. A sensitivity study is presented that allows for establishing an error budget for the aerosol retrievals. Assuming a monomodal log-normal aerosol particle size distribution with a geometric width of S = 1.5, median radii on the order of below 100 nm are retrieved. The median radii are found to generally decrease with increasing altitude. The retrieved aerosol extinction profiles are compared to observations with the OSIRIS (Optical Spectrograph and InfraRed Imager System) and the OMPS-LP (Ozone Mapping Profiling Suite Limb Profiler) satellite instruments in the 60∘ N to 80∘ N latitude band. The extinction profiles that were retrieved from the lidar measurements show good agreement with the observations of the two satellite instruments when taking the different wavelengths of the instruments into account.

Potential Approach for Single-Peak Extinction Fitting of Aerosol Profiles Based on In Situ Measurements for the Improvement of Surface PM2.5 Retrieval from Satellite AOD Product

The vertical distribution of aerosols is important for accurate surface PM2.5 retrieval and initial modeling forecasts of air pollution, but the observation of aerosol profiles on the regional scale is usually limited. Therefore, in this study, an approach to aerosol extinction profile fitting is proposed to improve surface PM2.5 retrieval from satellite observations. Owing to the high similarity of the single-peak extinction profile in the distribution pattern, the log-normal distribution is explored for the fitting model based on a decadal dataset (3248 in total) from Micro Pulse LiDAR (MPL) measurements. The logarithmic mean, standard deviation, and the height of peak extinction near-surface (Mode) are manually derived as the references for model construction. Considering the seasonal impacts on the planetary boundary layer height (PBLH), Mode, and the height of the surface layer, the extinction profile is then constructed in terms of the planetary boundary layer height (PBLH) and the total column aerosol optical depth (AOD). A comparison between fitted profiles and in situ measurements showed a high level of consistency in terms of the correlation coefficient (0.8973) and root-mean-square error (0.0415). The satellite AOD is subsequently applied for three-dimensional aerosol extinction, and the good agreement of the extinction coefficient with the PM2.5 within the surface layer indicates the good performance of the proposed fitting approach and the potential of satellite observations for providing accurate PM2.5 data on a regional scale.

Evaluation of the OMPS/LP stratospheric aerosol extinction product using SAGE III/ISS observations

Abstract. The Ozone Mapping and Profiler Suite Limb Profiler (OMPS/LP) has been taking limb-scattered measurements since April 2012. It is designed to produce ozone and aerosol vertical profiles at a 1.6 km vertical resolution over the entire sunlit globe. The Version 1.5 (V1.5) aerosol extinction retrieval algorithm provides aerosol extinction profiles using observed radiances at 675 nm. The algorithm assumes Mie theory and a gamma function aerosol size distribution for the stratospheric aerosol that is derived from results calculated by the Community Aerosol and Radiation Model for Atmospheres (CARMA). In this paper, we compare V1.5 LP aerosol profiles with SAGE III/ISS solar occultation observations for the period from June 2017 to May 2019, when both measurements were available to evaluate our ability to characterize background aerosol conditions. Overall, LP extinction profiles agree with SAGE III/ISS data to within ±25 % for altitudes between 19 and 27 km, even during periods perturbed by volcanic eruptions or intense forest fires. In this altitude range, the slope parameter of linear fitting of LP extinction values with respect to SAGE III/ISS measurements is close to 1.0, with Pearson correlation coefficients of r≥0.95, indicating that the LP aerosol data are reliable in that altitude range. Comparisons of extinction time series show that both instruments capture the variability of the stratospheric aerosol layer quite well, and the differences between the two instruments vary from 0 % to ±25 % depending on altitude, latitude, and time. In contrast, we find erroneous seasonal variations in the OMPS/LP Version 1.5 dataset, which usually exist below 20 km in the Southern Hemisphere due to the lack of sensitivity to particles when the scattering angle (SA) is greater than 145∘. We also find that LP-retrieved extinction is systematically higher than SAGE III/ISS observations at altitudes above 28 km and systematically lower below 19 km in the tropics with significant biases up to ±13 %. This is likely due in part to the fact that the actual aerosol size distribution is altitude dependent. There are also other reasons related to cloud contamination, wavelength limitations, aerosol loading, and the influence of the viewing configuration.

A multi-axis differential optical absorption spectroscopy aerosol profile retrieval algorithm for high-altitude measurements: application to measurements at Schneefernerhaus (UFS), Germany

Abstract. We present a new aerosol extinction profile retrieval algorithm for multi-axis differential optical absorption spectrometer (MAX-DOAS) measurements at high-altitude sites. The algorithm is based on the lookup table method. It is applied to retrieve aerosol extinction profiles from the long-term MAX-DOAS measurements (February 2012 to February 2016) at the Environmental Research Station Schneefernerhaus (UFS), Germany (47.417∘ N, 10.980∘ E), which is located near the summit of Zugspitze at an altitude of 2650 m. The lookup table consists of simulated O4 differential slant column densities (DSCDs) corresponding to numerous possible aerosol extinction profiles. The sensitivities of O4 absorption to several parameters were investigated for the design and parameterization of the lookup table. In the retrieval, simulated O4 DSCDs for each possible profile are derived by interpolating the lookup table to the observation geometries. The cost functions are calculated for each aerosol profile in the lookup table based on the simulated O4 DSCDs, the O4 DSCD observations, and the measurement uncertainties. Valid profiles are selected from all the possible profiles according to the cost function, and the optimal solution is defined as the weighted mean of all the valid profiles. A comprehensive error analysis is performed to better estimate the total uncertainty. Based on the assumption that the lookup table covers all possible profiles under clear-sky conditions, we determined a set of O4 DSCD scaling factors for different elevation angles and wavelengths. The profiles retrieved from synthetic measurement data can reproduce the synthetic profile. The results also show that the retrieval is insensitive to measurement noise, indicating the retrieval is robust and stable. The aerosol optical depths (AODs) retrieved from the long-term measurements were compared to coinciding and co-located sun photometer observations. High correlation coefficients (R) of 0.733 and 0.798 are found for measurements at 360 and 477 nm, respectively. However, especially in summer, the sun photometer AODs are systematically higher than the MAX-DOAS retrievals by a factor of ∼2. The discrepancy might be related to the limited measurement range of the MAX-DOAS and is probably also related to the decreased sensitivity of the MAX-DOAS measurements at higher altitudes. The MAX-DOAS measurements indicate the aerosol extinction decreases with increasing altitude during all seasons, which agrees with the co-located ceilometer measurements. Our results also show maximum AOD and maximum Ångström exponent in summer, which is consistent with observations at an AERONET station located ∼43 km from the UFS.

The Influence of Elevated Smoke Layers on Stratocumulus Clouds Over the SE Atlantic in the NASA Goddard Earth Observing System (GEOS) Model

AbstractPrevious evaluations of simulated aerosol transport over the south‐east Atlantic by global aerosol models, including the Goddard Earth Observing System (GEOS) atmospheric general circulation model, showed that the bulk of the modeled smoke aerosol layer resided ~1–2 km lower than Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) lidar observations. Using this finding as the motivation, this study examines the changes in model‐simulated cloud properties in response to redistributing the vertical placement of the aerosol over the ocean. Ten years (2006–2015) of CALIOP‐retrieved smoke aerosol extinction profiles were used to redistribute the model‐simulated aerosol mass on a monthly mean basis, keeping the column aerosol mass conserved. The results from the model sensitivity experiments show that elevating the aerosol layer to higher levels in agreement with CALIOP observations causes an increase in cloud fractions by ~33% for shallow marine boundary layers (MBL) and a decrease by ~30% for deeper MBL. For a shallow MBL, aerosol‐induced warming within the cloud layers for the lower altitude aerosol case decreases relative humidity at these levels and leads to a reduction of overall cloud amount compared to the elevated aerosol case. For a deeper MBL, however, aerosol heating within the upper cloud levels in the lower altitude aerosol case increases the underlying MBL stability, which suppresses the cloud vertical extent, enhances cloud cover, and delays the stratocumulus to cumulus transition. Finally, aerosol redistribution impacts on radiative forcing are investigated, which appear to be mainly driven by the changes in cloud area fractions rather than in‐cloud liquid water path changes between the model experiments.

Validation of MAX-DOAS retrievals of aerosol extinction, SO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;, and NO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; through comparison with lidar, sun photometer, active DOAS, and aircraft measurements in the Athabasca oil sands region

Abstract. Vertical profiles of aerosols, NO2, and SO2 were retrieved from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements at a field site in northern Alberta, Canada, during August and September 2013. The site is approximately 16 km north of two mining operations that are major sources of industrial pollution in the Athabasca oil sands region. Pollution conditions during the study ranged from atmospheric background conditions to heavily polluted with elevated plumes, according to the meteorology. This study aimed to evaluate the performance of the aerosol and trace gas retrievals through comparison with data from a suite of other instruments. Comparisons of aerosol optical depths (AODs) from MAX-DOAS aerosol retrievals, lidar vertical profiles of aerosol extinction, and the AERONET sun photometer indicate good performance by the MAX-DOAS retrievals. These comparisons and modelling of the lidar S ratio highlight the need for accurate knowledge of the temporal variation in the S ratio when comparing MAX-DOAS and lidar data. Comparisons of MAX-DOAS NO2 and SO2 retrievals to Pandora spectral sun photometer vertical column densities (VCDs) and active DOAS mixing ratios indicate good performance of the retrievals, except when vertical profiles of pollutants within the boundary layer varied rapidly, temporally, and spatially. Near-surface retrievals tended to overestimate active DOAS mixing ratios. The MAX-DOAS observed elevated pollution plumes not observed by the active DOAS, highlighting one of the instrument's main advantages. Aircraft measurements of SO2 were used to validate retrieved vertical profiles of SO2. Advantages of the MAX-DOAS instrument include increasing sensitivity towards the surface and the ability to simultaneously retrieve vertical profiles of aerosols and trace gases without requiring additional parameters, such as the S ratio. This complex dataset provided a rare opportunity to evaluate the performance of the MAX-DOAS retrievals under varying atmospheric conditions.