Optimization of Aeolus' aerosol optical properties by maximum-likelihood estimation

The European Space Agency (ESA) Earth Explorer Mission Aeolus was launched in August 2018, carrying the first Doppler wind lidar in space. Its primary payload, the Atmospheric LAser Doppler INstrument (ALADIN), is an ultraviolet (UV) high-spectral-resolution lidar (HSRL) measuring atmospheric backscatter from air molecules and particles in two separate channels. The primary mission product is globally distributed line-of-sight wind profile observations in the troposphere and lower stratosphere. Atmospheric optical properties are provided as a spin-off product. Being an HSRL, Aeolus is able to independently measure the particle extinction coefficients, co-polarized particle backscatter coefficients and the co-polarized lidar ratio (the cross-polarized return signal is not measured). This way, the retrieval is independent of a priori lidar ratio information. The optical properties are retrieved using the standard correct algorithm (SCA), which is an algebraic inversion scheme and therefore sensitive to measurement noise. In this work, we reformulate the SCA into a physically constrained maximum-likelihood estimation (MLE) problem and demonstrate a predominantly positive impact and considerable noise suppression capabilities. These improvements originate from the use of all available information by the MLE in conjunction with the expected physical bounds concerning positivity and the expected range of the lidar ratio. To consolidate and to illustrate the improvements, the new MLE algorithm is evaluated against the SCA on end-to-end simulations of two homogeneous scenes and for real Aeolus data collocated with measurements by a ground-based lidar and the Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite. The largest improvements were seen in the retrieval precision of the extinction coefficients and lidar ratio ranging up to 1 order of magnitude or more in some cases due to effective noise dampening. In real data cases, the increased precision of MLE with respect to the SCA is demonstrated by increased horizontal homogeneity and better agreement with the ground truth, though proper uncertainty estimation of MLE results is challenged by the constraints, and the accuracy of MLE and SCA retrievals can depend on calibration errors, which have not been considered.

First triple-wavelength lidar observations of depolarization and extinction-to-backscatter ratios of Saharan dust

Two layers of Saharan dust observed over Leipzig, Germany, in February and March 2021 were used to provide the first-ever lidar measurements of the dust lidar ratio (extinction-to-backscatter ratio) and linear depolarization ratio at all three classical lidar wavelengths (355, 532 and 1064 nm). The pure-dust conditions during the first event exhibit lidar ratios of 47 ± 8, 50 ± 5 and 69 ± 14 sr and particle linear depolarization ratios of 0.242 ± 0.024, 0.299 ± 0.018 and 0.206 ± 0.010 at wavelengths of 355, 532 and 1064 nm, respectively. The second, slightly polluted-dust case shows a similar spectral behavior of the lidar and depolarization ratio with values of the lidar ratio of 49 ± 4, 46 ± 5 and 57 ± 9 sr and the depolarization ratio of 0.174 ± 0.041, 0.298 ± 0.016 and 0.242 ± 0.007 at 355, 532 and 1064 nm, respectively. The results were compared with Aerosol Robotic Network (AERONET) version 3 (v3) inversion solutions and the Generalized Retrieval of Aerosol and Surface Properties (GRASP) at six and seven wavelengths. Both retrieval schemes make use of a spheroid shape model for mineral dust. The spectral slope of the lidar ratio from 532 to 1064 nm could be well reproduced by the AERONET and GRASP retrieval schemes. Higher lidar ratios in the UV were retrieved by AERONET and GRASP. The enhancement was probably caused by the influence of fine-mode pollution particles in the boundary layer which are included in the columnar photometer measurements. Significant differences between the measured and retrieved wavelength dependence of the particle linear depolarization ratio were found. The potential sources for these uncertainties are discussed.

Aeolus L2A aerosol optical properties product: standard correct algorithm and Mie correct algorithm

Aeolus carries the Atmospheric LAser Doppler INstrument (ALADIN), the first high-spectral-resolution lidar (HSRL) in space. Although ALADIN is optimized to measure winds, its two measurement channels can also be used to derive optical properties of atmospheric particles, including a direct retrieval of the lidar ratio. This paper presents the standard correct algorithm and the Mie correct algorithm, the two main algorithms of the optical properties product called the Level-2A product, as they are implemented in version 3.12 of the processor, corresponding to the data labelled Baseline 12. The theoretical basis is the same as in Flamant et al. (2008). Here, we also show the in-orbit performance of these algorithms. We also explain the adaptation of the calibration method, which is needed to cope with unforeseen variations of the instrument radiometric performance due to the in-orbit strain of the primary mirror under varying thermal conditions. Then we discuss the limitations of the algorithms and future improvements. We demonstrate that the L2A product provides valuable information about airborne particles; in particular, we demonstrate the capacity to retrieve a useful lidar ratio from Aeolus observations. This is illustrated using Saharan dust aerosol observed in June 2020.

Assessment of tropospheric CALIPSO Version 4.2 aerosol types over the ocean using independent CALIPSO-SODA lidar ratios

We assess the CALIPSO Version 4.2 (V4) aerosol typing and assigned lidar ratios over ocean using aerosol optical depth (AOD) retrievals from the Synergized Optical Depth of Aerosols (SODA) algorithm and retrieved columnar lidar ratio estimated by combining SODA AOD and CALIPSO attenuated backscatter (CALIPSO-SODA). Six aerosol types – clean marine, dusty marine, dust, polluted continental/smoke, polluted dust, and elevated smoke – are characterized using CALIPSO-SODA over ocean and the results are compared against the prescribed V4 lidar ratios, when only one aerosol type is present in the atmospheric column. For samples detected at 5-km or 20-km spatial resolutions and having AOD > 0.05, the CALIPSO-SODA lidar ratios are significantly different between different aerosol types, and are consistent with the type-specific values assigned in V4 to within 10 sr (except for polluted continental/smoke). This implies that the CALIPSO classification scheme generally categorizes aerosols correctly. We find remarkable daytime/nighttime regional agreement for clean marine aerosol over the open ocean (CALIPSO-SODA = 20–25 sr, V4 = 23 sr), elevated smoke over the southeast Atlantic (CALIPSO-SODA = 65–75 sr, V4 = 70 sr), and dust over the subtropical Atlantic adjacent to the African continent (CALIPSO-SODA = 40–50 sr, V4 = 44 sr). In contrast, daytime polluted continental/smoke lidar ratio is more than 20 sr smaller than the constant V4 vaue for that type, attributed in part to the challenge of classifying tenuous aerosol with low signal-to-noise ratio. Dust over most of the Atlantic Ocean features CALIPSO-SODA lidar ratios less than 40 sr, possibly suggesting the presence of dust mixed with marine aerosols or lidar ratio values that depend on source and evolution of the aerosol plume. The new dusty marine type introduced in V4 features similar magnitudes and spatial distribution as its clean marine counterpart with lidar ratio differences of less than 3 sr, and nearly identical values over the open ocean, implying that some modification of the classification scheme for the marine subtypes is warranted.

Measurement report: Comparison of airborne, in situ measured, lidar-based, and modeled aerosol optical properties in the central European background – identifying sources of deviations

A unique data set derived from remote sensing, airborne, and ground-based in situ measurements is presented. This measurement report highlights the known complexity of comparing multiple aerosol optical parameters examined with different approaches considering different states of humidification and atmospheric aerosol concentrations. Mie-theory-based modeled aerosol optical properties are compared with the respective results of airborne and ground-based in situ measurements and remote sensing (lidar and photometer) performed at the rural central European observatory at Melpitz, Germany. Calculated extinction-to-backscatter ratios (lidar ratios) were in the range of previously reported values. However, the lidar ratio is a function of the aerosol type and the relative humidity. The particle lidar ratio (LR) dependence on relative humidity was quantified and followed the trend found in previous studies. We present a fit function for the lidar wavelengths of 355, 532, and 1064 nm with an underlying equation of fLR(RH, γ(λ))=fLR(RH=0,λ)×(1-RH)-γ(λ), with the derived estimates of γ(355 nm) = 0.29 (±0.01), γ(532 nm) = 0.48 (±0.01), and γ(1064 nm) = 0.31 (±0.01) for central European aerosol. This parameterization might be used in the data analysis of elastic-backscatter lidar observations or lidar-ratio-based aerosol typing efforts. Our study shows that the used aerosol model could reproduce the in situ measurements of the aerosol particle light extinction coefficients (measured at dry conditions) within 13 %. Although the model reproduced the in situ measured aerosol particle light absorption coefficients within a reasonable range, we identified many sources for significant uncertainties in the simulations, such as the unknown aerosol mixing state, brown carbon (organic material) fraction, and the unknown aerosol mixing state wavelength-dependent refractive index. The modeled ambient-state aerosol particle light extinction and backscatter coefficients were smaller than the measured ones. However, depending on the prevailing aerosol conditions, an overlap of the uncertainty ranges of both approaches was achieved.

Biomass burning events measured by lidars in EARLINET – Part 2: Optical properties investigation

Biomass burning episodes measured at 14 stations of the European Aerosol Research Lidar Network (EARLINET) over 2008–2017 were analysed using the methodology described in "Biomass burning events measured by lidars in EARLINET – Part 1: Data analysis methodology" (Adam et al., 2020, this issue). The smoke layers were identified in lidar optical properties profiles. A number of 795 layers for which we measured at least one intensive parameter was analysed. These layers were geographically distributed as follows: 399 layers observed in South-East Europe, 119 layers observed in South-West Europe, 243 layers observed in North-East Europe, and 34 layers observed in Central Europe. The mean layer intensive parameters are discussed following two research directions: (I) the long-range transport of smoke particles from North America, and (II) the smoke properties (fresh versus aged), separating the smoke events into four continental source regions (European, North American, African, Asian or a mixture of two), based on back trajectory analysis. The smoke detected in Central Europe (Cabauw, Leipzig, and Hohenpeißenberg) was mostly transported from North America (87 % of fires). In North-East Europe (Belsk, Minsk, Warsaw) smoke advected mostly from Eastern Europe (Ukraine and Russia), but there was a significant contribution (31 %) from North America. In South-West Europe (Barcelona, Evora, Granada) smoke originated mainly from the Iberian Peninsula and North Africa (while 9 % were originating in North America). In the South-East Europe (Athens, Bucharest, Potenza, Sofia, Thessaloniki) the origin of the smoke was mostly local (only 3 % represented North America smoke). The following features, correlated with the increased smoke travel time (corresponding to aging) were found: the colour ratio of the lidar ratio (i.e., the ratio of the lidar ratio at 532 nm to the lidar ratio at 355 nm) and the colour ratio of the backscatter Ångström exponent (i.e., the ratio of the backscatter-related Angstrom exponent for the pair 532 nm – 1064 nm to the one for the pair 355 nm – 532 nm) increase, while the extinction Ångström exponent and the colour ratio of the particle depolarization ratio (i.e., the ratio of the particle linear depolarization ratio at 532 nm to the particle depolarization ratio at 355 nm) decrease. The smoke originating from all continental regions can be characterized on average as aged smoke, with a very few exceptions. In general, the long range transported smoke shows higher lidar ratio and lower depolarization ratio compared to the local smoke.

Retrieval of UVB aerosol extinction profiles from the ground-based Langley Mobile Ozone Lidar (LMOL) system

Aerosols emitted from wildfires are becoming one of the main sources of poor air quality in the US mainland. Their extinction in UVB (wavelength range 280–315 nm) is difficult to be retrieved using simple lidar techniques because of the impact of O3 absorption and lacking information of lidar ratio at those wavelengths. The 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) campaign in the New York City region allowed the characterization of lidar ratio for UVB aerosol retrieval. An algorithm for the aerosol extinction retrieval out of the Langley Mobile Ozone Lidar (LMOL) was used in conjunction with the NASA Langley High Altitude Lidar Observatory (HALO) 532 nm aerosol extinction product. This approach requires assuming 2 parameters, the lidar ratio at 292 nm and the Ångström Exponent (AE) between 532 nm and 292 nm. The objective of this work is to determine these two parameters and assess the retrieval error caused by improper assumption of lidar ratio. This work also accomplishes the first know 292 nm aerosol product inter-comparison between HALO and Tropospheric Ozone Lidar Network (TOLNet) ozone lidar. HALO results were compared with the aerosol data retrieved from the 292 nm band from LMOL with different approximations of the lidar ratio and the AE to determine optimal parameters. Using optimized parameters, the LMOL aerosol extinction can be retrieved with a 10 % accuracy up to 3 km. This work highlights the importance of the lidar ratio and AE in the retrieval and validation of 292 nm aerosol profiles obtained from UV-lidar. Errors arise from approaches that utilize a random priori lidar ratio and AE assumption. The lidar ratios at 292 nm determined in this work will also improve our understanding of the UVB optical properties of aerosol in the lower troposphere affected by transported wildfire emission.

A novel method of identifying and analysing oil smoke plumes based on synergic satellite data

Black carbon aerosols are the second largest contributor to global warming while also being linked to respiratory and cardiovascular disease. These particles are generally found in smoke plumes originating from biomass burning and fossil fuel combustion. They are also heavily concentrated in smoke plumes originating from oil fires exhibiting the largest ratio of black carbon to organic carbon. In this study, we identified and analyzed oil smoke plumes derived from 30 major industrial events within a 12-year timeframe. To our knowledge, this is the first study of its kind that utilized a synergetic approach based on satellite remote sensing techniques. One objective of this study is to highlight the importance of satellite remote sensing techniques in identifying these types of events. As opposed to ground stations, satellite data offers access to remote areas all over the globe which would otherwise be very difficult to reach. Satellite data offers access to these events which, as seen in this study, are mainly located in war prone or hazardous areas. This study focuses on the use of MODIS (Moderate Resolution Imaging Spectroradiometer) and CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) products regarding these types of aerosol while also highlighting their intrinsic limitations. By using data from both MODIS instruments onboard Terra and Aqua satellites we addressed the temporal evolution of the smoke plume while assessing Lidar specific properties and plume elevation using CALIPSO data. We present several aerosol properties in the form of plume specific averaged values. The MODIS ocean algorithms were successful in retrieving aerosol properties which, on average, ranged from −0.06 to 0.16 for plume specific AOD, −0.18 to 1.25 for Ångström exponent and 0.29 to 1.73 µm for the effective radius. CALIPSO measurements showed values of plume AOD ranging from 0 to 0.14 (532 nm) and 0 to 0.13 (1064 nm) except for one event where AOD values showed 1.52 (532 nm) and 1.42 (1064 nm). AE values ranged from 0.11 to 0.33 which were in agreeance with MODIS values. A large discrepancy can be found in one event where CALIPSO measured AOD values 5 times higher than MODIS. This event also produced the largest lidar ratio at 109 sr (532 nm) and 86 (1064 nm). Other lidar ratio values ranged from 37 to 55 sr however these unconstrained solutions were obtained for the entire layer of which the plumes were a part of and thus did not reflect specific plume conditions. Particulate backscatter values ranged from 0.002 to 0.0017 km−1 sr−1 while extinction coefficient values ranged from 0.10 to 1.65 km−1. On average backscatter and extinction coefficient values were 2 to 9 times higher than local background values. Particulate depolarization ratios ranged from 0.11 to 0.15 in 4 out of 6 cases while the remaining two ranged from 0.27 to 0.32 where dust was highly dominant. The values represented in this study are in good agreement with similar studies that used ground based and flight measurements. We believe that MODIS values are a conservative estimation of plume AOD since MODIS algorithms rely on general aerosol models and various atmospheric conditions within the look-up tables which do not reflect the highly absorbing nature of these smoke plumes. CALIPSO measurements are heavily dependent on lidar ratios which are not directly measured if plumes within the planetary boundary layer. We also believe that AOD values based on CALIPSO measurements are conservative in nature since heavy absorbing smoke would yield larger lidar ratios and AOD values. Based on this study we conclude that the MODIS land algorithms are not yet suited for retrieving aerosol properties for these types of smoke plumes due to the strong absorbing properties of these aerosols. We believe that these types of studies are a strong indicator for the need of improved aerosol models and retrieval algorithms.

Optical and Microphysical Properties of Aged Biomass Burning Aerosols and Mixtures, Based on 9-Year Multiwavelength Raman Lidar Observations in Athens, Greece

Mean optical and microphysical aerosol properties of long-range transported biomass burning (BB) particles and mixtures are presented from a 9-year (2011–2019) data set of multiwavelength Raman lidar data, obtained by the EOLE lidar over the city of Athens (37.58° N, 23.47° E), Greece. We studied 34 aerosol layers characterized as: (1) smoke; (2) smoke + continental polluted, and (3) smoke + mixed dust. We found, mainly, small-sized aerosols with mean backscatter-related (355 nm/532 nm, 532 nm/1064 nm) values and Ångström exponent (AE) values in the range 1.4–1.7. The lidar ratio (LR) value at 355 nm was found to be 57 ± 10 sr, 51 ± 5 sr, and 38 ± 9 sr for the aerosol categories (1), (2), and (3), respectively; while at 532 nm, we observed LR values of 73 ± 11 sr, 59 ± 10 sr, and 62 ± 12 for the same categories. Regarding the retrieved microphysical properties, the effective radius (reff) ranged from 0.24 ± 0.11 to 0.24 ± 0.14 μm for all aerosol categories, while the volume density (vd) ranged from 8.6 ± 3.2 to 20.7 ± 14.1 μm−3cm−3 with the higher values linked to aerosol categories (1) and (2); the real part of the refractive index (mR) ranged between 1.49 and 1.53, while for the imaginary part (mI), we found values within 0.0108 i and 0.0126 i. Finally, the single scattering albedo (SSA) of the propped particles varied from 0.915 to 0.936 at all three wavelengths (355–532–1064 nm). The novelty of this study is the provision of typical values of BB aerosol properties from the UV to the near IR, which can be used in forecasting the aerosol climatic effects in the European region.

Capabilities of an Automatic Lidar Ceilometer to Retrieve Aerosol Characteristics within the Planetary Boundary Layer

Continuous observation and quantitative retrieval of aerosol backscatter coefficients are important in the study of air quality and climate in metropolitan areas such as New York City. Ceilometers are ideal for this application, but aerosol backscatter coefficient retrievals from ceilometers are challenging and require proper calibration. In this study, we calibrate the ceilometer (Lufft CHM15k, 1064 nm) system constant with the molecular backscatter coefficient and evaluate the calibrated profiles with other independent methods, including the water-phase cloud method and comparison with the NASA Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) attenuated backscatter coefficient profile. Multiple-day calibration results show a stable system constant with a relative uncertainty of about 7%. We also evaluate the overlap correction for the CHM15k ceilometer (provided by Lufft) with a Vaisala CL-31 ceilometer, and the results show good consistency between two ceilometers’ range-corrected signal (RCS) profiles above 200 m. Next, we implement a forward iterative method to retrieve aerosol backscatter coefficients from continuous ceilometer measurements. In the retrieval, the lidar ratio is constrained by the co-located NASA AERONET radiometer aerosol optical depth (AOD) retrieval and agrees with the AERONET lidar-ratio products, derived from aerosol microphysical parameters. The aerosol backscatter coefficient retrievals are validated with co-located elastic-Raman lidar retrievals and indicate a good correlation (R2≥0.95) in the planetary boundary layer (PBL). Furthermore, a case study shows that the ceilometer retrieved aerosol extinction coefficient profiles can be used to estimate the AOD of the PBL and the aloft plumes. Finally, simulations of the uncertainty of aerosol backscatter coefficient retrieval show that a calibration error of 10% results in 10–20% of relative error in the aerosol backscatter coefficient retrievals, while relative error caused by a lidar-ratio error of 10% is less than 4% in the PBL.