Atmospheric aerosols are solid or liquid particles suspended in the air. The majority of them are produced by natural processes, including sea salt from oceans, mineral dust from (semi-)arid regions, carbon containing particles from wildfires, and sulfates and ash from volcanic activities. Anthropogenic aerosols are produced by industrial activities, power generation, transportation, agriculture, and human-induced biomass burning events. Depending on the meteorological conditions, aerosol particles can stay in the atmosphere for several hours to several months and can be transported over long distances, causing adverse effects on human health, visibility and climate. This thesis focuses on the aerosol optical properties, particularly the light absorption of the aerosol particles that has significant effects on the Earth’s climate system. This thesis starts with a general introduction of atmospheric aerosols, including its sources, categories, physical properties and measurement techniques (Chapter 1). Next, the Ultra-Violet Aerosol Index (UVAI) is introduced, which is calculated from satellite measurements of the radiance at two wavelengths in the UV. UVAI contains information of aerosol absorption, and it has a very long and almost continuous data record starting in 1978. Direct use of UVAI is challenging because it is not a geophysical quantity, but a numerical index. The objective of this thesis is to derive quantitative properties on aerosol absorption from the UVAI (e.g. single scattering albedo, absorption aerosol optical depth) that can be directly used in aerosol radiative transfer assessments. Two types of methods have been developed, i.e. physically-based methods and statistically-based methods. The first compares the observed UVAI to the one simulated by radiative transfer models. The second uses Machine Learning algorithms trained by existing data sets. The physically-based methods have been applied to quantify aerosol absorption of several large scale wildfires (Chapter 2 and 3). An important challenge of these method is that assumptions have to be made on the aerosol micro-physical properties, leading to significant uncertainties in the results, whereas theMachine Learning-based methods can avoid this kind of assumptions. Chapter 3 investigates the feasibility to quantify aerosol absorption from UVAI using a Machine Learning algorithm. Despite the higher computational efficiency and better results, the application of such data-driven methods is still restricted by the limited data on the aerosol vertical distribution. Therefore, in Chapter 4, a database of aerosol height is created from a chemistry transport model. This database is applied in Chapter 5, where a Deep Neural Network method is used to derive the quantitative aerosol absorptive properties from the OMI/Aura UVAI for the period from 2006 to 2019. In comparison to ground-based observations, the results of the Deep Neural Network agree better than satellite retrievals and also better than chemistry transport model simulations. This thesis demonstrates the feasibility of deriving quantitative aerosol absorptive properties from the satellite retrieved UVAI.We use traditional radiative transfer simulations meanwhile investigating the new possibilities of data-driven methods in aerosol remote sensing. Although the retrieval results are encouraging, there remain limitations and challenges which need to be addressed. These are discussed in Chapter 6 with corresponding suggestions and prospects. Despite the challenges, it is expected that a synthetic database of global aerosol absorption can be derived fromUVAI observations provided by multiple satellite products. Such a data set will make great contributions to quantify the effect of absorbing aerosols on the climate system.@en

Quantitative measurements of aerosol absorptive properties, e.g., the absorbing aerosol optical depth (AAOD) and the single scattering albedo (SSA), are important to reduce uncertainties of aerosol climate radiative forcing assessments. Currently, global retrievals of AAOD and SSA are mainly provided by the ground-based aerosol robotic network (AERONET), whereas it is still challenging to retrieve them from space. However, we found the AERONET AAOD has a relatively strong correlation with the satellite retrieved ultra-violet aerosol index (UVAI). Based on this, a numerical relation is built by a deep neural network (DNN) to predict global AAOD and SSA over land from the long-term UVAI record (2006-2019) provided by the ozone monitoring instrument (OMI) onboard Aura. The DNN predicted aerosol absorption is satisfying for samples with AOD at 550 nm larger than 0.1, and the DNN model performance is better for smaller absorbing aerosols (e.g., smoke) than larger ones (e.g., mineral dust). The comparison of the DNN predictions with AERONET shows a high correlation coefficient of 0.90 and a root mean square of 0.005 for the AAOD, and over 80% of samples are within the expected uncertainty of AERONET SSA (pm0.03).

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The TROPOspheric Monitoring Instrument (TROPOMI) level-2 aerosol layer height (ALH) product has now been released to the general public. This product is retrieved using TROPOMI's measurements of the oxygen A-band, radiative transfer model (RTM) calculations augmented by neural networks and an iterative optimal estimation technique. The TROPOMI ALH product will deliver ALH estimates over cloud-free scenes over the ocean and land that contain aerosols above a certain threshold of the measured UV aerosol index (UVAI) in the ultraviolet region. This paper provides background for the ALH product and explores its quality by comparing ALH estimates to similar quantities derived from spaceborne lidars observing the same scene. The spaceborne lidar chosen for this study is the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission, which flies in formation with NASA's A-train constellation since 2006 and is a proven source of data for studying ALHs. The influence of the surface and clouds is discussed, and the aspects of the TROPOMI ALH algorithm that will require future development efforts are highlighted. A case-by-case analysis of the data from the four selected cases (mostly around the Saharan region with approximately 800 co-located TROPOMI pixels and CALIOP profiles in June and December 2018) shows that ALHs retrieved from TROPOMI using the operational Sentinel-5 Precursor Level-2 ALH algorithm is lower than CALIOP aerosol extinction heights by approximately 0.5km. Looking at data beyond these cases, it is clear that there is a significant difference when it comes to retrievals over land, where these differences can easily go over 1km on average.

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The purpose of this study is to demonstrate the role of aerosol layer height (ALH) in quantifying the single scattering albedo (SSA) from ultraviolet satellite observations for biomass burning aerosols. In the first experiment, we retrieve SSA by minimizing the near-ultraviolet (near-UV) absorbing aerosol index (UVAI) difference between observed values and those simulated by a radiative transfer model. With the recently released S-5P TROPOMI ALH product constraining forward simulations, a significant gap in the retrieved SSA (0.25) is found between radiative transfer simulations with spectral flat aerosols and those with strong spectrally dependent aerosols, implying that inappropriate assumptions regarding aerosol absorption spectral dependence may cause severe misinterpretations of the aerosol absorption. In the second part of this paper, we propose an alternative method to retrieve SSA based on a long-term record of co-located satellite and ground-based measurements using the support vector regression (SVR) approach. This empirical method is free from the uncertainties due to the imperfection of a priori assumptions on aerosol microphysics seen in the first experiment. We present the potential capabilities of SVR using several fire events that have occurred in recent years. For all cases, the difference between SVR-retrieved SSA and AERONET are generally within ±0:05, and over half of the samples are within ±0:03. The results are encouraging, although in the current phase the model tends to overestimate the SSA for relatively absorbing cases and fails to predict SSA for some extreme situations. The spatial contrast in SSA retrieved by radiative transfer simulations is significantly higher than that retrieved by SVR, and the latter better agrees with SSA from MERRA-2 reanalysis. In the future, more sophisticated feature selection procedures and kernel functions should be taken into consideration to improve the SVR model accuracy. Moreover, the high-resolution TROPOMI UVAI and co-located ALH products will guide us to more reliable training data sets and more powerful algorithms to quantify aerosol absorption from UVAI records.

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The absorbing aerosol index (AAI) is a qualitative parameter directly calculated from satellite-measured reflectance. Its sensitivity to absorbing aerosols in combination with a long-term data record since 1978 makes it an important parameter for climate research. In this study, we attempt to quantify aerosol absorption by retrieving the single-scattering albedo (ω0) at 550 nm from the satellite-measured AAI. In the first part of this study, AAI sensitivity studies are presented exclusively for biomass-burning aerosols. Later on, we employ a radiative transfer model (DISAMAR) to simulate the AAI measured by the Ozone Monitoring Instrument (OMI) in order to derive ω0 at 550 nm. Inputs for the radiative transfer calculations include satellite measurement geometry and surface conditions from OMI, aerosol optical thickness (τ) from the Moderate Resolution Imaging Spectroradiometer (MODIS) and aerosol microphysical parameters from the AErosol RObotic NETwork (AERONET), respectively. This approach is applied to the Chile wildfires for the period from 26 to 30 January 2017, when the OMI-observed AAI of this event reached its peak. The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) overpasses missed the evolution of the smoke plume over the research region; therefore the aerosol profile is parameterized. The simulated plume is at an altitude of 4.5-4.9 km, which is in good agreement with available CALIOP backscatter coefficient measurements. The data may contain pixels outside the plume, so an outlier detection criterion is applied. The results show that the AAI simulated by DISAMAR is consistent with satellite observations. The correlation coefficients fall into the range between 0.85 and 0.95. The retrieved mean ω0 at 550 nm for the entire plume over the research period from 26 to 30 January 2017 varies from 0.81 to 0.87, whereas the nearest AERONET station reported ω0 between 0.89 and 0.92. The difference in geolocation between the AERONET site and the plume, the assumption of homogeneous plume properties, the lack of the aerosol profile information and the uncertainties in the inputs for radiative transfer calculation are primarily responsible for this discrepancy in ω0.@en