Theses and Dissertations from UMD
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Item INVESTIGATION OF AMBIENT METHANE CONCENTRATION, SOURCES, AND TRENDS IN THE BALTIMORE-WASHINGTON REGION(2024) Sahu, Sayantan; Dickerson, Russell Professor; Chemistry; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Methane, an important and not yet fully understood greenhouse gas, has a global warming potential 25 times that of carbon dioxide over 100 years, although with an atmospheric lifetime much shorter than carbon dioxide. Controlling methane emissions is a useful way to avoid some of the adverse effects of climate change at least on short time scales. Natural sources include wetlands, ruminants, and wildfires, while anthropogenic sources include the production, transmission, distribution, and use of natural gas, livestock, and landfills. In the US, natural gas and petroleum systems, anthropogenic sources, are the second-largest source of methane emissions. Urban areas are a significant source of anthropogenic methane emissions, primarily fugitive emissions from natural gas distribution and usage.We studied methane observations from five towers in the Baltimore-Washington (BWR) region – two urban towers ARL (Arlington, VA), NEB (Northeast Baltimore, MD), and one rural tower, BUC (Bucktown, MD). Methane measurements from these three towers displayed distinct seasonal and diurnal cycles with maxima at night and in the early morning, which indicated significant local emissions. We concluded from our analysis that anthropogenic methane emissions dominate at the urban sites whereas wetland emissions dominate at the rural site. We compared observed enhancements (mole fractions above the 5th percentile) to simulated methane enhancements using the WRF-STILT model driven by two EDGAR inventories – EDGAR 4.2 and EDGAR 5.0. We did a similar comparison between model and observations with vertical gradients. We concluded that both versions of EDGAR underestimated the regional anthropogenic emissions of methane, but version 5.0 had a more accurate spatial representation. We ran the model with WETCHARTs to account for wetland emissions which significantly reduced the bias between model and observations especially in summer at the rural site. We investigated winter methane observations from three towers in the BWR including a ten-year record, 2013-2022, from BUC, located ~100 km southeast of these urban areas. We combined the observations with a HYSPLIT clustering analysis for all years to determine the major synoptic patterns influencing methane mixing ratios at BUC. For methane concentrations above global background, the cluster analysis revealed four characteristic pathways of transport into BUC – from the west (W), southwest (SW), northwest (NW), and east (E) and these showed significant differences in methane mixing ratios. We corroborated our conclusions from BUC using 2018-2022 data from towers in Stafford, Virginia (SFD), and Thurmont, Maryland (TMD); results confirmed the influence of synoptic pattern, typically associated with frontal passage, on methane. No significant temporal trend over the global background was detected overall or within any cluster. For BUC, low concentrations were observed for air off the North Atlantic Ocean (E cluster) and flowing rapidly behind cold fronts (NW cluster). High methane mixing ratios were observed, as expected, in the W cluster due to the proximity of the BWR and oil and gas operations in the Marcellus. Less expected were high mixing ratios for the SW cluster – we attribute these to agricultural sources in North Carolina. Swine production, ~500 km to the SW, impacts methane in eastern Maryland as much or more than local urban emissions plus oil and gas operations 100–300 km to the west; this supports the high end of emission estimates for animal husbandry and suggests strategies for future research and mitigation.Item ATMOSPHERIC ORGANIC AEROSOLS: THE EFFECT OF PHYSIOCHEMICAL PROPERTIES ON HYGROSCOPICITY(2023) Malek, Kotiba; Asa-Awuku, Akua; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Aerosols, tiny solid or liquid particles, are ubiquitous in the atmosphere yet their impact on climate remains poorly understood. One prominent way aerosols are able to impact the climate is through their ability to uptake water and form clouds. The chemical diversity and aerosol interactions in the atmosphere can greatly complicate the investigation of aerosol-cloud interactions. This complexity is expressed with a large uncertainty associated with aerosols’ role on climate change. This dissertation investigates the aerosol-cloud interaction by measuring the water uptake of atmospherically relevant aerosols. Our results highlight the importance of accounting for various physiochemical properties when exploring the water uptake of atmospheric aerosols. One such property is liquid-liquid phase separation (LLPS) in ternary mixtures. Our work offers new evidence, insight, and a paradigm shift to the contribution of LLPS to supersaturated droplet activation. We complemented this finding with a theoretical model, that incorporates solubility, O:C ratio, and LLPS, for predicting κ-hygroscopicity of ternary mixtures. Another physiochemical property that was shown to play a key role in droplet activation of polymeric aerosols is chemical structure. Our study shows that polycatechol is more hygroscopic than polyguaiacol and the difference in hygroscopicity is attributed to the density of hydroxyl groups in both structures. Polycatechol has a higher density of hydroxyl groups than polyguaiacol, resulting in polycatechol having stronger water uptake affinity than polyguaiacol. When maintaining the same structural makeup by investigating the water uptake of two isomeric compounds, we discovered that solubility was the driving force in water uptake. The more soluble isomer o-aminophenol was more hygroscopic than p-aminophenol. Hence, a small change in the position of functional groups can impact solubility which in turn influence hygroscopicity. Lastly, we explored the presence of gas-phase organics on the water uptake of isomers with a wide range of solubilities. Our work highlights that gas-phase organics, specifically ethanol, can influence the water uptake of aerosols. Ethanol was shown to increase water uptake efficiencies based on solubility, with the least soluble compound showing stronger affinity to water uptake. Overall, this thesis advances our knowledge and understanding of aerosol-cloud interactions and its implications on climate change.Item REMOTE SENSING OF ATMOSPHERIC TRACE GASES FROM SPACEBORNE UV MEASUREMENTS(2022) Huang, Xinzhou; Yang, Kai; Dickerson, Russell R.; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Satellite measurements of atmospheric trace gases provide continuous long-term information for monitoring the atmospheric chemical environment and air quality at local, regional, and global scales. Trace gas retrievals play a critical role in chemical data assimilation, air quality modeling and forecast, and regulatory decision-making. In this dissertation, I present retrievals of three trace gases species (O3, SO2, and NO2) from measurements of Ultraviolet (UV) radiation made from the imaging spectrometers onboard operational satellites, including the Earth Polychromatic Imaging Camera (EPIC) onboard the Deep Space Climate Observatory (DSCOVR), the Ozone Mapping and Profiler Suite - Nadir Mapper (OMPS-NM) onboard Suomi-NPP (SNPP), and the OMPS-NM onboard NOAA-20 satellite. The retrievals of the trace gas vertical columns are achieved through the Direct Vertical Column Fitting (DVCF) algorithm, which is designed to maximize the absorption signature from the Earth’s atmosphere in the UV spectral range. This dissertation first demonstrates the theoretical basis and mathematical procedures of the DVCF algorithm used for retrieving total vertical columns of ozone (O3) and sulfur dioxide (SO2) from DSCOVR EPIC. We describe algorithm advances, including an improved O3 profile representation that enables profile adjustments from multiple spectral measurements and the spatial optimal estimation (SOE) scheme that reduces O3 artifacts resulted from EPIC’s band-to-band misregistrations. Furthermore, we present detailed error analyses to quantify retrieval uncertainties from various sources, assess EPIC-observed volcanic plumes, and validate O3 and SO2 retrievals with correlative data. The second part of this dissertation presents a suite of efforts to retrieve the tropospheric and stratospheric NO2 vertical columns from the new NOAA-20 OMPS hyperspectral Ultraviolet-Visible (UV-Vis) instrument, covering retrieval algorithm, Stratosphere-Troposphere Separation (STS) scheme, measurement sensitivity assessment, inter-comparison with the Ozone Monitoring Instrument (OMI), evaluation with ground-based Pandora spectrometers, as well as a case study of drastic NO2 changes during COVID-19 pandemic. The third part of my dissertation focuses on validation and algorithm improvements for the tropospheric NO2 retrievals from SNPP OMPS UV measurements. OMPS column NO2 was validated against coincidence measurements from two ground-based MAX-DOAS spectrometers deployed in eastern China. To achieve higher retrieval accuracy, we developed and implemented a series of algorithm improvements, including an explicit aerosol correction scheme to account for changes in measurement sensitivity caused by aerosol scattering and absorption, the replacement of climatological a priori NO2 profile with more accurate NO2 vertical distribution from high-resolution CMAQ model simulations, and the application of model-derived spatial weighting kernel to account for the effect of heterogeneous subpixel distribution. These improvements yield more accurate OMPS NO2 retrievals in better agreement with MAX-DOAS NO2 measurements. The analysis concluded that explicit aerosol correction and a priori profile adjustment are critical for improving satellite NO2 observations in highly polluted regions and spatial downscaling is helpful in resolving NO2 subpixel variations.Item THE HYGROSCOPICITY OF PLASTIC AEROSOLS(2023) Mao, Chun-Ning; Asa-Awuku, Akua; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Polymeric nanoparticles affect many aspects of human life. They directly absorb or scatter sunlight, or indirectly act as cloud condensation nuclei (CCN) to change the Earth’s climate. Additionally, micro-plastics released into the environment have the potential to degrade into nano-size particles. Plastic nanoparticles' sizes, number concentration, and hygroscopicity are important properties to understanding nano-plastics’ fates. In this work, I explored aerosol measurement techniques, aerosol hygroscopicity, and polymer nanoparticles to understand subsequent effects in the environment and on human health. The project was divided into three objectives:For the first objective, I developed the single-parameter hygroscopicity model for polymeric aerosols with Flory-Huggins Köhler theory. Traditional hygroscopicity, derived from Raoult’s law, depends on the molecular volume of the solute. For polymers with a high molecular volume, the predicted hygroscopicity from traditional Köhler theory is zero. However, the experimental results showed that polymers could take up water and readily act as CCN. I developed the expression of the hygroscopicity for polymers and showed the relation between the polymer-water interaction parameter and the water-uptake ability. I also considered water-insoluble polymers and the water-adsorption model combined with Köhler theory to define water-uptake. Thus the CCN activity of polystyrene and surface modified polystyrene particles were also measured. For the second objective, I predicted the fraction of the multiply charged particles, showing that the extinction cross section measured by Cavity Ring Down Spectroscopy (CRD) was influenced by a small amount of multiply charged particles using a Differential Mobility Analyzer (DMA). The initial results indicated that ~4% to ~6% of the total number concentration are triply and quadruply charged particles at 200 nm electrical mobility. This small percentage if neglected could induce errors greater than 5% in subsequent extinction cross section measurements. Thus, the errors induced with commercially available DMAs in the extinction cross section measurement were evaluated. For the third objective, I studied the fate of the nano-plastics in the environment. Results showed that low density polyethylene (LDPE) powders generated particles less than 100 nm at temperatures above 40 oC. I quantified the number concentration of 5 materials in water via traditional atmospheric aerosol measurement techniques. The five materials are cellulose, SiO2, LDPE, polyethylene terephthalate (PET), and polyvinyl chloride (PVC). They were all common materials used for food packaging. Furthermore, the hygroscopicities of the nano-plastics were measured. I demonstrated that the nano-plastics could act as CCN under a supersaturated environment and hence affect the climate. The results showed that the plastic materials (LDPE, PVC, PET) were more hygroscopic than cellulose. The nano-plastics could travel further and be found in remote and cold areas like Antarctica, the Arctic, and high mountains. The work in this objective provided evidence of wet deposition being a possible route for nano-plastics to come to the ground. Plastics are relatively new materials compared to papers, clays, and glasses, but have already been massively produced. The work in this thesis contributed to our understanding of the impact on nano-plastics to the environment. The interaction of the water and nano-plastics in the environment was studied. The measurements of size distribution and hygroscopicity of nano-plastics can be applied in the climate model to reduce the uncertainties in the indirect effect of the aerosols in future studies.Item AEROSOL-CLOUD-CLIMATE INTERACTIONS DUE TO CARBONACEOUS AEROSOLS(2022) Gohil, Kanishk; Asa-Awuku, Akua A; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Aerosols can affect the net radiation budget and global climate of the Earth either “directly” – through their radiative properties, or “indirectly” – through their cloud-forming abilities by acting as Cloud Condensation Nuclei (CCN). The interactions between aerosols and clouds are the most significant sources of uncertainty in the overall radiative forcing from due to a lack of understanding related to the droplet formation mechanism of aerosols. These uncertainties are majorly associated with the carbonaceous aerosols present in the atmosphere, notably due to their compositional diversity, vastly variable physicochemical properties, and unique water uptake characteristics. In this dissertation, new lab-based measurement techniques and computational methods have been developed to resolve the CCN activity and water uptake behavior of pure and mixed carbonaceous aerosol particles.The first part of this dissertation accomplishes two goals: 1. The development and application of a new CCN measurement method, and 2. The formulation of a new computational framework for CCN activity analysis of aerosols. The results in this dissertation demonstrate the significance of size-resolved morphology and dissolution properties of aerosol particles in improving their CCN activity analysis under varying ambient conditions. Furthermore, these results suggest that in the future, more comprehensive CCN analysis frameworks can be developed by explicitly treating other physical and chemical properties of the aerosols to further improve their CCN activity analysis. The second part of this dissertation focuses on large-scale analysis. The CCN analysis framework is implemented into a climate model to quantify the water uptake behavior of carbonaceous aerosols, and then study the subsequent variabilities associated with the physical and radiative properties of ambient aerosols and clouds. Statistical techniques are also developed in this work for chemical characterization of ambient aerosols. The characterization results show large regional compositional variations in ambient aerosol populations. These results also suggest that the knowledge of chemical species is necessary to quantify the water uptake properties of the aerosol population.Item Simulation and Projection of Global Temperature Change and Recovery of Extra-polar Ozone using Multiple Linear Regression Models(2022) McBride, Laura Anne; Salawitch, Ross J.; Chemistry; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Climate change and the depletion of the ozone layer are two important global environmental problems caused by the release of gases into the atmosphere. This dissertation uses multiple linear regression to quantify the natural and human components that affect Earth’s global mean surface temperature (GMST) and the thickness of the ozone layer. To analyze changes in Earth’s climate, the Empirical Model of Global Climate (EM-GC) is used to simulate and project variations in GMST. Numerous scenarios of greenhouse gas and aerosol emissions are considered to analyze the probability of achieving the 1.5 and 2.0°C warming goals set by the Paris Agreement. There is a 53% likelihood of the rise in GMST staying below 1.5°C if the world follows the greenhouse gas and aerosol emissions in SSP1-2.6, and a 64% probability of staying below 2.0°C if the world follows SSP4-3.4. The amount of warming attributed to humans from 1975 to 2014 based on the EM-GC is 0.157°C decade−1 (range of 0.120 to 0.195°C decade−1). Multi-model output from the Coupled Model Intercomparison Project Phase 6 (CMIP6) indicates humans contributed 0.221°C decade−1 (0.151 to 0.299°C decade−1) of warming from 1975 to 2014, which is notably faster warming than inferred from the historical climate record. The rise in GMST at 2×preindustrial concentrations of carbon dioxide is also examined. The effects of increasing methane emissions are discussed, as well as the timeline for emitting the remainder of the world’s carbon budget. Humans can emit another 150 ± 79 Gt C after 2019 to have a 66% likelihood of limiting warming to 1.5°C and another 400 ± 104 Gt C to have the same probability of limiting warming to 2.0°C. Given the estimated emission of 11.7 Gt C per year for 2019 due to human activities, carbon and methane emissions must be severely curtailed in the next 10 years to achieve the 1.5°C goal of the Paris Agreement. The results from the EM-GC are compared to other reduced complexity climate models (RCMs) as part of an international collaboration, as well as multi-model output from CMIP6. All RCMs, including the EM-GC, show that the CMIP6 global climate models warm too quickly. To analyze changes in the ozone layer due to human activities, a multiple linear regression model is used that includes equivalent effective stratospheric chlorine (EESC) as a measure of the human effect on ozone. Results using the updated EESC calculation indicate anthropogenic, very short-lived chlorine (VSL Cl) species not regulated by the Montreal Protocol have already caused a seven-year delay in the recovery of the ozone layer. Future simulations indicate that if human emissions of VSL Cl species continue to rise, the recovery of the ozone layer could be delayed up to 25 years.Item MEASUREMENTS OF AEROSOL PHYSICOCHEMICAL PROPERTIES(2022) Razafindrambinina, Patricia Nirina; Asa-Awuku, Akua A; Chemistry; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Tiny liquid or solid particles suspended in the air with sizes ranging between several nanometers to several microns, collectively referred to as aerosol particles, are ubiquitous in the atmosphere and have been shown to affect a planet’s radiative budget. Aerosol particles have the ability to directly reflect and absorb solar radiation leading to a cooling or heating the planet’s surface, respectively (aerosol direct effect). Aerosol particles can also indirectly affect the net radiative forcing through water uptake and cloud formation prior to reflecting and absorbing solar radiation (aerosol indirect effect). In my dissertation, I utilize lab-based measurements to measure the optical properties of mineral dust and Martian dust simulants, and quantify the water uptake and cloud condensation nuclei activity of secondary organic aerosols (SOA), and water-soluble organic compounds in various mixing states and relative humidities. This body of work provides directly-measured values that may reduce uncertainties in climate prediction when used as inputs in future climate and air quality models.Item APPLICATIONS OF THE OZONE MONITORING INSTRUMENT IN OBSERVING VOLCANIC SULFUR DIOXIDE PLUMES AND SULFATE DEPOSITION(2021) Fedkin, Niko Markovich; Dickerson, Russell R; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Sulfur dioxide (SO2), a gas emitted by both volcanoes and anthropogenic activity, is a major pollutant and a precursor to sulfate aerosols. Sulfates can be deposited back to the ground where they have adverse impact on the environment or reside in the stratosphere as aerosols and affect radiative forcing. I investigated two components that stem from SO2: the deposition of sulfate, and the remote sensing of the SO2 layer height, important for aviation safety and chemical modeling. In the first study, I used column SO2 data from the Ozone Monitoring Instrument (OMI), and sulfate wet deposition data from the National Atmospheric Deposition Program to investigate the temporal and spatial relationship between trends in SO2 emissions and the downward sulfate wet deposition over the northeastern U.S. from 2005 to 2015. The results showed that emission reductions are reflected in deposition reductions within this same region. Emission reductions along the Ohio River Valley led to decreases in sulfate deposition not only in eastern OH and western PA, but also further downwind at sites in Delaware and Maryland. The findings suggested that emissions and wet deposition are linked through not only the location of sources relative to the observing sites, but also photochemistry and weather patterns characteristic to the region in winter and summer. The second part of this dissertation focuses on SO2 layer height retrievals and their applications. To this end I applied the Full Physics Inverse Learning Machine (FP-ILM) algorithm to OMI radiances in the spectral range of 310-330 nm. This approach utilized radiative transfer calculations to generate a large dataset of synthetic radiance spectra for a wide range of geophysical parameters. The spectral information was then used to train a neural network to predict the SO2 height. The main advantage of the algorithm is its speed, retrieving plume height in less than 10 min for an entire OMI orbit. I also compared the SO2 height retrievals to other data sources and explored some potential applications, in particular their use in volcanic SO2 plume forecasts and estimating the total mass emitted from volcanic eruptions.Item EXAMINATION OF TROPOSPHERIC OZONE AND ITS PRECURSORS WITHIN AN AIR QUALITY MODEL AND IMPLICATIONS FOR AIR QUALITY AND CLIMATE(2021) Hembeck, Linda; Salawitch, Ross J; Canty, Timothy P; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Elevated levels of tropospheric ozone (O3) caused by emissions of NOx and VOCs negatively impact human health, crops, and ecosystems. Even if precursor emissions are reduced below current levels, predicted higher temperatures due to increased greenhouse gas emissions could impede resulting air quality benefits. Air quality models simulate the complex relationships that form O3 and are used to guide policy decisions directed at improving O3. The body of this work encompasses three projects related to improvements in the representation of O3 and precursors in air quality models. First, I examine the role of O3 and its precursors in air quality and climate change by evaluating ozone production efficiency (OPE) and O3 precursors within models. I modified a chemical mechanism and the emissions of NOx to accurately represent NOx, the reactivity of NOx with peroxy radicals, HCHO, isoprene, as well as organic and inorganic NOy reservoir species. Implementation of these modifications increased confidence in model simulations. Results indicate accepted inventories overestimated NOx emissions but underestimate total VOC reactivity and OPE. Second, I examined the dependence of surface O3 on temperature (climate penalty factor (CPF)) throughout a period of 11 years within an air quality model and measurements. Future increases in temperature could offset benefits from future reductions in the emission of O3 precursors. Determining and understanding the CPF is critical to formulating effective strategies to reduce future exceedances. I have demonstrated that the model can reproduce O3 sensitivity to temperature reasonably well. By controlling emissions specifically of NOx mankind has reduced its vulnerability. Third, I compare satellite-observed and modeled ammonia (NH3) under varying chemical environments over East Asia. Regulation of O3 precursor concentrations in the atmosphere has an indirect effect on NH3 concentrations. Air quality policy to reduce NOx and through that also nitric acid (HNO3) in the atmosphere can result in an increase in the concentration of NH3 because of its neutralizing ability. Therefore, a less acidic atmosphere sequesters less NH3. This preliminary work exposes different areas that need to be addressed to gain greater insight into NH3 emissions and chemistry.Item REMOTE SENSING OF AEROSOL AND THE PLANETARY BOUNDARY LAYER, AND EXPLORING THEIR INTERACTIONS(2022) SU, Tianning; Li, Zhanqing; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Aerosol-planetary boundary layer (PBL) interaction (API) is an important mechanism affecting the thermodynamics and convection in the lower atmosphere. API plays a critical role in the formation of severe pollution events and the development of convective clouds. Despite the progress made in understanding these processes, their magnitude and significance still have large uncertainties, varying significantly with aerosol distribution, aerosol optical property, and meteorological conditions. This study attempts to develop advanced remote sensing algorithms to retrieve information about the PBL and the aerosols contained within it. These remote sensing techniques are further used to elucidate the mechanisms governing API, enhancing our ability to predict air quality and model convective clouds, as well as understand the impact of aerosols on the climate system.In particular, we develop algorithms to improve the retrieval accuracy of aerosols and the PBL from satellite sensors and a ground-based lidar. For aerosol remote sensing, we use the deep neural network (DNN) to construct surface reflectance relationships (SRR) between different wavelengths. We then incorporate the DNN-constrained SRR into a traditional dark-target algorithm to retrieve the aerosol optical depth (AOD) using information from a current-generation geostationary satellite, i.e., Himawari-8, as input. As a result, the performance of AOD retrievals over East Asia is significantly improved. For PBL remote sensing, we explore different techniques for retrieving the PBL height (PBLH) from both a space-borne lidar (i.e., the Cloud-Aerosol Lidar with Orthogonal Polarization) and a ground-based lidar. We further develop a new method that combines lidar-measured aerosol backscatter with a stability-dependent model of PBLH diurnal variation. The new method circumvents or alleviates an inherent limitation of lidar-based PBLH detection when a residual layer of aerosols does not change in phase with the evolving thermodynamics. By separately considering surface-cloud coupling regimes, this method also offers high-quality retrievals of PBLH under cloudy conditions. Utilizing the enhanced retrievals of PBLH and synergistic measurements, we can also address some scientific questions concerning API, including the influencing factors of API and the role of aerosol vertical distributions. The correlation between the PBLH and the concentration of particulate matter with aerodynamic diameters less than 2.5 microns is generally negative. However, the magnitude, significance, and even the sign of their relationship vary greatly, depending on location and meteorological and aerosol conditions. In particular, API is considerably different under three aerosol vertical structure scenarios (i.e., well-mixed, decreasing and increasing with height). The vertical distribution of aerosol radiative forcing differs dramatically among the three types, with strong heating in the lower, middle, and upper PBL, respectively. Such a discrepancy in aerosol radiative forcing leads to different aerosol effects on atmospheric stability and entrainment processes. Absorbing aerosols are much less effective in stabilizing the lower atmosphere when aerosols decrease with height than in an inverted structure scenario.