Atmospheric aerosols are responsible for adverse health effects and uncertain climate forcing. Depending on their composition, they can directly affect climate by scattering or absorbing solar radiation and they can also indirectly affect by serving as cloud condensation nuclei (CCN). While the chemistry and physical properties of the inorganic components of the aerosols are more or less known, the same does not stand for the organic components. Hygroscopic water soluble organic material can enhance the water absorption of the particles, affecting their climate forcing. This dissertation explores the hygroscopic properties of atmospheric organic aerosol, the first part of the thesis is dedicated to the development and analysis of methods for the measurement of water soluble organic aerosol, while the second part investigates the hygroscopic properties and CCN activity of organic particulate matter emitted by different sources or produced in the atmosphere through oxidation of volatile organic compounds. / Τα ατμοσφαιρικά σωματίδια έχουν αρνητικές επιδράσεις στην ανθρώπινη υγεία αλλά και αβέβαιες επιπτώσεις στο κλίμα. Ανάλογα με τη σύστασή τους, μπορούν να επιδράσουν άμεσα στο κλίμα, σκεδάζοντας ή απορροφώντας ηλιακή ακτινοβολία, ενώ μπορούν ακόμα να δράσουν ως πυρήνες συμπύκνωσης συννέφων. Παρόλο που η χημεία και οι φυσικές ιδιότητες των ανόργανων συστατικών των αεροζόλ είναι γενικά γνωστές, δε συμβαίνει το ίδιο για τα οργανικά συστατικά. Υγροσκοπικά υδατοδιαλυτά οργανικά συστατικά μπορούν να αυξήσουν την απορρόφηση νερού από τα σωματίδια, επηρεάζοντας την επίδραση αυτών στο κλίμα. Αυτή η διατριβή διερευνά τις υγροσκοπικές ιδιότητες των ατμοσφαιρικών οργανικών σωματιδίων: Το πρώτο μέρος ασχολείται με την ανάπτυξη και την ανάλυση μεθόδων για τη μέτρηση των υδατοδιαλυτών ατμοσφαιρικών οργανικών σωματιδίων, ενώ στο δεύτερο διερευνώνται οι υγροσκοπικές ιδιότητες και η δράση ως πυρήνων συμπύκνωσης συννέφων οργανικών σωματιδίων που εκπέμπονται από διαφορετικές πηγές ή παράγονται στην ατμόσφαιρα μέσω οξείδωσης πτητικών οργανικών ενώσεων.

Ozone (O₃) and terpenoids react to produce secondary organic aerosol (SOA). This work explored novel ways that these reactions form SOA indoors, with five investigations, in two categories: investigations of (i) the impacts of particle controls on indoor SOA formation, and (ii) two fundamental aspects of indoor SOA formation. For category (i), two investigations examined the particle control devices of ion generators, which are air purifiers that are ineffective at removing particles and emit ozone during operation. With a terpenoid source present (an air freshener), ion generators acted as steady-state SOA generators, both in a 15 m³ chamber and 27 m³ room. The final investigation in category (i) modeled how heating, ventilating, and air-conditioning (HVAC) systems influence SOA formation. Influential HVAC parameters were flow rates, particle filtration, and indoor temperature for residential and commercial models, as well as ozone removal by particle-laden filters for the commercial model. For category (ii), the first investigation measured SOA formation from ozone reactions with single terpenoids and terpenoid mixtures in a 90 L Teflon-film chamber, at low and high ozone concentrations. For low ozone, experiments with only d-limonene yielded the largest SOA number formation, relative to other mixtures, some of which had three times the effective amount of reactive terpenoids. This trend was not observed for high ozone experiments, and these results imply that ozone-limited reactions with d-limonene form byproducts with high nucleation potential. The second investigation in category (ii) explored SOA formation from ozone reactions with surface-adsorbed terpenoids. A model framework was developed to describe SOA formation due to ozone/terpenoid surface reactions, and experiments in a 283 L chamber determined the SOA yield for ozone/d-limonene surface reactions. The observed molar yields were 0.14–0.16 over a range of relative humidities, and lower relative humidity led to higher SOA number formation from surface reactions. Building materials on which ozone/d-limonene surface reactions are predicted to lead to substantial SOA formation are those with initially low surface reactivity, such as glass, sealed materials, or metals. The results from category (ii) suggest significant, previously unexplored mechanisms of SOA number formation indoors. / text

Atmospheric aerosols are a highly relevant component of the climate system affecting atmospheric radiative transfer and the hydrological cycle. As opposed to other key atmospheric constituents with climatic relevance, atmospheric aerosol particles are highly heterogeneous in time and space with respect to their size, concentration, chemical composition and physical properties. Many aspects of their life cycle are not understood, making them difficult to represent in climate models and hard to control as a pollutant. Aerosol-cloud interactions in particular are infamous as a major source of uncertainty in future climate predictions. Field measurements are an important source of information for the modeling community and can lead to a better understanding of chemical and microphysical processes. In this study, field data from urban, marine, and arid settings are analyzed and the impact of meteorological conditions on the evolution of aerosol particles while in the atmosphere is investigated. Particular attention is given to organic aerosols, which are a poorly understood component of atmospheric aerosols. Local wind characteristics, solar radiation, relative humidity and the presence or absence of clouds and fog are found to be crucial factors in the transport and chemical evolution of aerosol particles. Organic aerosols in particular are found to be heavily impacted by processes in the liquid phase (cloud droplets and aerosol water). The reported measurements serve to improve the process-level understanding of aerosol evolution in different environments and to inform the modeling community by providing realistic values for input parameters and validation of model calculations.

La connaissance des sources primaires (combustion des énergies fossiles, combustion de la biomasse, éruptions des volcans, etc.) et secondaires (oxydation des composés organiques volatils (COV) suivie de la condensation formant des composés organiques particulaires) de l'aérosol organique ainsi que la caractérisation et la quantification de sa composition chimique restent un défit majeur, en particulier dans la région du Moyen Orient où les études de caractérisation de l'aérosol organique n'existent pas jusqu'à présent. Le Liban, un pays du Moyen Orient qui se situe au bord du bassin méditerranéen, représente un bon exemple pour la caractérisation des aérosols organiques dans cette région. Les travaux menés durant cette thèse s'inscrivent dans un objectif de l'étude de la qualité de l'air à Beyrouth (la capitale du Liban) en se concentrant plus spécifiquement sur les aérosols organiques. Tout d'abord, cette thèse a permis le développement d'un inventaire des émissions pour les gaz et les particules pour le Liban avec une résolution spatiale de 5 km x 5 km et pour la capitale Beyrouth avec une résolution spatiale de 1 km x 1 km. Les résultats obtenus indiquent que le transport routier est la source majoritaire responsable des émissions de monoxyde de carbone (CO), d'oxydes d'azote (NOX) et de composés organiques volatils non méthaniques (COVNM), tandis que les industries et les centrales électriques sont les principaux émetteurs des émissions de dioxyde de souffre (SO2) et des particules primaires. Ensuite, afin de caractériser les concentrations des polluants et plus spécialement la fraction organique des particules, deux campagnes de mesures intensives de 15 jours chacune ont été menées sur un site semi-urbain situé dans la banlieue de Beyrouth. Une première campagne estivale s'est déroulée en juillet 2011 et une deuxième campagne hivernale en février 2012. Ces campagnes, qui s'inscrivent dans le cadre du projet ECOCEM (Emission and Chemistry of Organic Carbon in East Mediterranean Beirut) ont permis une spéciation moléculaire et une catégorisation des sources en été et en hiver de l'aérosol organique au site de mesures où les campagnes ont été menées. En été, les précurseurs biogéniques tels que les monoterpènes et les sesquiterpènes qui aboutissent à la formation des aérosols organiques secondaires biogéniques sont la principale source à cause de l'insolation intensive et les températures élevées qui favorisent les émissions et les réactions de photo-oxydations. En hiver, la combustion de la biomasse est la principale source en raison de la combustion du bois dans le secteur résidentiel pour le chauffage. Enfin, les concentrations ambiantes des polluants à Beyrouth ont été simulées durant le mois de juillet 2011 à partir de données de l'inventaire des émissions développé dans le cadre de cette thèse en utilisant le modèle de chimie-transport Polyphemus/Polair3D. Les concentrations de polluants simulées avec le modèle ont été comparées aux concentrations mesurées durant la campagne estivale afin d'évaluer le modèle. Les résultats obtenus révèlent que le modèle est capable de simuler de manière satisfaisante les concentrations d'ozone (O3), de NOX et la plupart des composés présents dans les particules fines. Les différences entre le modèle et les mesures peuvent résulter des incertitudes dans les données d'entrée qui ont une très grande influence sur les sorties du modèle. Pour cela, une réduction des incertitudes engendrées par les données d'entrée et plus spécifiquement celles liées à l'inventaire des émissions est nécessaire. Par ailleurs, des mesures chimiques sur plusieurs sites sont aussi nécessaires dans le futur afin de mieux évaluer les simulations des concentrations de polluants / The chemical composition of PM2.5 includes both organic and inorganic compounds. Organic compounds, which constitute a significant fraction of the PM2.5 mass, can be emitted directly as primary aerosol from sources such as fossil-fuel combustion, biomass burning, and natural biogenic emissions, or formed in the atmosphere via chemical reactions leading to secondary organic aerosol (SOA) formation. SOA, which account for 20 – 80 % of total organic aerosol, are currently a major source of uncertainty in air quality modeling. The identification and quantification of the chemical composition of the organic fraction of PM2.5 and its source apportionment are of great interest, especially in the Middle East region where data on organic aerosols are currently lacking. Lebanon, a small developing country in the Middle East region located on the eastern shore of the Mediterranean basin represents a good example for characterizing organic aerosols in this region. To address this issue, the air quality in Beirut (the capital city of Lebanon) was investigated with a focus on organic aerosols. First, an air pollutant emission inventory was developed for Lebanon with a spatial resolution of 5 km x 5 km and for Beirut with a spatial resolution of 1 km x 1 km. The results obtained show that the road transport sector is the major contributor to carbon monoxide (CO), nitrogen oxides (NOx) and non-methane volatile organic compounds (VOC) emissions, whereas fossil fuel-fired power plants and large industrial plants are the major contributors to sulfur dioxide (SO2) and primary particulate matter (PM) emissions. Then, two intensive 15-day measurement campaigns were conducted at a semi-urban site located in a Beirut suburb to characterize air pollutant concentrations. The first measurement campaign took place in July 2011 and the second in February 2012. Measurements included PM2.5, organic carbon (OC) and elemental carbon (EC) mass concentrations as well as a molecular characterization of organic aerosols. Using these data, a source apportionment of organic aerosols was conducted for summer and winter. In summer, biogenic precursors such as monoterpenes and sesquiterpenes were the major source of OC due to intensive solar radiation and high ambient temperatures that promote biogenic VOC emissions and photo-oxidation reactions. In winter, biomass burning was the major source of organic aerosols because of the intensive use of wood burning for heating. Finally, air pollutant concentrations in Beirut were simulated for July 2011 with the Polyphemus/Polair3D chemical-transport model (CTM). The emission inventory mentioned above was used as input to the model. Meteorological simulations were conducted with the Weather Research and Forecasting model (WRF) using different configurations and the configuration leading to the best agreement with the observations was used to drive the air quality simulations. The simulated air pollutant concentrations were compared to the measured concentrations collected during the summer measurement campaign. The results show that the model reproduces satisfactorily the concentrations of ozone (O3), nitrogen dioxide (NO2), carbon monoxide (CO), and the major components of PM2.5. The differences obtained between the modeled and measured air pollutants concentrations are due in part to uncertainties in input data. Future studies should address the reduction of uncertainties such as those of the emission inventory. In addition, measurement campaigns involving several sites are needed to better characterize air pollution in Beirut and provide a more complete database to evaluate simulated air pollutant concentrations

Understanding the composition of atmospheric organic particulate matter (OPM) is essential for predicting its effects on climate, air quality, and health. However, the polar oxygenated fraction (PO-OPM), which includes a significant mass contribution from carboxylic acids, is difficult to speciate and quantitatively determine by current analytical methods such as gas chromatography-mass spectrometry (GC-MS). The method of chemical derivatization and two-dimensional GC with time of flight MS (GC×GC/TOF-MS) was examined in this study for its efficacy in: 1) quantifying a high percentage of the total organic carbon (TOC) mass of a sample containing PO-OPM; 2) quantitatively determining PO-OPM components including carboxylic acids at atmospherically relevant concentrations; and 3) tentatively identifying PO-OPM components. Two derivatization reagent systems were used in this study: BF₃/butanol for the butylation of carboxylic acids, aldehydes, and acidic ketones, and BSTFA for the trimethylsilylation (TMS) of carboxylic acids and alcohols. Three α-pinene ozonolysis OPM filter samples and a set of background filter samples were collected by collaborators in a University of California, Riverside environmental chamber. Derivatization/GC×GC TOF-MS was used to tentatively identify some previously unidentified α-pinene ozonolysis products, and also to show the characteristics of all oxidation products determined. Derivatization efficiencies as measured were 40-70% for most butyl derivatives, and 50-58% for most trimethylsilyl derivatives. A thermal optical method was used to measure the TOC on each filter, and a value of the quantifiable TOC mass using a gas chromatograph was calculated for each sample using GC×GC separation and the mass-sensitive response of a flame ionization detector (FID). The TOC quantified using TMS and GC×GC-FID (TMS/TOCGC×GC FID) accounted for 15-23% of the TOC measured by the thermal-optical method. Using TMS and GC×GC/TOF-MS, 8.85% of the thermal optical TOC was measured and 48.2% of the TMS/TOCGC×GC-FID was semi-quantified using a surrogate standard. The carboxylic acids tentatively identified using TMS and GC×GC/TOF-MS accounted for 8.28% of the TOC measured by thermal optical means. GC×GC TOF-MS chromatograms of derivatized analytes showed reduced peak tailing due in part to the lesser interactions of the derivatized analytes with the stationary phase of the chromatography column as compared to the chromatograms of underivatized samples. The improved peak shape made possible the greater separation, quantification, and identification of high polarity analytes. Limits of detection using derivatization and GC×GC/TOF-MS were μL injected for a series of C2-C6 di-acids, cis-pinonic acid, and dodecanoic acid using both butylation and TMS. Derivatization with GC×GC/TOF-MS was therefore effective for determining polar oxygenated compounds at low concentrations, for determining specific oxidation products not previously identified in OPM, and also for characterizing the probable functional groups and structures of α-pinene ozonolysis products.

This thesis characterizes the ambient fine organic carbon aerosol and investigates its sources through the development and deployment of new measurement techniques. The focus is on organic compounds that are soluble in water (WSOC), which comprise a large fraction of the organic aerosol, yet little has been known about its chemical nature. A method was developed for quantitative on-line measurements of WSOC by using a Particle-into-Liquid Sampler (PILS) to capture ambient particles into a flow of purified water, which is then forced through a liquid filter and the carbonaceous content quantified by a Total Organic Carbon (TOC) analyzer. This system allows for a continuous 6 minute (ground-based) or 3 s integrated measurement (airborne) with a limit of detection of 0.1 microgramsC/m3 and uncertainty of 10%. Furthermore, a new quantitative method was developed to group speciate the WSOC. In the first step, WSOC is separated by use of XAD-8 resin into its hydrophilic (WSOCxp) and hydrophobic (WSOCxr) fractions. This separation can be performed on-line by coupling the XAD-8 column with the PILS-TOC or off-line on WSOC extracted from integrated filter samples. If off-line, a second step involving size-exclusion chromatography (SEC) is used to chromatographically separate by organic functional groups the WSOCxp and recovered hydrophobic fraction (WSOCxrr). During this step, the WSOCxp is further separated into aliphatic acids with less than four carbons, neutrals, and bases. The WSOCxrr can be separated into acids and neutrals. Results showing the capabilities of the PILS-TOC both on the ground at the St. Louis Midwest Supersite and when airborne during the New England Air Quality Study/Intercontinental Transport and Chemical Transformation 2004 mission conducted in the northeastern U.S. will be presented. Ambient results from urban sites where a PILS-TOC was coupled with a XAD-8 column will be discussed. Data from the two-step speciation performed on samples collected from urban Atlanta summer and winter, and biomass burning in rural Georgia in a region of prescribed burning are presented. Finally, WSOC measurements obtained in Atlanta and its surrounding regions from both the speciation measurements and PILS-TOC will be used to investigate the sources of WSOC in the southeastern U.S.

An existing method for the measurement of atmospheric gaseous species was modified to collect data on aerosol concentrations. Data from biomass burning events in different regions (Canada, the Arctic and California) were collected during April to July, 2008 and the concentrations and evolution of secondary organic aerosols were discussed. And finally, data on the light absorbing properties of water soluble organic aerosols were collected in Atlanta, GA and compared with filter data for the same properties. The results presented in this thesis showed that a negative ion chemical ionization mass spectrometer (CIMS), can be modified by the addition of a thermally denuded inlet to measure aerosol phase sulfuric acid. This system can also be used to measure other aerosol phase organic acids. In the biomass burning plumes studied in the second part, no clear indication of formation of secondary aerosol or gaseous species was observed, except for peroxyacetyl nitrate (PAN). Filter data collected from FRM sites in the Southeastern U.S. showed that biomass burning is the most dominant source of water soluble light absorbing carbonaceous aerosol in this region. The data from a study in Atlanta, GA showed that the online PILS-LWCC-WSOC system might be used for measurements of light absorbing properties of aerosols and WSOC.

Land surface areas, which represent approximately 30% of the Earth’s surface, contribute largely to the complexity of the climate system by exchanging water, energy, momentum, and chemical materials with the overlying atmosphere. Because of the highly heterogeneous nature of the land surface and its rapid transformation due to human activities, future climate projections are less certain on regional scales than for the globe as a whole. The work presented in this dissertation is focused on a better understanding of regional-scale land–atmosphere interactions and their impacts on climate and air quality. Specifically, I concentrate my research on three typical regions in the United States (U.S.): 1) the Central U.S. (representing transition zones between arid and wet climates); 2) the Houston metropolitan region (representing a major urban area); and 3) the eastern U.S. (representing temperate forested regions). These regions are also chosen owing to the consideration of data availability. The first study concerns the roles of vegetation phenology and groundwater dynamics in regulating evapotranspiration and precipitation over the transition zones in summer months. It is found that the warm-season precipitation in the Central U.S. is sensitive to latent heat fluxes controlled by vegetation dynamics. Groundwater enhances the persistence of soil moisture memory from rainy periods to dry periods by transferring water to upper soil layers through capillary forces. Enhancement in soil moisture facilitates vegetation persistence in dry periods, producing more evaporation to the atmosphere and resulting in enhanced precipitation, which then increases soil moisture. The second study compares the impacts of future urbanization and climate change on regional air quality. The results show that the effect of land use change on surface ozone (O3) is comparable to that of climate change, but the details differ across the domain. The third study deals with the formation and distributions of secondary organic aerosols (SOA) — a largely overlooked but potentially important component in the climate system. Under future different climate scenarios, I found that biogenic emissions — an important precursor of SOA — are expected to increase everywhere over the U.S., with the largest increase found in the southeastern U.S. and the northwestern U.S., while changes in SOA do not necessarily follow those in biogenic emissions. Other factors such as partitioning coefficients, atmospheric oxidative capability, primary organic carbon, and anthropogenic emissions also play a role in SOA formation. Direct and indirect impacts from climate change complicate the future SOA formation. / text

Aerosols are either emitted directly into the atmosphere or are generated in the atmosphere; the latter process forms secondary organic aerosol (SOA). One of the important sources for SOA is the oxidation of volatile organic compounds (VOCs) by OH radicals, NOx, and O3. Aerosol can be visualized as suspended solid or liquid particle which is in equilibrium with surrounding gases. The products of SOA formation is a mixture of semi volatile organic compounds and a fraction of the products are condensable under atmospheric conditions. The condensable portion of aerosol is called particulate matter (PM) and these suspended particles can range in diameter from a few nanometers to microns. PM can impact climate through direct and indirect radiative forcing and can degrade air quality by reducing visibility and causing detrimental health effects. SOA can also form indoors, which also contributes to the health risk of PM. The severe impact of PM on human health and climate drives the scientific community to investigate the volatile organic compounds (VOCs) and their potential to form SOA, as well as the factors that alter the efficiency of SOA generation and the type of products. In a similar pursuit, the focus of this dissertation is the investigation of the SOA precursors that are emitted from trees and how they vary as a function of insect infestation. Also, the role of mixtures of VOCs as SOA precursors are investigated; commercial and lab made VOC mixtures are studied for SOA generation, product analysis, and absorption characteristics of aged SOA. Chapter 1 introduces PM, VOCs present in atmosphere, SOA generation, and speciation of products generated from the ozonolysis of VOCs. The impact of PM on human health and climate are summarized. A literature survey on the VOCs that are precursors to SOA and present in the outdoor and indoor environment is presented along with factors that may lead to variability in amount of VOCs. SOA generation from direct plant emissions and consumer products is surveyed. These studies show that VOC oxidation generate SOA which is important in the atmosphere due to climate and health effects and indoors due to health effects. A summary of SOA phase partitioning theories, the reaction mechanism for the formation of products from ozonolysis of the dominant biogenic SOA precursors (monoterpenes), and the factors that affect SOA generation is presented. Chapter 2 summarizes the results obtained from a field study assessing the impact of bark beetle infestation on SOA precursor emissions from forests in the Western United States. Samples of VOCs were collected by our collaborators from healthy and bark beetle infested trees using scent traps. We solvent extracted and analyzed by gas chromatography/mass spectrometry (GC/MS) nearly four hundred scent traps. An increase in the total and the individual VOCs emitted by infested trees was measured. A statistical analysis shows significant differences between the emissions from infested and healthy trees. A perspective is provided on potential impact of bark beetle infestation on regional SOA. The majority of the laboratory experiments for SOA generation have focused on individual VOCs as the single SOA precursor. However, as demonstrated in Chapter 2 for example, in a real environment multiple VOCs co-exist. Multiple SOA precursors undergo concurrent oxidation reactions, and it is not known if the products from concurrent oxidation of multiple precursors are the same as the sum of the products from individual SOA precursors. Mass closure analysis of field samples show that a significant fraction of the chemical identity of organic PM is unknown, but the chemistry impacts the toxicity of PM. Hence, it is important to understand SOA formation from realistic SOA mixtures. Chapter 3 describes the results of the SOA generation by ozonolysis of limonene and VOC mixtures containing limonene. We use an additive approach for building a surrogate VOC mixture close in composition to a commercially-available mixture. The yield of PM as a function of VOC precursor mixture was measured with respect to VOC composition using smog chamber SOA generation and scanning mobility particle sizing. PM in the chamber was collected onto filters and extracted, and the individual products of SOA were identified and quantified by GC/MS. The condensed-phase SOA products generated during these experiments for different VOC mixtures are compared. In Chapter 4, condensed-phase products sampled from SOA generated by the ozonolysis of α pinene and VOC mixtures containing α pinene, including two fir needle essential oils, are studied by extracting filter samples and analyzing the extracts by GC/MS. The products generated from VOC mixtures are characteristic of the most dominant VOC present in the mixture i.e. either limonene or α pinene. Some mixtures show the generation of new products which are not observed for corresponding individual VOC ozonolysis and hence can be used as marker for the corresponding VOC mixture. The distribution of α-pinene SOA products changes as the composition of the SOA precursor mixture changes. In Chapter 5, the UV visible absorption characteristics of ammonium ion aged SOA are discussed. Ammonium ion aging of aerosol leads impacts the radiative properties of aerosol and has the potential to impact aerosol's role in climate change. Filter samples containing SOA generated from two mixtures with different dominant monoterpenes (α-pinene-based Siberian fir needle oil and a limonene-based air freshener) were extracted. The absorption coefficients of the extracts were measured as a function of ammonium ion aging time using UV-visible absorption spectrometry. The conclusions from all above chapters are summarized in Chapter 6.

Atmospheric aerosols have been shown to have a significant impact on air quality and health in urban environments. Organic aerosols (OA) are one of the main constituents of submicron particulate matter. They are composed of thousands of different chemical species, which makes it challenging to identify and quantify their sources. OA sources have been previously studied; however quantitative knowledge of aerosol composition and their processes in urban environments is still limited. The results presented here investigate OA, their chemical composition and sources as well as their interaction with gases. On-line measurements of species in the particle and the gas phase were performed both from field-based and laboratory studies. Aerosol Mass Spectrometers (AMS) were used together with the Chemical Ionisation Mass Spectrometer (CIMS) and the Filter Inlet for Gases and AEROsols (FIGAERO). Two ambient datasets were analysed to develop methods for source apportionment, using the Multilinear Engine (ME-2), in order to gain new insights into aerosol sources in Manchester and London. Long-term measurements in London allowed the opportunity to perform seasonal analysis of OA sources and look into the relationship of hydrogen-like OA (HOA) and heavy- and light-duty diesel emissions. The seasonal analysis provided information about OA sources that was not possible to observe on the long-term analysis. During Bonfire Night in Manchester, with high aerosol concentrations, particularly biomass burning OA (BBOA), it was possible to identify particulate organic oxides of nitrogen (PON), with further identification of primary and secondary PON and their light absorbing properties. Through laboratory work, new insights into cooking organic aerosols (COA) were gained, a higher relative ion efficiency (RIEOA) value of around 3.3 for OA-AMS compared with the typical RIEOA of 1.4 was determined, which implies COA concentrations are overestimated when using the RIEOA value of 1.4. Dilution showed to have a significant effect on food cooking experiments, increasing both the gas/particle ratios and the O:C ratios. The data generated in this work, OA-AMS mass spectra and markers from both gas and particle phase identified with FIGAERO-CIMS, provide significant information that will contribute to the improvement of source apportionment in future studies. This work investigates OA, with a focus on primary organic aerosols originated from anthropogenic activities. These scientific findings increase our understanding of OA sources and can help to improve inventories and models as well as to develop plans and policies to mitigate the air pollution in urban environments.