Atmospheric aerosol is an important component of our atmosphere influencing human health, regional and global atmospheric chemistry and climate. The organic component of submicron aerosol contributes around 50% of its mass and is a complex mixture of tens of thousands of compounds. Real-time aerosol mass spectrometry was the major measurement tool used in this work. The Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) can quantitatively measure the chemical composition and size distribution of non-refractory submicron aerosol (NR-PM1). The mass spectra provided by the instrument every few minutes contain information about aerosol sources and processes. This thesis uses the HR-ToF-AMS measurements in two areas of Greece to quantify the contributions of organic aerosol sources to the corresponding organic aerosol levels. Local and regional air pollution sources were monitored and characterized in two sites during intensive campaigns. The first campaign took place during the fall of 2011 (September 24 to October 23) in Finokalia, Crete, a remote-background coastal site without any major human activity. The aim of the study was to quantify the extent of oxidation of the organic aerosol (OA) during autumn, a season neither too hot nor cold, with reduced solar radiation in comparison to summer. The second one took place during the winter of 2012 (February 26 to March 5), in the third major city of Greece, Patras. The measurements were conducted in the campus of the Technological Educational Institute of Patras (TEI), in order to quantify the severity of the wintertime air pollution problem in the area and its sources. The contributions of traffic and residential wood burning were the foci of that study. The Finokalia site is isolated and far away from anthropogenic sources of pollution, making it ideal for the study of organic aerosol coming from different directions, usually exposed to high levels of atmospheric oxidants. The fine PM measured during the Finokalia Atmospheric Measurement Experiment (FAME-11) by the AMS and a Multi Angle Absorption Photometer (MAAP) was mostly ammonium sulfate and bisulfate (60%), organic compounds (34%), and BC (5%). The aerosol sampled originated mainly from Turkey during the first days of the study, but also from Athens and Northern Greece during the last days of the campaign. By performing Positive Matrix Factorization (PMF) analysis on the AMS organic spectra for the whole dataset the organic aerosol (OA) composition could be explained by two components: a low volatility factor (LV-OOA) and a semi-volatile one (SV-OOA). Hydrocarbon-like organic aerosol (HOA) was not present, consistent with the lack of strong local sources. The second field campaign took place in the suburbs of the city of Patras, 4 km away from the city center during the winter of 2012. During this 10-day campaign, organics were responsible for 70% during the day and 80% during the evening of the total PM1. The OA mean concentration during that period was approximately 20 μg m-3 and reaching hourly maximum values as high as 85 μg m-3. Sulfate ions and black carbon followed with 10% and 7% of the PM1. PMF analysis of the organic mass spectra of PM1 explained the OA observations with four sources: cooking (COA), traffic (HOA), biomass burning (BBOA), and oxygenated aerosol (OOA), related to secondary formation and long range transport. On average, BBOA represented 58% of the total OM, followed by OOA with 18%, COA and HOA, with the last two contributing of the same percentage (12%). / --