This dissertation presents a scientific framework that facilitates enhanced understanding of aerosol source - receptor (S/R) relationships and their impact on the local, regional and global air quality by employing a complementary suite of modeling methods. The receptor - oriented Positive Matrix Factorization (PMF) technique is combined with Potential Source Contribution Function (PSCF), a trajectory ensemble model, to characterize sources influencing the aerosols measured at Gosan, Korea during spring 2001. It is found that the episodic dust events originating from desert regions in East Asia (EA) that mix with pollution along the transit path, have a significant and pervasive impact on the air quality of Gosan. The intercontinental and hemispheric transport of aerosols is analyzed by a series of emission perturbation simulations with the Sulfur Transport and dEposition Model (STEM), a regional scale Chemical Transport Model (CTM), evaluated with observations from the 2008 NASA ARCTAS field campaign. This modeling study shows that pollution transport from regions outside North America (NA) contributed ∼ 30 and 20% to NA sulfate and BC surface concentration. This study also identifies aerosols transported from Europe, NA and EA regions as significant contributors to springtime Arctic sulfate and BC. Trajectory ensemble models are combined with source region tagged tracer model output to identify the source regions and possible instances of quasi-lagrangian sampled air masses during the 2006 NASA INTEX-B field campaign. The impact of specific emission sectors from Asia during the INTEX-B period is studied with the STEM model, identifying residential sector as potential target for emission reduction to combat global warming. The output from the STEM model constrained with satellite derived aerosol optical depth and ground based measurements of single scattering albedo via an optimal interpolation assimilation scheme is combined with the PMF technique to characterize the seasonality and regional distribution of aerosols in Asia. This innovative analysis framework that combines the output from source - oriented chemical transport models with receptor models is shown to reduce the uncertainty in aerosol distributions, which in turn leads to better estimates of source - receptor relationships and impact assessments of aerosol radiative forcing and health effects due to air pollution.

This study presents airborne measurements of HO2NO2, HCl and SO2 using chemical ionization mass spectrometry (CIMS) during the Intercontinental Chemical Transport Experiment (INTEX) field campaign, an intensive study to characterize the chemical composition of the troposphere in the eastern United States, Mexico City, and the North Pacific which is the outflow region of Asia. The first direct in situ measurements of HO2NO2 were made in the free troposphere over the eastern U.S. during summer 2004. The highest mean mixing ratio of 76 pptv (median = 77 pptv, = 39 pptv) was observed in the altitude range of 8-9 km. Highly constrained steady state calculations of HO2NO2 using measured HOx levels are poorly correlated with observed HO2NO2 in the upper troposphere (8 km < z < 12 km; the median ratio of [HO2NO2]SS-MEA/[HO2NO2]MEA = 2.9). However, steady state HO2NO2 using model-derived HOx shows reasonable agreement with measurements in the free troposphere ([HO2NO2]SS-MEA/[HO2NO2]MEA = 1.3). The vertical distribution of HCl was measured over the north Pacific during May 2006 from the marine boundary layer (MBL) up to lower stratosphere. Recent stratospheric influence in the upper troposphere (8 km < z < 12 km) was efficiently identified from enhanced HCl (up to ~100 pptv) relative to very low background levels (< 2pptv). In the remote MBL, the acidification of seasalt aerosols by HNO3 appeared to be the major source of HCl, with level consistently over 20 pptv (up to 400 pptv). The distribution of SO2 was measured in the outflow region of the eastern U.S. and Asia; two major anthropogenic SO2 source regions. This study presents vertical and horizontal distributions of SO2 and relevant gas phase and aerosol parameters to characterize SO2 transport in the troposphere. SO2 in the boundary layer was efficiently transported to the upper troposphere by deep convection and frontal uplift processes. High SO2 in convective plume in the upper troposphere were strongly correlated with ultrafine aerosols.Conversely, SO2 from frontal uplift shows a strong correlation with non-volatile aerosols. Comparisons of SO2 products from global 3-D chemical transportation models (GEOS-CHEM and MOZART) with observations suggest that sulfur sources are relatively well described but that the oxidation mechanism needs refinement.

Ce travail de thèse a pour objectif de concevoir et réaliser un module informaticolinguistique apte à effectuer des analyses automatiques de textes thaï sous le système INTEX © . Basé fondamentalement sur les langues indo-européennes écrites avec l'alphabet latin, INTEX © rencontre quelques difficultés pour travailler sur une langue très différente comme le thaï. Le problème crucial est la segmentation en mots et en phrases, étant donné que le thaï n'a pas de séparateur de mot : une phrase est écrite en une séquence de lettres continues, et les séparateurs de phrase sont fréquemment ambigus. Aussi avons-nous développé et évalué deux méthodes de segmentation en mots, par expressions rationnelles et par transducteurs à nombre fini d'états, qui découpent respectivement des textes thaï en lettres et en syllabes. Nous avons également créé les dictionnaires électroniques du thaï qui servent à la fois à reconnaître les mots à partir des lettres ou des syllabes et à les étiqueter avec les codes syntaxiques et sémantiques. Deux méthodes de segmentation en phrases thaï, par la ponctuation et par mots-clés, sont également proposées et évaluées. Nous montrons enfin que, grâce à notre travail, INTEX © est capable d'analyser des documents thaï, malgré toutes les difficultés.