Improving chemical transport models for atmospheric simulations relies on future developments of mathematical methods and parallelization methods. Better mathematical methods allow simulations to more accurately model realistic processes and/or to run in a shorter amount of time. Parellization methods allow simulations to run in much shorter amounts of time, therefore allowing scientists to use more accurate or more detailed simulations (higher resolution grids, smaller time steps). The state-of-the-science GEOS-Chem model is modified to use the Kinetic Pre-Processor, giving users access to an array of highly efficient numerical integration methods and to a wide variety of user options. Perl parsers are developed to interface GEOS-Chem with KPP in addition to modifications to KPP allowing KPP integrators to interface with GEOS-Chem. A variety of different numerical integrators are tested on GEOS-Chem, demonstrating that KPP provided chemical integrators produce more accurate solutions in a given amount of time than the original GEOS-Chem chemical integrator. The STEM chemical transport model provides a large scale end-to-end application to experiment with running chemical integration methods and transport methods on GPUs. GPUs provide high computational power at a fairly cheap cost. The CUDA programming environment simplifies the GPU development process by providing access to powerful functions to execute parallel code. This work demonstrates the accleration of a large scale end-to-end application on GPUs showing significant speedups. This is achieved by implementing all relevant kernels on the GPU using CUDA. Nevertheless, further improvements to GPUs are needed to allow these applications to fully exploit the power of GPUs. / Master of Science

The Weather Research and Forecasting with Chemistry (WRF-Chem) Model is an “online” regional scale prediction system designed to simulate many detailed meteorological, gas-phase chemical and aerosol processes, with full coupling between the different components. The impacts of aerosol particles are complex and spatially heterogeneous, their impacts varying greatly at the regional scale. Modelling the properties and impacts in a systematic manner requires the coupling between different chemical phases, meteorological and physical parameterisations a model such as WRF-Chem offers. This manuscript documents several developments, and their evaluation, that have been made to the WRF-chem model to improve its representation of detailed gas-phase chemical and aerosol processes. The first study gives an overview of developments made for modeling the North-West European region, including the addition of a new semi-explicit chemical mechanism, N2O5 heterogeneous chemistry and modifications to the sea-spray emissions routine to include fine-mode organic material. The broad impacts of these developments were assessed in the study, while a follow up paper (included in supplementary material) investigated more deeply the impacts of N2O5 heterogeneous chemistry. The second study discusses modifications to WRF-Chem and emission products to improve modelled representation of biomass burning aerosol particles over Brazil. Model results were compared with aircraft measurements and found to represent aerosol particle size distributions and cloud condensation nuclei concentrations reasonably well, but too much biomass burning aerosol were transported up to high altitudes (4-8 km) by the model. In the third study, nested simulations (at higher resolutions than those used in the second study) over Brazil were used to evaluate the impact of aerosol particles on the local radiative balance, by comparing model results from simulations with and with- out aerosol-radiative feedbacks. The instantaneous clear sky aerosol-radiation forcings were found to have a net cooling of -5.0 W m−2 at the top of the atmosphere. Issues with resolving aerosol–cloud interactions, because of the convective parameterisation and differences in model setup across scales, made evaluating semi- and indirect effects impossible.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第21597号 / 理博第4504号 / 新制||理||1647(附属図書館) / 京都大学大学院理学研究科化学専攻 / (主査)教授 杉山 弘, 教授 秋山 芳展, 准教授 竹田 一旗 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

Recent structural studies evidenced the presence of a recurring well-known interaction between an oxygen atom and an aromatic nucleobase ring in structural motifs of nucleic acids. In particular, this type of interaction is observed between the O4' atom of the (deoxy)ribose moiety and the aromatic nucleobase in Z-DNA molecules and in a variety of structural RNA molecules. In this thesis, we comprehensively examine the hitherto undetected stacking interactions between an oxygen atom of a water (Ow) molecule and the aromatic nucleobase ring, using structural bioinformatics along with quantum mechanics. On the basis of the structural analysis of the high-resolution X-ray structures, we found out that the stacking distance between the Ow atom and the nucleobase plane varies between 3.1 and 4.0 Å. Further, the contact between the Ow-nucleobase plane can be categorized either as a lonepair-π type, where the Ow atom interacts directly with the aromatic surface of the nucleobase, or as an OH-π interaction, where one of the hydrogen atoms of the Ow points towards the nucleobase. Our quantum chemical analysis evidenced that the OH-π interaction is clearly favored in terms of energetics when compared to the lonepair-π, except for the uracil, where the lonepair-π kind of interaction seems to be energetically more stable, as also supported by electrostatic potential map calculations.

This work is aimed to study the capabilities of CMAQ and WRF-Chem models for predicting the PM10 and PM2.5 pollution in the west side of Saudi Arabia. To do this fairly, one-month simulations (April, 2021) are done in both models using same initial and boundary conditions, meteorology and anthropogenic emissions. Unique configurations in both models allow to compare differences in the chemical processes and natural emissions estimation of each model. Simulated PM (PM10 and PM2.5) surface concentrations and AOD are compared with available observations to assess models’ performance. Moreover, CMAQ is used to study a real air pollution episode generated by a fire in the Rabigh Electricity Power Station between April 8 and April 11, 2021.

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京都大学 / 新制・課程博士 / 博士(工学) / 甲第25268号 / 工博第5227号 / 新制||工||1997(附属図書館) / 京都大学大学院工学研究科都市環境工学専攻 / (主査)教授 藤森 真一郎, 教授 米田 稔, 教授 橋本 訓 / 学位規則第4条第1項該当 / Doctor of Agricultural Science / Kyoto University / DFAM

Nowadays, megacities all over the world are facing air quality issues, especially regarding the control of secondary pollutants such as tropospheric ozone (O3) but mainly fine particles (PM2.5 ; 2.5 m in diameter), as they have important impacts on both human health and climate change. Understanding the evolution of these particles in the atmosphere requires the description of emission sources as well as the physicochemical processes involved in their formation, growth and removal. In this study, the Weather Research and Forecasting with Chemistry (WRF-Chem) community model, a state-of-the-art coupled meteorology-chemistry modelling system, along with experimental data collected during the Narrowing the Uncertainties on Aerosol and Climate Change in São Paulo State (NUANCE-SPS, FAPESP thematic project) campaigns performed in 2012 and 2014, were used in order to examine the main properties of atmospheric aerosol particles over the Metropolitan Area of São Paulo (MASP), in southeastern Brazil, where changes in fuel blend and consumption in recent years have affected the evolution of pollutant concentrations. The combined application of aerosol data and WRF-Chem simulations made it possible to represent some of the most important aerosol properties such as particle number concentration (PNC) and cloud condensation nuclei (CCN) activation, besides allowing us to evaluate the contributions of anthropogenic and biomass burning sources to the PM2.5 loadings in the MASP. For instance, on-road vehicles have a potential to form new particles between 20 and 30 % in relation to the total PM2.5 mass, whereas biomass burning, on average, accounted for 824 % (515 g m3 ) of it. In addition, biomass burning accounted for up to 20 % of the baseline PNC- and CCN-weighted relative differences over the MASP (2300 cm3 and 1400 cm3 , respectively). The results indicate the potential importance of biomass burning sources for air quality in the MASP, and underscore the need for more accurate representations of aerosol emissions to reduce uncertainties in the model predictions. / Atualmente, megacidades ao redor do mundo enfrentam problemas de qualidade do ar, especialmente aqueles relacionados ao controle de poluentes secundários como o ozônio troposférico (O3), mas principalmente partculas finas (PM2.5 ; 2.5m em diâmetro). As partculas finas têm impactos significativos na saúde humana bem como no clima, através das mudanças climáticas. O entendimento da evolução destas partculas na atmosfera requer a descrição de suas fontes de emissão e também dos processos fsico-qumicos envolvidos na sua formação, crescimento e remoção. Neste estudo, o modelo Weather Research and Forecasting with Chemistry (WRF-Chem), um sistema de modelagem atmosférica estado-da-arte, juntamente com dados coletados durante duas campanhas experimentais realizadas em 2012 e 2014 no âmbito do projeto Narrowing the Uncertainties on Aerosol and Climate Change in São Paulo State (NUANCE-SPS, projeto temático FAPESP), foram usados para analisar as principais propriedades do aerossol atmosférico na Região Metropolitana de São Paulo (RMSP), no sudeste do Brasil, onde mudanças na composição e no consumo dos combustveis têm afetado a evolução da concentração de poluentes. A aplicação combinada de dados experimentais e simulações numéricas com o WRF-Chem permitiu a representação de algumas das propriedades mais importantes do aerossol atmosférico como concentração do número de partculas e ativação de núcleos de condensação de nuvens, assim como a avaliação da contribuição de fontes antropogênicas e de queimadas na concentração do PM2.5 . Por exemplo, fontes veiculares têm potencial para formar novas partculas entre 20 e 30 % em relação à massa total do PM2.5, enquanto fontes de queimadas contriburam, na média, entre 824 % (515 g m3 ) da massa total deste poluente. Outrossim, fontes de queimadas contriburam em até 20 % das concen- trações base do número de partculas e de núcleos de condensação de nuvens sobre a RMSP (2300 cm3 e 1400 cm3, respectivamente). Os resultados indicam o potencial impacto das queimadas na qualidade do ar na RMSP, e enfatizam a necessidade de aprimoramentos nos modelos de emissão de aerossol, visando reduzir incertezas nas previsões do modelo.