The monitoring and study of the earth�s atmosphere is becoming an increasingly important task given the current uncertainties in climate prediction. Areas where lidar has been used to further understanding of the atmosphere include monitoring of greenhouse gases, global warming, stratospheric ozone depletion, photochemical smog and aerosol photochemistry. However, the potentially severe long term effects of anthropogenic aerosols on earth�s biosphere are poorly understood. This project seeks to apply state of the art laser technology to develop an innovative multiwavelength lidar system capable of providing new information and new insights into the field of tropospheric aerosol lidar. Several novel tunable laser and laser-like sources have been investigated and developed for the purpose of tropospheric aerosol lidar at The National Institute of Water and Atmospheric Research (Niwa), Central Otago. Multiwavelength operation in the visible and near infrared portion of the spectrum has been emphasised with the sources developed collectively spanning the wavelength interval of 400-1369 nm. The laser sources investigated were the LiF:F2+ colour centre, Titanium Sapphire (Ti:sapphire) and barium nitrate Raman lasers. In addition to the laser sources, the β-barium borate optical parametric oscillator (BBO OPO) was characterised. For each of the sources, lidar relevant aspects were studied. The results recorded include conversion efficiency with respect to the pump source, linewidth and tuning characteristics, beam quality, temporal behaviour, and device reliability and ruggedness. It was found that the LiF:F2+ laser offered significantly lower threshold, broader tuning and higher output pulse energies than the Ti:sapphire laser in the 900-1000 nm region. The high optical gain of the LiF:F2+ medium facilitated cavity optical alignment and operation of the system. The high gain also resulted in temporal behaviour well suited to the existing Niwa lidar detection scheme. When using a 5 ns pump source, amplified spontaneous emission (ASE) was found to limit the laser tuning range and efficiency. The barium nitrate Raman laser was based on a simple linear cavity arrangement which resulted in a compact and robust device with no moving components. The stimulated Raman scattering process offers relatively narrow linewidth laser operation at the first and second Stokes wavelengths of 1197 nm and 1369 nm respectively. This laser offered efficient operation once the high operation threshold was reached. Second harmonic generation was used to extend the number of potential lidar transmitter lines produced. The barium nitrate Raman laser possessed high beam divergence and a maximum of three discrete transmitter wavelengths. The BBO OPO used a type I collinear signal resonant configuration. A plane-plane cavity configuration with pump reflection was found to provide simplicity of design, low threshold, highly efficient operation and output pointing stability. The BBO OPO signal wavelength could be tuned over the wavelength interval of 400-700 nm. The disadvantage of the plane cavity was high output beam divergence. However, this was successfully brought within the required limits through the use of a 40 mm long cavity in conjunction with an expanding and collimating telescope. As a result of the study, a Tunable lidar Transmitter (TLT) system based on the BBO OPO was designed and constructed at the Physics Department. The TLT was computer-controlled using custom written software and constructed in a self contained modular manner with all required mechanical, electrical and optical components. A user manual was also written to accompany the TLT. The TLT was installed at Niwa and was successfully used to gather preliminary multiwavelength lidar data. The TLT BBO OPO threshold occurred for a pump energy of 5.2 mJ (10.6 MW/cm2) and had a maximum slope efficiency of 53%. Signal efficiency varied from 24-41-35% over the intervals of 410-500-600 nm. A maximum signal energy of 21 mJ was obtained for a signal wavelength of 492 nm when using the maximum available pump energy of 42 mJ. OPO signal linewidth varied from 0.1-1-8 nm over the signal wavelength intervals of 400-600-700 nm. The associated OPO finesse varied between 370 and 100 as the signal wavelength was tuned over the wavelength interval of 400-600 nm. The temporal behaviour of the BBO OPO was a slowly varying function of pump energy and closely followed the temporal behaviour of the pump laser, making it well suited to the existing Italian lidar detection and timing scheme.

Many high-accuracy regional GPS continuously operating reference (CORS) networks have been established globally. These networks are used to facilitate better positioning services, such as high accuracy real-time positioning. GPSnet is the first state-wide CORS network in Australia. In order to maximize the benefits of the expensive CORS geospatial infrastructure, the state of Victoria in collaboration with three universities (RMIT University, the University of NSW and the University of Melbourne) embarked on research into regional atmospheric error modelling for Network-based RTK (NRTK) via an Australian Research Council project in early 2005. The core of the NRTK technique is the modelling of the spatially-correlated errors. The accuracy of the regional error model is a determining factor for the performance of NRTK positioning. In this research, a number of error models are examined and comprehensively analysed. Among them, the following three models are tested: 1) the Linear Interpolation Method (LIM); 2) the Distance-Based interpolation method (DIM); and 3) the Low-order surface model (LSM). The accuracy of the three models is evaluated using three different observation sessions and a variety of network configurations of GPSnet. Results show that the LIM and DIM can be used to significantly reduce the double-differenced (DD) residuals (up to 60% improvement), and the LIM is slightly better than the DIM (most at mm level). However the DD residuals with the LSM corrections are, in some cases, not only much worse than that of the LIM and DIM but also even must greater/worse than the DD residuals without any corrections applied at all. This indicates that there are no advantages by using the LSM for the error modelling for NRTK in GPSnet, even though it is the most commonly used method by researchers. The performance difference of the LIM for different GPSnet configurations is also tested. Results show that in most cases, the performance difference mainly caused by the number of reference stations used is not significant. This implies that more redundant reference stations may not contribute much to the accuracy improvement of the LIM. However, it may mitigate the station specific errors (if any). The magnitude of the temporal variations of both the tropospheric and ionospheric effects in GPSnet observations is also investigated. Test results suggest that the frequency of generating and transmitting the tropospheric corrections should not be significantly different from that for the ionospehric corrections. Thus 1Hz frequency (i.e. once every second) is recommended for the generation and transmission for both types of the atmospheric corrections for NRTK in GPSnet. The algorithms of the NRTK software package used are examined and extensive analyses are conducted. The performance and limitation of the NRTK system in terms of network ambiguity resolution are assessed. The methodology for generating virtual reference station (VRS) observations in the system is presented. The validation of the algorithms for the generated VRS observations is undertaken. It is expected that this research is significant for both the selection of regional error models and the implementation of the NRTK technique in GPSnet or in the Victorian region.

Thesis (M.Sc.). / Written for the Dept. of Atmospheric and Oceanic Sciences. Title from title page of PDF (viewed 2008/12/10). Includes bibliographical references.

Resumo: A quantificação do vapor d'água integrado na atmosfera (IWV - Integrated Water Vapor), ao contrário de outras variáveis meteorológicas, é algo que ainda se apresenta como um grande desafio para as Ciências Atmosféricas. Diversos mecanismos, envolvendo diferentes técnicas, têm sido empregados e testados para esse fim em diferentes regiões do globo por pesquisa dores das mais variadas áreas da ciência. Essa tese apresenta uma contribuição a esse tema ao empregar receptores GPS (Global Positioning System) em bases terrestres, localizados no Brasil, envolvendo instituições de pesquisa na área de Geodésia e de Meteorologia. Os objetivos principais desse trabalho são validar os valores do IWV obtidos a partir das observações GPS e contribuir com a viabilização da utilização de redes ativas de receptores GPS, existentes atualmente e futuras, no monitoramento do IWV como suporte às atividades da Meteorologia e Climatologia no Brasil. Os resultados obtidos mostram que, com a efetivação desse processo, poderá ser obtida uma fonte adicional de informações da umidade para Previsão Numérica de Tempo (PNT). Além disso, é mostrado também que a alta resolução temporal dos valores do IWV obtidos a partir das observações GPS pode contribuir para a melhoria dos resultados gerados por outras técnicas empregadas na mesma tarefa. Em contrapartida, um modelo de PNT é utilizado para gerar previsões da influência da troposfera nos sinais GPS, visando beneficiar aplicações GPS em tempo real. Os resultados gerados nesse trabalho são frutos da sinergia entre as duas áreas envolvidas e mostram que, atualmente, há boas perspectivas para essa parceria no Brasil. / Abstract: Quantification of Integrated Water Vapor (IWV), unlike other meteorological variables, still represents a significant challenge to the Atmospheric Sciences. In this task several techniques using different mechanisms have been employed and tested in different regions of the planet. Many researchers from several areas of science have been involved in this process. This thesis presents a contribution to this theme, employing ground-based GPS receivers installed on Brazilian territory, involving Geodesy and Meteorology research institutes. The main aim of this work is to contribute in order to make enable the use of the existing networks of continuously operating GPS receivers, and those that will be installed in the future, in IWV monitoring to support meteorological and climatological activities in Brazil. The results generated show that in this process it is possible to obtain an additional source of humidity information for Numerical Weather Prediction (NWP). Furthermore, the prospect of using the ground-based GPS receivers to monitor atmospheric water vapor is promising because thehigh temporal resolution of IWV values from GPS observations can improve the results generated from other techniques employed in the same task. At the same time, a NWP model is applied to generate predictions of the atmosphere's influence over radiofrequency signals, to improve real time GPS applications. The results of this work stem from the synergy between the two areas of science involved. They show that the current outlook for this partnership in Brazil is good, and that both Meteorology and Geodesy will benefit. / Orientador: João Francisco Galera Monico / Coorientador: João Augusto Toledo Machado / Banca: José Antonio Aravequia / Banca: Paul J. de Jonge / Banca: José Tadeu Garcia Tommaselli / Banca: Paulo de Oliveira Camargo / Doutor

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / O presente estudo teve como objetivo quantificar as emissões de Compostos Orgânicos Voláteis do Aterro Controlado Morro do Céu localizado na cidade de Niterói, Rio de Janeiro, Brasil. Para tanto, vinte amostras foram coletadas, usando uma bomba de ar operada a bateria durante dois dias de dezembro de 2009. Uma câmara de fluxo cilíndrica de PVC de 30L foi inserida 5 cm no solo do aterro, e as amostras foram coletadas através de uma válvula na parte superior da câmera. Os resultados indicaram um valor de 1.980 Kg Km-2 h-1. O modelo Gaussiano de dispersão atmosférica ISCST3 foi utilizado para calcular a difusão e transporte dos poluentes a fim de estimar as concentrações de COV no bairro, usando dados topográficos, meteorológicos e de emissões. Valores de 525 μg m-3 de COV foram encontrados a 500 metros do aterro. As emissões do aterro foram usadas em conjunto com dados meteorológicos, utilizando o modelo de trajetória OZIPR e o mecanismo químico SAPRC para demonstrar o impacto na formação do ozônio troposférico na região. É conhecido que o ozônio é formado pela reação entre COV, NOx e luz solar. A contribuição de valores elevados de COV provenientes das emissões do aterro conduzirá a uma nova situação com valores mais elevados de ozônio na região. Os resultados da modelagem indicaram um aumento maior que 1000% nos níveis de ozônio na região do aterro, se comparado com a modelagem do ozônio para a região metropolitana do Rio de Janeiro. Os resultados mostram ser necessário que maior atenção seja dada à política de gerenciamento de RSU no Brasil, incluindo a escolha adequada para o local de instalação, o monitoramento da área durante e após o período de operação e técnicas mais adequadas de disposição dos resíduos sólidos urbanos / The purpose of this work was to quantify the Volatile Organic Compounds emissions by a landfill (Morro do Céu), located in Niterói, Rio de Janeiro State, Brazil. Twenty 10-minute samples were collected using a battery-operated air pump operated at 500 mL min-1, over a period of four days in May and December, 2009. A cylindrical 30 L PVC flux chamber was used, the open, bottom side of which was inserted into the landfill soil to a depth of 5 cm. The samples were collected using a valve at the upper, closed side of the chamber. The results indicated an elevated value of 1,980 kg km-2 h-1. A Gaussian plume dispersion model, implemented by Aermod software, was used to calculate the diffusion and transport of pollutants, and the pollutant concentrations in the surroundings were estimated using the emission, meteorological, and topographical data. Maximum values of 525 μg m-3 for VOC were found at approximately 500 m from the landfill. The landfill emissions were also compiled with meteorological data, using the OZIPR trajectory model coupled with SAPRC chemical mechanism, to demonstrate their impact on the formation of tropospheric ozone. It is well known that ozone is formed by the reactions of VOC, NOx and sunlight. The contribution of high VOC levels from the landfill emissions was expected to lead to higher ozone values. The results indicated a 1000% increase in ozone in the region of the landfill, compared to the ozone values for the metropolitan region of Rio de Janeiro. The results show that it is both necessary and desirable that greater attention be given to the political management of municipal solid waste in the Brazil, including the location choice, the monitoring of landfill areas during and after their period of operation and techniques more appropriate of disposition of municipal solid waste

Neste trabalho foram estudados, através de simulações numéricas e medidas de concentração de poluentes próximo à superfície, algumas situações meteorológicas que determinaram episódios de destaque com relação ao poluente ozônio que ocorreram na Região Metropolitana de São Paulo (RMSP) entre 1999 e 2006. Primeiramente, foram avaliados dois modelos fotoquímicos, CIT e SPM-BRAMS, quanto à formação de ozônio e a correta representação dos processos de dispersão de poluentes na região. Após a avaliação dos modelos, foram determinadas características do escoamento atmosférico durante a ocorrência de episódios críticos do ponto de vista da qualidade do ar. Os resultados obtidos mostraram que a variabilidade nas concentrações do ozônio pode ser bem representada pelos modelos utilizados. Em geral, as concentrações simuladas com o SPM-BRAMS concordam bem com as observações em termos da fase do ciclo diurno, sendo os valores das concentrações um pouco subestimados com relação aos máximos observados. O modelo CIT, por sua vez, apresentou concentrações mais altas, principalmente nos horários de máximo, tendo também representado adequadamente o ciclo diurno. Nas simulações, com ambos os modelos, foi constatado que nos pontos referentes às estações de monitoramento localizadas na porção sudeste da RMSP, foram obtidos os piores resultados em termos de parâmetros estatísticos comumente utilizados na avaliação de resultados modelados. Com o SPM-BRAMS foram também realizadas simulações abrangendo o mês de janeiro de 2006, através das quais foram estudadas as condições atmosféricas em grande e mesoescala e o comportamento das concentrações de ozônio associadas. Durante este mês houve períodos de intensa atividade convectiva, relacionados a episódios de ZCAS, bem como períodos mais secos em que a atmosfera apresentava-se mais estável. Observou-se que durante episódios de chuva intensa há uma superestimativa das concentrações pelo modelo; no entanto, os resultados são bem próximos às observações em situações de céu claro e com ventos menos intensos. Os picos secundários noturnos na concentração de ozônio, observados com certa freqüência nos dados medidos, nem sempre foram bem representados pelo modelo, embora os picos máximos diurnos fossem bem representados. Os dias em que os picos noturnos foram simulados adequadamente pelo SPM-BRAMS foram caracterizados por alta pressão desde a superfície até níveis médios, com maior subsidência e estabilidade na atmosfera, favorecendo o transporte de ozônio a partir de níveis mais altos da atmosfera para a superfície. Os picos noturnos com concentrações acima de 20 ppbv foram os mais bem representados. / Throughout numerical simulations and near to surface measurements of pollutants concentrations, in this work some meteorological situations of relevance for high ozone concentrations episodes over the Metropolitan Area of Sao Paulo (MASP) were studied., between 1999 and 2006. Firstly, two photochemical models, CIT and SPM-BRAMS, were evaluated in the sense of the correct representation of ozone formation and the pollutant dispersion processes over the region. After the models evaluation, some characteristics of the atmospheric flow were determined during the occurrence of critical events from the air quality point of view. The results showed that the ozone concentrations variability was relatively well represented by the used models. In general, the concentrations simulated by the SPMBRAMS agree well with observations, in terms of the diurnal cycle phase, but the concentrations values were slightly underestimated compared to the observed maximum. The CIT model showed higher concentrations, especially during diurnal maximum peaks. The diurnal cycle was also adequately represented by this model. In simulations with both models, it was found that in the monitoring stations located in the southeastern portion of the MASP, the worst results were obtained in terms of statistical parameters commonly used in the evaluation of models results. The SPM-BRAMS was also used for simulations throughout the whole month of January 2006. With these simulations the atmospheric conditions in large and meso scales and the associated ozone concentrations behavior were studied. During this month periods of intense convective activity occurred, associated with SACZ episodes. Dry periods in which the atmosphere was more stable, were also observed during this month. It was observed that during episodes of intense precipitation, there is a tendency of concentration overestimation by the model; however, the results are very close to the observations in situations of clear sky and with milder winds. The nocturnal secondary peaks in the ozone concentration observed with some frequency in the measured data, were not always well represented by the model, while the maximum day time peak were well represented. The days when the nocturne peaks were properly simulated by SPM-BRAMS, were characterized by high pressure from the surface to mid-level, with more atmospheric subsidence and stability, promoting the transport of ozone from higher levels of the atmosphere to the surface. The nocturnal peaks with concentration above 20 ppbv were most well represented.

Esta tese de doutorado teve como objetivo avaliar o impacto na qualidade do ar da Região Metropolitana de São Paulo (RMSP) de mudanças do clima a partir de cenários de mudança global oriundos do IPCC (International Panel for Climate Change) e das mudanças nas fontes urbanas da RMSP, decorrentes da implantação de políticas de controle de emissões veiculares. A qualidade do ar foi estimada por meio do modelo WRF/Chem (Weather Research and Forecasting with Chemistry). Os cenários do IPCC que foram utilizados representam situações futuras, levando-se em conta o aquecimento global dentro de suas perspectivas otimista (SRES B1) e pessimista (SRES B2). Para a representação desses dois cenários foram utilizadas as saídas do modelo climático global CCSM3 (Community Climate System Model), as quais serviram como condições iniciais e de contorno para o modelo utilizado no trabalho. A avaliação da qualidade do ar foi realizada com base na análise da concentração de ozônio na RMSP, para os anos de 2020 e 2050. Também, foram considerados os eventuais impactos na qualidade do ar considerando-se mudanças nas fontes de emissão veicular. Dessa forma foram estudados cenários com mudanças climáticas ou com variação nas emissões veiculares para os anos de 2020 e 2050 e com ambas para o ano de 2050. Os resultados foram avaliados através de métodos estatísticos em comparação com o caso base, que representa o comportamento do ozônio no período de estudo compreendido entre os dias 08 e 16 do mês de novembro de 2011. As análises estatísticas dos resultados das simulações em comparação com os dados medidos mostraram que o modelo representou de forma satisfatória as condições ambientais observadas no período de estudo. Resultados das simulações de eventos futuros considerando os casos onde foram modificadas as condições meteorológicas para os anos de 2020 e 2050 e mantidas as emissões de 2011 mostraram pouca diferença das concentrações de ozônio sobre a RMSP. Por outro lado, resultados das simulações obtidos da alteração das emissões para os anos futuros, tendo como base as condições meteorológicas de 2011 apresentaram grande variação das concentrações de ozônio sobre a mesma área. Por fim, resultados obtidos a partir de simulações com alterações das condições meteorológicas e das emissões para o ano de 2050 para os dois cenários do IPCC mostraram as maiores diferenças entre os cenários simulados e ambos concordam na ocorrência de aumento de concentrações de ozônio no futuro. Pode-se explicar essa tendência de aumento a partir de duas hipóteses: o aumento da temperatura, favorecendo a ocorrência dos processos fotoquímicos e o maior controle das emissões por veículos pesados, levando a uma razão de Compostos Orgânicos Voláteis por Óxidos de Nitrogênio mais favorável para a formação do ozônio. / This PhD dissertation aims to assess the impact of climate change on regional air quality from global change scenarios estimated by IPCC and control vehicle emissions changes over the Metropolitan Area of São Paulo (MASP). The air quality was estimated by WRF/Chem model. For this purpose, the scenarios proposed by IPCC that represent future situations were used, taking into account global warming in an optimist (SRES B1) and pessimist (SRES A2) perspective. The output files from the global climate model CCSM3 (Community Climate System Model) based in these scenarios were used as initial and boundary conditions for the model used in this work and, based on a defined set of cases, possible impacts on ozone concentrations were evaluated over the MASP for 2020 and 2050. Also, possible impacts on air quality were considered based on changes in the emission sources. In this way, the following cases were studied: 1) the actual emission for the two meteorological scenarios during 2020 and 2050; 2) same meteorological condition of 2011 for scenarios of urban emission with public politics of emission control for 2020 and 2050, and; 3) a scenario with 2050´s emissions and IPCC meteorological conditions. Results were evaluated through statistical methods based on a control case, which represents the ozone concentrations during the period between November 08th and 16th of 2011. Results obtained with the control case simulation showed that the model represented satisfactorily environmental conditions observed during the study period. Simulation results of future events considering cases where weather conditions were modified for 2020 and 2050 and keeping the emissions of 2011 showed little difference in the ozone concentrations over the MASP. On the other hand, simulation results obtained from the change in emissions for future years, based on weather conditions of 2011, showed a large variation of ozone concentrations over the same area. Finally, results from simulations with changes in weather and emissions for 2050, considering the two IPCC scenarios, showed major differences between the simulated scenarios and both of them show similar results in the sense that high ozone concentrations are estimated for the future. This trend of increased concentrations can be explained by two assumptions: higher temperature, causing the occurrence of photochemical processes, and the implementation of control emissions by heavy vehicles, leading to a ratio of Volatile Organic Compounds by Oxides of Nitrogen more favorable to the formation of ozone.

A Região Metropolitana de São Paulo (RMSP) enfrenta sérios problemas relacionados à degradação da qualidade do ar devido às emissões de sua intensa frota veicular, apresentando constantes ultrapassagens dos Padrões de Qualidade do Ar de poluentes como o ozônio (PQAr ~80ppbv). O Ozônio é formado na atmosfera em condições complexas em presença de intensa radiação solar, altas temperaturas, baixa umidade relativa, ventos fracos e altas concentrações dos precursores, óxidos de nitrogênio (NOx = NO + NO2) e compostos orgânicos voláteis (COVs). Assim, o problema da poluição do ar em centros urbanos precisa ser tratado com metodologias mais modernas para que possam ser estabelecidos novos critérios para redução de seus precursores e o conhecimento das condições mais adequadas (relação entre os COVs e os NOx, além da especiação destes COVs) para a redução do ozônio troposférico. Neste contexto, modelos fotoquímicos de qualidade do ar têm sido usados para auxiliar na tomada de decisões ambientais estratégicas. O módulo químico SAPRC Statewide Air Pollution Research Center é um mecanismo detalhado para simular reações entre COVs e NOX, desenvolvido para ser aplicado para atmosferas urbanas e regionais dos Estados Unidos. Porém, devido características específicas do combustível (aproximadamente 30% da frota usa etanol), no Brasil a poluição urbana apresenta características próprias. Dessa forma, baseado em campanhas anteriores de amostragem de COVs, no presente estudo foram modificados o inventário de emissões e o módulo químico (SAPRC99) do modelo fotoquímico CIT a fim de melhorar a representação do ozônio quanto a sua formação e consumo na atmosfera da RMSP. Para isso, alguns COVs como xilenos, 1-buteno e trimetilbenzenos foram explicitados. As simulações para os dias 30 e 31 de outubro de 2006 mostraram aumentos de espécies como peroxiacetilnitrato e ozônio de aproximadamente 10% para o centro de formação de pluma sobre a RMSP. / The Metropolitan Area of São Paulo (MASP) suffers severe problems related to air quality degradation presenting constant air quality standard overpasses for pollutants like ozone (QSAir ~80ppbv), due to its intense vehicular fleet. Ozone is formed in the atmosphere under complex conditions in the presence of strong solar radiation, high temperatures, low relative humidity, weak winds and also high precursor concentrations, such as nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOCs). Therefore, the problem of air pollution in urban centers has to be treated using modern methodologies in order to establish new criteria for reduction of precursors and to know more adequate conditions (relation between VOCs and NOx, as well as speciation of these VOCs) in order to reduce tropospheric ozone. In this context, air quality photochemical models have been used to support strategic environmental decisions. SAPRC chemical mechanism Statewide Air Pollution Research Center developed to be applied in the United States urban atmospheres, consists of a detailed mechanism to simulate reactions between VOCs and NOx. However, due to specific fuel properties (about 30% of vehicular fleet uses ethanol), urban air pollution in Brazil presents its own characteristics, such as higher level of the oxygenated compounds. Hence, based on previous campaigns where VOCs had been sampled, the emission inventory and the chemical module (SAPRC99) were modified in order to improve ozone consumption and formation representation in the MASP atmosphere. As a result, some VOCs like xylenes, 1-butene and trimethilbenzens were explicated. Simulations for 30 and 31 of October 2006 presented increases in species formation like peroxyacetylnitrate and ozone about 10% in the centre of the MASP plume.

Doctorat en Sciences / info:eu-repo/semantics/nonPublished

Understanding changes in the burden and growth rate of atmospheric methane (CH4) has been the focus of several recent studies but still lacks scientific consensus. Here we investigate the role of decreasing anthropogenic carbon monoxide (CO) emissions since 2002 on hydroxyl radical (OH) sinks and tropospheric CH4 loss. We quantify this impact by contrasting two model simulations for 2002-2013: (1) a Measurement of the Pollution in the Troposphere (MOPITT) CO reanalysis and (2) a Control-Run without CO assimilation. These simulations are performed with the Community Atmosphere Model with Chemistry of the Community Earth System Model fully coupled chemistry climate model with prescribed CH4 surface concentrations. The assimilation of MOPITT observations constrains the global CO burden, which significantly decreased over this period by similar to 20%. We find that this decrease results to (a) increase in CO chemical production, (b) higher CH4 oxidation by OH, and (c) similar to 8% shorter CH4 lifetime. We elucidate this coupling by a surrogate mechanism for CO-OH-CH4 that is quantified from the full chemistry simulations.