Thesis. 1977. M.S.--Massachusetts Institute of Technology. Dept. of Meteorology. / Microfiche copy available in Archives and Science. / Bibliography : leaves 77-78. / M.S.

Thesis. 1977. M.S.--Massachusetts Institute of Technology. Dept. of Meteorology. / Microfiche copy available in Archives and Science. / Bibliography : leaves 81-83. / M.S.

Factors governing the efficiency of convective moistening in the tropical upper troposphere between 15

The upper troposphere-lower stratosphere (UTLS) is a transition region between the troposphere and the stratosphere. During the boreal summer, the UTLS is dominated by large-scale anticyclonic circulations over the Asian and North American monsoon regions, exhibiting complex dynamical and chemical characteristics. Re-cent studies have emphasized the important role of the summer monsoon systemin stratosphere-troposphere exchange of water vapor and chemical species, which strongly influences the atmospheric chemistry and climate system. The transport in the UTLS region occurs in both directions, stratosphere-troposphere transport (STT)and troposphere-stratosphere transport (TST). For example, observational studies indicate localized maxima of tropospheric pollutants and stratospheric water vapor(SWV) in the UTLS, which are controlled by deep convection and large-scale circulation. Meanwhile, stratospheric ozone (O3) can fold into tropospheric air and entrain into the planetary boundary layer (PBL) via deep STT, and thus affect air quality at the surface. In this thesis, we aim at improving the understanding of the transport processes in the UTLS that are linked to monsoon dynamics using observations and modelling tools.<div><br></div><div>First, we investigate the TST transport in association with the Asian summer monsoon. We examine the simulation of SWV in the Community Earth System Model, version 1 with the Whole Atmosphere Community Climate Model as its atmospheric component [CESM1(WACCM)]. CESM1(WACCM) generally tends to simulate a SWV maximum over the central Pacific Ocean instead of over the Asian continent as observed, but this bias is largely improved in the high vertical resolution version. The high vertical resolution model with increased vertical layers in the UTLS is found to have a less stratified UTLS over the central Pacific Ocean compared with the low vertical resolution model. It therefore simulates a steepened potential vorticity gradient over the central Pacific Ocean that better closes the upper-level anticyclone and confines the SWV within the enhanced transport barrier.<br></div><div><br></div><div>We further study the transport pathways connecting the Northern Hemisphere sur-face and the North American (NA) UTLS by diagnosing Boundary Impulse Response idealized tracers implemented at the Northern Hemisphere surface during summer. In ensemble average, air masses enter the NA UTLS region above Central America, and then slowly mix into the higher latitudes. However, fast transport pathways with modal age around two weeks are evident in some tracer ensembles. For these rapid transport pathways, the tracers first reach the UTLS region over the eastern Pacific and the Gulf of Mexico as a result of enhanced deep convection and vertical advection, followed by horizontal transport over the United States by a strengthened UTLS anticyclone circulation.<br></div><div><br></div><div>To the end, we evaluate the downward transport of stratospheric O3via STT using simulation from a state-of-the-art chemistry climate model implemented with an artificial stratospheric ozone tracer (O3S). We find that O3transported from the stratosphere makes a significant contribution to the surface O3variability where back-ground surface O3exceeds 95thpercentile, especially over the western U.S. Maximum covariance analysis is applied to O3anomalies paired with stratospheric O3traceranomalies to identify the stratospheric intrusion and the underlying dynamical mechanism. The first leading mode corresponds to deep stratospheric intrusions in the western and northern tier of the U.S., and intensified north easterlies in the mid-to-lower troposphere along the west coast, which also facilitate the transport to the eastern Pacific Ocean. The second leading mode corresponds to deep intrusions over the Intermountain Regions. Both modes are associated with eastward propagating baroclinic systems, which are amplified near the end of the North Pacific storm tracks, leading to strong descents over the western United States.<br></div>

International Telemetering Conference Proceedings / October 22-25, 2001 / Riviera Hotel and Convention Center, Las Vegas, Nevada / This student paper was produced as part of the team design competition in the University of Arizona course ECE 485, Radiowaves and Telemetry. It describes a telemetering system design recommendation for a small satellite capable of conducting scientific research regarding atmospheric water content. This paper focuses on the subsystems required to send the scientific data and monitored operational conditions from the satellite to, and commands to the satellite from, a ground station. A companion paper (Hittle, et. al.) focuses on the cross-link subsystem required to make the scientific measurements and on the power generation and distribution subsystem for the satellite.

International Telemetering Conference Proceedings / October 22-25, 2001 / Riviera Hotel and Convention Center, Las Vegas, Nevada / This student paper was produced as part of the team design competition in the University of Arizona course ECE 485, Radiowaves and Telemetry. It describes a telemetering system design recommendation for a small satellite capable of conducting scientific research regarding atmospheric water content. This paper focuses on the cross-link subsystem required to make the scientific measurements and on the power generation and distribution subsystem for the satellite. A companion paper (Cramer, et. al.) focuses on the subsystems required to send the scientific data and monitored operational conditions from the satellite to, and commands to the satellite from, a ground station. The central objective is to validate a new technique for precisely measuring water vapor profiles of clouds throughout the troposphere. This method involves the detection of 4 SHF tones sent out from the International Space Station (ISS), providing high-resolution amplitude and phase delay data.

The tropospheric reactions of toluene, acting as a model VOC, are investigated using an electron bombardment-matrix isolation system coupled with Fourier transform infrared spectroscopy. Initial experiments to produce the hydroxyl radicals used to initiate the toluene reactions via electron bombardment of water-argon mixtures are performed. The effects of electron current, water concentration, and gas flow rate are investigated. A more efficient method of initiating the toluene reactions, by directly creating benzyl radicals through electron bombardment of toluene is then investigated, and the effects of toluene concentration and electron current on the production of the benzyl radicals is quantified. Benzyl radicals are successfully produced, and identified via FT-IR. The next step is the formation of benzylperoxy radicals, via electron bombardment of toluene-oxygen-argon gas mixtures. Experiments are performed using increasing concentrations of toluene and oxygen, in an attempt to observe the benzylperoxy radical. Two new absorptions are observed in the infrared spectra and are tentatively identified as due to the peroxy group on the benzylperoxy radical. Computational work is also performed to confirm that benzylperoxy radicals can in fact be produced from benzyl radicals and oxygen. The vibrational frequencies of the benzylperoxy radical are also calculated, and used to confirm the possibility that the new absorptions seen in the infrared spectra could in fact be due to benzylperoxy radicals. The overall results from this work demonstrate that it is likely to be possible to use electron bombardment-matrix isolation systems to investigate tropospheric reactions of volatile organics, and that further experiments could be enhanced by structural modifications to the system. / Thesis (Master, Chemistry) -- Queen's University, 2013-11-26 15:57:59.4

Carbon monoxide (CO) is present in the troposphere as a product of fossil fuel combustion, biomass burning and the oxidation of volatile hydrocarbons. It is the principal sink of the hydroxyl radical (OH), thereby affecting the concentrations of greenhouse gases such as CH4 and O3. Consequently, CO has an atmospheric lifetime of 1-3 months, making it a good tracer for studying the long range transport of pollution. Satellite observations present a valuable tool to investigate tropospheric CO. The Atmospheric InfraRed Sounder (AIRS), onboard the Aqua satellite, is sensitive to tropospheric CO in ~50 of its 2378 channels. This sensitivity to CO, combined with the daily global coverage provided by AIRS, makes AIRS a potentially useful instrument for observing CO sources and transport. An optimal estimation retrieval scheme has been developed for AIRS, to provide CO profiles from near-surface altitudes to 150 hPa. Through a validation study, using CO profiles from in-situ aircraft measurements, this retrieval scheme has been shown to provide CO observations with strong correlations to in situ measurements. Compared to the operational AIRS v4 CO product this retrieval scheme is shown to provide total column CO retrievals with a reduced bias relative to the in situ measurements (~ -10% to ~ -1%). In addition, the optimal estimation retrieval is shown to provide improved estimation and characterization of the retrieval errors. Further validation work has been carried out through comparison with the established CO observations from the MOPITT instrument, onboard the Terra satellite. Good agreement (correlation coefficient > 0.9, and bias < 1.0 ppbv) between the instruments is observed in the mid-troposphere. At this level, the optimal estimation scheme is shown to remove a positive bias of ~10 ppbv, relative to MOPITT, that is present in the AIRS v4 CO product. The AIRS instrument is also shown to be less sensitive to CO in the lower troposphere than MOPITT. AIRS is also demonstrated to provide fewer pieces of independent information about the vertical structure of CO at tropical latitudes, where higher thermal contrast increases the sensitivity of MOPITT. Through time series analysis, the capability of AIRS to detect seasonal trends in CO is demonstrated. The potential of AIRS to be used to track, both horizontal and vertical, CO transport is explored. AIRS is shown to be capable of tracking horizontal transport, and to have potential to track vertical transport when combined with another satellite sensor.

Atmospheric formaldehyde (H2CO) is an intermediate product common to the degradation of many volatile organic compounds and therefore it is a central component of the tropospheric chemistry. While the global formaldehyde background is due to methane oxidation, emissions of non-methane volatile organic compounds (NMVOCs) from biogenic, biomass burning and anthropogenic continental sources result in important and localised enhancements of the H2CO concentration. Recent spaceborne nadir sensors provide an opportunity to quantify the abundance of tropospheric formaldehyde at the global scale, and thereby to improve our knowledge of NMVOC emissions. This is essential for a better understanding of the processes that control the production and the evolution of tropospheric ozone, a key actor in air quality and climate change, but also of the hydroxyl radical OH, the main cleansing agent of our troposphere. For this reason, H2CO satellite observations are increasingly used in combination with tropospheric chemistry transport models to constrain NMVOC emission inventories in so-called top-down inversion approaches. Such inverse modelling applications require well characterised satellite data products consistently retrieved over long time periods. This work reports on global observations of formaldehyde columns retrieved from the successive solar backscatter nadir sensors GOME, SCIAMACHY and GOME-2, respectively launched in 1995, 2002 and 2006. The retrieval procedure is based on the differential optical absorption spectroscopy technique (DOAS). Formaldehyde concentrations integrated along the mean atmospheric optical path are derived from the recorded spectra in the UV region, and further converted to vertical columns by means of calculated air mass factors. These are obtained from radiative transfer simulations, accounting for cloud coverage, surface properties and best-guess H2CO profiles, the latter being derived from the IMAGES chemistry transport model. A key task of the thesis has consisted in the optimisation of the H2CO retrieval settings from multiple sensors, taking into account the instrumental specificities of each sounder. As a result of these efforts, a homogeneous dataset of formaldehyde columns covering the period from 1996 to 2010 has been created. This comes with a comprehensive error budget that treats errors related to the spectral fit of the columns as well as those associated to the air mass factor evaluation. The time series of the GOME, SCIAMACHY and GOME-2 H2CO observations is shown to be consistent and stable over time. In addition, GOME-2 brings a significant reduction of the noise on spatiotemporally averaged observations, leading to a better identification of the emission sources. Our dataset is used to study the regional formaldehyde distribution, as well as its seasonal and interannual variations, principally related to temperature changes and fire events, but also to anthropogenic activities. Moreover, building on the quality of our 15-year time series, we present the first analysis of long-term changes in the H2CO columns. Positive trends, in the range of 1.5 to 4% yr-1, are found in Asia, more particularly in Eastern China and India, and are related to the known increase of anthropogenic NMVOC emissions in these regions. Finally, our dataset has been extensively used in several studies, in particular by the BIRA-IASB modelling team to constrain NMVOC emission fluxes. The results demonstrate the high potential of satellite data as top-down constraint for biogenic and biomass burning NMVOC emission inventories, especially in Tropical ecosystems, in Southeastern Asia, and in Southeastern US. / Le formaldéhyde (H2CO) joue un rôle central dans la chimie de la troposphère en tant que produit intermédiaire commun à la dégradation chimique de la plupart des composés organiques volatils dans l’atmosphère. L’oxydation du méthane est responsable de plus de la moitié de la concentration moyenne globale du formaldéhyde. Sur les continents en revanche, les hydrocarbures non-méthaniques (NMVOCs) émis par la végétation, les feux de biomasse et les activités humaines, augmentent de façon significative et localisée la concentration de H2CO. Les récents senseurs satellitaires à visée nadir offrent la possibilité de quantifier à l’échelle globale l’abondance du formaldéhyde dans la troposphère et de ce fait, d’améliorer notre connaissance des émissions de NMVOCs. Ceci est essentiel à la compréhension des mécanismes contrôlant la production et l’évolution de l’ozone troposphérique, élément clé pour la qualité de l’air et les changements climatiques, mais aussi du composé hydroxyle OH, le principal agent nettoyant de notre troposphère. C’est pourquoi, une méthode de plus en plus répandue pour améliorer les inventaires d’émissions des NMVOCs consiste en l’utilisation d’observations satellitaires de H2CO en combinaison avec un modèle de chimie et de transport troposphérique, dans une approche appelée modélisation inverse. Ce genre d’application demande des produits satellitaires bien caractérisés et dérivés de façon cohérente sur de longues périodes de temps. Le travail présenté dans ce manuscrit porte sur l’inversion des colonnes de formaldéhyde à partir de spectres de la radiation solaire rétrodiffusée par l’atmosphère terrestre, mesurés par les senseurs GOME, SCIAMACHY et GOME-2, lancés successivement en 1995, 2002 et 2006. La méthode d’inversion est basée sur la spectroscopie d’absorption optique différentielle (DOAS). Les concentrations de formaldéhyde intégrées le long du chemin optique moyen dans l’atmosphère sont dérivées à partir des spectres mesurés, et ensuite transformées en colonnes verticales par le biais de facteurs de conversion appelés facteurs de masse d’air. Ces derniers sont calculés à l’aide d’un modèle de transfert radiatif, en tenant compte de la présence de nuages, des propriétés de la surface terrestre et la distribution verticale supposée du formaldéhyde, fournie par le modèle IMAGES. Un des objectifs principaux de la thèse a été d’optimiser les paramètres d’inversion pour H2CO, et ceci pour les trois senseurs, tout en tenant compte des spécificités de chaque instrument. Ces efforts ont conduit à la création d’un jeu de données homogène, couvrant la période de 1996 à 2010. Les colonnes sont fournies avec un bilan d’erreur complet, incluant les erreurs liées à l’inversion des concentrations dans les spectres, ainsi que celles provenant de l’évaluation des facteurs de masse d’air. La série temporelle des observations de GOME, SCIAMACHY et GOME-2 présente une bonne cohérence et stabilité sur toute la période. Nous montrons aussi que la meilleure couverture terrestre de GOME-2 entraîne une réduction significative du bruit sur les observations moyennées, permettant une meilleure identification des sources d’émission. Notre jeu de données est exploité pour étudier la distribution régionale du formaldéhyde, ainsi que ses variations saisonnières et interannuelles, principalement liées aux variations de température et aux feux de végétation, mais aussi aux activités anthropiques. De plus, en s’appuyant sur la qualité de la série temporelle de 15 ans, nous présentons la première analyse des variations à long terme des concentrations de H2CO. Des tendances positives, de l’ordre de 1.5 à 4% par an, sont observées en Asie, en particulier dans l’est de la Chine et en Inde, liées à l’augmentation des émissions anthropiques d’hydrocarbures dans ces régions. Finalement, nos données ont été largement exploitées par le groupe de modélisation de l’IASB pour faire des études de modélisation inverse des émissions de NMVOCs. Les résultats démontrent le haut potentiel des données satellitaires pour contraindre les inventaires d’émissions dues à la végétation et aux feux de biomasse, particulièrement dans les écosystèmes tropicaux, en Asie du sud-est, et dans le sud-est des Etats-Unis.

Recent observational and modeling studies indicate a robust dynamical coupling between the stratosphere and troposphere during boreal winter. This coupling occurs in association with the Northern Annular Mode (NAM), which itself accounts for a significant fraction of the variability of the extratropical circulation. While monthly NAM dynamics have been studied previously, the mechanisms that give rise to NAM variability on short intraseasonal timescale are still unclear. We perform regression analyses, case studies, and composites based on periods of dynamical growth/decay to investigate the roles of the different proposed mechanisms in driving the atmospheric variability observed in association with the NAM on short intraseasonal timescales. More specifically, lag-regression analyses are used to identify the mean canonical structures present during the evolution of a typical NAM event. Illustrative case studies of robust stratospheric NAM events but with different tropospheric signals are contrasted in order to identify the underlying dynamical reasons for the observed differences. Finally, composite analyses of NAM tendencies are performed to isolate the structural and dynamical evolution of NAM events. Zonal-mean and three-dimensional eddy-flux diagnoses are used to examine the role of eddy-mean flow interaction in driving the wind tendencies characteristic of the NAM. In particular, Plumb flux analyses are employed to quantify the contribution of regional stationary wave anomalies toward the zonal mean wind tendency field. Potential vorticity inversions are also used to determine the role of stratospheric anomalies in inducing tropospheric circulations. The case study analyses indicate that preexisting tropospheric PV anomalies can mask the downward penetration of an initial stratospheric NAM signal into the troposphere. PV inversions further suggest that a minimum requirement for a direct downward stratospheric influence is that the stratospheric NAM signal be robust in the lower stratosphere. The dynamical composites show a remarkable degree of reverse symmetry between the zonal-mean dynamical evolution of positive and negative NAM events. Anomalous Eliassen-Palm fluxes are observed in the troposphere and stratosphere, consistent with index of refraction considerations and an indirect downward influence of the stratosphere on the troposphere. The patterns of anomalous wave driving, primarily due to low-frequency planetary scale waves, provide the main forcing of the zonal mean wind tendency field. Regional wave activity fluxes indicate that the wave driving pattern represents the manifestation of planetary scale anomalies over the North Atlantic.