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1

Tarbuck, Teresa Lynn. "Vibrational sum-frequency spectroscopic investigations of small tropospheric aerosol molecules at vapor/water interfaces /." view abstract or download file of text, 2006. http://proquest.umi.com/pqdweb?did=1188876901&sid=6&Fmt=2&clientId=11238&RQT=309&VName=PQD.

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Thesis (Ph. D.)--University of Oregon, 2006.
Typescript. Includes vita and abstract. Includes bibliographical references (leaves 172-186). Also available for download via the World Wide Web; free to University of Oregon users.
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2

Rawle, Christopher B., and n/a. "Coherent multiwavelength sources for tropospheric aerosol lidar." University of Otago. Department of Physics, 2005. http://adt.otago.ac.nz./public/adt-NZDU20070427.114533.

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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.
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3

Gao, Song. "Laboratory studies and field measurements of organic compounds in tropospheric aerosols /." Thesis, Connect to this title online; UW restricted, 2002. http://hdl.handle.net/1773/8579.

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4

Choi, Sungyeon. "Investigation of tropospheric bro using space-based total column bro measurements." Diss., Georgia Institute of Technology, 2012. http://hdl.handle.net/1853/43682.

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We derive tropospheric column BrO during the ARCTAS and ARCPAC field campaigns in spring 2008 using retrievals of total column BrO from the satellite UV nadir sensors OMI and GOME-2 using a radiative transfer model and stratospheric column BrO from a photochemical simulation. We conduct a comprehensive comparison of satellite-derived tropospheric BrO column to aircraft in-situ observations of BrO and related species. The aircraft profiles reveal that tropospheric BrO, when present during April 2008, was distributed over a broad range of altitudes rather than being confined to the planetary boundary layer (PBL). Perturbations to the total column resulting from tropospheric BrO are the same magnitude as perturbations due to longitudinal variations in the stratospheric component, so proper accounting of the stratospheric signal is essential for accurate determination of satellite-derived tropospheric BrO. We find reasonably good agreement between satellite-derived tropospheric BrO and columns found using aircraft in-situ BrO profiles, particularly when satellite radiances were obtained over bright surfaces (albedo >0.7), for solar zenith angle <80 degree and clear sky conditions. The rapid activation of BrO due to surface processes (the bromine explosion) is apparent in both the OMI and GOME-2 based tropospheric columns. The wide orbital swath of OMI allows examination of the evolution of tropospheric BrO on about hourly time intervals near the pole. Low surface pressure, strong wind, and high PBL height are associated with an observed BrO activation event, supporting the notion of bromine activation by high winds over snow. We also provide monthly climatological maps of free tropospheric BrO volume mixing ratio (VMR) derived using the so-called cloud slicing technique. In this approach, the derived slope of the total column BrO versus cloud pressure is proportional to free tropospheric BrO VMR. Estimated BrO VMR shows a minimum in the tropics and greater values at higher latitudes in both hemispheres. High tropospheric BrO VMR at high latitudes in spring could be influenced by near-surface bromine activation.
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5

Carpenter, Lucy J. "Measurements of peroxy radicals in clean and polluted atmospheres." Thesis, University of East Anglia, 1996. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.317982.

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6

Rinehart, Lynn Rebecca. "The origin of polar organic compounds in ambient fine particulate matter." abstract and full text PDF (free order & download UNR users only), 2005. http://0-gateway.proquest.com.innopac.library.unr.edu/openurl?url_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:dissertation&res_dat=xri:pqdiss&rft_dat=xri:pqdiss:3210293.

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7

Price, Heather Umbehocker. "Photochemical processing of long range transported Eurasian pollution in the Northeast Pacific troposphere /." Thesis, Connect to this title online; UW restricted, 2004. http://hdl.handle.net/1773/8645.

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8

Boer, Gregory Jon. "Investigation of high spectral resolution signatures and radiative forcing of tropospheric aerosol in the thermal infrared." Diss., Georgia Institute of Technology, 2010. http://hdl.handle.net/1853/34001.

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An investigation of the high spectral resolution signatures and radiative forcing of tropospheric aerosol in the thermal infrared was conducted. To do so and to support advanced modeling of optical properties, a high spectral resolution library of atmospheric aerosol optical constants was developed. This library includes new optical constants of sulfate-nitrate-ammonium aqueous solutions and the collection of a broad range of existing optical constants for aerosol components, particularly mineral optical constants. The mineral optical constants were used to model and study infrared dust optical signatures as a function of composition, size, shape and mixing state. In particular, spherical and non-spherical optical models of dust particles were examined and compared to high spectral resolution laboratory extinction measurements. Then the performance of some of the most common effective medium approximations for internal mixtures was examined by modeling the optical constants of the newly determined sulfate-nitrate-ammonium mixtures. The optical signature analysis was applied to airborne and satellite high spectral resolution thermal infrared radiance data impacted by Saharan dust events. A new technique to retrieve dust microphysical properties from the dust spectral signature was developed and compared to a standard technique. The microphysics retrieved from this new technique and from a standard technique were then used to investigate the effects of dust on radiative forcing and cooling rates in the thermal IR.
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9

Liu, Jiumeng. "Chemical and optical properties of organic aerosols in the atmosphere over continental US: formation, partitioning, and light absorption." Diss., Georgia Institute of Technology, 2013. http://hdl.handle.net/1853/50370.

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The chemical and optical properties of particulate organic compounds remain unclear, which leaves large uncertainties in the estimation of global radiative transfer balance. Gas and find particle (PM2.5) phase formic acid concentrations were measured with online instrumentation during separate one-month studies in the summer of 2010 in Los Angeles (LA), CA, and Atlanta, GA, and the gas-particle partitioning behavior was investigated and compared with that of water-soluble organic compounds (WSOC). The diurnal profiles clearly indicated that the photochemistry production serves as a strong source for the formation of organics, while the correlation between the gas and particle phase suggested that another partitioning route, the aqueous reactions, is also very important. Later, the optical properties of light-absorbing organic compounds were examined. Little is known about the optical importance of light absorbing particulate organic compounds (brown carbon), especially its extent and absorption relative to black carbon throughout the tropospheric column. Mie theory was applied to size-resolved spectrophotometric absorption measurements of methanol and water-extracts from cascade impactor substrates collected at three surface sites around Atlanta, GA, including both urban and rural. These results were applied to similar measurements of brown carbon in extracts from aircraft bulk filter samples collected over central USA. At the surface sites predicted light absorption by brown carbon relative to total absorption (brown carbon plus pure black carbon) was about 10% and 30% at 350 nm, versus 1 and 11% at 450 nm, for water and methanol extracts, respectively. The relative contribution of brown carbon was greater in the free troposphere and significantly increased with altitude. Although this approach has limitations, it demonstrates the ubiquity and significant potential contribution of brown carbon.
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10

Hains, Jennifer Carrie. "A chemical climatology of lower tropospheric trace gases and aerosols over the Mid-Atlantic region." College Park, Md. : University of Maryland, 2007. http://hdl.handle.net/1903/6784.

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Thesis (Ph. D.)--University of Maryland, College Park, 2007.
Thesis research directed by: Chemistry. Title from t.p. of PDF. Includes bibliographical references. Published by UMI Dissertation Services, Ann Arbor, Mich. Also available in paper.
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11

Chakrabarty, Rajan Kumar. "Characterization of size, morphology and fractal properties of aerosols emitted from spark ignition engines and from the combustion of wildland fuels." abstract and full text PDF (UNR users only), 2006. http://0-gateway.proquest.com.innopac.library.unr.edu/openurl?url_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:dissertation&res_dat=xri:pqdiss&rft_dat=xri:pqdiss:1436027.

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12

Capouet, Manuel J. F. "Modeling the oxidation of alpha-pinene and the related aerosol formation in laboratory and atmospheric conditions." Doctoral thesis, Universite Libre de Bruxelles, 2005. http://hdl.handle.net/2013/ULB-DIPOT:oai:dipot.ulb.ac.be:2013/210935.

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13

Liu, Zhen. "Characterizing the photochemical environment over China." Diss., Georgia Institute of Technology, 2012. http://hdl.handle.net/1853/43668.

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The rapid rising anthropogenic emissions driven by economic growth over China documented by satellite observations and bottom-up inventories have led to severely degraded air quality, and also have been suggested to be linked to the recent upward trends of tropospheric O₃ over the regions downwind of China. Multi-scale modeling analyses facilitated by ground-level, aircraft and satellite observations have been conducted to understand the atmospheric chemistry over China. Analyses using a 1-D photochemical model constrained by measurements at Beijing in August of 2007 suggest that reactive aromatic VOCs are the major source (~75%) of peroxy acetyl nitrate (PAN). Detailed radical budget analyses reveal the very fast ROₓ (OH + HO₂ + RO₂) production, recycling and destruction driven by VOC oxidation and heterogeneous processes. Photoenhanced aerosol surface uptake of NO₂ is found to be the predominant source of nitrous acid (HONO) during daytime (~70%). 3-D regional modeling analyses of tropospheric vertical column densities of glyoxal (CHOCHO) from SCIAMACHY show that anthropogenic emissions of aromatic VOCs are substantially underestimated (by a factor of 5 - 6, regionally varied) over China. Such an underestimation is the main cause of a large missing source of CHOCHO over the region in current global models, and could also partly explain the underestimation of organic aerosols in previous modeling studies.
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14

Schmidt, Anja. "Modelling tropospheric volcanic aerosol : from aerosol microphysical processes to Earth system impacts." Thesis, University of Leeds, 2011. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.540764.

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15

Badger, C. L. "A laboratory study of the properties of tropospheric aerosol particles." Thesis, University of Cambridge, 2006. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.596243.

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This thesis describes studies of the kinetics of N2O5 hydrolysis using proxies for tropospheric aerosols, measured using an atmospheric pressure aerosol flow tube. The rate of N2O5 hydrolysis has been shown previously to depend on particle phase and water content so these physical properties were characterised in detail for some aerosols. The N2O5 hydrolysis reaction was initially studied on sulphate aerosols, specifically sulphuric acid, ammonium sulphate and ammonium bisulphate. Good agreement was found between this work and previous studies in the literature. The effect of the organic component of tropospheric aerosol on the N2O5 hydrolysis reaction was then considered. Two classes of atmospherically relevant organic species were investigated: dicarboxylic acids and polycarboxylic acids (represented by humic acid). For single-component dicarboxylic acid aerosols, uptake was found to depend on aerosol liquid water content. It was shown that the reactivity of mixed dicarboxylic acid/sulphate aerosols can be predicted based on a knowledge of the liquid water content of the single-component aerosols. The phase transitions of aerosols containing humic acid and mixtures of humic acid and ammonium sulphate were studied prior to an investigation of their chemical reactivity. Ammonium sulphate phase transitions were modified when humic acid was present. The growth of these mixed aerosols could be predicted assuming that the organic and inorganic components take up water independently. The reactivity of ammonium sulphate aerosol was significantly lowered in the presence of humic acid. The results from these experimental measurements are considered within the context of NOx chemistry in the troposphere.
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16

Piel, Claudia. "Variabilität chemischer und physikalischer Parameter des Aerosols in der antarktischen Troposphäre = Variability of chemical and physical parameters of aerosol in the Antarctic troposphere /." Bremerhaven : Alfred-Wegener-Inst. für Polar- und Meeresforschung, 2004. http://www.gbv.de/dms/bs/toc/378550012.pdf.

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17

Vandermeer, Aaron D. "Lidar measurements of tropospheric aerosol from the Lidar In-space Technology Experiment." Thesis, National Library of Canada = Bibliothèque nationale du Canada, 1999. http://www.collectionscanada.ca/obj/s4/f2/dsk3/ftp04/mq43408.pdf.

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18

Newchurch, Michael Joseph. "A comparison of stratospheric aerosol and gas experiment I (SAGE I) and umkehr ozone profiles including a search for umkehr aerosol effects." Diss., Georgia Institute of Technology, 1986. http://hdl.handle.net/1853/25798.

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19

Stachlewska, Iwona Sylwia. "Investigation of tropospheric arctic aerosol and mixed-phase clouds using airborne lidar technique." Phd thesis, Universität Potsdam, 2005. http://opus.kobv.de/ubp/volltexte/2006/698/.

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An Airborne Mobile Aerosol Lidar (AMALi) was constructed and built at Alfred-Wegener-Institute for Polar and Marine Research (AWI) in Potsdam, Germany for the lower tropospheric aerosol and cloud research under tough arctic conditions. The system was successfully used during two AWI airborne field campaigns, ASTAR 2004 and SVALEX 2005, performed in vicinity of Spitsbergen in the Arctic. The novel evaluation schemes, the Two-Stream Inversion and the Iterative Airborne Inversion, were applied to the obtained lidar data. Thereby, calculation of the particle extinction and backscatter coefficient profiles with corresponding lidar ratio profiles characteristic for the arctic air was possible. The comparison of these lidar results with the results of other in-situ and remote instrumentation (ground based Koldewey Aerosol Raman Lidar (KARL), sunphotometer, radiosounding, satellite imagery) allowed to provided clean contra polluted (Arctic Haze) characteristics of the arctic aerosols. Moreover, the data interpretation by means of the ECMWF Operational Analyses and small-scale dispersion model EULAG allowed studying the effects of the Spitsbergens orography on the aerosol load in the Planetary Boundary Layer. With respect to the cloud studies a new methodology of alternated remote AMALi measurements with the airborne in-situ cloud optical and microphysical parameters measurements was proved feasible for the low density mixed-phase cloud studies. An example of such approach during observation of the natural cloud seeding (feeder-seeder phenomenon) with ice crystals precipitating into the lower supercooled stratocumulus deck were discussed in terms of the lidar signal intensity profiles and corresponding depolarisation ratio profiles. For parts of the cloud system characterised by almost negligible multiple scattering the calculation of the particle backscatter coefficient profiles was possible using the lidar ratio information obtained from the in-situ measurements in ice-crystal cloud and water cloud.
Das Airborne Mobile Aerosol Lidar (AMALi) wurde am Alfred-Wegener-Institut für Polar- und Meeresforschung in Potsdam für die Untersuchung arktischer Aerosole und Wolken der unteren Troposphäre entwickelt und gebaut. Das AMALi wurde erfolgreich in zwei AWI Flugzeugmesskampagnen, der ASTAR 2004 und der SvalEx 2005, die in Spitzbergen in der Arktis durchgeführt wurden, eingesetzt. Zwei neue Lidar Datenauswertungsmethoden wurden implementiert: die Two-Stream Inversion und die Iterative Airborne Inversion. Damit erwies sich die Berechnung der Profile der Teilchen Rückstreu- und Extinktionskoeffizienten mit einem entsprechenden Lidar Verhältnis, das charakteristisch für arktische Luft ist, als möglich. Der Vergleich dieser Auswertungen mit den Resultaten, die mit verschiedenen Fernerkundungs- und In-situ Instrumenten gewonnen worden waren (stationäres Koldewey Aerosol Raman Lidar KARL, Sonnenphotometer, Radiosondierung und Satellitenbilder) ermöglichten die Interpretation der Lidar-Resultate und eine Charakterisierung sowohl der reinen als auch der verschmutzten Luft. Außerdem konnten die Lidardaten mit operationellen ECMWF Daten und dem kleinskaligen Dispersionsmodel EULAG verglichen werden. Dadurch konnte der Einfluss der Spitzbergener Orographie auf die Aerosolladung der Planetaren Grenzschicht untersucht werden. Für Wolkenmessungen wurde eine neue Methode der alternativen Fernerkundung mit dem AMALi und flugzeuggetragenen In-situ Messgeräten verwendet, um optische und mikrophysikalische Eigenschaften der Wolken zu bestimmen. Diese Methode wurde erfolgreich implementiert und auf Mixed-Phase Wolken geringer optischen Dicke angewendet. Ein Beispiel hier stellt das Besamen der Wolken (sogenannte Feeder-Seeder Effekt) dar, bei dem Eiskristalle in eine niedrige unterkühlte Stratokumulus fallen. Dabei konnten Lidarsignale, Intensitätsprofile und die Volumendepolarisation gemessen werden. Zusätzlich konnten in den weniger dichten Bereichen der Wolken, in denen Vielfachstreuung vernachlässigbar ist, auch Profile des Teilchen Rückstreukoeffizienten berechnet werden, wobei Lidarverhältnisse genommen wurden, die aus In-situ Messungen für Wasser- und Eiswolken ermittelt wurden.
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20

Benson, David Ryan. "Laboratory Kinetic Studies On Binary and Ternary Homogenous Nucleation Under Lower Tropospheric Conditions." Kent State University / OhioLINK, 2010. http://rave.ohiolink.edu/etdc/view?acc_num=kent1289953146.

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21

Moreau, Louis. "Direct radiative effect of aerosols in the lower troposphere based on aircraft measurements." Thesis, McGill University, 1993. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=69643.

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It is now well established that aerosols, by scattering and absorbing solar radiation, affect the terrestrial heat engine. Depending on the net relfectivity and absorptivity of the haze column and on the surface albedo, the net effect could be a cooling or a warming. But better understanding of the influence of aerosols is handicapped by lack of data and by the fact that their composition and distribution is highly variable in space and time. For the same reasons, the incorporation of aerosols in climate models is usually rudimentary.
We have in-situ measurements of the vertical profile and size distribution of aerosols ($>$0.09 $ mu$m in radius) taken over several places in eastern Canada at different times of the year. These data have been incorporated in a simple multi-layer radiative transfer model to estimate the effects of aerosols on the local radiation budget. A broad range of refractive indexes has been used and the increase of the particles size with the relative humidity is included.
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22

Zaveri, Rahul A. "Development and Evaluation of a Comprehensive Tropospheric Chemistry Model for Regional and Global Applications." Diss., Virginia Tech, 1997. http://hdl.handle.net/10919/30673.

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Accurate simulations of the global radiative impact of anthropogenic emissions must employ a tropospheric chemistry model that predicts realistic distributions of aerosols of all types. The need for a such a comprehensive yet computationally efficient tropospheric chemistry model is addressed in this research via systematic development of the various sub-models/mechanisms representing the gas-, aerosol-, and cloud-phase chemistries. The gas-phase model encompasses three tropospheric chemical regimes - background and urban, continental rural, and remote marine. The background and urban gas-phase mechanism is based on the paradigm of the Carbon Bond approach, modified for global-scale applications. The rural gas-phase chemistry includes highly condensed isoprene and a-pinene reactions. The isoprene photooxidation scheme is adapted for the present model from an available mechanism in the literature, while an a-pinene photooxidation mechanism, capable of predicting secondary organic aerosol formation, is developed for the first time from the available kinetic and product formation data. The remote marine gas- phase chemistry includes a highly condensed dimethylsulfide (DMS) photooxidation mechanism, based on a comprehensive scheme available in the literature. The proposed DMS mechanism can successfully explain the observed latitudinal variation in the ratios of methanesulfonic acid to non-sea-salt sulfate concentrations. A highly efficient dynamic aerosol growth model is developed for condensing inorganic gases. Algorithms are presented for calculating equilibrium surface concentrations over dry and wet multicomponent aerosols containing sulfate, nitrate, chloride, ammonium, and sodium. This alternative model is capable of predictions as accurate for completely dissolved aerosols, and more accurate for completely dry aerosols than some of the similar models available in the literature. For cloud processes, gas to liquid mass-transfer limitations to aqueous-phase reactions within cloud droplets are examined for all absorbing species by using the two-film model coupled with a comprehensive gas and aqueous-phase reaction mechanisms. Results indicate appreciable limitations only for the OH, HO2, and NO3 radicals. Subsequently, an accurate highly condensed aqueous-phase mechanism is derived for global-scale applications.
Ph. D.
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23

Pan, Wenwei. "The role of aerosols in the troposphere : radiative forcing, model response, and uncertainty analysis." Thesis, Massachusetts Institute of Technology, 1996. http://hdl.handle.net/1721.1/55044.

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24

Bräuer, Peter. "Extension and application of a tropospheric aqueous phase chemical mechanism (CAPRAM) for aerosol and cloud models." Doctoral thesis, Universitätsbibliothek Leipzig, 2015. http://nbn-resolving.de/urn:nbn:de:bsz:15-qucosa-183743.

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The ubiquitous abundance of organic compounds in natural and anthorpogenically influenced eco-systems has put these compounds into the focus of atmospheric research. Organic compounds have an impact on air quality, climate, and human health. Moreover, they affect particle growth, secondary organic aerosol (SOA) formation, and the global radiation budget by altering particle properties. To investigate the multiphase chemistry of organic compounds and interactions with the aqueous phase in the troposphere, modelling can provide a useful tool. The oxidation of larger organic molecules to the final product CO2 can involve a huge number of intermediate compounds and tens of thousands of reactions. Therefore, the creation of explicit mechanisms relies on automated mechanism construction. Estimation methods for the prediction of the kinetic data needed to describe the degradation of these intermediates are inevitable due to the infeasibility of an experimental determination of all necessary data. Current aqueous phase descriptions of organic chemistry lag behind the gas phase descriptions in atmospheric chemical mechanisms despite its importance for the multiphase chemistry of organic compounds. In this dissertation, the gas phase mechanism Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) has been advanced by a protocol for the description of the oxidation of organic compounds in the aqueous phase. Therefore, a database with kinetic data of 465 aqueous phase hydroxyl radical and 129 aqueous phase nitrate radical reactions with organic compounds has been compiled and evaluated. The database was used to evaluate currently available estimation methods for the prediction of aqueous phase kinetic data of reactions of organic compounds. Among the investigated methods were correlations of gas and aqueous kinetic data, kinetic data of homologous series of various compound classes, reactivity comparisons of inorganic radical oxidants, Evans-Polanyi-type correlations, and structure-activity relationships (SARs). Evans-Polanyi-type correlations have been improved for the purpose of automated mechanism self-generation of mechanisms with large organic molecules. A protocol has been designed based on SARs for hydroxyl radical reactions and the improved Evans-Polanyi-type correlations for nitrate radical reactions with organic compounds. The protocol was assessed in a series of critical sensitivity studies, where uncertainties of critical parameters were investigated. The advanced multiphase generator GECKO-A was used to generate mechanisms, which were applied in box model studies and validated against two sets of aerosol chamber experiments. Experiments differed by the initial compounds used (hexane and trimethylbenzene) and the experimental conditions (UV-C lights off/on and additional in-situ hydroxyl radical source no/yes). Reasonable to good agreement of the modelled and experimental results was achieved in these studies. Finally, GECKO-A was used to create two new CAPRAM version, where, for the first time, branchingratios for different reaction pathways were introduced and the chemistry of compounds with up to four carbon atoms has been extended. The most detailed mechanism comprises 4174 compounds and 7145 processes. Detailed investigations were performed under real tropospheric conditions in urban and remote continental environments. Model results showed significant improvements, especially in regard to the formation of organic aerosol mass. Detailed investigations of concentration-time profiles and chemical fluxes refined the current knowledge of the multiphase processing of organic compounds in the troposphere, but also pointed at current limitations of the generator protocol, the mechanisms created, and current understanding of aqueous phase processes of organic compounds
Das zahlreiche Vorkommen organischer Verbindungen in natürlichen und anthropogen beeinflussten Ökosystemen hat diese Verbindungen in den Fokus der Atmosphärenforschung gerückt. Organische Verbindungen beeinträchtigen die Luftqualität, die menschliche Gesundheit und das Klima. Weiterhin werden Partikelwachstum und -eigenschaften, sekundäre organische Partikelbildung und dadurch der globale Strahlungshaushalt durch sie beeinflusst. Um die troposphärische Multiphasenchemie organischer Verbindungen und Wechselwirkungen mit der Flüssigphase zu untersuchen, sind Modellstudien hilfreich. Die Oxidation großer organischer Moleküle führt zu einer Vielzahl an Zwischenprodukten. Der Abbau erfolgt in unzähligen Reaktionen bis hin zum Endprodukt CO2. Bei der Entwicklung expliziter Mechanismen muss deshalb für diese Verbindungen auf computergestützte, automatisierte Methoden zurückgegriffen werden. Abschätzungsmethoden für die Vorhersage kinetischer Daten zur Beschreibung des Abbaus der Zwischenprodukte sind unabdingbar, da eine experimentelle Bestimmung aller benötigten Daten nicht realisierbar ist. Die derzeitige Beschreibung der Flüssigphasenchemie unterliegt deutlich den Beschreibungen der Gasphase in atmosphärischen Chemiemechanismen trotz deren Relevanz für die Multiphasenchemie. In dieser Arbeit wurde der Gasphasenmechanismusgenerator GECKO-A (“Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere”) um ein Protokoll zur Oxidation organischer Verbindungen in der Flüssigphase erweitert. Dazu wurde eine Datenbank mit kinetischen Daten von 465 Hydroxylradikal- und 129 Nitratradikalreaktionen mit organischen Verbindungen angelegt und evaluiert. Mit Hilfe der Datenbank wurden derzeitige Abschätzungsmethoden für die Vorhersage kinetischer Daten von Flüssigphasenreaktionen organischer Verbindungen evaluiert. Die untersuchten Methoden beinhalteten Korrelationen kinetischer Daten aus Gas- und Flüssigphase, homologer Reihen verschiedener Stoffklassen, Reaktivitätsvergleiche, Evans-Polanyi-Korrelationen und Struktur-Reaktivitätsbeziehungen. Für die Mechanismusgenerierung großer organischer Moleküle wurden die Evans-Polanyi-Korrelationen in dieser Arbeit weiterentwickelt. Es wurde ein Protokol für die Mechanismusgenerierung entwickelt, das auf Struktur-Reaktivitätsbeziehungen bei Reaktionen von organischen Verbindungen mit OH-Radikalen und auf den erweiterten Evans-Polanyi-Korrelationen bei NO3-Radikalreaktionen beruht. Das Protokoll wurde umfangreich in einer Reihe von Sensitivitätsstudien getestet, um Unsicherheiten kritischer Parameter abzuschätzen. Der erweiterte Multiphasengenerator GECKO-A wurde dazu verwendet, neue Mechanismen zu generieren, die in Boxmodellstudien gegen Aerosolkammerexperimente evaluiert wurden. Die Experimentreihen unterschieden sich sowohl in der betrachteten Ausgangssubstanz (Hexan und Trimethylbenzen) und dem Experimentaufbau (ohne oder mit UV-C-Photolyse und ohne oder mit zusätzlicher partikulärer Hydroxylradikalquelle). Bei den Experimenten konnte eine zufriedenstellende bis gute Übereinstimmung der experimentellen und Modellergebnisse erreicht werden. Weiterhin wurde GECKO-A verwendet, um zwei neue CAPRAM-Versionen mit bis zu 4174 Verbindungen und 7145 Prozessen zu generieren. Erstmals wurden Verzweigungsverhältnisse in CAPRAM eingeführt. Außerdem wurde die Chemie organischer Verbindungen mit bis zu vier Kohlenstoffatomen erweitert. Umfangreiche Untersuchungen unter realistischen troposphärischen Bedingungen in urbanen und ländlichen Gebieten haben deutliche Verbesserungen der erweiterten Mechanismen besonders in Bezug auf Massenzuwachs des organischen Aerosolanteils gezeigt. Das Verständnis der organischen Multiphasenchemie konnte durch detaillierte Untersuchungen zu den Konzentrations-Zeit-Profilen und chemischen Flüssen vertieft werden, aber auch gegenwärtige Limitierungen des Generators, der erzeugten Mechanismen und unseres Verständnisses für Flüssigphasenprozesse organischer Verbindungen aufgezeigt werden
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25

Faloon, Kathleen Helen. "The development of a laboratory system to investigate the interactions of tropospheric aerosol and HOx radicals." Thesis, University of Birmingham, 2011. http://etheses.bham.ac.uk//id/eprint/2993/.

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This thesis describes the development and application of a laboratory system to investigate the loss of peroxy radicals to aerosol. The laboratory system consisted of an aerosol flow tube coupled to a custom-built PEroxy Radical Chemical Amplifier (PERCA). Aerosol was generated using an atomiser and their distribution measured using a SMPS. New values of the HO2 uptake coefficient, γ , were obtained for wet and dry sodium chloride aerosol and dry ammonium sulphate aerosol. The mass accommodation coefficient, α, was also determined for NaCl. A box model was used to determine the implications of the new uptake coefficient of HO2 loss to NaCl aerosol for tropospheric chemistry in the marine boundary layer.
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26

Schrödner, Roland. "Modeling the tropospheric multiphase aerosol-cloud processing using the 3-D chemistry transport model COSMO-MUSCAT." Doctoral thesis, Universitätsbibliothek Leipzig, 2016. http://nbn-resolving.de/urn:nbn:de:bsz:15-qucosa-199294.

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Die chemische Zusammensetzung und die physikalischen Eigenschaften von troposphärischen Gasen, Partikeln und Wolken hängen aufgrund zahlreicher Prozesse stark voneinander ab. Insbesondere chemische Multiphasenprozesse in Wolken können die physiko-chemischen Eigenschaften der Luft und troposphärischer Partikel klein- und großräumig verändern. Diese chemische Prozessierung des troposphärischen Aerosols innerhalb von Wolken beeinflusst die chemischen Umwandlungen in der Atmosphäre, die Bildung von Wolken, deren Ausdehnung und Lebensdauer, sowie die Transmissivität von einfallender und ausgehender Strahlung durch die Atmosphäre. Damit sind wolken-chemische Prozesse relevant für das Klima auf der Erde und für verschiedene Umweltaspekte. Daher ist ein umfassendes Verständnis dieser Prozesse wichtig. Die explizite Behandlung chemischer Reaktionen in der Flüssigphase stellt allerdings eine Herausforderung für atmosphärische Computermodelle dar. Detaillierte Beschreibungen der Flüssigphasenchemie werden deshalb häufig nur für Boxmodelle verwendet. Regionale Chemie-Transport-Modelle und Klimamodelle berücksichtigen diese Prozesse meist nur mit vereinfachten chemischen Mechanismen oder Parametrisierungen. Die vorliegende Arbeit hat zum Ziel, den Einfluss der chemischer Mehrphasenprozesse innerhalb von Wolken auf den Verbleib relevanter Spurengase und Partikelbestandteile mit Hilfe des state‑of‑the‑art 3D-Chemie-Transport-Modells COSMO-MUSCAT zu untersuchen. Zu diesem Zweck wurde das Model um eine detaillierte Beschreibung chemischer Prozesse in der Flüssigphase erweitert. Zusätzlich wurde das bestehende Depositionsschema verbessert, um auch die Deposition von Nebeltropfen zu berücksichtigen. Die durchgeführten Modellerweiterungen ermöglichen eine bessere Beschreibung des troposphärischen Multiphasensystems. Das erweiterte Modellsystem wurde sowohl für künstliche 2D-Bergüberströmungsszenarien als auch für reale 3D-Simulationen angewendet. Mittels Prozess- und Sensitivitätsstudien wurde der Einfluss (i) des Detailgrades der verwendeten Mechanismen zur Beschreibung der Flüssigphasenchemie, (ii) der Größenauflösung des Tropfenspektrums und (iii) der Tropfenanzahl auf die chemischen Modellergebnisse untersucht. Die Studien belegen, dass die Auswirkungen der Wolkenchemie aufgrund ihres signifikanten Einflusses auf die Oxidationskapazität in der Gas- und Flüssigphase, die Bildung von organischer und anorganischer Partikelmasse sowie die Azidität der Wolkentropfen und Partikel in regionalen Chemie-Transport-Modellen berücksichtigt werden sollten. Im Vergleich zu einer vereinfachten Beschreibung der Wolkenchemie führt die Verwendung des detaillierten chemischen Flüssigphasenmechanismus C3.0RED zu verringerten Konzentrationen wichtiger Oxidantien in der Gasphase, einer höheren Nitratmasse in der Nacht, geringeren nächtlichen pH-Werten und einer veränderten Sulfatbildung. Darüber hinaus ermöglicht eine detaillierte Wolkenchemie erst Untersuchungen zur Bildung sekundärer organischer Partikelmasse in der Flüssigphase. Die größenaufgelöste Behandlung der Flüssigphasenchemie hatte nur geringen Einfluss auf die chemischen Modellergebnisse. Schließlich wurde das erweiterte Modell für Fallstudien zur Feldmesskampagne HCCT‑2010 genutzt. Zum ersten Mal wurde dabei ein chemischer Mechanismus mit der Komplexität von C3.0RED verwendet. Die räumlichen Effekte realer Wolken z. B. auf troposphärische Oxidantien oder die Bildung anorganischer Masse wurden untersucht. Der Vergleich der Modellergebnisse mit verfügbaren Messungen hat viele Übereinstimmungen aber auch interessante Unterschiede aufgezeigt, die weiter untersucht werden müssen
In the troposphere, a vast number of interactions between gases, particles, and clouds affect their physico-chemical properties, which, therefore, highly depend on each other. Particularly, multiphase chemical processes within clouds can alter the physico-chemical properties of the gas and the particle phase from the local to the global scale. This cloud processing of the tropospheric aerosol may, therefore, affect chemical conversions in the atmosphere, the formation, extent, and lifetime of clouds, as well as the interaction of particles and clouds with incoming and outgoing radiation. Considering the relevance of these processes for Earth\'s climate and many environmental issues, a detailed understanding of the chemical processes within clouds is important. However, the treatment of aqueous phase chemical reactions in numerical models in a comprehensive and explicit manner is challenging. Therefore, detailed descriptions of aqueous chemistry are only available in box models, whereas regional chemistry transport and climate models usually treat cloud chemical processes by means of rather simplified chemical mechanisms or parameterizations. The present work aims at characterizing the influence of chemical cloud processing of the tropospheric aerosol on the fate of relevant gaseous and particulate aerosol constituents using the state-of-the-art 3‑D chemistry transport model (CTM) COSMO‑MUSCAT. For this purpose, the model was enhanced by a detailed description of aqueous phase chemical processes. In addition, the deposition schemes were improved in order to account for the deposition of cloud droplets of ground layer clouds and fogs. The conducted model enhancements provide a better insight in the tropospheric multiphase system. The extended model system was applied for an artificial mountain streaming scenario as well as for real 3‑D case studies. Process and sensitivity studies were conducted investigating the influence of (i) the detail of the used aqueous phase chemical representation, (ii) the size-resolution of the cloud droplets, and (iii) the total droplet number on the chemical model output. The studies indicated the requirement to consider chemical cloud effects in regional CTMs because of their key impacts on e.g., oxidation capacity in the gas and aqueous phase, formation of organic and inorganic particulate mass, and droplet acidity. In comparison to rather simplified aqueous phase chemical mechanisms focusing on sulfate formation, the use of the detailed aqueous phase chemistry mechanism C3.0RED leads to decreased gas phase oxidant concentrations, increased nighttime nitrate mass, decreased nighttime pH, and differences in sulfate mass. Moreover, the treatment of detailed aqueous phase chemistry enables the investigation of the formation of aqueous secondary organic aerosol mass. The consideration of size-resolved aqueous phase chemistry shows only slight effects on the chemical model output. Finally, the enhanced model was applied for case studies connected to the field experiment HCCT-2010. For the first time, an aqueous phase mechanism with the complexity of C3.0RED was applied in 3‑D chemistry transport simulations. Interesting spatial effects of real clouds on e.g., tropospheric oxidants and inorganic mass have been studied. The comparison of the model output with available measurements revealed many agreements and also interesting disagreements, which need further investigations
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27

COSTA, RENATA F. da. "Estudo das propriedades opticas dos aerossois no estado de Sao Paulo com a tecnica de Lidar Raman." reponame:Repositório Institucional do IPEN, 2010. http://repositorio.ipen.br:8080/xmlui/handle/123456789/9586.

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Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)
Dissertacao (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP
FAPESP:08/01954-0
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28

SOUZA, RENATA F. de. "Estudo do perfil vertical de aerossóis na troposfera utilizando a técnica de LIDAR." reponame:Repositório Institucional do IPEN, 2004. http://repositorio.ipen.br:8080/xmlui/handle/123456789/9294.

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Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)
Dissertacao (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares, IPEN/CNEN-SP
FAPESP:01/07304-8
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29

t'Kint, de Roodenbeke Axelle. "A novel broad-band LIDAR for the measurement of profiles of tropospheric aerosol and temperature : techniques and first profiles." Thesis, University of Cambridge, 1998. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.624815.

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30

Köllner, Franziska [Verfasser]. "Aerosol particles in the summertime Arctic lower troposphere: Chemical composition, sources, and formation / Franziska Köllner." Mainz : Universitätsbibliothek Mainz, 2020. http://d-nb.info/1204528756/34.

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31

Weigelt, Andreas. "An optical particle counter for the regular application onboard a passenger aircraft: instrument modification, characterization and results from the first year of operation." Doctoral thesis, Universitätsbibliothek Leipzig, 2015. http://nbn-resolving.de/urn:nbn:de:bsz:15-qucosa-172724.

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To understand the contribution of aerosol particles to radiative forcing and heterogeneous chemical processes in the upper troposphere and lowermost stratosphere (UT/LMS), the knowledge of the particle size distribution is mandatory. Unfortunately, measurements in the UT/LMS are costly. Research aircrafts are expensive and thus their application is limited in time and space. Satellite remote sensing measurements provide a good temporal and spatial (horizontal) coverage, but only a limited vertical resolution and currently cannot resolve the particle size distribution. Therefore, within this thesis an optical particle counter (OPC) unit was modified for the application onboard a passenger long-haul aircraft within the CARIBIC project (www.caribic-atmospheric.com). The CARIBIC OPC unit provides regular and cost-efficient particle size distribution measurements of accumulation mode particles in the UT/LMS. In April 2010, the new OPC unit was installed for the first time onboard the Lufthansa Airbus A340 600 (D-AIHE) for the measurement of the volcanic ash cloud from the Eyjafjallajökull eruption (April to May 2010). Since June 2010 the OPC unit measures on usually four intercontinental flights per month the UT/LMS particle size distribution in the particle size range 125 to 1300 nm particle diameter. As the data acquisition stores the scattering raw signal and all housekeeping data as well, during the post flight data analysis the temporal- and size channel resolution can be flexible set. Within this work the data were analyzed with 32 size channels and 300 seconds. As aircraft-borne measurements are always time-consuming, the development of the OPC unit and the analysis routine, as well as its characterization and certification took more than two thirds of the total working time of this thesis. Therefore, the analysis of the data is limited to the first year of regular measurements until May 2011. Nevertheless, this dataset is sufficient to demonstrate the scientific relevance of these measurements. To validate the OPC data, a comparison to particle size distributions measured from board research aircraft was carried out. The analysis of the volcanic ash flights in April and May 2010 showed strongly enhanced particle mass concentrations inside the plumes and agreed in some regions very well to the particle mass concentration predicted by a dispersion model. A further case study shows the occurrence of a surprising large (1000 km) and high concentrated pollution plume over eastern Asia close to Osaka (Japan). Inside the plume the highest particle number- and mass concentrations measured with the OPC unit in the analysis period were observed (except volcanic ash flights). A detailed analysis of the in parallel measured trace gasses as well as meteorological- and LIDAR data showed, the observed plume originate from biomass burning and industrial emissions in eastern China. A third case study gives a first attempt of a mass closure/validation between the particle masses derived by the CARIBIC OPC unit and the CARIBIC impactor particle samples. First statistical analyses to the vertical, meridional, and seasonal variation of the accumulation mode particle size distribution and therefrom derived parameter indicate a stratospheric vertical increasing gradient for the particle number- and mass concentration. In general in the mid-latitude LMS the concentration of accumulation mode particles was found to be on average 120% higher than in the mid-latitude UT. The mid-latitude LMS particle size distribution shows a seasonal variation with on average 120% higher concentrations during spring compared to fall. This results can be explained with general dynamics in the stratosphere (Brewer-Dobson Circulation) and in the tropopause region (stratosphere-troposphere-exchange, STE). An anti-correlation of gaseous mercury to the stratospheric particle surface area concentration (R²=0.97) indicates that most likely stratospheric aerosol particles do act as a sink for gaseous mercury. Finally, two comparisons of the OPC data to data from satellite remote sensing and a global aerosol model underline the OPC potential and the benefits of creating an in situ measured reference dataset
Um die Rolle von Aerosolpartikeln beim Strahlungsantrieb und der heterogenen chemischen Prozessen in der oberen Troposphäre und untersten Stratosphäre (OT/US) verstehen zu können, ist es unabdingbar die Partikelgrößenverteilung zu kennen. Messungen der Partikelgrößenverteilung in dieser Region sind allerdings aufwendig. Der Einsatz von Forschungsflugzeugen ist teuer und deshalb zeitlich und räumlich nur begrenzt. Satellitenmessungen bieten zwar eine gute zeitliche und räumliche (horizontal) Abdeckung, aber nur eine begrenzte vertikale Auflösung. Weiterhin können bisherige Satellitenmessungen die Partikelgrößenverteilung nicht auflösen. Im Rahmen dieser Arbeit wurde deshalb ein optischer Partikelzähler (OPC) Messeinschub für den Einsatz an Bord eines Langstrecken-Passagierflugzeugs aufgebaut (CARIBIC Projekt, www.caribic-atmospheric.com). Mit diesem Messeinschub kann regelmäßig und kosteneffizient die Partikelgrößenverteilung des Akkumulationsmodes in der OT/US gemessen werden. Im April 2010 wurde der neue OPC Einschub erstmals an Bord des Lufthansa Airbus A340-600 (D-AIHE) installiert um die Vulkanasche der Eyjafjallajökull Eruption (April bis Mai 2010) zu messen. Seit Juni 2010 misst der OPC Einschub auf durchschnittlich vier Interkontinentalflügen pro Monat die Partikelgrößenverteilung der OT/US im Größenbereich zwischen 125 und 1300 nm Partikeldurchmesser. Während des Fluges speichert die Datenerfassung alle Rohsignale ab und ermöglicht dadurch eine nutzerspezifische Datenauswertung nach dem Flug (z. B. Anzahl der Größenkanäle oder Zeitauflösung). Im Rahmen dieser Arbeit wurden die Daten mit 32 Größenkanälen und 300 Sekunden analysiert. Da fluggetragene Messungen immer sehr aufwendig sind, beanspruchte die Entwicklung des OPC Einschubs und des Analysealgorithmus, sowie die Charakterisierung und Zertifizierung mehr als zwei Drittel der Gesamtarbeitszeit dieser Arbeit. Daher ist die Analyse der Messdaten auf das erste Jahr der regulären Messungen bis Mai 2011 beschränkt. Dennoch ist dieser Datensatz geeignet um die wissenschaftliche Relevanz dieser Messungen zu demonstrieren. Um die OPC-Daten zu validieren, wurde ein Vergleich mit bisherigen OPC Messungen von Bord Forschungsflugzeugen durchgeführt. Die Analyse der Vulkanascheflüge im April und Mai 2010 zeigte in der Abluftfahne stark erhöhte Partikelmassekonzentrationen, welche in einigen Vergleichsregionen sehr gut mit der Vorhersage eines Disperionsmodells übereinstimmten. Eine weitere Fallstudie zeigt das Auftreten einer überraschend großen (1000 km) und hoch konzentrierten Abluftfahne über Ostasien nahe Osaka (Japan). In der Abluftfahne wurde die im Analysezeitraum höchste mit dem CARIBIC OPC gemessene Partikelanzahl- und Massenkonzentration beobachtet (ausgenommen Vulkanascheflüge). Eine detaillierte Analyse der parallel gemessenen Spurengase, sowie meteorologischer Daten und LIDAR Profile zeigte, dass die beobachtete Abluftfahne eine Mischung aus Biomasseverbrennungs- und Industrieabgasen aus Ost-China war. Eine dritte Fallstudie stellt einen ersten Versuch einer Massenschließung/Validierung zwischen der aus den CARIBIC OPC-Daten abgeleiteten Partikelmasse und der Partikelmasse aus CARIBIC Impaktorproben dar. Erste statistische Analysen zur vertikalen, meridionalen und saisonalen Variabilität der Partikelgrößenverteilung im Akkumulationsmode und daraus abgeleiteten Parametern zeigen einen vertikal ansteigenden Gradienten für die Partikelanzahl- und Massenkonzentration. Generell war in der US der mittleren Breiten die Konzentration von Akkumulationsmode Partikeln im Mittel um 120% höher als in der OT der mittleren Breiten. Weiterhin wurde in der US der mittleren Breiten eine jahreszeitliche Schwankung gefunden. Im Frühling war die mit dem OPC gemessene Partikelkonzentrationen im Mittel um 120% höher als im Herbst. Diese Befunde lassen sich mit der atmosphärischen Dynamik in der Stratosphäre (Brewer-Dobson Zirkulation) und in der Tropopausenregion (Stratosphäre-Troposphäre-Austauschprozesse) erklären. Eine gefundene negative Korrelation von gasförmigen Quecksilber mit der stratosphärischen Partikeloberflächenkonzentration (R²=0.97) ist ein starker Indikator dafür, dass in der US Aerosolpartikel eine Senke für gasförmiges Quecksilber darstellen. Zum Abschluss unterstreichen zwei Vergleiche der OPC-Daten mit Satellitenmessungen und Ergebnissen eines globalen Aerosolmodels das Potential und den Nutzen der CARIBIC OPC Daten als in-situ gemessenen Referenzdatensatz
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32

Seifert, Patric. "Dust-related ice formation in the troposphere: A statistical analysis based on 11 years of lidar observations of aerosols and clouds over Leipzig." Doctoral thesis, Universitätsbibliothek Leipzig, 2011. http://nbn-resolving.de/urn:nbn:de:bsz:15-qucosa-71167.

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Im Rahmen der vorliegenden Arbeit wurde der Zusammenhang zwischen heterogener Eisbildung und Temperatur auf Basis eines 11-Jahres Lidardatensatzes untersucht, wobei besonders der potenzielle Einfluss von Wüstenstaubaerosol auf die heterogene Gefriertemperatur von unterkühlten Wasserwolken überprüft wurde. Der zugrundeliegende Lidardatensatz entstand im Rahmen von zwischen 1997 und 2008 am Leibniz-Institut für Troposphärenforschung (IfT) in Leipzig durchgeführten Lidarmessungen. Mehr als 2300 zeitlich und räumlich defifinierte Wolkenschichten wurden anhand des gemessenen linearen Depolarisationsverhältnisses als Flüssigwasserwolken oder als eisbeinhaltende Wolken klassifiziert. Dazu war es nötig, den störenden Einfluss von spiegelnden Reflektionen horizontal ausgerichteter Eiskristalle auf das gemessene Depolarisationsverhältnis zu charakterisieren. Die für die Auswertung benötigten Wolkenoberkantentemperaturen wurden aus Modelldaten oder, falls zeitnah verfügbar, aus Radiosondenprofifilen ermittelt. Die statistische Auswertung des Wolkendatensatzes ergab, dass der Anteil an eisbeinhaltenden Wolken mit abnehmender Temperatur stark zunimmt. Wurde in Wolken mit Oberkantentemperaturen zwischen 0 und -5 °C in nur 1% aller Fälle Eis detektiert, enthielten zwischen -10 und -15 °C bereits 40% der in dem Temperaturbereich beobachteten Wolken Eis. Bei Wolkenoberkantentemperaturen unterhalb von -25 °C wurde in nahezu 100% aller Fälle Eis in den Wolken beobachtet. Ein ähnlicher Zusammenhang zwischen Temperatur und dem Anteil an eisbeinhaltenden Wolken wurde bereits in zahlreichen auf Flugzeugmessungen basierenden Studien gefunden. In einem weiteren Schritt wurde der Wolkendatensatz mittels drei verschiedener Ansätze in einen staubbelasteten sowie einen staubfreien Teil getrennt. Dies geschah Anhand einer Trajektorien-Clusteranalyse sowie der Trennung bezüglich der von einem Mineralstaubvorhersagemodell berechneten Mineralstaubbelastung in Wolkenhöhe beziehungsweise in der gesamten Luftsäule über Leipzig. Die Trennung ergab, dass staubbelastete Wolken im Temperaturbereich zwischen -5 und -25 °C 10-30% mehr Eis beinhalten als staubfreie Wolken. Die Ergebnisse dieser Untersuchung legen deshalb nahe, dass Mineralstaub Eisbildung in unterkühlten Wolken maßgeblich fördert. Der Vergleich des Leipziger Wolkendatensatzes mit einem auf den Kapverden gesammelten Datensatz tropischer Wolken zeigte, dass trotz vergleichbarem Einfluss von Mineralstaubaerosol Eisbildung in den Tropen erst bei um 10 K tieferen Temperaturen einsetzt. Als mögliche Einflussfaktoren wurden Unterschiede in der atmosphärischen Dynamik und die Wirkung effektiverer Eiskeime über Mitteleuropa diskutiert
The formation and presence of ice crystals in clouds strongly determines meteorological processes as precipitation formation but also climatological parameters as the radiation budget of the atmosphere. The process of ice formation, however, is not straightforward because ice crystals and liquid water droplets can coexist at temperatures from -38 °C to 0 °C. In this temperature range, aerosol particles, so-called ice nuclei, must be present to trigger ice formation in a supercooled droplet. From laboratory studies it is known that mineral dust particles are efficient ice nuclei. We present a statistical analysis of lidar-based observations of 2300 free-tropospheric clouds that was used to investigate the effect of mineral dust particles on the ice-formation temperature. The observations were performed at Leipzig, Germany (51° N, 12 °E). The time and height as well as the phase state (ice, liquid-water) of the observed clouds can easily be derived from the lidar data. The dust load in every observed cloud layer was determined by means of model data. From the analysis it was found that dust-affected clouds produce ice 50% more frequently than dust-free clouds at temperatures between -20 and -10 °C. In a last step we compared the relationship between ice-containing clouds and temperature of the Leipzig dataset with a similar data set from Cape Verde (15 °N, 23.5 °W). Even though dust is omnipresent in the troposphere at this location, the study of more than 200 spatially well-defined altocumulus clouds did not show a significant number of ice clouds at temperatures above -15 °C. Possible explanations for the observed differences between the Leipzig and the Cape Verde data set are contrasts in atmospheric dynamics over Central Europe and western Africa or the presence of anthropogenic aerosol over Europe that may provide additional effective ice nuclei besides Saharan dust
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33

Suh, Inseon. "Photochemistry of aromatic hydrocarbons: implications for ozone and secondary organic aerosol formation." Texas A&M University, 2003. http://hdl.handle.net/1969.1/3893.

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Aromatic hydrocarbons constitute an important fraction (~20%) of total volatile organic compounds (VOCs) in the urban atmosphere. A better understanding of the aromatic oxidation and its association in urban and regional ozone and organic aerosol formation is essential to assess the urban air pollution. This dissertation consists of two parts: (1) theoretical investigation of the toluene oxidation initiated by OH radical using quantum chemical and kinetic calculations to understand the mechanism of O3 and SOA precursors and (2) experimental investigation of atmospheric new particle formation from aromatic acids. Density functional theory (DFT) and ab initio multiconfigurational calculations have been performed to investigate the OH-toluene reaction. The branching ratios of OH addition to ortho, para, meta, and ipso positions are predicted to be 0.52, 0.34, 0.11, and 0.03, respectively, significantly different from a recent theoretical study of the same reaction system. Aromatic peroxy radicals arising from initial OH and subsequent O2 additions to the toluene ring are shown to cyclize to form bicyclic radicals rather than undergoing reaction with NO under atmospheric conditions.Isomerization of bicyclic radicals to more stable epoxide radicals possesses significantly higher barriers and hence has slower rates than O2 addition to form bicyclic peroxy radicals. At each OH attachment site, only one isomeric pathway via the bicyclic peroxy radical is accessible to lead to ring cleavage. Decomposition of the bicyclic alkoxy radicals leads primarily to formation of glyoxal and methyl glyoxal along with other dicarbonyl compounds. Atmospheric aerosols often contain a considerable fraction of organic matter, but the role of organic compounds in new nanometer-sized particle formation is highly uncertain. Laboratory experiments show that nucleation of sulfuric acid is considerably enhanced in the presence of aromatic acids. Theoretical calculations identify the formation of an unusually stable aromatic acid-sulfuric acid complex, which likely leads to a reduced nucleation barrier. The results imply that the interaction between organic and sulfuric acids promotes efficient formation of organic and sulfate aerosols in the polluted atmosphere because of emissions from burning of fossil fuels, which strongly impact human health and global climate.
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34

Ricketts, Hugo Michael Anthony. "A lidar system to measure aerosol and ozone profiles in the atmospheric boundary layer and free troposphere." Thesis, University of Manchester, 2009. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.509406.

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35

Dadashazar, Hossein, Rachel A. Braun, Ewan Crosbie, Patrick Y. Chuang, Roy K. Woods, Haflidi H. Jonsson, and Armin Sorooshian. "Aerosol characteristics in the entrainment interface layer in relation to the marine boundary layer and free troposphere." COPERNICUS GESELLSCHAFT MBH, 2018. http://hdl.handle.net/10150/627046.

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This study uses airborne data from two field campaigns off the California coast to characterize aerosol size distribution characteristics in the entrainment interface layer (EIL), a thin and turbulent layer above marine stratocumulus cloud tops, which separates the stratocumulus-topped boundary layer (STBL) from the free troposphere (FT). The vertical bounds of the EIL are defined in this work based on considerations of buoyancy and turbulence using thermodynamic and dynamic data. Aerosol number concentrations are examined from three different probes with varying particle diameter (Dp) ranges: > 3 nm, > 10 nm, and 0.11–3.4 µm. Relative to the EIL and FT layers, the sub-cloud (SUB) layer exhibited lower aerosol number concentrations and higher surface area concentrations. High particle number concentrations between 3 and 10 nm in the EIL are indicative of enhanced nucleation, assisted by high actinic fluxes, cool and moist air, and much lower surface area concentrations than the STBL. Slopes of number concentration versus altitude in the EIL were correlated with the particle number concentration difference between the SUB and lower FT layers. The EIL aerosol size distribution was influenced by varying degrees from STBL aerosol versus subsiding FT aerosol depending on the case examined. These results emphasize the important role of the EIL in influencing nucleation and aerosol–cloud–climate interactions.
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36

Bräuer, Peter [Verfasser], Hartmut [Akademischer Betreuer] Herrmann, and Bernard [Gutachter] Aumont. "Extension and application of a tropospheric aqueous phase chemical mechanism (CAPRAM) for aerosol and cloud models / Peter Bräuer ; Gutachter: Bernard Aumont ; Betreuer: Hartmut Herrmann." Leipzig : Universitätsbibliothek Leipzig, 2015. http://d-nb.info/1239659903/34.

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37

RODRIGUES, PATRICIA F. "Avaliação da higroscopicidade de aerossóis urbanos pela técnica LIDAR Raman." reponame:Repositório Institucional do IPEN, 2014. http://repositorio.ipen.br:8080/xmlui/handle/123456789/23498.

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Submitted by Maria Eneide de Souza Araujo (mearaujo@ipen.br) on 2015-02-24T19:21:41Z No. of bitstreams: 0
Made available in DSpace on 2015-02-24T19:21:41Z (GMT). No. of bitstreams: 0
Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)
Tese (Doutorado em Tecnologia Nuclear)
IPEN/T
Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP
FAPESP:09/14758-7
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38

Schrödner, Roland [Verfasser], Eberhard [Akademischer Betreuer] Renner, Eberhard [Gutachter] Renner, Ralf [Akademischer Betreuer] Wolke, Andreas [Akademischer Betreuer] Tilgner, and Nadine [Gutachter] Chaumerliac. "Modeling the tropospheric multiphase aerosol-cloud processing using the 3-D chemistry transport model COSMO-MUSCAT / Roland Schrödner ; Gutachter: Eberhard Renner, Nadine Chaumerliac ; Eberhard Renner, Ralf Wolke, Andreas Tilgner." Leipzig : Universitätsbibliothek Leipzig, 2016. http://d-nb.info/1240398093/34.

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39

Farah, Antoine. "Analysis of the physical and chemical properties of atmospheric aerosol at the Puy de Dôme station." Thesis, Université Clermont Auvergne‎ (2017-2020), 2018. http://www.theses.fr/2018CLFAC049/document.

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Les particules d'aérosol sont importantes en raison de leurs impacts directs et indirects sur le climat. Dans la couche limite (CL), ces particules ont une durée de vie relativement courte en raison de leur élimination fréquente par dépôt humide. En revanche, lorsque les aérosols sont transportés dans la troposphère libre (TL), leur durée de vie dans l'atmosphère augmente de manière significative, ce qui les rend représentatifs de vastes zones spatiales. Dans le cadre de ces travaux de thèse, nous avons utilisé une combinaison de mesures in situ effectuées à la station PUY (Puy de Dôme, 45 ° 46 'N, 2 ° 57'E, 1465 m d'altitude), ainsi que des profils LIDAR obtenus depuis Clermont-Ferrand pour identifier les conditions de TL et caractériser davantage les propriétés physiques et chimiques des aérosols dans cette zone de l'atmosphère peu documentée. Dans un premier temps, une combinaison de quatre critères a été utilisée pour déterminer le positionnement de la station PUY en TL ou en CL. Les résultats montrent que la station est située en CL avec des fréquences allant de 50% en hiver à 97% en été. Cette classification a ensuite été utilisée pour évaluer, sur un an de mesures, les différences qui existent entre la TL et la CL en termes de caractéristiques physique (distribution en taille) et chimique (fraction non réfractaire) de l’aérosol, et vis-à-vis des concentrations en carbone suie (BC). Sur la base de cette ségrégation, nous avons observé pour la plupart des saisons que les concentrations en particules des modes Aitken et accumulation ainsi que la concentration en BC sont plus élevées dans la CL que dans la TL. Cette observation est cohérente avec le fait que la majorité des sources d’aérosol sont situées dans la CL. Au contraire, des concentrations plus élevées en particules dans les modes Aitken et accumulation (notamment organiques) et en BC sont observées en TL au printemps. Ces aérosols organiques ont été identifiés comme étant âgés / moins âgés ; ils coïncident avec la présence de fortes concentrations en sulfate et en BC et sont probablement originaires de processus de combustion de biomasse, à la suite desquels ils sont directement injectés en TL sous l’effet d’une convection thermique intense. Aucune différence significative entre les concentrations de CL et de TL n'a été observée pour les particules du mode nucléation, et ce quelle que soit la saison, ce qui suggère une source supplémentaire continue de particules du mode nucléation dans la TL en hiver et en automne. Les concentrations en particules du mode grossier sont en revanche plus élevées dans la TL que dans la CL pour toutes les saisons, et en particulier en été. Cela indique un transport longue distance efficace des grosses particules dans la TL depuis des sources lointaines (marines et désertiques), probablement favorisé par les vitesses de vent accrues dans la TL par rapport à la CL. Nous avons ensuite calculé les rétro-trajectoires des masses d'air que nous avons combinées aux estimations de hauteur de couche limite du modèle ECMWF ERA-Interim pour estimer le temps passé par les masses d’air dans la TL depuis leur dernier contact avec la CL, et pour évaluer l'impact de ce paramètre sur les propriétés des aérosols. Nous avons observé que même après 75 heures sans aucun contact avec la CL, les aérosols de la TL conservent les propriétés spécifiques du type de masse d'air auquel ils appartiennent. Ce manuscrit présente également une étude des mesures simultanées au PUY et à une station urbaine à basse altitude, AtmoAura. Les résultats montrent que lorsque le PUY est en TL, les concentrations des PM1 (particules de diamètre inférieur à 1 µm) sont plus faibles au PUY qu’à AtmoAura, ce qui confirme notre classification. Lorsque le PUY est en CL, la composition en aérosol est similaire pour les deux sites, ce qui a permis de quantifier la contribution de la pollution urbaine locale issue de la ville de Clermont-Ferrand
Aerosol particles are important due to their direct and indirect impacts on climate. Within the planetary boundary layer (BL), these particles have a relatively short lifetime due to their frequent removal process by wet deposition. When aerosols are transported into the free troposphere (FT), their atmospheric lifetime increases significantly, making them representative of large spatial areas. In this work, we use a combination of in situ measurements performed at the high altitude PUY (Puy de Dôme, 45°46’ N, 2°57’E, 1465 m asl) station, together with LIDAR profiles at Clermont-Ferrand for characterizing FT conditions, and further characterize the physical and chemical properties of aerosol in this poorly documented area of the atmosphere. First, a combination of four criteria was used to identify whether the PUY station lies within the FT or within the BL. Results show that the PUY station is located in BL with frequencies ranging from 50% during the winter, up to 97% during the summer. Then, the classification is applied to a year-long dataset of particle size distribution and NR-PM1 data’s to study the differences in particle physical and chemical characteristics and BC concentrations between the FT and the BL. Based on this segregation, we observed higher concentrations in the BL compared to FT for BC, Aitken and accumulation mode particle concentrations for most seasons, as expected from larger sources originating from the surface. However, BC, Aitken mode, accumulation mode and organic aerosols concentrations were higher in the FT compared to BL during spring. These organic aerosols were identified as aged/less aged, and were correlated with sulphate and BC and we suspect that the higher concentrations of particles observed in the FT compared to BL during spring originate from direct injection of BB aerosols in the FT through strong heat convection. No significant difference between the BL and the FT concentrations was observed for the nucleation mode particles for all seasons, suggesting a continuous additional source of nucleation mode particles in the FT during winter and autumn. Coarse mode particle concentrations were found higher in the FT than in the BL for all seasons and especially during summer. This indicates an efficient long-range transport of large particles in the FT from distant sources (marine and desert) due to higher wind speeds in the FT compared to BL. For FT air masses, we used 204-h air mass back-trajectories combined with boundary layer height estimations from ECMWF ERA-Interim to assess the time they spent in the FT since their last contact with the BL and to evaluate the impact of this parameter on the aerosol properties. We observed that even after 75 h without any contact with the BL, FT aerosols preserve specific properties of their air mass type. This manuscript is also presenting a study of simultaneous measurements at PUY and an urban low altitude station AtmoAura. Results show that when the PUY is influenced by FT air masses, the PM1 species are lower at the PUY compared to AtmoAura confirming our classification. When the PUY is predicted to lay within the BL, the aerosol composition was similar among the two sites for several species, which allowed for a quantification of the local urban pollution contribution for the species enhanced within the city of Clermont-Ferrand
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40

Leitão, Alexandre Joana [Verfasser], John P. [Akademischer Betreuer] Burrows, and Otto [Akademischer Betreuer] Schrems. "The relevance of aerosol in the retrieval of tropospheric NO2 from satellite - a study of model data applicability / Joana Leitão Alexandre. Gutachter: John P. Burrows ; Otto Schrems. Betreuer: John P. Burrows." Bremen : Staats- und Universitätsbibliothek Bremen, 2011. http://d-nb.info/1071898558/34.

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41

Schmale, Julia Yvonne [Verfasser]. "Aircraft-based in-situ aerosol mass spectrometry: Chemical characterization and source identification of submicron particulate matter in the free and upper troposphere and lower stratosphere / Julia Yvonne Schmale." Mainz : Universitätsbibliothek Mainz, 2011. http://d-nb.info/1031800891/34.

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42

Chauvigné, Aurélien. "Impact radiatif des aérosols de haute altitude." Thesis, Clermont-Ferrand 2, 2016. http://www.theses.fr/2016CLF22757/document.

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La présence des particules d’aérosols dans l’atmosphère influencent le bilan radiatif de notre planète et ainsi son équilibre climatique. Selon les différents mécanismes d’émission et processus de transports atmosphériques, les aérosols peuvent être entrainés dans la troposphère libre et ainsi y résider pendant plusieurs semaines. Les contributions optiques et radiatives des aérosols de troposphère libre par rapport à celles de la colonne atmosphérique sont encore mal évaluées du fait de la difficulté d’accès et du manque de mesures sur de longues périodes. Ces travaux de thèse se sont donc appuyés sur deux sites d’altitude présentant des topographies adéquates pour l’analyse des aérosols de troposphère libre : le site ACTRIS/GAW du puy de Dôme (PUY, 1 465 m, France) et le site ACTRIS/GAW de Chacaltaya (CHC, 5 240 m, Bolivie). Ces deux sites disposent d’un large jeu de données in-situ et de télédétection. Les résultats montrent ainsi l’importance de la prise en compte de la structure verticale de l’atmosphère et de l’effet de l’humidité sur les propriétés des aérosols dans l’analyse des mesures. Pour la première fois à notre connaissance, l’utilisation de ces techniques instrumentales depuis la station de mesures météorologiques la plus haute du monde (Chacaltaya) a permis d’établir les propriétés optiques des aérosols dans cette région largement influencée par la ville de La Paz et par les émissions de la forêt amazonienne. Les résultats montrent que l’influence des feux de forêt amazoniens à la fin de la saison sèche peut accroitre les propriétés optiques de l’aérosol à cette altitude d’un facteur de 3,5 en moyenne et celles de la troposphère libre de 28 à 80%. La station est d’ailleurs régulièrement influencée par les conditions de la troposphère libre (30% du temps en journée et 60% la nuit). Ce manuscrit présente également des méthodes originales pour la détermination des contributions optiques et radiatives des aérosols de troposphère libre avec l’utilisation conjointe des mesures in-situ, photométriques et LIDAR. Les résultats établissent ainsi des contributions optiques de la troposphère libre au-dessus du puy de Dôme variant de 20%en hiver à 80% en été en moyenne. L’utilisation du modèle de transfert radiatif SBDART permet d’évaluer les contributions radiatives correspondantes qui oscillent entre 13 et 40% pour les courtes longueurs d’onde, soit des forçages radiatifs de -1 W.m-2 à -10 W.m-2. Les différentes sources d’aérosols en surface influencent donc fortement la composition de la troposphère libre, qu’il est alors nécessaire de prendre en compte dans le bilan radiatif global de notre planète
Atmospheric aerosols impact the earth radiative budget and its climate. Depending on their emission mechanisms and atmospheric transport processes, aerosols can be injected into the free tropophere where their lifetime is increased to up to several weeks. Optical and radiative properties of free tropospheric aerosols are still poorly known because of the difficulties to access high altitudes over long periods of time. The present work is based on two high altitude sites measurements: the ACTRIS/GAW station of puy de Dôme (PUY, 1 465 m, France) and the ACTRIS/GAW station of Chacaltaya (CHC, 5 240 m, Bolivia). These two sites are equipped with a unique set of both in-situ and remote sensing measurements. Results first show the importance of taking into account the vertical atmospheric structure and the hygroscopic properties of aerosols when combining in situ and remote sensing measurements. Measurements from the highest atmospheric station in the world (Chacaltaya), provide for the first time to our knowledge, the aerosol optical properties from this region of the world, segregated into mixing layer aerosols and free tropospheric aerosols.The site is both influenced by anthropogenic emissions from the nearby city, La Paz and pristine emissions from the Amazonian forest. From these measurements, we observe that biomass burning emissions can increase column aerosol optical properties by an average factor of 3,5 and the free tropospheric aerosol optical properties between 28 and 80%. The station is regularly influenced by free tropospheric conditions (30% of the time during daytime and 60% during nighttime). This manuscript is also presenting original methods for retrieving the optical and radiative aerosol contributions from the free tropospheric layer to the total atmospheric column using a combination of in-situ, photometric and LIDAR measurements. Results show that free tropospheric contributions above puy de Dôme station vary from 20% during winter to 80% during summer. The use of the radiative transfer model SBDART allows to evaluate the corresponding shortwave radiative contributions of free tropospheric aerosols between 13 and 40% (between -1 and -10 W.m-2). Thus, the different surface aerosol emissions influence significantly the free tropospheric composition which is essential for radiative budget determination
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43

Seifert, Patric [Verfasser], Albert [Akademischer Betreuer] Ansmann, Jost [Gutachter] Heintzenberg, and Kenneth [Gutachter] Sassen. "Dust-related ice formation in the troposphere: A statistical analysis based on 11 years of lidar observations of aerosols and clouds over Leipzig / Patric Seifert ; Gutachter: Jost Heintzenberg, Kenneth Sassen ; Betreuer: Albert Ansmann." Leipzig : Universitätsbibliothek Leipzig, 2011. http://d-nb.info/1237894700/34.

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44

Chiang, Chih-Wei, and 江智偉. "The optical properties measurements of tropospheric Aerosols." Thesis, 2005. http://ndltd.ncl.edu.tw/handle/50414759106890934268.

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博士
國立中央大學
物理研究所
93
Dual-wavelength, depolarization, and Raman Lidar observations for the tropospheric aerosols in the height region 1-5 km, using data of 126 days for background aerosols and 40 days for special aerosols events (dust and biomass burning) during the period 2002/2-2004/5, are presented in this paper. Lidar measurements revealed the optical properties, source, transport processes, seasonal variation, and humidity effect of aerosols. Data were analyzed in conjunction with Sun-photometer, Radiosonde, Visibility, satellite image (TOMS), and trajectory studies (HYSPLIT). The larger aerosols loading occurred below 3 km and had a distinct feature of seasonal variation. The maximum and minimum aerosol optical thickness, in the height region of 1-5 km, for the spring and fall seasons respectively. There are different characteristics for various aerosols which are recognized by using depolarization Lidar. The dust aerosols events have larger depolarization ratio varied mainly between 0.12 and 0.27. The height distribution of the particles size derived from the dual-wavelength Lidar. Raman Lidar measured the results of humidity were not only coincidence with Radiosonde but also had the potential to understand the interaction of aerosols and humidity.
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45

Cziczo, Daniel J. "Laboratory studies of phase transitions in common tropospheric aerosols /." 1999. http://wwwlib.umi.com/dissertations/fullcit/9943058.

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46

Adams, Peter Jonathan. "Representing Tropospheric Aerosols and Their Climatic Effects in Global Models." Thesis, 2002. https://thesis.library.caltech.edu/6137/2/Adams_pj_2002.pdf.

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In order to better understand and quantify the direct and indirect effect of aerosols on climate, an earlier general circulation model (GCM) simulation of tropospheric sulfate has been extended by incorporating aerosol thermodynamics and microphysics. The thermodynamic simulation allows the prediction of nitrate, ammonium, and aerosol water concentrations. It is estimated that nitrate contributes as much to total aerosol mass as sulfate on regional scales in parts of Europe and North America. The direct radiative forcing associated with the sulfate-nitrate-ammonium-water mixture is estimated to be —1.14 W M^(-2) for the present day. Based on a future emissions scenario, this could increase to as much as —2.13 W^(-2) by the year 2100, an increase that results from increased nitrate concentrations. Although currently a minor contributor to aerosol direct radiative forcing, nitrate is predicted to exceed sulfate in its contribution by the end of the century for this emissions scenario. It is also found that direct radiative forcing estimates are highly sensitive to aerosol behavior at relative humidity above 90%, highlighting the shortcomings of global models in their treatment of aerosol water uptake under partly cloudy conditions. The microphysical simulation allows the prediction of tropospheric aerosol number concentrations and size distributions, key parameters in determining the indirect effect of aerosols on clouds. A two-moment sectional algorithm is used to simulate the microphysical processes of condensation/evaporation and coagulation. It has been tested by performing a simulation of sulfate microphysics. Predicted aerosol number concentrations generally agree with observations to within 25%. The microphysical simulation also reproduces key features of the tropospheric aerosol such as increasing number concentrations with altitude and land-sea contrasts in cloud condensation nuclei concentrations. It is found that there are important uncertainties in the source rates of new particles to the atmosphere, whether from in situ nucleation or emissions of particulates, that can significantly impact predicted aerosol number and cloud condensation nuclei concentrations.
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47

Liao, Hong. "Interactions between Tropospheric Chemistry and Aerosols in a Unified GCM Simulation." Thesis, 2002. https://thesis.library.caltech.edu/6370/1/Liao_h_2002.pdf.

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Anthropogenic changes in the atmospheric abundances of tropospheric ozone and aerosols make significant contributions to climate change. In turn, climate change affects the abundances of ozone and aerosols, resulting in complicated feedbacks. To move toward understanding interactions and feedbacks among tropospheric chemistry, aerosol formation, and climate change, a unified tropospheric chemistry-aerosol model is developed within the Goddard Institute for Space Studies general circulation model. The model includes a detailed simulation of tropospheric ozone-NO_x-hydrocarbon chemistry and a thermodynamic representation of sulfate/nitrate/ammonium aerosols. Two-way coupling between aerosols and chemistry provides consistent chemical fields for aerosol dynamics and aerosol mass for heterogeneous processes and calculations of gas-phase photolysis rates. Although the current version of the unified model does not include prognostic treatments of black carbon, organic carbon, and mineral dust aerosols, we include effects of these particles on photolysis and heterogeneous processes by using three-dimensional off-line fields. The unified model is applied to examine interactions between tropospheric chemistry and aerosols. This dissertation is the first step in the development of a fully-coupled climate/chemistry/aerosol model.
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48

石井, 昌憲, and Shoken Ishii. "Arctic Tropospheric Aerosols Observed by Lidar during Winter Seasons at Eureka, Canada : Optical Properties and Source Regions of Aerosol layers." Thesis, 2001. http://hdl.handle.net/2237/16338.

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Rashki, Alireza. "Seasonality and mineral, chemical and optical properties of dust storms in the Sistan region of Iran, and their influence on human health." Thesis, 2012. http://hdl.handle.net/2263/27734.

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Atmospheric aerosols are suspensions of solid and/or liquid particles in the air from natural and anthropogenic sources. Aerosols are ubiquitous in the air and are often observable as dust, smoke and haze. Dust is considered to be one of the major components of tropospheric aerosols over the globe. Natural and human processes contribute to aerosol emissions. Each year, several billion tons of soil-dust is entrained into the atmosphere playing a vital role in solar irradiance attenuation, and affects marine environments, atmospheric dynamics and weather. Air pollution has recently become a serious environmental problem. Over recent years in the public health domain particulate matter (PM) concentration has become a topic of considerable importance, since epidemiological studies have shown that exposure to particulates with aerodynamic diameters of < 10 ìm (PM10) and especially < 2.5 ìm (PM2.5) induces an increase of lung cancer, morbidity and cardiopulmonary mortality. Mineral dust plays an important role in the optical, physical and chemical processes in the atmosphere, while dust deposition adds exogenous mineral and organic material to terrestrial surfaces, having a significant impact on the Earth’s ecosystems and biogeochemical cycles. The role of dust aerosols in atmospheric processes, i.e. Earth’s radiation balance, cloud microphysics, etc, strongly depends on a variety of physico-chemical parameters, size distribution, dust sources, atmospheric lifetime and mixing processes in the atmosphere. Analysis of the physical properties and chemical composition of dust aerosols is important to determine aerosol sources, mixing processes, transport pathways and their effects on human health. Atmospheric aerosols affect the global climatic system in many ways, i.e. by attenuating the solar radiation reaching the ground, modifying the solar spectrum, re-distributing the earth-atmosphere energy budget and influencing cloud microphysics and the hydrological cycle. Satellite remote for sensing provides an important observational means for monitoring dust production and for improving the understanding of the effects of regional-scale atmospheric processes on dust emission and transport. The Sistan region is located in southeastern Iran, close to the Iranian borders with Pakistan and Afghanistan. The climate is arid, with low annual average precipitation of ~55 mm occurring mainly in the winter (December to February) and evaporation exceeding ~4000 mm.year-1. During summer (June – September), the area is under the influence of a low pressure system attributed to the Indian thermal low that extends further to the west as a consequence of the south Asian monsoon system. These low pressure conditions are the trigger for the development of the Levar northerly wind, commonly known as the “120-day wind”, causing frequent dust and sand storms and contributing to the deterioration of air quality. Therefore, one of the main factors affecting the weather conditions over the region is the strong winds rendering Sistan as one of the windiest deserts in the world. Severe droughts during the past decades, especially after 1999, have caused desiccation of the Hamoun lakes which is located in the northern part of Sistan, leaving a fine layer of sediment that is easily lifted by the wind, thus modifying the basin to one of the most active sources of dust in southwest Asia. The strong winds blow fine sand off the exposed Hamoun lake beds and deposit it to form huge dunes that may cover a hundred or more villages along the former lakeshore. Hamoun dry lake beds are mainly composed of quaternary lacustrine silt and clay material as well as Holocene fluvial sand, silt and clay. These materials have been carried to the basin by the rivers, while along their courses neogene fluvial sand, eolian sand, silt and clay are the main constituents. This thesis analyses the aerosol characteristics, dust loading and air quality over the Sistan region based on first time measurements conducted. The dust loading was measured using dust traps near the Hamoun basin during the period August 2009 to July 2010. Dust loading from the Hamoun basin appears to have a significant contributing influence on the development of extreme dust storms, especially during the summer days. This influence firstly seems to depend on the intensity and duration of dust storms, and secondarily, on the distance from the source region, the wind speed and altitude. The grain-size distribution of the dust loading is strongly influenced by the distance from the dust source. Furthermore, the particle size distribution exhibited a shift towards lower values as the altitude increases, with this feature found to be more obvious amongst larger sized particles, while the frequency of particles below 2.5 ìm seemed not to be affected by altitude. In general, the analysis revealed significant spatio-temporal variability of regional dust loading and characteristics. This finding necessitates more systematic observations at as many locations as possible around the Hamoun basin in order to improve the understanding of force dynamics, transport mechanisms as well as to quantify the dust amounts emitted from the Hamoun basin. To assess air quality characteristics in two cities of Zabol and Zahedan affected by the Sistan dust storms, systematic airborne PM concentrations were measured during the period September 2010 to September 2011 and July 2008 to March 2010, respectively. The results showed that the PM10 concentrations were considerably higher than the corresponding European Union air quality annual standard and the mean PM2.5 concentration (32 ìgm-3) also overcame the Air Quality Index (AQI) annual PM2.5 standards. This poor air quality is affected by dust storms from the Sistan desert. The drainage of the Hamoun wetlands, in association with the intense Levar winds in summer, is the main factor responsible for the frequent and massive dust storms over the Sistan region. Hamoun, as an intense dust source region, caused a dramatic increase in PM10 concentrations and a deterioration of air quality (65% of the days were considered unhealthy for sensitive people and 34.9% as hazardous) in Zabol city. The maximum PM10 concentrations occurred between 8:00 to 11:00 Local Sidereal Time (LST) in Zabol and between 12:00 and 20:00 LST in Zahedan, indicating that Sistan dust storms reach Zahedan after six to nine hours. The strong correlation between daily PM2.5 and PM10 concentrations indicated that they have similar sources and an increase of PM10 significantly affects PM2.5. Considering the air pollution standards defined by the United state Environmental Protection Agency (USEPA), determining that only on one day per year may the AQI be higher than 100 ìg.m-3, it was found that the values of AQI in Zahedan overcame this level for 86 days out of 399, expressing a fraction of 21.5%. It should be noted that on 25 days (6.3%) the atmospheric conditions were very unhealthy or hazardous for the whole population and this requires more attention by officials, managers and urban planners. Windblown transport and deposition of dust is widely recognized as an important physical and chemical concern to climate, human health and ecosystems. To mitigate the impact of these phenomena, this thesis examines for the first time, the mineralogical and chemical properties of dust over Sistan by collecting aerosol and soil samples. These data were analyzed to investigate the chemical and mineralogical characteristics of dust, relevance of inferred sources and contributions to air pollution. Dust aerosol characterization included chemical analysis of major and trace elements by X-Ray Fluorescence (XRF) and mineral analysis by X-Ray Diffraction (XRD). The results showed that quartz, calcite, muscovite, plagioclase and chlorite are the main mineralogical components of the dust, in descending order, over Sistan, and were present in all the selected airborne dust samples. In contrast, significantly lower percentages for enstatite, halite, dolomite, microcline, gypsum, diopside, orthoclase and hornblende were found, since these elements occurred only in some of the samples. On the other hand, silicone dioxide (SiO2), Calcium oxide (CaO), Aluminum oxide (Al2O3), Sodium oxide (Na2O), Magnesium Oxide (MgO) and Iron (III) Oxide (Fe2O3) were the major elements characterising the dust, while large amounts of Fluorine (F), Chlorine (Cl) and Sulfur (S) were also found as trace elements. The mineralogy and chemical composition of airborne dust at both stations were nearly the same and quite similar to the soil samples collected at several locations downwind. This suggests that the dust over Sistan is locally emitted, i.e. from the Hamoun basin, and in a few cases can also be long-range transported to distant regions. On the other hand, individual dust storms showed significant differences between either evaporite-dominated aerosols or those characterized by deflation from alluvial silts. These possibly reflect either localized climatic cyclicity or desiccation cycles. However, in some cases the soil samples showed poor comparisons with aerosol compositions, suggesting that dynamic sorting, soil-forming processes and climatic influences, such as rainfall, altered the mineralogy and chemistry in these partially eolian deposits. Estimates of Enrichment Factors (EF) for all studied elements show that all of them have very low EF values, suggesting natural origin from local materials. The results suggest that a common dust source region can be inferred, which is the eroded sedimentary environment in the extensive Hamoun dry lakes. Scanning Electronic Microscope (SEM) analyses of the samples indicated that airborne dust has rounded irregular, prismatic and rhombic shapes, with only the finer particles and a few cases of the coarser dust being spherical. This thesis analyses the aerosol patterns over the arid environment of Sistan region by means of multiple satellite platforms aiming to reveal the spatio-temporal and vertical distribution of dust aerosols. The dataset used includes records of Aerosol Index (AI) from the Total Ozone Mapping Spectrometer (TOMS) on board the Nimbus-7 (1979–92) and the Earth Probe (mid-1996 to 2001) satellites and six-year AI records from OMI aboard Aura. Moreover, the Aerosol Optical Depth (AOD) is analyzed through 11-year records from Multi-angle Imaging Spectro Radiometer (MISR) aboard Terra (2000-2010) and from seven-year Deep Blue records from MODIS aboard Aqua (2002-2011). The main focus is to determine similarities and differences in dust climatology provided by these sensors over the Sistan region and surroundings. The results showed a marked seasonal cycle with high aerosol loading during summer and lower in winter, while MISR, MODIS Deep Blue and OMI climatologies agree in both terms of monthly and seasonally mean spatial and temporal aerosol patterns revealing similar seasonal behavior over the region. After prolonged drought conditions in 1999 at Hamoun lakes (northern of Sistan) the dust-aerosol load over the area has increased. The higher aerosol concentrations during summer are interpreted as a result of the Levar northerly winds and the drying of Hamoun lakes. The satellite monitoring highlights Sistan and Hamoun basin as major dust source regions in south Asia, spreading dust aerosols over Afghanistan, Pakistan and Arabian Sea.
Thesis (PhD)--University of Pretoria, 2012.
Geography, Geoinformatics and Meteorology
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Sakai, Tetsu, and 哲. 酒井. "Optical Properties of Free Tropospheric Aerosol Particles Related to the Relative Humidity as Derived from Raman Lidar Observations at Nagoya: Contributions of Aerosols from the Asian Continent and the Pacific Ocean." Thesis, 2000. http://hdl.handle.net/2237/6418.

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