Dissertations / Theses on the topic 'Aerosol microphysical properties'

A new retrieval algorithm has been developed based on the Optimal Estimation (OE) approach, which retrieves lognormal aerosol size distribution parameters from multiwavelength aerosol extinction data, as measured by the Stratospheric Aerosol and Gas Experiment (SAGE) II in the lower stratosphere. Retrieving these aerosol properties becomes increasingly more difficult under aerosol background conditions, when tiny particles (« 0.1 µm) prevail, to which the experiment is nearly or entirely insensitive. A successful retrieval algorithm must then be able (a) to fill the 'blind spot' with suitable information about the practically invisible particles, and (b) to identify 'the best' of many possible solutions. The OE approach differs from other previously used aerosol retrieval techniques by taking a statistical approach to the multiple solution problem, in which the entire range of possible solutions are considered (including the smallest particles) and characterized by probability density functions. The three main parts of this thesis are (1) the development of the new OE retrieval algorithm, (2) the validation of this algorithm on the basis of synthetic extinction data, and (3) application of the new algorithm to SAGE II measurements of stratospheric background aerosol. The validation results indicate that the new method is able to retrieve the particle size of typical background aerosols reasonably well, and that the retrieved uncertainties are a good estimate of the true errors. The derived surface area densities (A), and volume densities (V ) tend to be closer to the correct solutions than the directly retrieved number density (N), median radius (R), and lognormal distribution width (S). Aerosol properties as retrieved from SAGE II measurements (recorded in 1999) are observed to be close to correlative in situ data. In many cases the OE and in situ data agree within the (OE and/or the in situ ) uncertainties. The retrieved error estimates are of the order of 69% (σN), 33% (σR), 14% (σS), 23% (σA), 12% (σV), and 13% (σReff ). The OE number densities are generally larger, and the OE median particle sizes are generally smaller than those N and R retrieved by Bingen et al. (2004a), who suggest that their results underestimate (N) or overestimate (R) correlative in situ data due to the 'small particle problem'. The OE surface area estimates are generally closer to correlative in situ profiles (courtesy of T. Deshler, University of Wyoming), and larger than Principal Component Analysis (PCA) retrieval solutions of A (courtesy of L. W. Thomason, NASA LaRC) that have been observed to underestimate correlative in situ data by 40-50%. These observations suggest that the new OE retrieval algorithm is a successful approach to the aerosol retrieval problem, which is able to add to the current knowledge by improving current estimates of aerosol properties in the lower stratosphere under low aerosol loading conditions.

To assess information about the optical, microphysical, and radiative properties of aerosol particles the lidar technique and sun photometers are commonly used. Information that result from both lidar and sun photometer data can provide a distinct image of the vertical aerosol properties. The algorithm developed at the Institute of Physics of the National Academy of Science of Belarus (IPNASB) uses lidar measurements at the three wavelengths 355, 532, and 1064 nm and mean backscatter and extinction coefficients retrieved from radiometric data to obtain profiles of fine-mode and coarse-mode concentrations. Within the master thesis the IPNASB algorithm was tested for specific aerosol situations. Three cases are considered representing Saharan dust, smoke and industrial aerosol from East Europe, and volcanic aerosol from the Eyjafjallajokull eruption. The retrieved microphysical aerosol properties are in good to acceptable agreement with findings of well-established methods.

Im Rahmen der vorliegenden Arbeit wurde eine neuartige Lidartechnik in ein leistungsstarkes Lidar-System implementiert. Mit Hilfe des realisierten Aufbaus wurden Aerosol-Wolken-Wechselwirkungen in Flüssigwasserwolken über Leipzig untersucht. Die angewandte Messmethode beruht auf der Detektion von Licht, das an Wolkentröpfchen mehrfach in Vorwärtsrichtung gestreut und an Stickstoffmolekülen inelastisch zurückgestreut wurde. Dabei werden zwei Gesichtsfelder unterschiedlicher Größe verwendet. Ein Vorwärtsiterations-Algorithmus nutzt die gewonnenen Informationen zur Ermittlung von Profilen wolkenmikrophysikalischer Eigenschaften. Es können der Extinktionskoeffizient, der effektive Tröpfchenradius, der Flüssigwassergehalt sowie die Tröpfchenanzahlkonzentration bestimmt werden. Weiterhin wird die exakte Erfassung der Wolkenunterkantenhöhe durchdie eingesetzte Messtechnik ermöglicht. Darüber hinaus ist die Bestimmung von Aerosoleigenschaften mit dem eingesetzten Lidargerät möglich. Die Qualität des realisierten Messaufbaus wurde geprüft und eine Fehleranalyse durchgeführt. Unter anderem wurde der aus einer Wolkenmessung bestimmte Flüssigwassergehalt mit einem Mikrowellen-Radiometer bestätigt. Anhand von Fallbeispielen konnte das Potential dieser Messtechnik demonstriert werden. Die Bedeutung von Profilinformationen von Wolkeneigenschaften für die Untersuchung von Aerosol-Wolken-Wechselwirkungen wurde gezeigt. Weiterhin wurde mit Hilfe eines Doppler-Windlidars der Einfluss der Vertikalwindgeschwindigkeit auf Wolkeneigenschaften und damit Aerosol-Wolken-Wechselwirkungen verdeutlicht. Neunundzwanzig Wolkenmessungen wurden für eine statistische Auswertung bezüglich Aerosol-Wolken-Wechselwirkungen genutzt. Dabei konnte erstmalig die Abhängigkeit von Aerosol-Wolken-Wechselwirkungen von der Wolkeneindringtiefe untersucht werden. Es wurde festgestellt, dass diese auf die untersten 70m von Wolken beschränkt sind. Weiterhin wurden deutlich stärkere Aerosol-Wolken-Wechselwirkungen in Wolkengebieten festgestellt, die von Aufwinden dominiert werden. Für der Quantifizierung der Stärke von Aerosol-Wolken-Wechselwirkungen wurden ACIN-Werte genutzt, welche den Zusammenhang zwischen der Tröpfchenanzahlkonzentration und dem Aerosol-Extinktionskoeffizienten beschreiben. Dabei wurde zwischen der Untersuchung der entsprechenden mikrophysikalischen Prozesse und deren Bedeutung für die Wolkenalbedo und damit dem Strahlungsantrieb der Wolken unterschieden. Für die erstgenannte Zielstellung wurde ein ACIN-Wert von 0.80 +/- 0.40 ermittelt, für Letztere 0.13 +/- 0.07.

Clouds play an important role in precipitation, solar radiation budget and electrification of Earth's atmosphere. The presence of small ice crystals in clouds and their morphology can complicate parametrisation and climate modelling, consequently leading to a net cooling feedback on climate. In situ airborne measurements provide single particle characterisation with high temporal and spatial resolution allowing better understanding of atmosphericprocesses of ice nucleation and growth. Simulations of the preindustrial clouds and accurate characterisation and comparison of the instruments require a well-controlled and often pristine environment. The experimental chamber setup allows simulations of these and other conditions. The microphysical features of the micrometric ice particles in clouds were examined in a laboratory setup, at numerous sub-zero temperatures [-10 to -50 ⁰C]. The following instruments were sampling the content of the CLOUD chamber air volume: Cloud and Aerosol Spectrometer with Polarisation (CASPOL), Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition), 3-View Cloud Particle Imager (3V-CPI), and the Scattering-Intensity-Measurements-for-the-Optical-detectioN-of-icE (SIMONE-Junior). Cluster analysis was applied to the data collected with CASPOL and compared with results from the other probes. We were able to discriminate and map the aerosol and cloud particles in the pristine chamber environment using polarisation ratios (Dpol/Backscatter and Dpol/Forwardscatter) of the scattered light. We demonstrate the sensitivity of the instruments in detecting secondary organic aerosol (SOA) phase transitions. Then, we show the ability of the viscous SOA to nucleate ice in a series of SPectrometer for Ice Nuclei (SPIN) measurements. The detected viscous SOA ice nucleation efficiency may affect global modelling and estimations of ice water content in the atmosphere. Subsequently, the analysis and discrimination technique used in the CLOUD chamber was applied to airborne measurements to test its efficiency and to retrieve the composition of clouds. Data from four flight campaigns on board of the FAAM BAe-146 were analysed: Aerosol-Cloud Coupling and Climate Interactions in the Arctic (ACCACIA), COnvective-Precipitation-Experiment (COPE) in south England, CIRrus Coupled Cloud-Radiation EXperiment (CIRCCREX), and PIKNMIX in Scotland. In these and other flights, we were able to identify unique clusters such as salts, minerals, organics, volcanic ash, water and ice, confirming some of the offline laboratory elemental analysis results, and providing complementary information. Single particle polarisation measurements were compared with bulk depolarisation, diffraction patterns, and imaging. Most of the optical instruments still suffer from ambiguity in phase derivation (i.e. water/ice) of optically spherical small shapes. We discuss some of the limitations of optical cloud particle discrimination in different ambient conditions and offer possible solutions to reduce the uncertainty, e.g., surface complexity derivation from scatteringpatterns. Our findings will help to develop better instruments and improve the models which are used for weather forecasts and climate change predictions.

Im Rahmen dieser Dissertation wurden die mikrophysikalischen Eigenschaften von Aerosolpartikeln im Passatklima und deren Einfluss auf Passatwolken untersucht. Die Arbeit basiert auf Messungen mit der hubschrauber-getragenen Messplattform ACTOS. Es wurden zwei Intensivmesskampagnen im November 2010 und April 2011 durchgeführt, welche 31 Forschungsflüge in der Nähe der östlichsten Karibik-Insel Barbados umfassen. Die gemessenen Partikel-Anzahl-Größenverteilungen weisen meist eine bimodale Verteilung auf, welche typisch für marines Aerosol ist. Im Vergleich zu kontinentalen Verhältnissen ist die Totalanzahlkonzentration der Aerosolpartikel von 100-1000 cm-3 gering. Eine statistische Analyse einzelner Wolken lässt auf typische Anzahlkonzentrationen von aktivierten Partikeln bis zu 400 cm-3 und minimale Aktivierungsdurchmesser in der Größenordnung von 40 nm bis 180 nm mit entsprechenden maximalen kritischen Übersättigungen zwischen 0.1 und 0.9% schließen. Zusätzlich wurden wesentliche Einflussfaktoren auf die Anzahlkonzentration aktivierter Partikel identifiziert: 1) Vertikalwind an der Wolkenunterkante und 2) Anzahlkonzentration der verfügbaren Aerosolpartikel, die als Wolkenkondensationskeime dienen können. Mit Hilfe von Beobachtungsdaten und einer umfassenden Sensitivitätsstudie unter Verwendung eines Luftpaketmodells mit spektraler Wolkenmikrophysik wurde die Sensitivität der Wolkentropfenkonzentration gegenüber Änderungen in den physikalischen Eigenschaften und der Hygroskopizität von Aerosolpartikeln untersucht. Die beobachteten Ergebnisse in Form von sogenannten \"aerosol-cloud interaction metrics\" (ACI, Maß für den Einfluss von Änderungen einer bestimmten Aerosoleigenschaft auf eine bestimmte Wolkeneigenschaft) zeigen eine sehr hohe Sensitivität der Tropfenanzahlkonzentration gegenüber Änderungen in der Partikelanzahlkonzentration (in der Nähe des physikalisch sinnvollen Maximums von eins). Diese abgeleiteten ACI-Metriken eignen sich als Basis für Abschätzungen des indirekten Strahlungsantriebes auf der Grundlage von Beobachtungen. Zusätzliche Modellrechnungen umfassen die gemessenen Partikeleigenschaften während der gesamten Kampagnen. Die Ergebnisse unterstreichen besonders die Bedeutung der physikalischen Partikeleigenschaften. Die Suszeptibilität der Tropfenanzahlkonzentration gegenüber Änderungen in der Partikelanzahlkonzentration (Wertebereich: 0-1) ist am größten (> 0.9) für den Fall eines stark ausgeprägten Akkumulations-Mode und nimmt ab, je stärker der Aitken-Mode ausgeprägt ist (> 0.6). Im Gegensatz dazu ist die Sensitivität der Tropfenanzahlkonzentration gegenüber Änderungen in der Hygroskopizität der Partikel generell geringer (< 0.4). Die hier präsentierten Ergebnisse stellen eine umfangreiche Charakterisierung der Aerosol- und Wolkeneigenschaften im Passatklima dar und können helfen, die vorhergesagte Sensitivität der Wolkeneigenschaften in Klimamodellen gegenüber Änderungen der Aerosoleigenschaften zu evaluieren und deren Unsicherheiten zu reduzieren
Within the scope of this dissertation, microphysical properties of aerosol particles in the trade wind regime and their influence on microphysical properties of trade wind cumulus clouds have been investigated. The study is based on measurements performed with the helicopter-borne measurement platform ACTOS. Two intensive measurement periods were carried out in November 2010 and April 2011, including 31 research flights close to the easternmost Caribbean island - Barbados. Aerosol particle number size distributions show a bimodal structure, which is typical for marine aerosol particles. The total particle concentrations of approximately 100-1000 cm-3 are compared to continental conditions relatively low. A statistical analysis of individual clouds reveals typical number concentrations of activated particles up to 400 cm-3 and minimum activation diameters between 40 and 180 nm with corresponding critical supersaturations between 0.1 and 1%. Additionally, major factors affecting the number concentration of activated particles are identifed: 1) vertical wind velocity at cloud base and, 2) number concentration of available aerosol particles as potential cloud condensation nuclei. With the help of observational data and a comprehensive sensitivity study using a spectral cloud microphysical parcel model, the sensitivity of the cloud droplet number concentration towards changes in the microphysical aerosol particle properties and their hygroscopicity has been investigated. Observational results in terms of so-called aerosol-cloud interactions metrics (describes a measure of the influence of changes in one specific aerosol property on one specific cloud property) show a very high sensitivity (close to the physical meaningful maximum of unity) of the number concentration of activated particles towards changes in the particle number concentration. These aerosol-cloud interaction metrics can be used as basis for observationally-based radiative forcing estimates. Additional model calculations cover the entire range of the observed aerosol properties during both campaigns. The results underline particularly the importance of the physical aerosol properties. The calculated susceptibility (valuation: 0-1) of the droplet number concentration towards changes in the particle number concentration is highest (> 0.9) for accumulation mode dominated particle number size distributions and decreases for Aitken mode dominated size distributions (> 0.6). In contrast, for the modeled parameter space, the sensitivity towards changes in the particle hygroscopicity is generally below 0.4. The findings presented in this study represent a comprehensive characterization of aerosol and cloud microphysical properties in the trade wind regime. These findings may help to evaluate the predicted sensitivity of cloud microphysical properties by climate models towards changes in particle microphysical properties and reduce the uncertainties in climate sensitivity estimates

La connaissance de la répartition verticale des propriétés optiques et microphysiques des aérosols est cruciale pour étudier l'évolution et le transport des aérosols, ainsi que leurs impacts sur la santé humaine, l'environnement local et le climat mondial. Dans ce travail nous avons développé un algorithme BOREAL pour restituer les propriétés microphysiques des aérosols à partir de combinaisons de mesures lidar d'extinction, de rétrodiffusion et de dépolarisation spectrales. Basé sur une estimation de vraisemblance maximale, l'algorithme de restitution utilise une approche d'itération non linéaire pour rechercher la meilleure adéquation entre les mesures et les contraintes. Les propriétés microphysiques des aérosols restituées comprennent la distribution de taille des particules, leur concentration volumique, leur rayon efficace, l'indice de réfraction complexe (CRI) et l'albédo de diffusion simple (SSA).Les performances de BOREAL, sa précision et la sensibilité des mesures sont évaluées à l'aide de données simulées. En général, la précision de la restitution est meilleure pour les particules de mode fin que pour les particules de mode grossier. Les simulations démontrent l'importance de l'exploitation de contraintes a priori pour améliorer la précision de la restitution du CRI et du SSA. Outre les particules sphériques, la performance de la restitution des particules non sphériques est également évaluée en intégrant trois modèles de diffusion de particules différents, à savoir les modèles Sphérique, Sphéroïdale et Irrégulier-Hexaédrique (IH), dans BOREAL. Les résultats montrent que l'intégration des mesures de dépolarisation dans l'inversion est essentielle pour mieux contraindre et stabiliser la restitution. De plus, l'approximation des particules non sphériques par des sphères dégrade manifestement la qualité de la restitution. Enfin, BOREAL est utilisé pour restituer les propriétés aérosols au cours d'événements de feux de biomasse, de poussières désertiques et les d'aérosols continentaux pollués détectés depuis la plateforme ATOLL. Les résultats sont analysés et comparés aux restitutions d'AERONET ainsi qu'aux résultats d'études précédentes, ce qui démontrer la robustesse de BOREAL pour l'application de données réelles et la caractérisation d'aérosols.Ce travail contribue aux études menées dans le cadre du Labex CaPPA et d'ACTRIS en quantifiant les propriétés microphysiques des aérosols à partir des observations lidar
Vertical information on aerosol optical and microphysical properties is of significant importance to study aerosol evolution, transport, as well as their impacts on human health, local environment and global climate. This thesis developed an algorithm, the Basic algOrithm for REtrieval of Aerosol with Lidar (BOREAL), for retrieving heigh-resolved aerosol microphysical properties from combinations of extinction, backscattering and depolarization lidar measurements. Based on maximum likelihood estimation, the retrieval algorithm uses a nonlinear iteration approach to search for the best fit to both measurements and constraints. The retrieved aerosol microphysical properties include particle size distribution, volume concentration, effective radius, complex refractive index (CRI) and single scattering albedo (SSA).The performance of BOREAL, retrieval accuracy and measurement sensitivity are assessed through simulated data. In general, retrieval accuracy is higher for fine-mode particles than coarse-mode particles. The simulations demonstrate the importance of exploiting a priori constraint to improve the retrieval accuracy of CRI and SSA. Apart from spherical particles, performance of retrieving non-spherical particles is also evaluated by integrating three different particle scattering models, i.e., the Sphere, Spheroid and Irregular-Hexahedral (IH) models, into BOREAL. The results show incorporating depolarization measurements into inversion is essential to better constrain and stabilize the retrieval. Besides, approximating non-spherical particles to spheres will evidently degrade retrieval quality in cases of lidar measurements. In addition, BOREAL is applied to real lidar observations of different aerosol types, including biomass burning, dust and continental polluted aerosols at the ATOLL observatory. Results are analyzed and compared with retrievals from AERONET and previous studies, which demonstrates the robustness of BOREAL for real data application and aerosol characterization.Overall, this work contributes to Labex CaPPA and ACTRIS efforts to better quantify aerosol microphysical properties using lidar measurements

Les aérosols atmosphériques constituent l’une des plus grandes incertitudes dans l’étude des processus de changement climatique. La diversité des leurs sources et mécanismes de formation rendent la distribution spatiale des aérosols très inhomogène ce qui nécessite la mise en place d’une instrumentation et de méthodes d’observation sophistiquées. Un nouveau photomètre solaire aéroporté PLASMA permet d’effectuer des mesures d’épaisseur optique des aérosols sur une large gamme spectrale (0.34−2.25 μm) et à différentes altitudes. La détermination de la distribution verticale des propriétés optiques des aérosols peut ainsi être utilisée pour valider les algorithmes d’inversion des mesures lidar. Il est possible de remonter à la distribution de taille des particules d’aérosol à différents niveaux. En outre, l’instrument peut être installé sur un véhicule afin de mesurer les profils horizontaux du contenu des aérosols. Cette étude est consacrée à la caractérisation et à l’étalonnage de l’instrument et à l’analyse de plusieurs jeux de données. De nombreuses mesures au sol, aéroportées et depuis un véhicule ont réalisées et sont comparées aux mesures d’autres instruments. L’étude de la sensibilité de l’algorithme d’inversion de Oleg Dubovik a montré qu’il est possible d’obtenir la distribution en tailles des particules à partir de mesures d’épaisseur optique quand l’indice de réfraction est connu avec une certaine précision. Les mesures aéroportées ont ainsi été inversées et les distributions de tailles obtenues pour différentes altitudes. Cette information permettra de mieux comprendre les processus de formation et la répartition spatiale des aérosols dans l’atmosphère
Atmospheric aerosols still represents one of the greatest uncertainty in the study of the processes of climate change. The diversity of aerosol sources and their formation mechanisms make the spatial distribution of aerosols very inhomogenous and requires numerous instruments and different approaches for their analysis. A new multi-wavelength airborne sun photometer PLASMA (Photomètre Léger Aéroporté pour la Surveillance des Masses d’Air) developed in the Laboratory of Atmospheric Optics allows providing on-board measurements of aerosol optical depth over a wide (0.34 − 2.25 μm) spectral range and at different altitudes. The information of vertical distribution of aerosol optical properties can be then used to validate the lidar processing algorithms. It is possible to retrieve from PLASMA measurements the size distribution of the aerosol particles at different levels. Also, the instrument can be installed on an automobile in order to measure the horizontal profiles of AOT. This study is dedicated to characterization and calibration of PLASMA and to the analysis of several data sets. Numerous ground-based, airborne and automobile measurements were held and compared with other instruments. Sensitivity study of the Dubovik’s inversion algorithm showed that it is possible to get the particle’s size distribution from only AOD measurements assuming a value of the refractive index within a limited domain. Airborne PLASMA measurements were inverted and size distributions of the aerosol particles were obtained at different altitudes. This new information is helpful to better understand the formation and spatial distribution of aerosols in the atmosphere

Les aérosols atmosphériques constituent l’une des plus grandes incertitudes dans l’étude des processus de changement climatique. La diversité des leurs sources et mécanismes de formation rendent la distribution spatiale des aérosols très inhomogène ce qui nécessite la mise en place d’une instrumentation et de méthodes d’observation sophistiquées. Un nouveau photomètre solaire aéroporté PLASMA permet d’effectuer des mesures d’épaisseur optique des aérosols sur une large gamme spectrale (0.34−2.25 μm) et à différentes altitudes. La détermination de la distribution verticale des propriétés optiques des aérosols peut ainsi être utilisée pour valider les algorithmes d’inversion des mesures lidar. Il est possible de remonter à la distribution de taille des particules d’aérosol à différents niveaux. En outre, l’instrument peut être installé sur un véhicule afin de mesurer les profils horizontaux du contenu des aérosols. Cette étude est consacrée à la caractérisation et à l’étalonnage de l’instrument et à l’analyse de plusieurs jeux de données. De nombreuses mesures au sol, aéroportées et depuis un véhicule ont réalisées et sont comparées aux mesures d’autres instruments. L’étude de la sensibilité de l’algorithme d’inversion de Oleg Dubovik a montré qu’il est possible d’obtenir la distribution en tailles des particules à partir de mesures d’épaisseur optique quand l’indice de réfraction est connu avec une certaine précision. Les mesures aéroportées ont ainsi été inversées et les distributions de tailles obtenues pour différentes altitudes. Cette information permettra de mieux comprendre les processus de formation et la répartition spatiale des aérosols dans l’atmosphère
Atmospheric aerosols still represents one of the greatest uncertainty in the study of the processes of climate change. The diversity of aerosol sources and their formation mechanisms make the spatial distribution of aerosols very inhomogenous and requires numerous instruments and different approaches for their analysis. A new multi-wavelength airborne sun photometer PLASMA (Photomètre Léger Aéroporté pour la Surveillance des Masses d’Air) developed in the Laboratory of Atmospheric Optics allows providing on-board measurements of aerosol optical depth over a wide (0.34 − 2.25 μm) spectral range and at different altitudes. The information of vertical distribution of aerosol optical properties can be then used to validate the lidar processing algorithms. It is possible to retrieve from PLASMA measurements the size distribution of the aerosol particles at different levels. Also, the instrument can be installed on an automobile in order to measure the horizontal profiles of AOT. This study is dedicated to characterization and calibration of PLASMA and to the analysis of several data sets. Numerous ground-based, airborne and automobile measurements were held and compared with other instruments. Sensitivity study of the Dubovik’s inversion algorithm showed that it is possible to get the particle’s size distribution from only AOD measurements assuming a value of the refractive index within a limited domain. Airborne PLASMA measurements were inverted and size distributions of the aerosol particles were obtained at different altitudes. This new information is helpful to better understand the formation and spatial distribution of aerosols in the atmosphere

This thesis addresses a series of questions related to the problem of achieving reliable and physically consistent representations of aerosol-cloud interaction in global circulation models (GCM). In-situ data and modeling tools are used to develop and evaluate novel parameterization schemes for the process of aerosol activation for applications in GCM simulations. Atmospheric models of different complexity were utilized, ranging from detailed Lagrangian parcel model simulations of the condensational growth of droplets, to one-dimensional single column model with aerosol and cloud microphysics, and finally GCM simulations performed with the Community Atmosphere Model (CAM). A scheme for mapping the sub-grid scale variability of cloud droplet number concentrations (CDNC) to a number of microphysical process rates in a GCM was tested, finding that neglecting this impact can have substantial influences in the integrated cloud properties. A comprehensive comparison and evaluation of two widely used, physically-based activation parameterizations was performed in the framework of CAM5.1. This was achieved by utilizing a numerical adjoint sensitivity approach to comprehensively investigate their response under the wide range of aerosol and dynamical conditions encountered in GCM simulations. As a result of this, the specific variables responsible for the observed differences in the physical response across parameterizations are encountered, leading to further parameterization improvement.

Atmospheric particles are ubiquitous in the Earth’s atmosphere and have potential to influence atmospheric chemistry, visibility, global climate and human health, particularly downwind from major pollution sources. The main objective of this thesis was to investigate questions pertaining to the microphysical, chemical and optical properties of aerosol particles by using in situ data collected during four experiments carried out in different regions of the Northern Hemisphere.

The first two papers of this thesis reports on airborne measurements of the aerosol optical properties performed over the North Atlantic and the Los Angeles basin. Airmasses from Europe and North Africa are usually advected in over the North Atlantic, alternating with the background marine conditions. The results showed that the aerosols are not uniformly distributed in the area and variability in the aerosol fields occurs at sub-synoptic scales. It was also observed that the single scattering coefficient varied as the polluted plumes aged, suggesting a relationship between this quantity and transport time. The measurements performed around the Los Angeles basin showed that the area’s complex topography and local meteorological circulations exert a strong control on the distribution of the aerosol in the basin. Large spatio-temporal gradients in the aerosol optical properties were observed along a transect flown from the shore towards the mountains. Profiles flown over sites located on the mountains displayed a stratified configuration with elevated aerosol layers.

Airborne data of residual particles collected in orographic wave clouds over Scandinavia were analyzed using a single particle analysis technique. Mineral dust, organic aerosols and sea salt were the main group of particles identified. Residuals composed predominantly of mineral dust were found in glaciated clouds while organic residuals were found in liquid clouds. The results suggest that organic material may inhibit freezing and have considerable influence on supercooled clouds that form through heterogeneous pathways.

The partitioning of the aerosol particles between cloud droplets and interstitial air has been addressed in terms of their microphysical properties using data obtained at a mountain-top site in Sweden during a stratocumulus event. The results showed that the scavenging efficiency varied during the cloud event, and Aitken-mode particles were also efficiently scavenged in addition to accumulation-mode particles. It is hypothesized that alterations of the aerosol chemical composition occurred during the measurement period, modifying the hygroscopic nature of the particles and decreasing their activation diameter.

Cette thèse vise à montrer rapport d'un lidar multispectral, en particulier en ajoutant des longueurs d'onde dans le proche infrarouge proche, pour la caractérisation des aérosols. En effet par rapport à un lidar mono-longueur d'onde, l'information contenue dans les profils multispectraux permet de remonter aux propriétés microphysiques des aérosols (distribution en aille et composition). Pour cela un simulateur de signaux lidar multispectraux a été adapté à notre étude afin de pouvoir développer et tester deux méthodes permettant de retrouver les propriétés microphysiques des aérosols le long de la ligne e visée à partir de signaux lidar synthétiques. La première méthode, basée sur l'inversion des signaux lidar, permet de retrouver la répartition en taille des aérosols et donc d'en déduire notamment leur concentration et leur rayon modal. Cette méthode nécessite des informations a priori sur les aérosols. Un bilan d'erreur a été réalisé en introduisant des incertitudes sur ces paramètres a priori et montre que les résultats obtenus sur la concentration et le rayon modal sont précis (respectivement 16% et 17% d'erreur). Cette méthode présente l'avantage de ne pas nécessiter d'étalonnage absolu de l'instrument. La deuxième méthode est basée sur la minimisation de l'écart entre des signaux simulés et les signaux que l'on étudie. Même si la précision obtenue sur la répartition en taille retrouvée est plus faible (35% et 40 % d'erreur sur la concentration t le rayon modal) et que la constante d'étalonnage de l'instrument doit être connue, cette méthode a l'avantage de retrouver la composition des aérosols dans 74 % des cas
The purpose of this thesis is to show the contribution of a multispectral Iidar for the characterisation of aerosols, in particular hen wavelengths in near infrared are added. Indeed, compared with a mono-wavelength Iidar, the information contained in multispectral profiles allow to retrieve the microphysical properties of aerosols (particule size distribution and composition). To this end, we adapted a multispectral Iidar signal simulator to our study in order to develop and test two methods which objective is to obtain the microphysical properties of aerosol along the line-of-sight from synthetic lidar signals. The first method, based on the inversion of lidar signals, enables to find the length distribution of aerosols and therefore to educe their concentration and their modal radius. This method requires a priori information about the aerosols. An error budget was made by introducing uncertainties on the a priori parameters. It shows that the results obtained regarding the concentration and modal radius are accurate (respectively 16% and 17% uncertainty). The advantage of this method is that it does not require absolute calibration of the instrument. The principle of the second method is to minimize the difference between the studied and the simulated signals. Even if the accuracy on the size distribution is lower (35% and 40% on the concentration and modal radius) and the calibration constant of the instrument has to be known, this method has the advantage to find the concentration of the aerosols in 74% of the cases. Finally, the first method was validated on real data, coming from a collaboration with the RSLab (Barcelona), by comparing ur results with those obtained by this team (7% difference on the modal radius)

Dans cette thèse, nous analysons les principales caractéristiques des aérosols atmosphériques sur un site urbain en Afrique de l’Ouest : la ville de Ouagadougou. Cette analyse est suivie de l’évaluation du forçage radiatif produit par cette population d’aérosols au sommet de l’atmosphère, dans la couche atmosphérique ainsi qu’à la surface terrestre. Une étude climatologique des propriétés optiques (épaisseurs optiques, exposant d’Angström, albédo de simple diffusion, facteur d’asymétrie) et microphysiques (distribution granulométrique, indice complexe de réfraction) a été effectuée sur la base des données de mesures et d’inversions photométriques du réseau AERONET. L’analyse de ces données a permis de définir à diverses échelles de temps les différentes variabilités des propriétés étudiées. Ces propriétés ont mis en exergue les effets combinés de l’activité anthropique, du cycle de production des poussières minérales d’origine saharienne, de la succession saisonnière et la dynamique du climat spécifiques à cette région de la terre. La composition du panache d’aérosols a également été déduite de l’analyse des données optiques, et les conclusions tirées se sont avérées être en bon accord avec des mesures chimiques effectuées au LSCE sur des échantillons obtenus par prélèvement manuel sur filtres. Le bilan radiatif a été évalué en utilisant le modèle GAME. Cette simulation a montré une forte corrélation du forçage avec la succession des saisons sèche et humide, avec des valeurs extrêmes au mois d’Août (humide) et de Mars (sec avec poussières maximales). Les résultats traduisent un refroidissement en surface pouvant atteindre -41 W/m 2 en Mars, un réchauffement de la couche atmosphérique qui va de 15 à 35 W/m 2 environ et un refroidissement au sommet de l’atmosphère compris entre -2 et -6 W/m 2 . La représentation du forçage calculé en fonction de l’albédo de simple diffusion a montré une tendance linéaire avec un coefficient de corrélation traduisant une fiabilité de nos résultats de l’ordre de 88%. La cohérence des valeurs simulées a été aussi montrée par une comparaison avec des résultats obtenus dans la région Ouest Africaine par d’autres chercheurs utilisant des techniques différentes. De même, la représentation de l’efficacité radiative simulée en fonction de celle inversée par AERONET a montré un très bon accord
In this thesis, we analyze the main characteristics of atmospheric aerosols on an urban site in West Africa: Ouagadougou. This analysis is followed by an assessment of the radiative forcing produced by this population of aerosols at the top of the atmosphere, in the atmospheric layer and at the Earth's surface. A climatological study of the optical properties (optical thickness, Angstrom exponent, single scattering albedo, asymmetry factor) and microphysical properties (particle size distribution, complex refractive index) was performed on basis of data obtained from photometric measurement and inversions of AERONET network. The analysis of these data allowed us to define the different variabilities of the properties studied at various time scales. These properties have highlighted the combined effects of human activity, the cycle production of mineral dust from the Sahara region, the seasonal succession and the climate dynamics known in this region of the earth. The composition of the aerosol plume was also deduced from the analysis of optical data, and the conclusions were found to be in good agreement with chemical analysis carried out at LSCE on samples obtained by sampling on filters at Ouagadougou. The radiation balance was assessed using the GAME model. This simulation showed a strong relationship of the radiative forcing with the succesion of wet and dry seasons, with extreme values in August (wet) and Mars (dry with maximum dust emissions). The results showed a cooling at the surface that can reach -41 W / m 2 in March, a warming of the atmosphere, ranging from 15 to 35 W / m 2 about and a cooling at the top of the atmosphere between -2 and -6 W / m 2 . The representation of the radiative forcing calculated as a function of the single scattering albedo showed a linear trend with a correlation coefficient reflecting relatively good reliability of our results (about 88%). The consistency of simulated values was also shown by a comparison with the results obtained in the West African region by other researchers using different techniques. Similarly, the representation of the radiative efficiency simulated as a function of the inverted AERONET one showed a very good agreement

The direct and indirect effects of aerosols on the hurricane ‘Katrina’ have been investigated using the WRF model with a two-moment bulk microphysical scheme and modified Goddard shortwave radiation scheme. Simulations of the hurricane ‘Katrina’ are conducted under the three aerosol scenarios: 1) the clean case with an aerosol number concentration of 200 cm-1, 2) the polluted case with a number concentration of 1000 cm-1, and 3) the aerosol radiative effects (AR) case with same aerosol concentration as polluted case but with a modified shortwave radiation scheme. The polluted and AR cases have much larger amounts of cloud water and water vapor in troposphere, and the increased cloud water can freeze to produce ice water paths. A tropical cyclone in dirty and dusty air has active rainbands outside the eyewall due to aerosol indirect effects. The aerosol direct effect can lead to the suppressing of convection and weakening of updraft intensity by warming the troposphere and cooling the surface temperature. However, these thermal changes in atmosphere are concerned with the enhanced amounts of cloud hydrometeors and modification of downdraft and corresponding the low level winds in rainband regions. Thus, the AR case can produce the enhanced precipitation even in the weakest hurricane. When comparing the model performance between aerosol indirect and direct effect by ensemble experiments, the adjustment time of the circulation due to modification of the aerosol radiative forcing by aerosol layers may take a longer time than the hurricane lifetime, and the results from the simulated hurricane show that it is more sensitive to aerosol indirect effects which are related to the cloud microphysics process changes. From this aerosol study, we can suggest that aerosols can influence the cloudiness, precipitation, and intensity of hurricanes significantly, and there may be different results in the meso-scale convective clouds cases. The hurricane system is a large and complex convective system with enormous heating energy and moistures. Moreover, relationships between various hydrometeors in hurricane systems are difficult to isolate and thus, it needs further study with more realistic cloud microphysical processes, aerosol distributions, and parameterizations.

To understand the interaction between aerosols and climate, equilibrium simulations with a general circulation model are carried out in Part I to study the effects of future climate change on aerosol distributions, as well as the climate responses to future aerosol changes. The predicted warmer climate induced by carbon dioxide modifies the climate-sensitive emissions, alters the thermodynamic partitioning, and enhances wet removal of the aerosols. The direct radiative perturbations of aerosols, and the modification of clouds by aerosols can potentially change the temperature distribution, the hydrological cycle, and the atmospheric circulation; the pattern of climatic impacts from aerosols are differentiated from those of anthropogenic greenhouse gases. In Part II, the aerosol retrieval algorithm of the remote sensing instrument, the Multi-angle Imaging SpectroRadiometer (MISR), is assessed for the retrieval of biomass burning aerosols. By comparisons with coincident ground measurements and theoretical sensitivity tests, specific refinements to particle and mixture properties assumed in the algorithm for biomass burning aerosols are proposed. Representative case studies confirm the theoretical results and underline the key role of surface characterization in the remote sensing of aerosols.