Abstract : This is a study concerning comparisons between the Dubovik Aerosol optical depth (AOD) retrievals from AEROCAN (ARONET) stations and AOD estimates from simulations provided by a chemical transport model (GEOS-Chem : Goddard Earth Observing System Chemistry). The AOD products associated with the Dubovik product are divided into total, fine and coarse mode components. The retrieval period is from January 2009 to January 2013 for 5 Arctic stations (Barrow, Alaska; Resolute Bay, Nunavut; 0PAL and PEARL (Eureka), Nunavut; and Thule, Greenland). We also employed AOD retrievals from 10 other mid-latitude Canadian stations for comparisons with the Arctic stations. The results of our investigation were submitted to Atmosphere-Ocean. To briefly summarize those results, the model generally but not always tended to underestimate the (monthly) averaged AOD and its components. We found that the subdivision into fine and coarse mode components could provide unique signatures of particular events (Asian dust) and that the means of characterizing the statistics (log-normal frequency distributions versus normal distributions) was an attribute that was common to both the retrievals and the model. / Résumé : Cette étude compare des épaisseurs optiques d’aérosols (AOD) à 5 stations arctiques d’AEROCAN (AERONET), obtenues d’une part à l’aide de l’algorithme d'inversion de Dubovik appliqué à des mesures in situ, et d’autre part du modèle de transport chimique (GEOS-Chem : Goddard Earth Observing Système Chemistry). Les produits d’AOD associés à l’algorithme d’inversion sont divisés en composantes totales, fines et grossières. Pour chacune des 5 stations (Barrow, Alaska, Resolute Bay, au Nunavut, 0PAL et PEARL (Eureka), Nunavut, et Thulé, au Groenland), la période de récupération est de janvier 2009 à janvier 2013. Nous avons également utilisé les mesureurs d’AOD de dix autres stations canadiennes de latitudes moyennes, à des fins de comparaison. Les résultats de l’étude ont été soumis à la revue Atmosphere-Ocean. Pour résumer brièvement ces résultats, le modèle a généralement, mais pas toujours, eu tendance à sous-estimer l'AOD moyenne et de ses composantes. Nous avons constaté que la subdivision en composantes fine et grossière pourrait fournir des signatures uniques d'événements particuliers (poussière asiatique) et que les moyens de caractériser des statistiques (les distributions de fréquence log-normale versus les distributions normales) était un attribut qui était commun aux deux les mesureurs et le modèle.

This master thesis analyses light scattering on atmospheric aerosols, which has been measured at Košetice observatory in Pelhřimov region since 2012. In the thesis, data are processed for period from 1. 1. 2014 to 31. 12. 2015 which provide representative values of scattering and backscattering light measurement. Angstroem exponent was calculated based on which data corrections were performed. Data were processed using hour steps and compared with meteorological and emissions concentrations data. Correlations were calculated and regressions models estimated in order to verify correctness of measurement and to explore impact of meteorological conditions and emissions concentrations PM2,5 and PM10 on scattering coefficients. Performed analyses imply, that light scattering is higher for higher concentrations of PM2,5 and PM10 and for higher relative air humidity and lower for higher outdoor temperature, total precipitations, and wind speed. In addition, it was showed that light scattering is influenced by wind direction, which determines compositions of aerosols in the sample. Key words: atmospheric aerosol, light scattering, time series evaluation

I advanced the understanding of particle morphology and its implications for the behavior and effects of atmospheric aerosol particles. I have developed new experimental methods for the Aerosol Optical Tweezers (AOT) system and expanded the AOT’s application into studying realistic secondary organic aerosol (SOA) particle phases. The AOT is a highly accurate system developed to study individual particles in real-time for prolonged periods of time. While previous AOT studies have focused on binary or ternary chemical systems, I have investigated complex SOA, and how they interact with other chemical phases, and the surrounding gas-phase. This work has led to new insights into liquid-liquid phase separation and the resulting particle morphology, the surface tension, solubility, and volatility of SOA, and diffusion coefficients of SOA phases. I designed a new aerosol optical tweezers chamber for delivering a uniformly mixed aerosol flow to the trapped droplet’s position. I used this chamber to determine the phase-separation morphology and resulting properties of complex mixed droplets. A series of experiments using simple compounds are presented to establish my ability to use the cavity enhanced Raman spectra to distinguish between homogenous single-phase, and phase-separated core-shell or partially-engulfed morphologies. I have developed a new algorithm for the analysis of whispering gallery modes (WGMs) present in the cavity enhanced Raman spectra retrieved from droplets trapped in the AOT. My algorithm improves the computational scaling when analyzing core-shell droplets (i.e. phase-separated or biphasic droplets) in the AOT, making it computationally practical to analyze spectra collected over many hours at a few Hz. I then demonstrate for the first time the capture and analysis of SOA on a droplet suspended in an AOT. I examined three initial chemical systems of aqueous NaCl, aqueous glycerol, and squalane at ~ 75% relative humidity. For each system I added α-pinene SOA – generated directly in the AOT chamber – to the trapped droplet. The resulting morphology was always observed to be a core of the initial droplet surrounded by a shell of the added SOA. By combining my AOT observations of particle morphology with results from SOA smog chamber experiments, I conclude that the α-pinene SOA shell creates no major diffusion limitations for water, glycerol, and squalane under humid conditions. My AOT experiments highlight the prominence of phase-separated core-shell morphologies for secondary organic aerosols interacting with a range of other chemical phases. The unique analytical capabilities of the aerosol optical tweezers provide a new approach for advancing the understanding of the chemical and physical evolution of complex atmospheric particulate matter, and the important environmental impacts of aerosols on atmospheric chemistry, air quality, human health, and climate change.

Atmospheric aerosols are the major component in the shorter-term variability governing the radiative balance of the climate system, particularly on regional scales. However, knowledge of the myriad of properties and processes associated with aerosols is often limited, which results in major uncertainties when assessing their climate effects. One such aspect is the chemical make-up of the atmospheric aerosol burden.Airborne measurements of aerosol properties across Northern Europe are presented here in order to facilitate constraint of the properties, processes and effects of aerosols in this highly populated and industrialised region. An Aerodyne Aerosol Mass Spectrometer (AMS) delivered highly time-resolved measurements of aerosol chemical components, which included organic matter, sulphate, nitrate and ammonium.The chemical composition of the aerosol burden was strongly determined by the dominant meteorological conditions in Northern Europe. Pollution loadings in North- Western Europe were strongly enhanced when air masses originated from Continental Europe. Conversely, much cleaner conditions were associated with air masses from the Atlantic Ocean.Organic matter was found to be ubiquitous across Northern Europe and predominantly secondary in nature, which is consistent with other analyses in polluted regions of the Northern Hemisphere. Furthermore, its concentration was generally comparable to, or exceeded that of, sulphate. Significant chemical processing of the organic aerosol component was observed. Highly oxidised secondary organic aerosol dominated, as the distance from source and photochemical processing increased.Ammonium nitrate was found to be a major component of the aerosol burden in Northern Europe, with peak contributions occurring in North-Western Europe, due to the co-location of its emission precursors (NH3 and NOx) in the region. Ammonium nitrate was found to be the dominant sub-micron chemical constituent during periods associated with enhanced pollution episodes. Its concentration was shown to be modulated by the thermodynamic structure of the lower troposphere, with enhanced concentrations prevalent at the top of the boundary layer. This phenomenon greatly enhanced the radiative impact of the aerosol burden; the increased mass and water uptake by the aerosol significantly amplified the aerosol optical depth in the region.The results presented in this thesis highlight a highly dynamic region, where major changes in emissions have played a significant role in determining the chemical composition of the aerosol burden. As substantial reductions in sulphur dioxide emissions have occurred over the past two decades in Northern Europe, the relative contribution of sulphate aerosols to the regional aerosol burden has decreased. Consequently, it is more pertinent to consider the roles of organic matter and ammonium nitrate, as their influence becomes more pronounced than sulphate on regional and global climate.

We present a method for deriving the radiative effects of absorbing aerosols in cloudy scenes from satellite retrievals only. We use data of 2005–2007 from various passive sensors aboard satellites of the “A-Train” constellation. The study area is restricted to the tropical- and subtropical Atlantic Ocean. To identify the dependence of the local planetary albedo in cloudy scenes on cloud liquid water path and aerosol optical depth (AOD), we perform a multiple linear regression. The OMI UV-Aerosolindex serves as an indicator for absorbing-aerosol presence. In our method, the aerosol influences the local planetary albedo through direct- (scattering and absorption) and indirect (Twomey) aerosol effects. We find an increase of the local planetary albedo (LPA) with increasing AOD of mostly scattering aerosol and a decrease of the LPA with increasing AOD of mostly absorbing aerosol. These results allow us to derive the direct aerosol effect of absorbing aerosols in cloudy scenes, with the effect of cloudy-scene aerosol absorption in the tropical- and subtropical Atlantic contributing (+21.2±11.1)×10−3 Wm−2 to the global top of the atmosphere radiative forcing.

Die entsprechend der Quellstärke größte Fraktion des atmosphärischen Aerosols ist der natürliche Grobstaub (Seesalz, Mineralstaub und primär biologische Partikel). Nahezu alle natürlichen Grobstaubpartikel in trockener Phase weisen mehr oder weniger starke Abweichungen von der sphärischen Form auf. Der Einfluss der Asphärizität auf die aerodynamischen und optischen Eigenschaften kann durch sogenannte Formfaktoren unter Verwendung einer Referenzgröße berücksichtigt werden. Für wissenschaftliche Fragestellungen, die sowohl auf aerodynamischen wie auch optischen Aspekten beruhen, bedarf es einer vollständigen Betrachtung des Einflusses der Partikelmorphologie, um ein physikalisch plausibles Ergebnis zu erhalten. Gegenstand dieser Arbeit ist die Analyse der Relationen zwischen aerodynamischen und optischen Eigenschaften. Ziel ist die approximative Darstellung der optischen Formfaktoren durch den aerodynamischen Formfaktor als Maßzahl der Asphärizität. Hierfür wurden sowohl geometrische Formparameter als auch aerodynamische und optische Formfaktoren für ein Ensemble von regelmäßigen und unregelmäßigen Partikeln simuliert. Der Approximation der optischen Formfaktoren durch den aerodynamischen Formfaktor werden theoretische Überlegungen und Ergebnisse numerischer Simulationen vorangestellt. Die optischen Formfaktoren sind dabei primär eine Funktion des Größenparameters (Partikelgröße und Wellenlänge) und des aerodynamischen Formfaktors. In Laborexperimenten wurden beide Abhängigkeiten unter Verwendung von Proben mit Partikeln unterschiedlicher Asphärizität validiert. Die resultierende Approximation ermöglicht eine einfache und konsistente Beschreibung des Einflusses der Partikelmorphologie auf die aerodynamischen und optischen Eigenschaften. Dies ist eine unabdingbare Voraussetzung für eine genauere Analyse von Partikeleigenschaften, die aus aerodynamisch und optisch basierten In-situ-Messungen abgeleitet werden.

The European Centre for Medium-range Weather Forecast (ECMWF) provides an aerosol re-analysis starting from year 2003 for the Monitoring Atmospheric Composition and Climate (MACC) project. The re-analysis assimilates total aerosol optical depth retrieved by the Moderate Resolution Imaging Spectroradiometer (MODIS) to correct for model departures from observed aerosols. The reanalysis therefore combines satellite retrievals with the full spatial coverage of a numerical model. Re-analysed products are used here to estimate the shortwave direct and first indirect radiative forcing of anthropogenic aerosols over the period 2003–2010, using methods previously applied to satellite retrievals of aerosols and clouds. The best estimate of globally-averaged, all-sky direct radiative forcing is −0.7±0.3Wm−2. The standard deviation is obtained by a Monte-Carlo analysis of uncertainties, which accounts for uncertainties in the aerosol anthropogenic fraction, aerosol absorption, and cloudy-sky effects. Further accounting for differences between the present-day natural and pre-industrial aerosols provides a direct radiative forcing estimate of −0.4±0.3Wm−2. The best estimate of globally-averaged, all-sky first indirect radiative forcing is −0.6±0.4Wm−2. Its standard deviation accounts for uncertainties in the aerosol anthropogenic fraction, and in cloud albedo and cloud droplet number concentration susceptibilities to aerosol changes. The distribution of first indirect radiative forcing is asymmetric and is bounded by −0.1 and −2.0Wm−2. In order to decrease uncertainty ranges, better observational constraints on aerosol absorption and sensitivity of cloud droplet number concentrations to aerosol changes are required.

An increasing trend in surface solar radiation (solar brightening) has been observed over Europe since the 1990s, linked to economic developments and air pollution regulations and their direct as well as cloud-mediated effects on radiation. Here, we find that the all-sky solar brightening trend (1990–2005) over Europe from seven out of eight models (historical simulations in the Fifth Coupled Model Intercomparison Project) scales well with the regional and global mean effective forcing by anthropogenic aerosols (idealized “present-day” minus “preindustrial” runs). The reason for this relationship is that models that simulate stronger forcing efficiencies and stronger radiative effects by aerosol-cloud interactions show both a stronger aerosol forcing and a stronger solar brightening. The all-sky solar brightening is the observable from measurements (4.06 ± 0.60Wm−2 decade−1), which then allows to infer a global mean total aerosol effective forcing at about −1.30Wm−2 with standard deviation ±0.40Wm−2.

Large uncertainties exist in estimations of aerosol direct radiative forcing and indirect radiative forcing, and the values derived from globalmodeling differ substantially with satellite-based calculations. Following the approach of Quaas et al. (2008; hereafter named Quaas2008),we reassess satellite-based clear- and cloudy-sky radiative forcings and their seasonal variations by employing updated satellite products from 2004 to 2011 in combination with the anthropogenic aerosol optical depth (AOD) fraction obtained frommodel simulations using the Goddard Earth Observing System-Chemistry-Advanced ParticleMicrophysics (GEOS-Chem-APM). Our derived annual mean aerosol clear-sky forcing (-0.59 W m-2) is lower, while the cloudy-sky forcing (-0.34 W m-2) is higher than the corresponding results (-0.9Wm-2 and -0.2W m-2, respectively) reported in Quaas2008. Our study indicates that the derived forcings are sensitive to the anthropogenic AOD fraction and its spatial distribution but insensitive to the temporal resolution used to obtain the regression coefficients, i.e.,monthly or seasonal based. The forcing efficiency (i.e., the magnitude per anthropogenic AOD) for the clear-sky forcing based on this study is 19.9Wm-2, which is about 5% smaller than Quaas2008’s value of 21.1Wm-2. In contrast, the efficiency for the cloudy-sky forcing of this study (11 W m-2) is more than a factor of 2 larger than Quaas2008’s value of 4.7 W m-2. Uncertainties tests indicate that anthropogenic fraction of AOD strongly affects the computed forcings while using aerosol index instead of AOD from satellite data as aerosol proxy does not appear to cause any significant differences in regression slopes and derived forcings.

Ship tracks are regarded as the most obvious manifestations of the effect of anthropogenic aerosol particles on clouds (indirect effect). However, it is not yet fully quantified whether there are climatically relevant effects on large scales beyond the narrow ship tracks visible in selected satellite images. A combination of satellite and reanalysis data is used here to analyze regions in which major shipping lanes cut through otherwise pristine marine environments in subtropical and tropical oceans. We expect the region downwind of a shipping lane is affected by the aerosol produced by shipping emissions but not the one upwind. Thus, differences in microphysical and macrophysical cloud properties are analyzed statistically. We investigate microphysical and macrophysical cloud properties as well as the aerosol optical depth and its fine-mode fraction for the years 2005–2007 as provided for by retrievals of the two Moderate Resolution Imaging Spectroradiometer instruments. Water-cloud properties include cloud optical depth, cloud droplet effective radius, cloud top temperature, and cloud top pressure. Large-scale meteorological parameters are taken from ERA-Interim reanalysis data and microwave remote sensing (sea surface temperature). We analyze the regions of interest in a Eulerian and Lagrangian sense, i.e., sampling along shipping lanes and sampling along wind trajectories, respectively. No statistically significant impacts of shipping emissions on large-scale cloud fields could be found in any of the selected regions close to major shipping lanes. In conclusion, the net indirect effects of aerosols from ship emissions are not large enough to be distinguishable from the natural dynamics controlling cloud presence and formation.