Aerosols change the Earth's energy balance. Black carbon (BC) aerosols are a product of incomplete combustion of fossil fuels and biomass burning and cause a net warming through aerosol radiation interactions (ari) and aerosol cloud interactions (aci). BC aerosols have potentially strong implications on the Arctic climate, yet the net global climate effect of BC is very uncertain. Best estimates assume a net warming effect, roughly half to that of CO2. However, the time scales during which CO2 emissions affect the global climate are on the order of hundreds of years, while BC is a short-lived climate pollutant (SLCP) with atmospheric life times of days to weeks. Climate models or atmospheric transport models struggle to emulate the seasonality and amplitude of BC concentrations in the Arctic, which are low in summer and high in winter/spring during the so called Arctic haze season. The high uncertainties regarding BC's climate impact are not only related to ari and aci, but also due to model parameterizations of BC lifetime and transport, and the highly uncertain estimates of global and regional BC emissions. Given the high uncertainties in technology-based emission inventories (EI), there is a need for an observation-based assessment of sources of BC in the atmosphere. We study short-term and long-term observations of elemental carbon (EC), the mass-based analog of optically-defined BC. EC aerosol concentrations and carbon-isotope-based (δ13C and ∆14C) sources were constrained (top-down) for three Arctic receptor sites in Abisko (northern Sweden), Tiksi (East Siberian Russia), and Zeppelin (on Svalbard, Norway). The radiocarbon (∆14C) signature allows to draw conclusion on the EC sources (fossil fuels vs. biomass burning) with high accuracy (&lt;5% variation). Stable carbon isotopic fingerprints (δ13C) give qualitative information of the consumed fuel type, i.e. coal, C3-plants (wood), liquid fossil fuels (diesel) or gas flaring (methane and non-methane hydrocarbons). These fingerprints can be used in conjunction with Bayesian statistics, to estimate quantitative source contributions of the sources. Finally, our observations were compared to predictions from a state of the art atmospheric transport model (coupled to BC emissions), conducted by our collaborators at NILU (Norwegian Institute for Air Research). Observed BC concentrations showed a high seasonality throughout the year, with elevated concentrations in the winter, at all sites. The highest concentrations were measured on Svalbard during a short campaign (Jan-Mar 2009) focusing on BC pollution events. Long-term observations showed that Svalbard (2013) had overall the lowest annual BC concentrations, followed by Abisko (2012) and Tiksi (2013). Isotope constraints on BC combustion sources exhibited a high seasonality and big amplitude all across the Eurasian Arctic. Uniform seasonal trends were observed in all three year-round studies, showing fractions of biomass burning of 60-70% in summer and 10-40% in winter. Europe was the major source region (&gt;80%) for BC emissions arriving at Abisko and the main sources were liquid fossil fuels and biomass burning (wood). The model agreed very well with the Abisko observations, showing good model skill and relatively well constrained sources in the European regions of the EI. However, for the Svalbard and East Siberian Arctic observatories the model-observation agreement was not as good. Here, Russia, Europe and China were the major contributors to the mostly liquid fossil and biomass burning BC emissions. This showed that the EI still needs to be improved, especially in regions where emissions are high but observations are scarce (low ratio of observations to emitted pollutant quantity). Strategies for BC mitigation in the (Eurasian) Arctic are probably most efficient, if fossil fuel (diesel) emissions are tackled during winter and spring periods, all across Eurasia. / <p>At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 2: Manuscript. Paper 3: Manuscript.</p>

Le réchauffement climatique dans l’Arctique canadien est deux fois plus rapide que la moyenne globale, ce qui accélère la fonte de la banquise et bouleverse radicalement la faune, la flore et les communautés de la région tout entière. Ce réchauffement est causé non seulement par la hausse des émissions de gaz à effet de serre, mais également par des agents de forçage climatique de courte durée comme les aérosols troposphériques. Toutefois, le forçage radiatif des aérosols dans la région polaire est beaucoup moins bien estimé que celui des gaz à effet de serre, notamment le CO2, et demeure toujours incertain. Cette grande incertitude résulte principalement de la grande variabilité spatiotemporelle des propriétés chimiques et physiques des aérosols, en plus de la complexité des boucles de rétroaction observées en Arctique. D’ailleurs, les données sur les caractéristiques des aérosols et de leur répartition à travers la région sont très limitées, et ce, plus particulièrement dans le Haut-Arctique canadien. Pour remédier à ce problème, une série de mesures a été effectuée sur une période de 3 ans (2016-2019) dans le laboratoire de recherche sur l’environnement atmosphérique polaire (PEARL, 80N 86O) situé près de la station météorologique d’Eureka, au Nunavut, Canada. La distribution en taille des aérosols a été mesurée en se servant de plusieurs instruments, dont un compteur optique de particules (OPC), un granulomètre de mobilité électrique à balayage (SMPS) et un granulomètre aérodynamique (APS). Les propriétés optiques des aérosols ont été déterminées avec deux extinctiomètres photoacoustiques (PAX) qui opèrent respectivement à des longueurs d’onde de 405 et 870 nm. Les observations réalisées à l’observatoire PEARL démontrent une forte variation saisonnière dans les propriétés optiques et microphysiques des aérosols polaires. Pendant l’hiver et le printemps, l’atmosphère arctique est envahie par une brume sèche d’origine anthropique qui se traduit par une forte augmentation dans la taille, la concentration en nombre et les propriétés optiques extensives des aérosols. Les épisodes de brume arctique commencent généralement en mi-décembre, où des évènements de poussières minérales ont aussi été observés, et se terminent en mai où la formation et le grossissement de nouvelles particules s’amorcent. Le début du printemps mesure les concentrations d’aérosol en mode accumulation les plus élevées durant l’année. Les aérosols les plus sombres qui composent la brume arctique ont été identifiés comme étant de la suie ou du carbone noir transporté dans l’Arctique à partir de l’Eurasie et de l’Alaska. Quelques relations systématiques entre les propriétés optiques et la distribution de taille des aérosols ont également été calculées et révèlent une différence majeure entre les aérosols interagissant avec la lumière à 405 et 870 nm. / Global warming in the Canadian Arctic is twice as fast as the global average, accelerating the melting of sea ice and radically disrupting the fauna, the flora, and the communities of the whole region. Arctic warming is caused not only by rising greenhouse gas emissions, but also by the short-lived climate forcing agents such as tropospheric aerosols. However, aerosol radiative forcing in the polar region is less precisely estimated than that of greenhouse gases, notably CO2, and remains highly uncertain. This large uncertainty arises mainly from the high spatiotemporal variability in aerosol chemical and physical properties, in addition to the complexity of the feedback loops observed in the Arctic. Furthermore, datasets on aerosol characteristics and their distribution across the region are very limited, particularly in the Canadian High Arctic. To address this issue, a series of measurements were conducted over a 3-year period (2016-2019) at the Polar Atmospheric Environment Research Laboratory (PEARL, 80N 86W) near Eureka weather station, in Nunavut, Canada. Aerosol size distribution was measured using several instruments including an Optical Particle Counter (OPC), a Scanning Mobility Particle Sizer (SMPS), an Aerodynamic Particle Sizer (APS). Aerosol optical properties were determined by two Photoacoustic Extinctiometers (PAXs) which operate at wavelengths of 405 nm and 870 nm, respectively. Observations made at the PEARL observatory show a strong seasonal variation in the optical and microphysical properties of polar aerosols. In the winter and spring, the Arctic atmosphere is impacted by an anthropogenic haze that results in a sharp increase in aerosol size, number concentration, and optical properties. Arctic haze episodes typically occur in mid-December, when mineral dust events have also been observed, and end in May when formation and growth of new particles begin. Early spring exhibits the highest accumulation-mode aerosol concentrations during the year. The darkest Arctic haze aerosols have been identified as soot or black carbon transported into the Arctic from Eurasia and Alaska. Some systematic relationships among aerosol optical properties and size distribution have also been calculated and reveal a major difference between aerosols interacting with light at 405 nm and 870 nm.

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.