Potential source regions and processes of aerosol in the summer Arctic

Sub-micrometer particle size distributions measured during four summer cruises of the Swedish icebreaker Oden 1991, 1996, 2001, and 2008 were combined with dimethyl sulfide gas data, back trajectories, and daily maps of pack ice cover in order to investigate source areas and aerosol formation processes of the boundary layer aerosol in the central Arctic. With a clustering algorithm, potential aerosol source areas were explored. Clustering of particle size distributions together with back trajectories delineated five potential source regions and three different aerosol types that covered most of the Arctic Basin: marine, newly formed and aged particles over the pack ice. Most of the pack ice area with < 15% of open water under the trajectories exhibited the aged aerosol type with only one major mode around 40 nm. For newly formed particles to occur, two conditions had to be fulfilled over the pack ice: the air had spent 10 days while traveling over ever more contiguous ice and had traveled over less than 30% open water during the last 5 days. Additionally, the air had experienced more open water (at least twice as much as in the cases of aged aerosol) during the last 4 days before arrival in heavy ice conditions at Oden. Thus we hypothesize that these two conditions were essential factors for the formation of ultrafine particles over the central Arctic pack ice. In a comparison the Oden data with summer size distribution data from Alert, Nunavut, and Mt. Zeppelin, Spitsbergen, we confirmed the Oden findings with respect to particle sources over the central Arctic. Future more frequent broken-ice or open water patches in summer will spur biological activity in surface water promoting the formation of biological particles. Thereby low clouds and fogs and subsequently the surface energy balance and ice melt may be affected

Reconciling aerosol light extinction measurements from spaceborne lidar observations and in situ measurements in the Arctic

© Author(s) 2014. This work is distributed under the Creative Commons Attribution 3.0 License.In this study we investigate to what degree it is possible to reconcile continuously recorded particle light extinction coefficients derived from dry in situ measurements at Zeppelin station (78.92° N, 11.85° E; 475 m above sea level), Ny-Ålesund, Svalbard, that are recalculated to ambient relative humidity, as well as simultaneous ambient observations with the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite. To our knowledge, this represents the first study that compares spaceborne lidar measurements to optical aerosol properties from short-term in situ observations (averaged over 5 h) on a case-by-case basis. Finding suitable comparison cases requires an elaborate screening and matching of the CALIOP data with respect to the location of Zeppelin station as well as the selection of temporal and spatial averaging intervals for both the ground-based and spaceborne observations. Reliable reconciliation of these data cannot be achieved with the closest-approach method, which is often used in matching CALIOP observations to those taken at ground sites. This is due to the transport pathways of the air parcels that were sampled. The use of trajectories allowed us to establish a connection between spaceborne and ground-based observations for 57 individual overpasses out of a total of 2018 that occurred in our region of interest around Svalbard (0 to 25° E, 75 to 82° N) in the considered year of 2008. Matches could only be established during winter and spring, since the low aerosol load during summer in connection with the strong solar background and the high occurrence rate of clouds strongly influences the performance and reliability of CALIOP observations. Extinction coefficients in the range of 2 to 130 Mmg-1 at 532 nm were found for successful matches with a difference of a factor of 1.47 (median value for a range from 0.26 to 11.2) between the findings of in situ and spaceborne observations (the latter being generally larger than the former). The remaining difference is likely to be due to the natural variability in aerosol concentration and ambient relative humidity, an insufficient representation of aerosol particle growth, or a misclassification of aerosol type (i.e., choice of lidar ratio) in the CALIPSO retrieval.Peer reviewe

New trajectory-driven aerosol and chemical process model Chemical and Aerosol Lagrangian Model (CALM)

A new Chemical and Aerosol Lagrangian Model (CALM) has been developed and tested. The model incorporates all central aerosol dynamical processes, from nucleation, condensation, coagulation and deposition to cloud formation and in-cloud processing. The model is tested and evaluated against observations performed at the SMEAR II station located at Hyytiälä (61° 51&apos; N, 24° 17&apos; E) over a time period of two years, 2000–2001. The model shows good agreement with measurements throughout most of the year, but fails in reproducing the aerosol properties during the winter season, resulting in poor agreement between model and measurements especially during December–January. Nevertheless, through the rest of the year both trends and magnitude of modal concentrations show good agreement with observation, as do the monthly average size distribution properties. The model is also shown to capture individual nucleation events to a certain degree. This indicates that nucleation largely is controlled by the availability of nucleating material (as prescribed by the [H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;]), availability of condensing material (in this model 15% of primary reactions of monoterpenes (MT) are assumed to produce low volatile species) and the properties of the size distribution (more specifically, the condensation sink). This is further demonstrated by the fact that the model captures the annual trend in nuclei mode concentration. The model is also used, alongside sensitivity tests, to examine which processes dominate the aerosol size distribution physical properties. It is shown, in agreement with previous studies, that nucleation governs the number concentration during transport from clean areas. It is also shown that primary number emissions almost exclusively govern the CN concentration when air from Central Europe is advected north over Scandinavia. We also show that biogenic emissions have a large influence on the amount of potential CCN observed over the boreal region, as shown by the agreement between observations and modeled results for the receptor SMEAR II, Hyytiälä, during the studied period

An investigation of processes controlling the evolution of the boundary layer aerosol size distribution properties at the Swedish background station Aspvreten

International audienceAerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E). Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing different stages of the aerosol lifecycle. The atmospheric aerosol size distributions were interpreted as belonging to fresh, intermediate and aged types of size distribution. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-Lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features that are likely to be related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability of the aerosol size distribution. Processing by clouds and precipitation is shown to be especially crucial in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions indicating signs of recent new particle formation (~30% of the observed size distributions) represent the first stage in the lifecycle. Aging of the aerosol size distribution may follow two branches: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area) in environments similar to the one studied

Seasonal variation of aerosol water uptake and its impact on the direct radiative effect at Ny-Ålesund, Svalbard

© Author(s) 2014. This work is distributed under the Creative Commons Attribution 3.0 LicenseIn this study we investigated the impact of water uptake by aerosol particles in ambient atmosphere on their optical properties and their direct radiative effect (ADRE, W m-2) in the Arctic at Ny-Ålesund, Svalbard, during 2008. To achieve this, we combined three models, a hygroscopic growth model, a Mie model and a radiative transfer model, with an extensive set of observational data. We found that the seasonal variation of dry aerosol scattering coefficients showed minimum values during the summer season and the beginning of fall (July-August-September), when small particles (< 100 nm in diameter) dominate the aerosol number size distribution. The maximum scattering by dry particles was observed during the Arctic haze period (March-April-May) when the average size of the particles was larger. Considering the hygroscopic growth of aerosol particles in the ambient atmosphere had a significant impact on the aerosol scattering coefficients: the aerosol scattering coefficients were enhanced by on average a factor of 4.30 ± 2.26 (mean ± standard deviation), with lower values during the haze period (March-April-May) as compared to summer and fall. Hygroscopic growth of aerosol particles was found to cause 1.6 to 3.7 times more negative ADRE at the surface, with the smallest effect during the haze period (March-April-May) and the highest during late summer and beginning of fall (July-August-September).Peer reviewe

Multi-year Measurements of Black Carbon Aerosol over Barrow and Ny-Alesund in the Arctic

第6回極域科学シンポジウム分野横断セッション：[IA] 急変する北極気候システム及びその全球的な影響の総合的解明―GRENE北極気候変動研究事業研究成果報告2015―11月19日（木）　国立極地研究所１階交流アトリウ

Inverse modeling of cloud-aerosol interactions – Part 1: Detailed response surface analysis

This is the final version of the article. Available from EGU via the DOI in this record.New methodologies are required to probe the sensitivity of parameters describing cloud droplet activation. This paper presents an inverse modeling-based method for exploring cloud-aerosol interactions via response surfaces. The objective function, containing the difference between the measured and model predicted cloud droplet size distribution is studied in a two-dimensional framework, and presented for pseudo-adiabatic cloud parcel model parameters that are pair-wise selected. From this response surface analysis it is shown that the susceptibility of cloud droplet size distribution to variations in different aerosol physiochemical parameters is highly dependent on the aerosol environment and meteorological conditions. In general the cloud droplet size distribution is most susceptible to changes in the updraft velocity. A shift towards an increase in the importance of chemistry for the cloud nucleating ability of particles is shown to exist somewhere between marine average and rural continental aerosol regimes. We also use these response surfaces to explore the feasibility of inverse modeling to determine cloud-aerosol interactions. It is shown that the "cloud-aerosol" inverse problem is particularly difficult to solve due to significant parameter interaction, presence of multiple regions of attraction, numerous local optima, and considerable parameter insensitivity. The identifiability of the model parameters will be dependent on the choice of the objective function. Sensitivity analysis is performed to investigate the location of the information content within the calibration data to confirm that our choice of objective function maximizes information retrieval from the cloud droplet size distribution. Cloud parcel models that employ a moving-centre based calculation of the cloud droplet size distribution pose additional difficulties when applying automatic search algorithms for studying cloud-aerosol interactions. To aid future studies, an increased resolution of the region of the size spectrum associated with droplet activation within cloud parcel models, or further development of fixed-sectional cloud models would be beneficial. Despite these improvements, it is demonstrated that powerful search algorithms remain necessary to efficiently explore the parameter space and successfully solve the cloud-aerosol inverse problem.We gratefully acknowledge the financial support of the Bert Bolin Centre for Climate research. We gratefully appreciate G. J. Roelofs, IMAU, Utrecht, the Netherlands, for providing us with the pseudo-adiabatic cloud parcel model used in this study. We gratefully acknowledge Hamish Struthers valuable discussions and his help to improve the readability of the manuscript. Some of the calculations made during the course of this study have been made possible using the LISA cluster from the SARA centre for parallel computing at the University of Amsterdam, the Netherlands. AS acknowledges support from an Office of Naval Research YIP award (N00014-10-1-0811).The authors acknowledge the Swedish Environmental Monitoring Program a

A pseudo-Lagrangian model study of the size distribution properties over Scandinavia: transport from Aspvreten to Värriö

International audienceThe evolution of the aerosol size distribution during transport between Aspvreten (58.8° N, 17.4° E) and Värriö (67.46° N, 29.35° E) was studied using a pseudo-Lagrangian approach. Aerosol dynamic processes were studied and interpreted utilizing a state-of-the-art aerosol dynamic box model UHMA (University of Helsinki Multicomponent Aerosol model) complemented with OH, NO3, O3 and terpene chemistry. In the model simulations, the growth and formation of aerosol particles was controlled by sulphuric acid, ammonia, water and an unidentified low volatile organic compound. This organic compound was assumed to be a product of terpene oxidation with a yield of 13% in the base case conditions. Changes of aerosol size distribution properties during transport between the stations were examined in twelve clear sky cases. On average, the modelled number agreed fairly well with observations. Mass concentration was overestimated by 10%. Apart from dilution, the only removal mechanism for aerosol mass is dry deposition. A series of sensitivity tests performed revealed that the absolute magnitude of dry deposition effects on the aerosol size distribution is slow overall. Furthermore, nucleation does not leave a significant contribution to aerosol number in the selected cases. The sensitivity of the modelled size distribution to concentration of precursor gases and oxidants is, however, obvious. In order to explain observed mass increase during transport we conclude that a yield of low volatile products from oxidation of terpenes of 10?15% is required to explain observed growth rates. Coagulation is acknowledged to be highly important in modelled cases

Inverse modelling of cloud-aerosol interactions – Part 2: Sensitivity tests on liquid phase clouds using a Markov chain Monte Carlo based simulation approach

This paper presents a novel approach to investigate cloud-aerosol interactions by coupling a Markov chain Monte Carlo (MCMC) algorithm to an adiabatic cloud parcel model. Despite the number of numerical cloud-aerosol sensitivity studies previously conducted few have used statistical analysis tools to investigate the global sensitivity of a cloud model to input aerosol physiochemical parameters. Using numerically generated cloud droplet number concentration (CDNC) distributions (i.e. synthetic data) as cloud observations, this inverse modelling framework is shown to successfully estimate the correct calibration parameters, and their underlying posterior probability distribution. &lt;br&gt;&lt;/br&gt; The employed analysis method provides a new, integrative framework to evaluate the global sensitivity of the derived CDNC distribution to the input parameters describing the lognormal properties of the accumulation mode aerosol and the particle chemistry. To a large extent, results from prior studies are confirmed, but the present study also provides some additional insights. There is a transition in relative sensitivity from very clean marine Arctic conditions where the lognormal aerosol parameters representing the accumulation mode aerosol number concentration and mean radius and are found to be most important for determining the CDNC distribution to very polluted continental environments (aerosol concentration in the accumulation mode &gt;1000 cm&lt;sup&gt;−3&lt;/sup&gt;) where particle chemistry is more important than both number concentration and size of the accumulation mode. &lt;br&gt;&lt;/br&gt; The competition and compensation between the cloud model input parameters illustrates that if the soluble mass fraction is reduced, the aerosol number concentration, geometric standard deviation and mean radius of the accumulation mode must increase in order to achieve the same CDNC distribution. &lt;br&gt;&lt;/br&gt; This study demonstrates that inverse modelling provides a flexible, transparent and integrative method for efficiently exploring cloud-aerosol interactions with respect to parameter sensitivity and correlation