Browsing by Author "Ogren, J.A."
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- ItemAerosol decadal trends - Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations(München : European Geopyhsical Union, 2013) Asmi, A.; Collaud Coen, M.; Ogren, J.A.; Andrews, E.; Sheridan, P.; Jefferson, A.; Weingartner, E.; Baltensperger, U.; Bukowiecki, N.; Lihavainen, H.; Kivekäs, N.; Asmi, E.; Aalto, P.P.; Kulmala, M.; Wiedensohler, A.; Birmili, W.; Hamed, A.; O'Dowd, C.; Jennings, S.G.; Weller, R.; Flentje, H.; Fjaeraa, A.M.; Fiebig, M.; Myhre, C.L.; Hallar, A.G.; Swietlicki, E.; Kristensson, A.; Laj, P.We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.
- ItemCharacterization and intercomparison of aerosol absorption photometers: Result of two intercomparison workshops(München : European Geopyhsical Union, 2011) Müller, T.; Henzing, J.S.; de Leeuw, G.; Wiedensohler, A.; Alastuey, A.; Angelov, H.; Bizjak, M.; Collaud Coen, M.; Engström, J.E.; Gruening, C.; Hillamo, R.; Hoffer, A.; Imre, K.; Ivanow, P.; Jennings, G.; Sun, J.Y.; Kalivitis, N.; Karlsson, H.; Komppula, M.; Laj, P.; Li, S.-M.; Lunder, C.; Marinoni, A.; Martins dos Santos, S.; Moerman, M.; Nowak, A.; Ogren, J.A.; Petzold, A.; Pichon, J.M.; Rodriquez, S.; Sharma, S.; Sheridan, P.J.; Teinilä, K.; Tuch, T.; Viana, M.; Virkkula, A.; Weingartner, E.; Wilhelm, R.; Wang, Y.Q.Absorption photometers for real time application have been available since the 1980s, but the use of filter-based instruments to derive information on aerosol properties (absorption coefficient and black carbon, BC) is still a matter of debate. Several workshops have been conducted to investigate the performance of individual instruments over the intervening years. Two workshops with large sets of aerosol absorption photometers were conducted in 2005 and 2007. The data from these instruments were corrected using existing methods before further analysis. The inter-comparison shows a large variation between the responses to absorbing aerosol particles for different types of instruments. The unit to unit variability between instruments can be up to 30% for Particle Soot Absorption Photometers (PSAPs) and Aethalometers. Multi Angle Absorption Photometers (MAAPs) showed a variability of less than 5%. Reasons for the high variability were identified to be variations in sample flow and spot size. It was observed that different flow rates influence system performance with respect to response to absorption and instrumental noise. Measurements with non absorbing particles showed that the current corrections of a cross sensitivity to particle scattering are not sufficient. Remaining cross sensitivities were found to be a function of the total particle load on the filter. The large variation between the response to absorbing aerosol particles for different types of instruments indicates that current correction functions for absorption photometers are not adequate.
- ItemConstrained two-stream algorithm for calculating aerosol light absorption coefficient from the Particle Soot Absorption Photometer(München : European Geopyhsical Union, 2014) Müller, T.; Virkkula, A.; Ogren, J.A.We present a new correction scheme for filter-based absorption photometers based on a constrained two-stream (CTS) radiative transfer model and experimental calibrations. The two-stream model was initialized using experimentally accessible optical parameters of the filter. Experimental calibrations were taken from the literature and from dedicated experiments for the present manuscript. Uncertainties in the model and calibration experiments are discussed and uncertainties for retrieval of absorption coefficients are derived. For single-scattering albedos lower than 0.8, the new CTS method and also other correction schemes suffer from the uncertainty in calibration experiments, with an uncertainty of about 20% in the absorption coefficient. For high single-scattering albedos, the CTS correction significantly reduces errors. At a single-scattering albedo of about 0.98 the error can be reduced to 30%, whereas errors using the Bond correction (Bond et al., 1999) are up to 100%. The correction scheme was tested using data from an independent experiment. The tests confirm the modeled performance of the correction scheme when comparing the CTS method to other established correction methods.
- ItemExplaining global surface aerosol number concentrations in terms of primary emissions and particle formation(München : European Geopyhsical Union, 2010) Spracklen, D.V.; Carslaw, K.S.; Merikanto, J.; Mann, G.W.; Reddington, C.L.; Pickering, S.; Ogren, J.A.; Andrews, E.; Baltensperger, U.; Weingartner, E.; Boy, M.; Kulmala, M.; Laakso, L.; Lihavainen, H.; Kivekäs, N.; Komppula, M.; Mihalopoulos, N.; Kouvarakis, G.; Jennings, S.G.; O'Dowd, C.; Birmili, W.; Wiedensohler, A.; Weller, R.; Gras, J.; Laj, P.; Sellegri, K.; Bonn, B.; Krejci, R.; Laaksonen, A.; Hamed, A.; Minikin, A.; Harrison, R.M.; Talbot, R.; Sun, J.We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
- ItemIntercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity(München : European Geopyhsical Union, 2014) Mann, G.W.; Carslaw, K.S.; Reddington, C.L.; Pringle, K.J.; Schulz, M.; Asmi, A.; Spracklen, D.V.; Ridley, D.A.; Woodhouse, M.T.; Lee, L.A.; Zhang, K.; Ghan, S.J.; Easter, R.C.; Liu, X.; Stier, P.; Lee, Y.H.; Adams, P.J.; Tost, H.; Lelieveld, J.; Bauer, S.E.; Tsigaridis, K.; van Noije, T.P.C.; Strunk, A.; Vignati, E.; Bellouin, N.; Dalvi, M.; Johnson, C.E.; Bergman, T.; Kokkola, H.; von Salzen, K.; Yu, F.; Luo, G.; Petzold, A.; Heintzenberg, J.; Clarke, A.; Ogren, J.A.; Gras, J.; Baltensperger, U.; Kaminski, U.; Jennings, S.G.; O'Dowd, C.D.; Harrison, R.M.; Beddows, D.C.S.; Kulmala, M.; Viisanen, Y.; Ulevicius, V.; Mihalopoulos, N.; Zdimal, V.; Fiebig, M.; Hansson, H.-C.; Swietlicki, E.; Henzing, J.S.Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.
- ItemMobility particle size spectrometers: Harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions(München : European Geopyhsical Union, 2012) Wiedensohler, A.; Birmili, W.; Nowak, A.; Sonntag, A.; Weinhold, K.; Merkel, M.; Wehner, B.; Tuch, T.; Pfeifer, S.; Fiebig, M.; Fjäraa, A.M.; Asmi, E.; Sellegri, K.; Depuy, R.; Venzac, H.; Villani, P.; Laj, P.; Aalto, P.; Ogren, J.A.; Swietlick, E.; Williams, P.; Roldin, P.; Quincey, P.; Hüglin, C.; Fierz-Schmidhauser, R.; Gysel, M.; Weingartner, E.; Riccobono, F.; Santos, S.; Grüning, C.; Faloon, K.; Beddows, D.; Harrison, R.; Monahan, C.; Jennings, S.G.; O'Dowd, C.D.; Marinoni, A.; Horn, H.-G.; Keck, L.; Jiang, J.; Scheckman, J.; McMurry, P.H.; Deng, Z.; Zhao, C.S.; Moerman, M.; Henzing, B.; de Leeuw, G.; Löschau, G.; Bastian, S.Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.
- ItemRecommendations for reporting "black carbon" measurements(München : European Geopyhsical Union, 2013) Petzold, A.; Ogren, J.A.; Fiebig, M.; Laj, P.; Li, S.-M.; Baltensperger, U.; Holzer-Popp, T.; Kinne, S.; Pappalardo, G.; Sugimoto, N.; Wehrli, C.; Wiedensohler, A.; Zhang, X.-Y.Although black carbon (BC) is one of the key atmospheric particulate components driving climate change and air quality, there is no agreement on the terminology that considers all aspects of specific properties, definitions, measurement methods, and related uncertainties. As a result, there is much ambiguity in the scientific literature of measurements and numerical models that refer to BC with different names and based on different properties of the particles, with no clear definition of the terms. The authors present here a recommended terminology to clarify the terms used for BC in atmospheric research, with the goal of establishing unambiguous links between terms, targeted material properties and associated measurement techniques.