We use a global aerosol microphysics model in combination with an offline radiative transfer model to quantify the radiative effect of biogenic secondary organic aerosol (SOA) in the present-day ...atmosphere. Through its role in particle growth and ageing, the presence of biogenic SOA increases the global annual mean concentration of cloud condensation nuclei (CCN; at 0.2% supersaturation) by 3.6-21.1%, depending upon the yield of SOA production from biogenic volatile organic compounds (BVOCs), and the nature and treatment of concurrent primary carbonaceous emissions. This increase in CCN causes a rise in global annual mean cloud droplet number concentration (CDNC) of 1.9-5.2%, and a global mean first aerosol indirect effect (AIE) of between +0.01 W m-2 and -0.12 W m-2. The radiative impact of biogenic SOA is far greater when biogenic oxidation products also contribute to the very early stages of new particle formation; using two organically mediated mechanisms for new particle formation, we simulate global annual mean first AIEs of -0.22 W m-2 and -0.77 W m-2. The inclusion of biogenic SOA substantially improves the simulated seasonal cycle in the concentration of CCN-sized particles observed at three forested sites. The best correlation is found when the organically mediated nucleation mechanisms are applied, suggesting that the first AIE of biogenic SOA could be as large as -0.77 W m-2. The radiative impact of SOA is sensitive to the presence of anthropogenic emissions. Lower background aerosol concentrations simulated with anthropogenic emissions from 1750 give rise to a greater fractional CCN increase and a more substantial first AIE from biogenic SOA. Consequently, the anthropogenic indirect radiative forcing between 1750 and the present day is sensitive to assumptions about the amount and role of biogenic SOA. We also calculate an annual global mean direct radiative effect of between -0.08 W m-2 and -0.78 W m-2 in the present day, with uncertainty in the amount of SOA produced from the oxidation of BVOCs accounting for most of this range.
Secondary new particle formation affects atmospheric aerosol and cloud droplet numbers and thereby, the aerosol effects on climate. In this paper, the frequency of nucleation events and the ...associated particle formation and growth rates, along with their seasonal variation, was analysed based on over ten years of aerosol measurements conducted at the Pallas GAW station in northern Finland. The long-term measurements also allowed a detailed examination of factors possibly favouring or suppressing particle formation. Effects of meteorological parameters and air mass properties as well as vapour sources and sinks for particle formation frequency and event parameters were inspected. In addition, the potential of secondary particle formation to increase the concentration of cloud condensation nuclei (CCN) sized particles was examined. Findings from these long-term measurements confirmed previous observations: event frequency peaked in spring and the highest growth rates were observed in summer, affiliated with increased biogenic activity. Events were almost exclusively observed in marine air masses on sunny cloud-free days. A low vapour sink by the background particle population as well as an elevated sulphuric acid concentration were found to favour particle formation. These were also conditions taking place most likely in marine air masses. Inter-annual trend showed a minimum in event frequency in 2003, when also the smallest annual median of growth rate was observed. This gives further evidence of the importance and sensitivity of particle formation for the condensing vapour concentrations at Pallas site. The particle formation was observed to increase CCN80 (>80 nm particle number) concentrations especially in summer and autumn seasons when the growth rates were the highest. When the growing mode exceeded the selected 80 nm limit, on average in those cases, 211 ± 114% increase of CCN80 concentrations was observed.
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.
Particles in the atmosphere are of concern due to their toxic properties and effects on climate. In coastal areas, ship emissions can be a significant anthropogenic source. In this study we ...investigated the contribution from ship emissions to the total particle number and mass concentrations at a remote location. We studied the particle number concentration (12 to 490 nm in diameter), the mass concentration (12 to 150 nm in diameter) and number and volume size distribution of aerosol particles in ship plumes for a period of 4.5 months at Høvsøre, a coastal site on the western coast of Jutland in Denmark. During episodes of western winds, the site is about 50 km downwind of a major shipping lane and the plumes are approximately 1 hour old when they arrive at the site. We have used a sliding percentile-based method for separating the plumes from the measured background values and to calculate the ship plume contribution to the total particle number and PM0.15 mass concentration (mass of particles below 150 nm in diameter, converted from volume assuming sphericity) at the site. The method is not limited to particle number or volume concentration, but can also be used for different chemical species in both particle and gas phase. The total number of analyzed ship plumes was 726, covering on average 19% of the time when air masses were arriving at the site over the shipping lane. During the periods when plumes were present, the particle concentration exceeded the background values on average by 790 cm−3 by number and 0.10 μg m−3 by mass. The corresponding daily average values were 170 cm−3 and 0.023 μg m−3, respectively. This means that the ship plumes contributed between 11 and 19% to the particle number concentration and between 9 and 18% to PM0.15 during days when air was arriving over the shipping lane. The estimated annual contribution from ship plumes, where all wind directions were included, was in the range of 5–8% in particle number concentration and 4–8% in PM0.15.
Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface ...aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-Å lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
Biogenic volatile organic compounds (BVOCs) emitted by vegetation play an important role for aerosol mass loadings since the oxidation products of these compounds can take part in the formation and ...growth of secondary organic aerosols (SOA). The concentrations and properties of BVOCs and their oxidation products in the atmosphere are poorly characterized, which leads to high uncertainties in modeled SOA mass and properties. In this study, the formation of SOA has been modeled along an air-mass trajectory over northern European boreal forest using two aerosol dynamics box models where the prediction of the condensable organics from the gas-phase oxidation of BVOC is handled with schemes of varying complexity. The use of box model simulations along an air-mass trajectory allows us to compare, under atmospheric relevant conditions, different model parameterizations and their effect on SOA formation. The result of the study shows that the modeled mass concentration of SOA is highly dependent on the organic oxidation scheme used to predict oxidation products. A near-explicit treatment of organic gas-phase oxidation (Master Chemical Mechanism version 3.2) was compared to oxidation schemes that use the volatility basis set (VBS) approach. The resulting SOA mass modeled with different VBS schemes varies by a factor of about 7 depending on how the first-generation oxidation products are parameterized and how they subsequently age (e.g., how fast the gas-phase oxidation products react with the OH radical, how they respond to temperature changes, and if they are allowed to fragment during the aging process). Since the VBS approach is frequently used in regional and global climate models due to its relatively simple treatment of the oxidation products compared to near-explicit oxidation schemes, a better understanding of the above-mentioned processes is needed. Based on the results of this study, fragmentation should be included in order to obtain a realistic SOA formation. Furthermore, compared to the most commonly used VBS schemes, the near-explicit method produces less – but more oxidized – SOA.
Concurrent measurement of aerosols, cloud condensation nuclei (CCN) and cloud droplet activation were carried out as a part of the third Pallas Cloud Experiment (PaCE-3) which took place at a ground ...based site located on northern Finland during the autumn of 2009. In this study, we investigate relationships between the aerosol properties, CCN and size resolved cloud droplet activation. During the investigated cloudy periods, the inferred number of cloud droplets (CDNC) varied typically between 50 and 150 cm super(-3) and displayed a linear correlation both with the number of particles having sizes over 100 nm and with the CCN concentrations at 0.4% supersaturation. Furthermore, the diameter corresponding to the 50% activation fraction, D sub(50), was generally in the range of 80 to 120 nm. The measured CCN concentrations were compared with predictions of a numerical model which used the measured size distribution and size resolved hygroscopicity as input. Assuming that the droplet surface tension is equal to that of water, the measured and predicted CCN concentrations were generally within 30%. We also simulated size dependent cloud droplet activation with a previously developed air parcel model. By forcing the model to reproduce the experimental values of CDNC, adiabatic estimates for the updraft velocity and the maximum supersaturation reached in the clouds were derived. Performed sensitivity studies showed further that the observed variability in CDNC was driven mainly by changes in the particle size distribution while the variations in the updraft velocity and hygroscopicity contributed to a lesser extent. The results of the study corroborate conclusions of previous studies according to which the number of cloud droplets formed in clean air masses close to the Arctic is determined mainly by the number of available CCN.
This study presents analysis of in situ measurements conducted over the period 2005–2014 in the Indian Himalayas to give a thorough overview of the factors and causes that drive aerosol properties. ...Aerosol extensive properties (namely, particle number concentration, scattering coefficient, equivalent black carbon, PM2.5, and PM10) have 1.5–2 times higher values in the early to late afternoon than during the night, and a strong seasonality. The interannual variability is ±20% for both PM2.5 and total particle number concentration. Analysis of the data shows statistically significant decreasing trends of −2.3 μg m−3 year−1 and −2.7 μg m−3 year−1 for PM2.5 and PM10, respectively, over the study period. The mountainous terrain site (Mukteshwar, MUK) is primarily under the influence of air from the plains. This is due to convective transport processes that are enhanced by local and mesoscale topography, leading to pronounced valley/mountain winds and consequently to atmospheric boundary layer air lifting from the plains below. The transport from plains is evident in seasonal‐diurnal patterns observed at MUK. The timing of the patterns corresponds with changes in turbulence and water vapor (q). According to our analysis, using these as proxies is a viable method for examining boundary layer influence in the absence of direct atmospheric boundary layer height measurements. Comparing the measurements with climate models shows that even regional climate models have problems capturing the orographic influence accurately at MUK, highlighting the importance of long‐term direct measurements at multiple points to understand aerosol behavior in mountainous areas.
Key Points
Long‐term aerosol observations were conducted in the central Himalaya, and turbulence and water vapor were used to describe mixing layer diurnal cycle
Aerosol variables clearly present clusters of highest concentration during the afternoon hours in the premonsoon and postmonsoon season
Transport and valley wind influence to the atmospheric boundary layer are the predominant reasons for the poor performance of climate models
In order to quantify the effects of absorbing contaminants on snow, a series of spectral reflectance measurements were conducted. Chimney soot, volcanic sand, and glaciogenic silt were deposited on a ...natural snow surface in a controlled way as a part of the Soot on Snow (SoS) campaign. The bidirectional reflectance factors of these soiled surfaces and untouched snow were measured using the Finnish Geodetic Institute's Field Goniospectropolariradiometer, FIGIFIGO. A remarkable feature is the fact that the absorbing contaminants on snow enhanced the metamorphism of snow under strong sunlight in our experiments. Immediately after deposition, the contaminated snow surface appeared darker than the natural snow in all viewing directions, but the absorbing particles sank deep into the snow in minutes. The nadir measurement remained the darkest, but at larger zenith angles, the surface of the contaminated snow changed back to almost as white as clean snow. Thus, for a ground observer the darkening caused by impurities can be completely invisible, overestimating the albedo, but a nadir-observing satellite sees the darkest points, underestimating the albedo. Through a reciprocity argument, we predict that at noon, the albedo perturbation should be lower than in the morning or afternoon. When sunlight stimulates sinking more than melting, the albedo should be higher in the afternoon than in the morning, and vice versa when melting dominates. However, differences in the hydrophobic properties, porosity, clumping, or size of the impurities may cause different results than observed in these measurements.
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