Estimating seasonal variations in cloud droplet number concentration over the boreal forest from satellite observations

Seasonal variations in cloud droplet number concentration (NCD) in low-level stratiform clouds over the boreal forest are estimated from MODIS observations of cloud optical and microphysical properties, using a sub-adiabatic cloud model to interpret vertical profiles of cloud properties. An uncertainty analysis of the cloud model is included to reveal the main sensitivities of the cloud model. We compared the seasonal cycle in NCD, obtained using 9 yr of satellite data, to surface concentrations of potential cloud activating aerosols, measured at the SMEAR II station at Hyytiälä in Finland. The results show that NCD and cloud condensation nuclei (CCN) concentrations have no clear correlation at seasonal time scale. The fraction of aerosols that actually activate as cloud droplet decreases sharply with increasing aerosol concentrations. Furthermore, information on the stability of the atmosphere shows that low NCD is linked to stable atmospheric conditions. Combining these findings leads to the conclusion that cloud droplet activation for the studied clouds over the boreal forest is limited by convection. Our results suggest that it is important to take the strength of convection into account when studying the influence of aerosols from the boreal forest on cloud formation, although they do not rule out the possibility that aerosols from the boreal forest affect other types of clouds with a closer coupling to the surfac

Ternary nucleation of H_2SO_4, NH_3 and H_2O

A classical theory of the ternary homogeneous nucleation of sulfuric acid—ammonia—water is presented. For NH3 mixing ratios exceeding 1 ppt, the presence of ammonia enhances the binary (sulfuric acid—water) nucleation rate by several orders of magnitude. However, the limiting component for ternary nucleation—as for binary nucleation—is sulfuric acid. The sulfuric acid concentration needed for significant ternary nucleation is several orders of magnitude below that required in binary case

Commentary on cloud modelling and the mass accommodation coefficient of water

International audienceThe mass accommodation coefficient of water is a quantity for which different experimental techniques have yielded conflicting values in the range 0.04-1. From the viewpoint of cloud modelling, this is an unfortunate situation, since the value of the mass accommodation coefficient affects the model results, e.g. the number concentration of activated cloud droplets. In this commentary we note that in cloud modelling, the primary quantity of interest is the droplet growth rate rather than the mass accommodation coefficient, and that experimental investigations of droplet growth rates provide more direct verification of cloud models than do measurements of the mass accommodation coefficient. Furthermore, we argue that the droplet growth rates calculated in cloud model studies are consistent with experimental results obtained so far only if a mass accommodation coefficient of unity is applied

Characterization of air ions in boreal forest air during BIOFOR III campaign

International audienceThe behavior of the concentration of positive small (or cluster) air ions and naturally charged nanometer aerosol particles (aerosol ions) has been studied on the basis of measurements carried out in a boreal forest at the Hyytiälä SMEAR station, Finland, during the BIOFOR III campaign in spring 1999. Statistical characteristics of the concentrations of cluster ions, two classes of aerosol ions of the sizes of 2.5?8 nm and 8?ca 20 nm and the quantities that determine the balance of small ions in the atmosphere have been given for the nucleation event days and non-event days. The dependence of small ion concentration on the ion loss (sink) due to aerosol particles was investigated applying a model of bipolar diffusion charging of particles by small ions. The small ion concentration and the ion sink were closely correlated (correlation coefficient 87%) when the fog events and the hours of high relative humidity (above 97%), as well as nocturnal calms and weak wind (wind speed-1 had been excluded. In the case of nucleation burst events, variations in the concentration of small positive ions were in accordance with the changes caused by the ion sink due to aerosols; no clear indication of positive ion depletion by ion-induced nucleation was found. The estimated average ionization rate of air at the Hyytiälä station in early spring, when the ground was partly covered with snow, was about 4.8 ion pairs cm-3 s-1. The study of the charging state of nanometer aerosol particles (2.5?8 nm) revealed a strong correlation (correlation coefficient 88%) between the concentrations of particles and their charged fraction (positive air ions) during nucleation bursts. The estimated charged fraction of particles, which varied from 3% to 6% considering various nucleation event days, confirms that these particles are almost quasi-steady state charged. Also the particles and air ions in the size range of 8?ca 20 nm showed a good qualitative consistency; the correlation coefficient was 92%

The analysis of size-segregated cloud condensation nuclei counter (CCNC) data and its implications for cloud droplet activation

Ambient aerosol, CCN (cloud condensation nuclei) and hygroscopic properties were measured with a size-segregated CCNC (cloud condensation nuclei counter) in a boreal environment of southern Finland at the SMEAR (Station for Measuring Ecosystem-Atmosphere Relations) II station. The instrumental setup operated at five levels of supersaturation <i>S</i> covering a range from 0.1–1% and measured particles with a size range of 20–300 nm; a total of 29 non-consecutive months of data are presented. The median critical diameter <i>D</i>_c ranged from 150 nm at <i>S</i> of 0.1% to 46 nm at <i>S</i> of 1.0%. The median aerosol hygroscopicity parameter &kappa; ranged from 0.41 at <i>S</i> of 0.1% to 0.14 at <i>S</i> of 1.0%, indicating that ambient aerosol in Hyytiälä is less hygroscopic than the global continental or European continental averages. It is, however, more hygroscopic than the ambient aerosol in an Amazon rainforest, a European high Alpine site or a forested mountainous site. A fairly low hygroscopicity in Hyytiälä is likely a result of a large organic fraction present in the aerosol mass comparative to other locations within Europe. A considerable difference in particle hygroscopicity was found between particles smaller and larger than ~100 nm in diameter, possibly pointing out to the effect of cloud processing increasing &kappa; of particles > 100 nm in diameter. The hygroscopicity of the smaller, ~50 nm particles did not change seasonally, whereas particles with a diameter of ~150 nm showed a decreased hygroscopicity in the summer, likely resulting from the increased VOC emissions of the surrounding boreal forest and secondary organic aerosol (SOA) formation. For the most part, no diurnal patterns of aerosol hygroscopic properties were found. Exceptions to this were the weak diurnal patterns of small, ~50 nm particles in the spring and summer, when a peak in hygroscopicity around noon was observed. No difference in CCN activation and hygroscopic properties was found on days with or without atmospheric new particle formation. During all seasons, except summer, a CCN-inactive fraction was found to be present, rendering the aerosol of 75–300 nm in diameter as internally mixed in the summer and not internally mixed for the rest of the year

Urban aerosol number size distributions

International audienceAerosol number size distributions have been measured since 5 May 1997 in Helsinki, Finland. The presented aerosol data represents size distributions within the particle diameter size range 8-400nm during the period from May 1997 to March 2003. The daily, monthly and annual patterns of the aerosol particle number concentrations were investigated. The temporal variation of the particle number concentration showed close correlations with traffic activities. The highest total number concentrations were observed during workdays; especially on Fridays, and the lowest concentrations occurred during weekends; especially Sundays. Seasonally, the highest total number concentrations were observed during winter and spring and lower concentrations were observed during June and July. More than 80% of the number size distributions had three modes: nucleation mode (30nm), Aitken mode (20-100nm) and accumulation mode (90nm). Less than 20% of the number size distributions had either two modes or consisted of more than three modes. Two different measurement sites were used; in the first (Siltavuori, 5.5.1997-5.3.2001), the arithmetic means of the particle number concentrations were 7000cm, 6500cm, and 1000cm respectively for nucleation, Aitken, and accumulation modes. In the second site (Kumpula, 6.3.2001-28.2.2003) they were 5500cm, 4000cm, and 1000cm. The total number concentration in nucleation and Aitken modes were usually significantly higher during workdays than during weekends. The temporal variations in the accumulation mode were less pronounced. The lower concentrations at Kumpula were mainly due to building construction and also the slight overall decreasing trend during these years. During the site changing a period of simultaneous measurements over two weeks were performed showing nice correlation at both sites

Parameterization of ion-induced nucleation rates based on ambient observations

Atmospheric ions participate in the formation of new atmospheric aerosol particles, yet their exact role in this process has remained unclear. Here we derive a new simple parameterization for ion-induced nucleation or, more precisely, for the formation rate of charged 2-nm particles. The parameterization is semi-empirical in the sense that it is based on comprehensive results of one-year-long atmospheric cluster and particle measurements in the size range ~1–42 nm within the EUCAARI (European Integrated project on Aerosol Cloud Climate and Air Quality interactions) project. Data from 12 field sites across Europe measured with different types of air ion and cluster mobility spectrometers were used in our analysis, with more in-depth analysis made using data from four stations with concomitant sulphuric acid measurements. The parameterization is given in two slightly different forms: a more accurate one that requires information on sulfuric acid and nucleating organic vapor concentrations, and a simpler one in which this information is replaced with the global radiation intensity. These new parameterizations are applicable to all large-scale atmospheric models containing size-resolved aerosol microphysics, and a scheme to calculate concentrations of sulphuric acid, condensing organic vapours and cluster ions