| 1. |
- Gagne, S., et al.
(författare)
-
Factors influencing the contribution of ion-induced nucleation in a boreal forest, Finland
- 2010
-
Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 10:8, s. 3743-3757
-
Tidskriftsartikel (refereegranskat)abstract
- We present the longest series of measurements so far (2 years and 7 months) made with an Ion-DMPS at the SMEAR II measurement station in Hyytiala, Southern Finland. We show that the classification into overcharged (implying some participation of ion-induced nucleation) and undercharged (implying no or very little participation of ion-induced nucleation) days, based on Ion-DMPS measurements, agrees with the fraction of ion-induced nucleation based on NAIS measurements. Those classes are based on the ratio of ambient charged particle to steady-state charged particle concentration, known as the charging state. We analyzed the influence of different parameters on the contribution of ion-induced nucleation to the total particle formation rate. We found that the fraction of ion-induced nucleation is typically higher on warmer, drier and sunnier days compared to colder days with less solar radiation and a higher relative humidity. Also, we observed that bigger concentrations of new particles were produced on days with a smaller fraction of ion-induced nucleation. Moreover, sulfuric acid saturation ratios were smaller for days with a bigger fraction of ion-induced nucleation. Finally, we propose explanations on how these different parameters could influence neutral and ion-induced nucleation, and show that the different mechanisms seem to take place at the same time during an event. For example, we propose that these observed differences could be due to high temperature and low vapors' saturation ratios (water and sulfuric acid) increasing the height of the energy barrier a particle has to reach before it can grow and thus limiting neutral nucleation.
|
|
| 2. |
- Hakkinen, S. A. K., et al.
(författare)
-
Long-term volatility measurements of submicron atmospheric aerosol in Hyytiala, Finland
- 2012
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:22, s. 10771-10786
-
Tidskriftsartikel (refereegranskat)abstract
- The volatility of submicron atmospheric aerosol particles was investigated at a boreal forest site in Hyytiala, Finland from January 2008 to May 2010. These long-term observations allowed for studying the seasonal behavior of aerosol evaporation with a special focus on compounds that remained in the aerosol phase at 280 degrees C. The temperature-response of evaporation was also studied by heating the aerosol sample step-wise to six temperatures ranging from 80 degrees C to 280 degrees C. The mass fraction remaining after heating (MFR) was determined from the measured particle number size distributions before and after heating assuming a constant particle density (1.6 g cm(-3)). On average 19% of the total aerosol mass remained in the particulate phase at 280 degrees C. The particles evaporated less at low ambient temperatures during winter as compared with the warmer months. Black carbon (BC) fraction of aerosol mass correlated positively with the MFR at 280 degrees C, but could not explain it completely: most of the time a notable fraction of this nonvolatile residual was something other than BC. Using additional information on ambient meteorological conditions and results from an Aerodyne aerosol mass spectrometer (AMS), the chemical composition of MFR at 280 degrees C and its seasonal behavior was further examined. Correlation analysis with ambient temperature and mass fractions of polycyclic aromatic hydrocarbons (PAHs) indicated that MFR at 280 degrees C is probably affected by anthropogenic emissions. On the other hand, results from the AMS analysis suggested that there may be very low-volatile organics, possibly organonitrates, in the non-volatile (at 280 degrees C) fraction of aerosol mass.
|
|
| 3. |
- Hakkinen, S. A. K., et al.
(författare)
-
Semi-empirical parameterization of size-dependent atmospheric nanoparticle growth in continental environments
- 2013
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:15, s. 7665-7682
-
Tidskriftsartikel (refereegranskat)abstract
- The capability to accurately yet efficiently represent atmospheric nanoparticle growth by biogenic and anthropogenic secondary organics is a challenge for current atmospheric large-scale models. It is, however, crucial to predict nanoparticle growth accurately in order to reliably estimate the atmospheric cloud condensation nuclei (CCN) concentrations. In this work we introduce a simple semi-empirical parameterization for sub-20 nm particle growth that distributes secondary organics to the nanoparticles according to their size and is therefore able to reproduce particle growth observed in the atmosphere. The parameterization includes particle growth by sulfuric acid, secondary organics from monoterpene oxidation (SORG(MT)) and an additional condensable vapor of non-monoterpene organics (background). The performance of the proposed parameterization was investigated using ambient data on particle growth rates in three diameter ranges (1.5-3 nm, 3-7 nm and 7-20 nm). The growth rate data were acquired from particle / air ion number size distribution measurements at six continental sites over Europe. The longest time series of 7 yr (2003-2009) was obtained from a boreal forest site in Hyytiala, Finland, while about one year of data (2008-2009) was used for the other stations. The extensive ambient measurements made it possible to test how well the parameterization captures the seasonal cycle observed in sub-20 nm particle growth and to determine the weighing factors for distributing the SORG(MT) for different sized particles as well as the background mass flux (concentration). Besides the monoterpene oxidation products, background organics with a concentration comparable to SORGMT, around 6x10(7) cm(-3) (consistent with an additional global SOA yield of 100 Tg yr(-1)) was needed to reproduce the observed nanoparticle growth. Simulations with global models suggest that the background could be linked to secondary biogenic organics that are formed in the presence of anthropogenic pollution.
|
|
| 4. |
- Hong, J., et al.
(författare)
-
Hygroscopicity, CCN and volatility properties of submicron atmospheric aerosol in a boreal forest environment during the summer of 2010
- 2014
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:9, s. 4733-4748
-
Tidskriftsartikel (refereegranskat)abstract
- A Volatility-Hygroscopicity Tandem Differential Mobility Analyzer (VH-TDMA) was applied to study the hygroscopicity and volatility properties of submicron atmospheric aerosol particles in a boreal forest environment in Hyytiala, Finland during the summer of 2010. Aitken and accumulation mode internally mixed particles (50 nm, 75 nm and 110 nm in diameter) were investigated. Hygroscopicity was found to increase with particle size. The relative mass fraction of organics and SO42- is probably the major contributor to the fluctuation of the hygroscopicity for all particle sizes. The Cloud Condensation Nuclei Counter (CCNC)-derived hygroscopicity parameter kappa was observed to be slightly higher than kappa calculated from VH-TDMA data under sub-saturated conditions, potential reasons for this behavior are discussed shortly. Also, the size-resolved volatility properties of particles were investigated. Upon heating, more small particles evaporated compared to large particles. There was a significant amount of aerosol volume (non-volatile material) left, even at heating temperatures of 280 degrees C. Using size resolved volatility-hygroscopicity analysis, we concluded that there was always hygroscopic material remaining in the particles at different heating temperatures, even at 280 degrees C. This indicates that the observed non-volatile aerosol material did not consist solely of black carbon.
|
|
| 5. |
- Kyro, E. -M, et al.
(författare)
-
Trends in new particle formation in eastern Lapland, Finland : effect of decreasing sulfur emissions from Kola Peninsula
- 2014
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:9, s. 4383-4396
-
Tidskriftsartikel (refereegranskat)abstract
- The smelter industry in Kola Peninsula is the largest source of anthropogenic SO2 in the Arctic part of Europe and one of the largest within the Arctic domain. Due to socio-economic changes in Russia, the emissions have been decreasing especially since the late 1990s resulting in decreased SO2 concentrations close to Kola in eastern Lapland, Finland. At the same time, the frequency of new particle formation days has been decreasing distinctively at SMEAR I station in eastern Lapland, especially during spring and autumn. We show that sulfur species, namely sulfur dioxide and sulfuric acid, have an important role in both new particle formation and subsequent growth and that the decrease in new particle formation days is a result of the reduction of sulfur emissions originating from Kola Peninsula. In addition to sulfur species, there are many other quantities, such as formation rate of aerosol particles, condensation sink and nucleation mode particle number concentration, which are related to the number of observed new particle formation (NPF) days and need to be addressed when linking sulfur emissions and NPF. We show that while most of these quantities exhibit statistically significant trends, the reduction in Kola sulfur emissions is the most obvious reason for the rapid decline in NPF days. Sulfuric acid explains approximately 20-50% of the aerosol condensational growth observed at SMEAR I, and there is a large seasonal variation with highest values obtained during spring and autumn. We found that (i) particles form earlier after sunrise during late winter and early spring due to high concentrations of SO2 and H2SO4; (ii) several events occurred during the absence of light, and they were connected to higher than average concentrations of SO2; and (iii) high SO2 concentrations could advance the onset of nucleation by several hours. Moreover, air masses coming over Kola Peninsula seemed to favour new particle formation.
|
|
| 6. |
- Manninen, H. E., et al.
(författare)
-
EUCAARI ion spectrometer measurements at 12 European sites - analysis of new particle formation events
- 2010
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:16, s. 7907-7927
-
Tidskriftsartikel (refereegranskat)abstract
- We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range similar to 1-42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1-30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.
|
|
| 7. |
- Nieminen, T., et al.
(författare)
-
Parameterization of ion-induced nucleation rates based on ambient = servations
- 2011
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:7, s. 3393-3402
-
Tidskriftsartikel (refereegranskat)abstract
- 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 similar to 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.
|
|
| 8. |
- Paasonen, P., et al.
(författare)
-
On the roles of sulphuric acid and low-volatility organic vapours in the initial steps of atmospheric new particle formation
- 2010
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:22, s. 11223-11242
-
Tidskriftsartikel (refereegranskat)abstract
- Sulphuric acid and organic vapours have been identified as the key components in the ubiquitous secondary new particle formation in the atmosphere. In order to assess their relative contribution and spatial variability, we analysed altogether 36 new particle formation events observed at four European measurement sites during EUCAARI campaigns in 2007-2009. We tested models of several different nucleation mechanisms coupling the formation rate of neutral particles (J) with the concentration of sulphuric acid ([H2SO4]) or low-volatility organic vapours ([org]) condensing on sub-4 nm particles, or with a combination of both concentrations. Furthermore, we determined the related nucleation coefficients connecting the neutral nucleation rate J with the vapour concentrations in each mechanism. The main goal of the study was to identify the mechanism of new particle formation and subsequent growth that minimizes the difference between the modelled and measured nucleation rates. At three out of four measurement sites - Hyytiala (Finland), Melpitz (Germany) and San Pietro Capofiume (Italy) - the nucleation rate was closely connected to squared sulphuric acid concentration, whereas in Hohenpeissenberg (Germany) the low-volatility organic vapours were observed to be dominant. However, the nucleation rate at the sulphuric acid dominant sites could not be described with sulphuric acid concentration and a single value of the nucleation coefficient, as K in J=K [H2SO4](2), but the median coefficients for different sites varied over an order of magnitude. This inter-site variation was substantially smaller when the heteromolecular homogenous nucleation between H2SO4 and organic vapours was assumed to take place in addition to homogenous nucleation of H2SO4 alone, i.e., J=K-SA1[H2SO4](2)+K-SA2[H2SO4][org]. By adding in this equation a term describing homomolecular organic vapour nucleation, K-s3[org](2), equally good results were achieved. In general, our results suggest that organic vapours do play a role, not only in the condensational growth of the particles, but also in the nucleation process, with a site-specific degree.
|
|
| 9. |
- Yli-Juuti, T., et al.
(författare)
-
Growth rates of nucleation mode particles in Hyytiala during 2003-2009 : variation with particle size, season, data analysis method and ambient conditions
- 2011
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:24, s. 12865-12886
-
Tidskriftsartikel (refereegranskat)abstract
- The condensational growth rate of aerosol particles formed in atmospheric new particle formation events is one of the most important factors influencing the lifetime of these particles and their ability to become climatically relevant. Diameter growth rates (GR) of nucleation mode particles were studied based on almost 7 yr of data measured during the years 2003-2009 at a boreal forest measurement station SMEAR II in Hyytiala, Finland. The particle growth rates were estimated using particle size distributions measured with a Differential Mobility Particle Sizer (DMPS), a Balanced Scanning Mobility Analyzer (BSMA) and an Air Ion Spectrometer (AIS). Two GR analysis methods were tested. The particle growth rates were also compared to an extensive set of ambient meteorological parameters and trace gas concentrations to investigate the processes/constituents limiting the aerosol growth. The median growth rates of particles in the nucleation mode size ranges with diameters of 1.5-3 nm, 3-7 nm and 7-20 nm were 1.9 nm h(-1), 3.8 nm h(-1), and 4.3 nm h(-1), respectively. The median relative uncertainties in the growth rates due to the size distribution instrumentation in these size ranges were 25 %, 19 %, and 8 %, respectively. For the smallest particles (1.5-3 nm) the AIS data yielded on average higher growth rate values than the BSMA data, and higher growth rates were obtained from positively charged size distributions as compared with negatively charged particles. For particles larger than 3 nm in diameter no such systematic differences were found. For these particles the uncertainty in the growth rate related to the analysis method, with relative uncertainty of 16 %, was similar to that related to the instruments. The growth rates of 7-20 nm particles showed positive correlation with monoterpene concentrations and their oxidation rate by ozone. The oxidation rate by OH did not show a connection with GR. Our results indicate that the growth of nucleation mode particles in Hyytiala is mainly limited by the concentrations of organic precursors.
|
|
