Characteristics of the three years continuous data on new particle formation events observed at a boreal forest site

Author(s):  
J. M. Mäkelä

2018 ◽  
Vol 18 (16) ◽  
pp. 11779-11791 ◽  
Author(s):  
Ximeng Qi ◽  
Aijun Ding ◽  
Pontus Roldin ◽  
Zhengning Xu ◽  
Putian Zhou ◽  
...  

Abstract. Highly oxygenated multifunctional compounds (HOMs) play a key role in new particle formation (NPF), but their quantitative roles in different environments of the globe have not been well studied yet. Frequent NPF events were observed at two “flagship” stations under different environmental conditions, i.e. a remote boreal forest site (SMEAR II) in Finland and a suburban site (SORPES) in polluted eastern China. The averaged formation rate of 6 nm particles and the growth rate of 6–30 nm particles were 0.3 cm−3 s−1 and 4.5 nm h−1 at SMEAR II compared to 2.3 cm−3 s−1 and 8.7 nm h−1 at SORPES, respectively. To explore the differences of NPF at the two stations, the HOM concentrations and NPF events at two sites were simulated with the MALTE-BOX model, and their roles in NPF and particle growth in the two distinctly different environments are discussed. The model provides an acceptable agreement between the simulated and measured concentrations of sulfuric acid and HOMs at SMEAR II. The sulfuric acid and HOM organonitrate concentrations are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower at SORPES compared to SMEAR II. The model simulates the NPF events at SMEAR II with a good agreement but underestimates the growth of new particles at SORPES, indicating a dominant role of anthropogenic processes in the polluted environment. HOMs from monoterpene oxidation dominate the growth of ultrafine particles at SMEAR II while sulfuric acid and HOMs from aromatics oxidation play a more important role in particle growth. This study highlights the distinct roles of sulfuric acid and HOMs in NPF and particle growth in different environmental conditions and suggests the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas like eastern China.



Author(s):  
Michael Boy ◽  
Boris Bonn ◽  
Miikka Dal Maso ◽  
Hannele Hakola ◽  
Anne Hirsikko ◽  
...  


2007 ◽  
Vol 7 (1) ◽  
pp. 211-222 ◽  
Author(s):  
M. Ehn ◽  
T. Petäjä ◽  
H. Aufmhoff ◽  
P. Aalto ◽  
K. Hämeri ◽  
...  

Abstract. The hygroscopic growth of aerosol particles present in a boreal forest was measured at a relative humidity of 88%. Simultaneously the gas phase concentration of sulfuric acid, a very hygroscopic compound, was monitored. The focus was mainly on days with new particle formation by nucleation. The measured hygroscopic growth factors (GF) correlated positively with the gaseous phase sulfuric acid concentrations. The smaller the particles, the stronger the correlation, with r=0.20 for 50 nm and r=0.50 for 10 nm particles. The increase in GF due to condensing sulfuric acid is expected to be larger for particles with initially smaller masses. During new particle formation, the changes in solubility of the new particles were calculated during their growth to Aitken mode sizes. As the modal diameter increased, the solubility of the particles decreased. This indicated that the initial particle growth was due to more hygroscopic compounds, whereas the later growth during the evening and night was mainly caused by less hygroscopic or even hydrophobic compounds. For all the measured sizes, a diurnal variation in GF was observed both during days with and without particle formation. The GF was lowest at around midnight, with a mean value of 1.12–1.24 depending on particle size and if new particle formation occurred during the day, and increased to 1.25–1.34 around noon. This can be tentatively explained by day- and nighttime gas-phase chemistry; different vapors will be present depending on the time of day, and through condensation these compounds will alter the hygroscopic properties of the particles in different ways.



2020 ◽  
Author(s):  
Dominik Stolzenburg ◽  
Runlong Cai ◽  
Lauri Ahonen ◽  
Tiia Laurila ◽  
Sebastian Holm ◽  
...  

<p>New particle formation (NPF) by gas-to-particle conversion occurs frequently in many different environments around the globe (Nieminen et al., 2018). NPF is the major contributor to the global cloud condensation nuclei budget (Gordon et al., 2017) and also impacts urban air quality (Guo et al., 2014). It is therefore crucial to understand how the newly formed particles can survive and grow to larger particles under different environmental conditions. Depending on the environment different condensable vapours and also different aerosol dynamics govern the NPF process.</p><p>In order to investigate the dynamics of aerosol growth in the sub-10 nm regime, where the newly formed particles are most vulnerable for losses to pre-existing aerosol, we tested several combining instrument inversion approaches. This allows to combine the measurements of several different particle sizing instruments in the sub-10 nm range, where each instrument offers different benefits and weaknesses. If the instruments are combined during the inversion, this could significantly reduce the error of the inferred particle size-distributions. Model results show that the regularization approach proposed by Wolfenbarger and Seinfeld (1990) yield the most stable inversion for data heavily influenced by measurement errors.</p><p>We than apply the tested inversion techniques to measurements in three different environments where an array of different state-of-the-art sub-10 nm sizing instruments was deployed: The SMEAR-II station in Hyytiälä, Finland, representative for a rural boreal forest background site, the SMEAR-III station in Helsinki, Finland, representative for a medium-polluted middle-scale European city, and at the Beijing University of Chemical Technology, China, an urban site in a global megacity.</p><p>We demonstrate that the combining instrument approach can enable a more detailed analysis of the cluster dynamics, e.g. by the application of size- and time resolving growth rate analysis tools (Pichelstorfer et al., 2018). This will lead to a better understanding of the role of coagulation and condensation in the particle growth process and will help to explain the different dynamics which lead to NPF in fundamentally different environments.</p><p><strong>References:</strong></p><p>Gordon, H. et al.: Causes and importance of new particle formation in the present-day and preindustrial atmospheres, J. Geophys. Res.-Atmos., 122, doi:10.1002/2017JD026844, 2017.</p><p>Guo, S. et al.: Elucidating severe urban haze formation in China, P. Nat. Acad. Sci. USA, 111(49), 17373 LP – 17378, doi:10.1073/pnas.1419604111, 2014.</p><p>Nieminen, T. et al.: Global analysis of continental boundary layer new particle formation based on long-term measurements, Atmos. Chem. Phys., (April), 1–34, doi:10.5194/acp-2018-304, 2018.</p><p>Pichelstorfer, L et al.: Resolving nanoparticle growth mechanisms from size- and time-dependent growth rate analysis, Atmos. Chem. Phys., 18(2), 1307–1323, doi:10.5194/acp-18-1307-2018, 2018.</p><p>Wolfenbarger, J. K. and Seinfeld, J. H.: Inversion of aerosol size distribution data, J. Aerosol Sci., 21(2), 227–247, doi:https://doi.org/10.1016/0021-8502(90)90007-K, 1990.</p>



2014 ◽  
Vol 14 (19) ◽  
pp. 10823-10843 ◽  
Author(s):  
B. Bonn ◽  
E. Bourtsoukidis ◽  
T. S. Sun ◽  
H. Bingemer ◽  
L. Rondo ◽  
...  

Abstract. It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulfuric acid. However, the activation process of sulfuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus on the PARADE campaign measurements conducted during August/September 2011 at Mt Kleiner Feldberg in central Germany. During this campaign a set of radicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulfuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products, in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilised Criegee intermediates (sCI). This novel laboratory-derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during daytime and NO3 during night-time. Because the RO2 lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should be taken into account when studying the impact of new particles in climate feedback cycles.



2009 ◽  
Vol 9 (6) ◽  
pp. 26627-26651 ◽  
Author(s):  
K. Lehtipalo ◽  
M. Kulmala ◽  
M. Sipilä ◽  
T. Petäjä ◽  
M. Vana ◽  
...  

Abstract. The detailed mechanism of secondary new particle formation in the atmosphere is still under debate. It is proposed that particle formation happens via activation of 1–2 nm atmospheric neutral molecular clusters and/or large molecules. Since traditional instrumentation does not reach these sizes, the hypothesis has not yet been verified. By directly measuring particle size distributions down to mobility diameters of about 1.3 nm with a pulse-height CPC we provide evidence of the nucleation mechanism in coastal environment (Mace Head, Ireland) and in boreal forest (Hyytiälä, Finland). In both places neutral sub-3 nm condensation nuclei (nano-CN) were continuously present, even when no new particle formation was detected. In Mace Head, however, the concentration of the nano-CN was far too low to account for the particle formation rates during particle bursts. Thus the results imply that on coastal sites new particle formation initiates, as proposed earlier, via homogenous nucleation from biogenic iodine vapors. In contrary, activation of pre-existing nano-CN remains a possible explanation in the boreal forest, but the observed concentrations are not the limiting factor for the particle formation events.



2021 ◽  
Author(s):  
Anastasiia Demakova ◽  
Olga Garmash ◽  
Ekaterina Ezhova ◽  
Mikhail Arshinov ◽  
Denis Davydov ◽  
...  

<p>New Particle Formation (NPF) is a process in which a large number of particles is formed in the atmosphere via gas-to-particle conversion. Previous research shows the important role of formation of new particles for atmosphere, clouds and climate (Kerminen, V.-M. et al. 2018).</p><p>              There exist measurements from different parts of the world which show that NPF is happening worldwide (Kerminen, V.-M. et al. 2018). Measurements at SMEAR II station in Hyytiälä, Finland (Hari P. and Kulmala M., 2005), show that NPF is a common process in Finland’s boreal forests. However, measurements at Zotto station in Siberia, Russia, show that NPF events are very rare in that area (Wiedensohler A. et al., 2018). Measurements in Siberian boreal forests are sparse. We have conducted new measurements at Fonovaya station near Tomsk (Siberia, Russia) using Neutral cluster Air Ion Spectrometer (NAIS), Particle Size Magnifier (PSM), Differential Mobility Particle Sizer (DMPS) and the Atmospheric Pressure interface Time-Of-Flight mass spectrometer (APi-TOF). Those instruments measure aerosol particle number size distribution (NAIS, DMPS), ion number size distribution (NAIS), size distribution of small particles (PSM) and chemical composition of aerosol particles (APi-TOF). The novelty of this work is that such complex measurements have not been done in Siberia before.</p><p>              Here we report the first results of our research on NPF phenomenon in Siberian boreal forest. We present detailed statistics of NPF events, as well as formation rates (J) and growth rates (GR) of aerosol particles. The results from Fonovaya station are compared with those from SMEAR II station and from SMEAR Estonia station in Järvselja, Estonia.</p><p>               </p><p> </p><p> </p><p>Literature</p><ul><li>[1] Kerminen V.-M. et al. “Atmospheric new particle formation and growth: review of field observations”. In: Environmental Research Letters 10 (2018), p. 103003.</li> <li>[2] Wiedensohler A. et al. “Infrequent new particle formation over the remote boreal forest of Siberia”. In: Atmospheric Environment 200 (2019), pp. 167–169.</li> <li>[3] Dada L. et al. “Long-term analysis of clear-sky new particle formation events and nonevents in Hyytiälä”. In: Atmospheric Chemistry and Physics 10 (2017), pp. 6227–6241.</li> </ul><p> </p>



2018 ◽  
Vol 45 (4) ◽  
pp. 2038-2046 ◽  
Author(s):  
Michael J. Lawler ◽  
Matti P. Rissanen ◽  
Mikael Ehn ◽  
R. Lee Mauldin ◽  
Nina Sarnela ◽  
...  


2019 ◽  
Author(s):  
Meinrat Andreae ◽  
Tracey Andreae ◽  
Florian Ditas


2005 ◽  
Vol 5 (5) ◽  
pp. 8851-8877
Author(s):  
F. Cavalli ◽  
M. C. Facchini ◽  
S. Decesari ◽  
L. Emblico ◽  
M. Mircea ◽  
...  

Abstract. Size-segregated aerosol samples were collected during the QUEST field campaign at Hyytiälä, a boreal forest site in Southern Finland, during spring 2003. Aerosol samples were selectively collected during both particle formation events and periods in which no particle formation occurred. A comprehensive characterisation of the aerosol chemical properties (water-soluble inorganic and organic fraction) and an analysis of the relevant meteorological parameters revealed how aerosol chemistry and meteorology combine to determine a favorable "environment" for new particle formation. The results indicated that all events, typically favored during northerly air mass advection, were background aerosols (total mass concentrations range between 1.97 and 4.31 μg m−3), with an increasingly pronounced marine character as the northerly air flow arrived progressively from the west and, in contrast, with a moderate SO2-pollution influence as the air arrived from more easterly directions. Conversely, the non-event aerosol, transported from the south, exhibited the chemical features of European continental sites, with a marked increase in the concentrations of all major anthropogenic aerosol constituents. The higher non-event mass concentration (total mass concentrations range between 6.88 and 16.30 μg m−3) and, thus, a larger surface area, tended to suppress new particle formation, more efficiently depleting potential gaseous precursors for nucleation. The analysis of water-soluble organic compounds showed that clean nucleation episodes were dominated by aliphatic biogenic species, while non-events were characterised by a large abundance of anthropogenic oxygenated species. Interestingly, a significant content of α-pinene photo-oxidation products was observed in the events aerosol, accounting for, on average, 72% of their WSOC; while only moderate amounts of these species were found in the non-event aerosol. If the organic vapors condensing onto accumulation mode particles are responsible also for the growth of newly formed thermodynamically stable clusters, our finding allows one to postulate that, at the site, α-pinene photo-oxidation products (and probably also photo-oxidation products from other terpenes) are the most likely species to contribute to the growth of nanometer-sized particles.



Sign in / Sign up

Export Citation Format

Share Document