Chemical composition of aerosol during particle formation events in boreal forest

Tellus B ◽  
2001 ◽  
Vol 53 (4) ◽  
pp. 380-393 ◽  
Author(s):  
J. M. MÄKELÄ ◽  
S. YLI‐KOIVISTO ◽  
V. HILTUNEN ◽  
W. SEIDL ◽  
E. SWIETLICKI ◽  
...  
2021 ◽  
Author(s):  
Luis M. F. Barreira ◽  
Arttu Ylisirniö ◽  
Iida Pullinen ◽  
Angela Buchholz ◽  
Zijun Li ◽  
...  

Abstract. Secondary organic aerosols (SOA) formed from biogenic volatile organic compounds (BVOCs) constitute a significant fraction of atmospheric particulate matter and have been recognized to affect significantly the climate and air quality. Many laboratory and field experiments have studied SOA particle formation and growth in the recent years. Most of them have focused on a few monoterpenes and isoprene. However, atmospheric SOA particulate mass yields and chemical composition result from a much more complex mixture of oxidation products originating from many BVOCs, including terpenes other than isoprene and monoterpenes. Thus, a large uncertainty still remains regarding the contribution of BVOCs to SOA. In particular, organic compounds formed from sesquiterpenes have not been thoroughly investigated, and their contribution to SOA remains poorly characterized. In this study, a Filter Inlet for Gases and Aerosols (FIGAERO) combined with a high-resolution time-of-flight chemical ionization mass spectrometer (CIMS), with iodide ionization, was used for the simultaneous measurement of gas and particle phase atmospheric SOA. The aim of the study was to evaluate the relative contribution of sesquiterpene oxidation products to SOA in a spring-time hemi-boreal forest environment. Our results revealed that monoterpene and sesquiterpene oxidation products were the main contributors to SOA particles. The chemical composition of SOA particles was compared for times when either monoterpene or sesquiterpene oxidation products were dominant and possible key oxidation products for SOA particle formation were identified. Surprisingly, sesquiterpene oxidation products were the predominant fraction in the particle phase at some periods, while their gas phase concentrations remained much lower than those of monoterpene products. This can be explained by quick and effective partitioning of sesquiterpene products into the particle phase or their efficient removal by dry deposition. The SOA particle volatility determined from measured thermograms increased when the concentration of sesquiterpene oxidation products in SOA particles was higher than that of monoterpenes. Overall, this study demonstrates the important role of sesquiterpenes in atmospheric chemistry and suggests that the contribution of their products to SOA particles is being underestimated in comparison to the most studied terpenes.


Tellus B ◽  
2001 ◽  
Vol 53 (4) ◽  
pp. 380-393 ◽  
Author(s):  
J. M. Mäkelä ◽  
S. Yli-Koivisto ◽  
V. Hiltunen ◽  
W. Seidl ◽  
E. Swietlicki ◽  
...  

Tellus B ◽  
2001 ◽  
Vol 53 (4) ◽  
pp. 380-393 ◽  
Author(s):  
J. M. MAKELA ◽  
S. YLI-KOIVISTO ◽  
V. HILTUNEN ◽  
W. SEIDL ◽  
E. SWIETLICKI ◽  
...  

Tellus B ◽  
2008 ◽  
Vol 60 (4) ◽  
Author(s):  
Miikka Dal Maso ◽  
Antti Hyvärinen ◽  
Mika Komppula ◽  
Peter Tunved ◽  
Veli-Matti Kerminen ◽  
...  

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.


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 ◽  
Vol 20 (10) ◽  
pp. 5911-5922 ◽  
Author(s):  
Hing Cho Cheung ◽  
Charles Chung-Kuang Chou ◽  
Celine Siu Lan Lee ◽  
Wei-Chen Kuo ◽  
Shuenn-Chin Chang

Abstract. The chemical composition of fine particulate matter (PM2.5), the size distribution and number concentration of aerosol particles (NCN), and the number concentration of cloud condensation nuclei (NCCN) were measured at the northern tip of Taiwan during an intensive observation experiment from April 2017 to March 2018. The parameters of aerosol hygroscopicity (i.e., activation ratio, activation diameter and kappa of CCN) were retrieved from the measurements. Significant variations were found in the hygroscopicity of aerosols (kappa – κ – of 0.18–0.56, for water vapor supersaturation – SS – of 0.12 %–0.80 %), which were subject to various pollution sources, including aged air pollutants originating in eastern and northern China and transported by the Asian continental outflows and fresh particles emitted from local sources and distributed by land–sea breeze circulations as well as produced by processes of new particle formation (NPF). Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aerosols associated with Asian continental outflows were characterized by lower NCN and NCCN values and by higher kappa values of CCN, whereas higher NCN and NCCN values with lower kappa values of CCN were observed in the aerosols associated with local air masses. Besides, it was revealed that the kappa value of CCN exhibited a decrease during the early stage of an event of new particle formation, which turned to an increasing trend over the later period. The distinct features in the hygroscopicity of aerosols were found to be consistent with the characteristics in the chemical composition of PM2.5. This study has depicted a clear seasonal characteristic of hygroscopicity and CCN activity under the influence of a complex mixture of pollutants from different regional and/or local pollution sources. Nevertheless, the mixing state and chemical composition of the aerosols critically influence the aerosol hygroscopicity, and further investigations are necessary to elucidate the atmospheric processing involved in the CCN activation in coastal areas.


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>


2004 ◽  
Vol 35 ◽  
pp. 137-160
Author(s):  
F. Cavalli ◽  
M.C. Facchini ◽  
S. Decesari ◽  
L. Emblico ◽  
M. Mircea ◽  
...  

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