Parameterization for Atmospheric New-Particle Formation: Application to a System Involving Sulfuric Acid and Condensable Water-Soluble Organic Vapors

2004 ◽  
Vol 38 (10) ◽  
pp. 1001-1008 ◽  
Author(s):  
Veli-Matti Kerminen ◽  
Tatu Anttila ◽  
Kari Lehtinen ◽  
Markku Kulmala
Keyword(s):  
Sulfuric Acid ◽  
Particle Formation ◽  
Water Soluble ◽  
New Particle Formation ◽  
Organic Vapors

scholarly journals Particle hygroscopicity during atmospheric new particle formation events: implications for the chemical species contributing to particle growth

2013 ◽  
Vol 13 (13) ◽  
pp. 6637-6646 ◽  
Author(s):  
Z. Wu ◽  
W. Birmili ◽  
L. Poulain ◽  
Z. Wang ◽  
M. Merkel ◽  
...  
Keyword(s):  
Growth Rate ◽  
Sulfuric Acid ◽  
Chemical Species ◽  
Particle Growth ◽  
Particle Formation ◽  
Water Soluble ◽  
Alternative Methods ◽  
Normal Distribution Function ◽  
Particle Fraction ◽  
New Particle Formation

Abstract. This study examines the hygroscopicity of newly formed particles (diameters range 25–45 nm) during two atmospheric new particle formation (NPF) events in the German mid-level mountains during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) field experiment. At the end of the NPF event involving clear particle growth, we measured an unusually high soluble particle fraction of 58.5% at 45 nm particle size. The particle growth rate contributed through sulfuric acid condensation only accounts for around 6.5% of the observed growth rate. Estimations showed that sulfuric acid condensation explained, however, only around 10% of that soluble particle fraction. Therefore, the formation of additional water-soluble matter appears imperative to explain the missing soluble fraction. Although direct evidence is missing, we consider water-soluble organics as candidates for this mechanism. For the case with clear growth process, the particle growth rate was determined by two alternative methods based on tracking the mode diameter of the nucleation mode. The mean particle growth rate obtained from the inter-site data comparison using Lagrangian consideration is 3.8 (± 2.6) nm h−1. During the same period, the growth rate calculated based on one site data is 5.0 nm h−1 using log-normal distribution function method. In light of the fact that considerable uncertainties could be involved in both methods, we consider both estimated growth rates consistent.

scholarly journals Particle hygroscopicity during atmospheric new particle formation events: implications for the chemical species contributing to particle growth

2012 ◽  
Vol 12 (5) ◽  
pp. 11415-11443
Author(s):  
Z. Wu ◽  
W. Birmili ◽  
L. Poulain ◽  
M. Merkel ◽  
B. Fahlbusch ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Soluble Fraction ◽  
Chemical Species ◽  
Particle Growth ◽  
Particle Formation ◽  
Water Soluble ◽  
Mountain Range ◽  
New Particle Formation ◽  
Particle Mobility ◽  
Significant Difference

Abstract. This study examines the hygroscopicity of newly formed particles (smaller than 50 nm in particle mobility diameter) during two atmospheric new particle formation events with and without clear growth process at mid-level mountain range in Central Germany based on HCCT field campaign. Particle hygroscopicity measurements show that the particle soluble fractions at the end of event for two events are, respectively 60% (45 nm particles for the event with clear growth) and 20% (30 nm particles for the event without clear growth), stressing that non-soluble organic compounds may play a key role in particle growth during new particle formation event. Such significant difference in particle hygroscopicity also suggests that the chemical species responsible for nucleation particle growth are considerably different between the two selected NPF events. During both events, the hygroscopicity of newly formed particles decreased with particle growth, indicating that more less-hygroscopic compounds contribute to the subsequent condensation in contrast to the earlier stage. Sulfuric acid was considered to be responsible of the NPF event and represent the highly hygroscopic compounds. However, calculation demonstrated that sulfuric acid condensation failed to fully explain the observed soluble fraction in the nucleation mode particles. Therefore, we hypothesize that some water-soluble matters may explain the missing soluble fraction.

scholarly journals Investigation of the connections between atmospheric new particle formation and organics at an urban site of Beijing

2013 ◽  
Vol 13 (2) ◽  
pp. 3419-3450 ◽  
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
Z. J. Wu ◽  
D. L. Yue ◽  
J. Zheng ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Correlation Coefficients ◽  
Particle Formation ◽  
Nucleation Theory ◽  
Urban Site ◽  
New Particle Formation ◽  
Organic Vapors ◽  
Data Set ◽  
High Background ◽  
Nucleation Mechanisms

Abstract. The role of low-volatility organic vapors in atmospheric new particle formation has been studied based on a data set of 17 nucleation events observed during the CAREBeijing 2008 campaign. The particle formation rates show good correlations with sulfuric acid and organic vapors implying that both play an important role in the atmospheric new particle formation. High correlation coefficients are observed in all investigated nucleation mechanisms. The best fit (R = 0.73, slope = 1.1) between the observed and modelled particle formation rates is achieved with the homogenous nucleation theory of sulfuric acid (both homomolecularly and hetermolecularly) with separate coefficients in J=KSA1[H2SO4]2+KSA2[H2SO4][Org]. The contributions of the sulfuric acid and the organics involving terms have been 43% and 57%, respectively. In addition, the higher particle formation rates are observed on polluted nucleation days, indicating the organic vapors should be involved in the new particle formation process in the polluted urban environment of Beijing with high background aerosol loading.

scholarly journals Open ocean and coastal new particle formation from sulfuric acid and amines around the Antarctic Peninsula

2021 ◽  
Author(s):  
James Brean ◽  
Manuel Dall’Osto ◽  
Rafel Simó ◽  
Zongbo Shi ◽  
David C. S. Beddows ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Antarctic Peninsula ◽  
Particle Formation ◽  
Open Ocean ◽  
New Particle Formation ◽  
The Antarctic

scholarly journals Modelling studies of HOMs and their contributions to new particle formation and growth: comparison of boreal forest in Finland and a polluted environment in China

2018 ◽  
Vol 18 (16) ◽  
pp. 11779-11791 ◽  
Author(s):  
Ximeng Qi ◽  
Aijun Ding ◽  
Pontus Roldin ◽  
Zhengning Xu ◽  
Putian Zhou ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Boreal Forest ◽  
Environmental Conditions ◽  
Eastern China ◽  
Particle Growth ◽  
Particle Formation ◽  
Forest Site ◽  
Polluted Environment ◽  
New Particle Formation ◽  
Multifunctional Compounds

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.

scholarly journals Long-term analysis of clear-sky new particle formation events and non-events in Hyytiälä

2016 ◽  
Author(s):  
Lubna Dada ◽  
Pauli Paasonen ◽  
Tuomo Nieminen ◽  
Stephany Buenrostro Mazon ◽  
Jenni Kontkanen ◽  
...  
Keyword(s):  
Formation Rate ◽  
Threshold Value ◽  
Particle Formation ◽  
New Particle Formation ◽  
Organic Vapors ◽  
Clear Sky ◽  
Sky Conditions ◽  
Oxidized Products ◽  
Condensation Sink

Abstract. New particle formation (NPF) events have been observed all around the world and are known to be a major source of atmospheric aerosol particles. Here we combine 20 years of observations in a boreal forest at the SMEAR II station (Station for Measuring Ecosystem-Atmosphere Relations) in Hyytiälä, Finland, by utilizing previously accumulated knowledge, and by focusing on clear-sky (non-cloudy) conditions. We first investigated the effect of cloudiness on NPF and then compared the NPF event and non-event days during clear-sky conditions. In this comparison we considered, for example, the effects of calculated particle formation rates, condensation sink, trace gas concentrations and various meteorological quantities. The formation rate of 1.5 nm particles was calculated by using proxies for gaseous sulfuric acid and oxidized products of low volatile organic compounds. As expected, our results indicate an increase in the frequency of NPF events under clear-sky conditions. Also, focusing on clearsky conditions enabled us to find a clear separation of many variables related to NPF. For instance, oxidized organic vapors showed higher concentration during the clear-sky NPF event days, whereas the condensation sink (CS) and some trace gases had higher concentrations during the non-event days. The calculated formation rate of 3 nm particles showed a notable difference between the NPF event and non-event days during clear-sky conditions, especially in winter and spring. For spring time, we are able to find a threshold value for the combined values of ambient temperature and CS, above which practically no clear-sky NPF event could be observed. Finally, we present a probability distribution for the frequency of NPF events at a specific CS and temperature.

scholarly journals Hygroscopic properties of ultrafine aerosol particles in the boreal forest: diurnal variation, solubility and the influence of sulfuric acid

2007 ◽  
Vol 7 (1) ◽  
pp. 211-222 ◽  
Author(s):  
M. Ehn ◽  
T. Petäjä ◽  
H. Aufmhoff ◽  
P. Aalto ◽  
K. Hämeri ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Boreal Forest ◽  
Diurnal Variation ◽  
Gas Phase ◽  
Aerosol Particles ◽  
Particle Formation ◽  
Time Of Day ◽  
New Particle Formation ◽  
Hygroscopic Growth ◽  
Hygroscopic Properties

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.

scholarly journals Atmospheric new particle formation at the research station Melpitz, Germany: connection with gaseous precursors and meteorological parameters

2018 ◽  
Vol 18 (3) ◽  
pp. 1835-1861 ◽  
Author(s):  
Johannes Größ ◽  
Amar Hamed ◽  
André Sonntag ◽  
Gerald Spindler ◽  
Hanna Elina Manninen ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Solar Radiation ◽  
Gas Phase ◽  
Meteorological Parameters ◽  
Particle Formation ◽  
Number Concentration ◽  
Independent Effect ◽  
Research Station ◽  
New Particle Formation ◽  
Automated Method

Abstract. This paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2–20 nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level.

scholarly journals Modeling particle nucleation and growth over northern California during the 2010 CARES campaign

2015 ◽  
Vol 15 (21) ◽  
pp. 12283-12313 ◽  
Author(s):  
A. Lupascu ◽  
R. Easter ◽  
R. Zaveri ◽  
M. Shrivastava ◽  
M. Pekour ◽  
...  
Keyword(s):  
Size Distribution ◽  
Particle Number ◽  
Particle Formation ◽  
Number Concentration ◽  
Aerosol Size Distribution ◽  
Particle Nucleation ◽  
Particle Number Concentration ◽  
New Particle Formation ◽  
Organic Vapors ◽  
Diurnal Variability

Abstract. Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4, while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapor parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates are predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary-layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10–40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. We found that newly formed particles could explain up to 20–30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ~ 36 %.

scholarly journals The Synergistic Role of Sulfuric Acid, Bases, and Oxidized Organics Governing New‐Particle Formation in Beijing

2021 ◽  
Vol 48 (7) ◽  
Author(s):  
Chao Yan ◽  
Rujing Yin ◽  
Yiqun Lu ◽  
Lubna Dada ◽  
Dongsen Yang ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Particle Formation ◽  
New Particle Formation
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