scholarly journals New particle formation in the Front Range of the Colorado Rocky Mountains

2008 ◽  
Vol 8 (6) ◽  
pp. 1577-1590 ◽  
Author(s):  
M. Boy ◽  
T. Karl ◽  
A. Turnipseed ◽  
R. L. Mauldin ◽  
E. Kosciuch ◽  
...  

Abstract. New particle formation is of interest because of its influence on the properties of aerosol population, and due to the possible contribution of newly formed particles to cloud condensation nuclei. Currently no conclusive evidence exists as to the mechanism or mechanisms of nucleation and subsequent particle growth. However, nucleation rates exhibit a clear dependence on ambient sulphuric acid concentrations and particle growth is often attributed to the condensation of organic vapours. A detailed study of new particle formation in the Front Range of the Colorado Rocky Mountains is presented here. Gas and particle measurement data for 32 days was analyzed to identify event days, possible event days, and non-event days. A detailed analysis of nucleation and growth is provided for four days on which new particle formation was clearly observed. Evidence for the role of sesquiterpenes in new particle formation is presented.

2007 ◽  
Vol 7 (6) ◽  
pp. 15581-15617 ◽  
Author(s):  
M. Boy ◽  
T. Karl ◽  
A. Turnipseed ◽  
R. L. Mauldin ◽  
E. Kosciuch ◽  
...  

Abstract. New particle formation is of interest because of its influence on the properties of aerosol population, and due to the possible contribution of newly formed particles to cloud condensation nuclei. Currently no conclusive evidence exists as to the mechanism or mechanisms of nucleation and subsequent particle growth. However, nucleation rates exhibit a clear dependence on ambient sulphuric acid concentrations and particle growth is often attributed to the condensation of organic vapours. A detailed study of new particle formation in the Front Range of the Colorado Rocky Mountains is presented here. Gas and particle measurement data for 32 days was analyzed to identify event days, possible event days, and non-event days. A detailed analysis of nucleation and growth is provided for four days on which new particle formation was clearly observed. Evidence for the role of sesquiterpenes in new particle formation is presented.


2008 ◽  
Vol 8 (2) ◽  
pp. 6313-6353 ◽  
Author(s):  
L. Laakso ◽  
H. Laakso ◽  
P. P. Aalto ◽  
P. Keronen ◽  
T. Petäjä ◽  
...  

Abstract. We have analyzed one year (July 2006–July 2007) of measurement data from a relatively clean background site located in dry savannah in South Africa. The annual-median trace gas concentrations were equal to 0.7 ppb for SO2, 1.4 ppb for NOx, 36 ppb for O3 and 105 ppb for CO. The corresponding PM1, PM2.5 and PM10 concentrations were 9.0, 10.5 and 18.8 μg m−3, and the annual median total particle number concentration in the size range 10–840 nm was 2340 cm−3. Gases and particles had a clear seasonal and diurnal variation, which was associated with field fires and biological activity together with local meteorology. Atmospheric new-particle formation was observed to take place in more than 90% of the analyzed days. The days with no new particle formation were cloudy or rainy days. The formation rate of 10 nm particles varied in the range of 0.1–28 cm−3 s−1 (median 1.9 cm−3 s−1) and nucleation mode particle growth rates were in the range 3–21 nm h−1 (median 8.5 nm h−1). Due to high formation and growth rates, observed new particle formation gives a significant contribute to the number of cloud condensation nuclei budget, having a potential to affect the regional climate forcing patterns.


2008 ◽  
Vol 8 (16) ◽  
pp. 4823-4839 ◽  
Author(s):  
L. Laakso ◽  
H. Laakso ◽  
P. P. Aalto ◽  
P. Keronen ◽  
T. Petäjä ◽  
...  

Abstract. We have analyzed one year (July 2006–July 2007) of measurement data from a relatively clean background site located in dry savannah in South Africa. The annual-median trace gas concentrations were equal to 0.7 ppb for SO2, 1.4 ppb for NOx, 36 ppb for O3 and 105 ppb for CO. The corresponding PM1, PM2.5 and PM10 concentrations were 9.0, 10.5 and 18.8 μg m−3, and the annual median total particle number concentration in the size range 10–840 nm was 2340 cm−3. During Easterly winds, influence of industrial sources approximately 150 km away from the measurement site was clearly visible, especially in SO2 and NOx concentrations. Of gases, NOx and CO had a clear annual, and SO2, NOx and O3 clear diurnal cycle. Atmospheric new-particle formation was observed to take place in more than 90% of the analyzed days. The days with no new particle formation were cloudy or rainy days. The formation rate of 10 nm particles varied in the range of 0.1–28 cm−3 s−1 (median 1.9 cm−3 s−1) and nucleation mode particle growth rates were in the range 3–21 nm h−1 (median 8.5 nm h−1). Due to high formation and growth rates, observed new particle formation gives a significant contribute to the number of cloud condensation nuclei budget, having a potential to affect the regional climate forcing patterns.


2020 ◽  
Vol 20 (16) ◽  
pp. 10029-10045 ◽  
Author(s):  
James Brean ◽  
David C. S. Beddows ◽  
Zongbo Shi ◽  
Brice Temime-Roussel ◽  
Nicolas Marchand ◽  
...  

Abstract. Atmospheric aerosols contribute some of the greatest uncertainties to estimates of global radiative forcing and have significant effects on human health. New particle formation (NPF) is the process by which new aerosols of sub-2 nm diameter form from gas-phase precursors and contributes significantly to particle numbers in the atmosphere, accounting for approximately 50 % of cloud condensation nuclei globally. Here, we study summertime NPF in urban Barcelona in north-eastern Spain utilising particle counting instruments down to 1.9 nm and a Nitrate Chemical Ionisation Atmospheric Pressure interface Time of Flight Mass Spectrometer (CI-APi-ToF). The rate of formation of new particles is seen to increase linearly with sulfuric acid concentration, although particle formation rates fall short of chamber studies of H2SO4–DMA–H2O while exceeding those of H2SO4–BioOxOrg–H2O nucleation, although a role of highly oxygenated molecules (HOMs) cannot be ruled out. The sulfuric acid dimer : monomer ratio is significantly lower than that seen in experiments involving sulfuric acid and dimethylamine (DMA) in chambers, indicating that stabilisation of sulfuric acid clusters by bases is weaker in this dataset than in chambers, either due to rapid evaporation due to high summertime temperatures or limited pools of stabilising amines. Such a mechanism cannot be verified in these data, as no higher-order H2SO4–amine clusters nor H2SO4–HOM clusters were measured. The high concentrations of HOMs arise from isoprene, alkylbenzene, monoterpene and polycyclic aromatic hydrocarbon (PAH) oxidation, with alkylbenzenes providing greater concentrations of HOMs due to significant local sources. The concentration of these HOMs shows a dependence on temperature. The organic compounds measured primarily fall into the semivolatile organic compound (SVOC) volatility class arising from alkylbenzene and isoprene oxidation. Low-volatility organic compounds (LVOCs) largely arise from oxidation of alkylbenzenes, PAHs and monoterpenes, whereas extremely low-volatility organic compounds (ELVOCs) arise from primarily PAH and monoterpene oxidation. New particle formation without growth past 10 nm is also observed, and on these days oxygenated organic concentrations are lower than on days with growth by a factor of 1.6, and thus high concentrations of low-volatility oxygenated organics which primarily derive from traffic-emitted volatile organic compounds (VOCs) appear to be a necessary condition for the growth of newly formed particles in Barcelona. These results are consistent with prior observations of new particle formation from sulfuric acid–amine reactions in both chambers and the real atmosphere and are likely representative of the urban background of many European Mediterranean cities. A role for HOMs in the nucleation process cannot be confirmed or ruled out, and there is strong circumstantial evidence of the participation of HOMs across multiple volatility classes in particle growth.


2015 ◽  
Vol 15 (11) ◽  
pp. 15655-15681
Author(s):  
R. Weller ◽  
K. Schmidt ◽  
K. Teinilä ◽  
R. Hillamo

Abstract. We measured condensation particle (CP) concentrations and particle size distributions at the coastal Antarctic station Neumayer (70°39' S, 8°15' W) during two summer campaigns (from 20 January to 26 March 2012 and 1 February to 30 April 2014) and during polar night between 12 August and 27 September 2014 in the particle diameter (Dp) range from 2.94 to 60.4 nm (2012) and from 6.26 to 212.9 nm (2014). During both summer campaigns we identified all in all 44 new particle formation (NPF) events. From 10 NPF events, particle growth rates could be determined to be around 0.90 ± 0.46 nm h−1 (mean ± SD; range: 0.4 to 1.9 nm h−1). With the exception of one case, particle growth was generally restricted to the nucleation mode (Dp < 25 nm) and the duration of NPF events was typically around 6.0 ± 1.5 h (mean ± SD; range: 4 to 9 h). Thus in the main, particles did not grow up to sizes required for acting as cloud condensation nuclei. NPF during summer usually occurred in the afternoon in coherence with local photochemistry. During winter, two NPF events could be detected, though showing no ascertainable particle growth. A simple estimation indicated that apart from sulfuric acid, the derived growth rates required other low volatile precursor vapours.


2018 ◽  
Vol 4 (11) ◽  
pp. eaat9744 ◽  
Author(s):  
T. Jokinen ◽  
M. Sipilä ◽  
J. Kontkanen ◽  
V. Vakkari ◽  
P. Tisler ◽  
...  

Formation of new aerosol particles from trace gases is a major source of cloud condensation nuclei (CCN) in the global atmosphere, with potentially large effects on cloud optical properties and Earth’s radiative balance. Controlled laboratory experiments have resolved, in detail, the different nucleation pathways likely responsible for atmospheric new particle formation, yet very little is known from field studies about the molecular steps and compounds involved in different regions of the atmosphere. The scarcity of primary particle sources makes secondary aerosol formation particularly important in the Antarctic atmosphere. Here, we report on the observation of ion-induced nucleation of sulfuric acid and ammonia—a process experimentally investigated by the CERN CLOUD experiment—as a major source of secondary aerosol particles over coastal Antarctica. We further show that measured high sulfuric acid concentrations, exceeding 107 molecules cm−3, are sufficient to explain the observed new particle growth rates. Our findings show that ion-induced nucleation is the dominant particle formation mechanism, implying that galactic cosmic radiation plays a key role in new particle formation in the pristine Antarctic atmosphere.


2017 ◽  
Vol 17 (24) ◽  
pp. 15181-15197 ◽  
Author(s):  
Robert Wagner ◽  
Chao Yan ◽  
Katrianne Lehtipalo ◽  
Jonathan Duplissy ◽  
Tuomo Nieminen ◽  
...  

Abstract. The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e., in conditions in which neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.5 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.5 nm. At this size, more than 90 % of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.5 nm. Observations at Hyytiälä, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.


2014 ◽  
Vol 14 (4) ◽  
pp. 2169-2183 ◽  
Author(s):  
E. Herrmann ◽  
A. J. Ding ◽  
V.-M. Kerminen ◽  
T. Petäjä ◽  
X. Q. Yang ◽  
...  

Abstract. Aerosols and new particle formation were studied in the western part of the Yangtze River Delta (YRD) at the Station for Observing Regional Processes of the Earth System, Nanjing University (SORPES-NJU). Air ions in the diameter range 0.8–42 nm were measured using an air ion spectrometer, and a differential mobility particle sizer (DMPS) provided particle number size distributions between 6 and 800 nm. Additionally, meteorological data, trace gas concentrations, and PM2.5 values were recorded. During the measurement period from 18 November 2011 to 31 March 2012, the mean total particle concentration was found to be 23 000 cm−3 and the mean PM2.5 value was 90 μg m−3, well above national limits. We observed 26 new particle formation events occurred during the measurement period, producing 6 nm particles at a rate of about 1 cm−3 s−1. Typical particle growth rates were between 6 and 7 nm h−1. On average, new particle formation and growth were estimated to enhance cloud condensation nuclei concentration by about a factor of two during these event days. Ion measurements showed the typical cluster band below 2 nm, with total ion concentrations between about 600 and 1000 cm−3. A peculiar feature of the ion measurements were heightened ion cluster concentrations during the nights before the event days. At 2 nm, the formation rate of charged particles was only about 0.2% of the total rate, pointing towards an only marginal role of ion-induced nucleation. Based on observations, a simple empirical criterion was deducted to estimate particle formation probability. Dominated by radiation and relative humidity, the criterion can predict the occurrence of particle formation with a 90% accuracy. In a similar fashion, a reasonably accurate estimate of particle formation rates was derived. Combined, these parameters allow for a description of particle formation based on a few basic measured variables.


2017 ◽  
Author(s):  
Robert Wagner ◽  
Chao Yan ◽  
Katrianne Lehtipalo ◽  
Jonathan Duplissy ◽  
Tuomo Nieminen ◽  
...  

Abstract. The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nano-particle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e. in conditions where neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.2 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.2 nm. At this size, more than 90 % of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.2 nm. Observations at Hyytiälä, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.


2015 ◽  
Vol 15 (19) ◽  
pp. 11399-11410 ◽  
Author(s):  
R. Weller ◽  
K. Schmidt ◽  
K. Teinilä ◽  
R. Hillamo

Abstract. We measured condensation particle (CP) concentrations and particle size distributions at the coastal Antarctic station Neumayer (70°39´ S, 8°15´ W) during two summer campaigns (from 20 January to 26 March 2012 and 1 February to 30 April 2014) and during the polar night between 12 August and 27 September 2014 in the particle diameter (Dp) range from 2.94 to 60.4 nm (2012) and from 6.26 to 212.9 nm (2014). During both summer campaigns we identified all in all 44 new particle formation (NPF) events. From 10 NPF events, particle growth rates could be determined to be around 0.90 ± 0.46 nm h−1 (mean ± SD; range: 0.4–1.9 nm h−1). With the exception of one case, particle growth was generally restricted to the nucleation mode (Dp < 25 nm) and the duration of NPF events was typically around 6.0 ± 1.5 h (mean ± SD; range: 4–9 h). Thus, in the surrounding area of Neumayer, particles did not grow up to sizes required for acting as cloud condensation nuclei. NPF during summer usually occurred in the afternoon in coherence with local photochemistry. During winter, two NPF events could be detected, though showing no ascertainable particle growth. A simple estimation indicated that apart from sulfuric acid, the derived growth rates required other low volatile precursor vapours.


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