scholarly journals New Particle Formation: A Review of Ground-Based Observations at Mountain Research Stations

Atmosphere ◽  
2019 ◽  
Vol 10 (9) ◽  
pp. 493 ◽  
Author(s):  
Karine Sellegri ◽  
Clemence Rose ◽  
Angela Marinoni ◽  
Angelo Lupi ◽  
Alfred Wiedensohler ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
New Particle Formation ◽  
High Altitudes ◽  
Positive Ions ◽  
Low Altitude ◽  
Term Data

New particle formation (NPF) was predicted to contribute to a major fraction of free tropospheric particle number and cloud condensation nuclei (CCN) concentrations by global models. At high altitudes, pre-existing particle concentrations are low, leading to limited condensational sinks for nucleation precursor gases, and temperatures are cooler compared to lower altitudes, whereas radiation is higher. These factors would all be in favor of nucleation to occur with an enhanced frequency at high altitudes. In the present work, long term data from six altitude stations (and four continents) at various altitudes (from 1465 to 5240 m a.s.l) were used to derive statistically relevant NPF features (frequency, formation rates, and growth rates) and seasonal variability. The combined information together with literature data showed that the frequencies of NPF events at the two Southern hemisphere (SH) stations are some of the highest reported thus far (64% and 67%, respectively). There are indications that NPF would be favored at a preferential altitude close to the interface of the free troposphere (FT) with the planetary boundary layer (PBL) and/or at the vicinity with clouds, which otherwise inhibit the occurrence of NPF. Particle formation rates are found to be lower at high altitudes than at low altitude sites, but a higher fraction of particles are formed via the charged pathway (mainly related to positive ions) compared to boundary layer (BL) sites. Low condensational sinks (CS) are not necessarily needed at high altitudes to promote the occurrence of NPF. For stations at altitudes higher than 1000 m a.s.l., higher CSs favor NPF and are thought to be associated with precursor gases needed to initiate nucleation and early growth.

scholarly journals New Particle Formation and impact on CCN concentrations in the boundary layer and free troposphere at the high altitude station of Chacaltaya (5240 m a.s.l.), Bolivia

2016 ◽  
Author(s):  
C. Rose ◽  
K. Sellegri ◽  
I. Moreno ◽  
F. Velarde ◽  
M. Ramonet ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Particle Number ◽  
Particle Growth ◽  
Particle Formation ◽  
Number Concentration ◽  
Particle Number Concentration ◽  
Free Troposphere ◽  
New Particle Formation ◽  
Radiative Processes ◽  
The Impact

Abstract. Global models predict that new particle formation (NPF) is, in some environments, responsible for a substantial fraction of the total atmospheric particle number concentration and subsequently contribute significantly to cloud condensation nuclei (CCN) concentrations. NPF events were frequently observed at the highest atmospheric observatory in the world, Chacaltaya (5240 m a.s.l.), Bolivia. The present study focuses on the impact of NPF on CCN population. Neutral cluster and Air Ion Spectrometer and mobility particle size spectrometer measurements were simultaneously used to follow the growth of particles from cluster sizes down to ~ 2 nm up to CCN threshold sizes set to 50, 80 and 100 nm. Using measurements performed between January 1 and December 31 2012, we found that 61% of the 94 analysed events showed a clear particle growth and significant enhancement of the CCN-relevant particle number concentration. We evaluated the contribution of NPF events relative to the transport of pre-existing particles to the site. The averaged production of 50 nm particles during those events was 5072 cm−3, and 1481 cm−3 for 100 nm particles, with a larger contribution of NPF compared to transport, especially during the wet season. The data set was further segregated into boundary layer (BL) and free troposphere (FT) conditions at the site. The NPF frequency of occurrence was higher in the BL (48 %) compared to the FT (39 %). Particle condensational growth was more frequently observed for events initiated in the FT, but on average faster for those initiated in the BL, when the amount of condensable species was most probably larger. As a result, the potential to form new CCN was higher for events initiated in the BL (67 % against 56 % in the FT). In contrast, higher CCN number concentration increases were found when the NPF process initially occurred in the FT, under less polluted conditions. This work highlights the competition between particle growth and the removal of freshly nucleated particles by coagulation processes. The results support model predictions which suggest that NPF is an effective source of CCN in some environments, and thus may influence regional climate through cloud related radiative processes.

scholarly journals Wintertime new particle formation and its contribution to cloud condensation nuclei in the Northeastern United States

2020 ◽  
Vol 20 (4) ◽  
pp. 2591-2601
Author(s):  
Fangqun Yu ◽  
Gan Luo ◽  
Arshad Arjunan Nair ◽  
James J. Schwab ◽  
James P. Sherman ◽  
...  
Keyword(s):  
United States ◽  
Particle Number ◽  
Hydrological Cycle ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
New Particle Formation ◽  
Northeastern United States ◽  
Condensation Nuclei ◽  
Upper Troposphere ◽  
Inorganic Species

Abstract. Atmospheric particles can act as cloud condensation nuclei (CCN) and modify cloud properties and precipitation and thus indirectly impact the hydrological cycle and climate. New particle formation (NPF or nucleation), frequently observed at locations around the globe, is an important source of ultrafine particles and CCN in the atmosphere. In this study, wintertime NPF over the Northeastern United States (NEUS) is simulated with WRF-Chem coupled with a size-resolved (sectional) advanced particle microphysics (APM) model. Model-simulated variations in particle number concentrations during a 2-month period (November–December 2013) are in agreement with corresponding measurements taken at Pinnacle State Park (PSP), New York, and Appalachian State University (APP), North Carolina. We show that, even during wintertime, regional nucleation occurs and contributes significantly to ultrafine-particle and CCN number concentrations over the NEUS. The model shows that, due to low biogenic emissions during this period, wintertime regional nucleation is solely controlled by inorganic species and the newly developed ternary ion-mediated nucleation scheme is able to capture the variations in observed particle number concentrations (ranging from ∼200 to 20 000 cm−3) at both PSP and APP. Total particle and CCN number concentrations dramatically increase following NPF events and have the highest values over the Ohio Valley region, where elevated [SO2] is sustained by power plants. Secondary particles dominate particle number abundance over the NEUS, and their fraction increases with altitude from ≳85 % near the surface to ≳95 % in the upper troposphere. The secondary fraction of CCN also increases with altitude, from 20 %–50 % in the lower boundary layer to 50 %–60 % in the middle troposphere to 70 %–85 % in the upper troposphere.

Regional modelling of aerosol interaction with deep convection and the effect on new particle formation over Amazonia

2020 ◽  
Author(s):  
Xuemei Wang ◽  
Daniel Grosvenor ◽  
Hamish Gordon ◽  
Meinrat O. Andreae ◽  
Ken Carslaw
Keyword(s):  
Boundary Layer ◽  
Cloud Condensation Nuclei ◽  
Deep Convection ◽  
Particle Formation ◽  
Nucleation Mechanism ◽  
Transport Processes ◽  
Radiative Properties ◽  
Free Troposphere ◽  
New Particle Formation ◽  
New Particles

<p>It has been estimated that over 50% of the present-day global low-level cloud condensation nuclei (CCN) are formed from new particle formation (NPF), and that this process has a substantial effect on the radiative properties of shallow clouds (Gordon et al. 2017). In contrast, we have a very limited understanding of how NPF affects deep convective clouds. Deep clouds could interact strongly with NPF because they extend into the high free troposphere where most new particles are formed, and they are responsible for most of the vertical transport of the nucleating vapours. Andreae et al. (2018) hypothesised from ACRIDICON-CHUVA campaign that organic gas molecules are transported by deep convection to the upper troposphere where they are oxidised and produce new particles, which are then be entrained into the boundary layer and grow to CCN-relevent sizes.</p><p>Here we study the interaction of deep convection and NPF using the United Kingdom Chemistry and Aerosols (UKCA) model coupled with the Cloud-AeroSol Interacting Microphyics (CASIM) embedded in the regional configuration of UK Met Office Hadley Centre Global Environment Model (HadGEM3). We simulate several days over a 1000 km region of the Amazon at 4 km resolution. We then compare the regional model, which resolves cloud up- and downdrafts, with the global model with parameterised convection and low resolution.</p><p>Our simulations highlight three findings. Firstly, solely using a binary H<sub>2</sub>SO<sub>4</sub>-H<sub>2</sub>O nucleation mechanism strongly underestimates total aerosol concentrations compared to observations by a factor of 1.5-8 below 3 km over the Amazon. This points to the potential role of an additional nucleation mechanism, most likely involving biogenic compounds that occurs throughout more of the free troposphere. Secondly, deep convection transports insoluble gases such as DMS and monoterpenes vertically but not SO<sub>2</sub> or H<sub>2</sub>SO<sub>4</sub>. The time scale for DMS oxidation (~ 1 day) is much longer than for monoterpene (1-2 hours), which points to the importance of simulating biogenic nucleation over the Amazon in a cloud-resolving model, while lower-resolution global models may adequately capture DMS effects on H<sub>2</sub>SO<sub>4</sub> nucleation. Finally, we also examine the Andreae et al (2018) hypothesis of aerosol supply to the boundary layer by quantifying cloud-free and cloudy up- and downdraft transport. The transport of newly formed aerosols into the boundary layer is 8 times greater in cloud-free regions than in the clouds, but these transport processes are of similar magnitude for large aerosols.</p>

scholarly journals Submicron aerosols at thirteen diversified sites in China: size distribution, new particle formation and corresponding contribution to cloud condensation nuclei production

2014 ◽  
Vol 14 (10) ◽  
pp. 15149-15189 ◽  
Author(s):  
J. F. Peng ◽  
M. Hu ◽  
Z. B. Wang ◽  
X. F. Huang ◽  
P. Kumar ◽  
...  
Keyword(s):  
Size Distribution ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
New Particle Formation ◽  
Condensation Nuclei ◽  
Accumulation Mode ◽  
Nucleation Mode ◽  
Secondary Formation ◽  
Urban Sites

Abstract. Understanding the particle number size distributions in diversified atmospheric environments is important in order to design mitigation strategies related to submicron particles and their effect on regional air quality, haze and human health. In this study, we conducted 15 different field measurement campaigns, each one-month long, between 2007 and 2011 at 13 individual sites in China. These were 5 urban sites, 4 regional sites, 3 coastal/background sites and one ship cruise measurement along eastern coastline of China. Size resolved particles were measured in the 15–600 nm size range. The median particle number concentrations (PNC) were found to vary in the range of 1.1–2.2 × 104 cm−3 at urban sites, 0.8–1.5 × 104 cm−3 at regional sites, 0.4–0.6 × 104 cm−3 at coastal/background sites, and 0.5 × 104 cm−3 during cruise measurements. Peak diameters at each of these sites varied greatly from 24 nm to 115 nm. Particles in the 15–25 nm (nucleation mode), 25–100 nm (Aitken mode) and 100–600 nm (accumulation mode) range showed different characteristics at each of the studied sites, indicating the features of primary emissions and secondary formation in these diversified atmospheric environments. Diurnal variations show a build-up of accumulation mode particles belt at regional sites, suggesting the contribution of regional secondary aerosol pollution. Frequencies of new particle formation (NPF) events were much higher at urban and regional sites than at coastal sites and cruise measurement. The average growth rates (GRs) of nucleation mode particles were 8.0–10.9 nm h−1 at urban sites, 7.4–13.6 nm h−1 at regional sites and 2.8–7.5 nm h−1 at both coastal and cruise measurement sites. The high gaseous precursors and strong oxidation at urban and regional sites not only favored the formation of particles, but also accelerated the growth rate of the nucleation mode particles. No significant difference in condensation sink (CS) during NPF days were observed among different site types, suggesting that the NPF events in background area were more influenced by the pollutant transport. In addition, average contributions of NPF events to potential cloud condensation nuclei (CCN) at 0.2% super-saturation in the afternoon of all sampling days were calculated as 11% and 6% at urban sites and regional sites, respectively. On the other hand, NPF events at coastal and cruise measurement sites had little impact on potential production of CCN. This study provides a large dataset of aerosol size distribution in diversified atmosphere of China, improving our general understanding of emission, secondary formation, new particles formation and corresponding CCN activity of submicron aerosols in Chinese environments.

scholarly journals Impact of temperature dependence on the possible contribution of organics to new particle formation in the atmosphere

2017 ◽  
Vol 17 (8) ◽  
pp. 4997-5005 ◽  
Author(s):  
Fangqun Yu ◽  
Gan Luo ◽  
Alexey B. Nadykto ◽  
Jason Herb
Keyword(s):  
North America ◽  
Temperature Dependence ◽  
Radiative Forcing ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Lower Troposphere ◽  
Particle Formation ◽  
Strong Impact ◽  
New Particle Formation ◽  
Aerosol Model

Abstract. Secondary particles formed via new particle formation (NPF) dominate cloud condensation nuclei (CCN) abundance in most parts of the troposphere and are important for aerosol indirect radiative forcing (IRF). Laboratory measurements have shown that certain organic compounds can significantly enhance the binary nucleation of sulfuric acid and H2O. According to our recent study comparing particle size distributions measured in nine forest areas in North America with those predicted by a global size-resolved aerosol model, current H2SO4–organics nucleation parameterizations appear to significantly overpredict NPF and particle number concentrations in summer. The lack of temperature dependence in the current H2SO4–organics nucleation parameterization has been suggested to be a possible reason for the observed overprediction. In this work, H2SO4–organics clustering thermodynamics from quantum chemical studies has been employed to develop a scheme to incorporate temperature dependence into H2SO4–organics nucleation parameterization. We show that temperature has a strong impact on H2SO4–organics nucleation rates and may reduce the nucleation rate by  ∼  1 order of magnitude per 10 K of temperature increase. The particle number concentrations in summer over North America based on the revised scheme is a factor of more than 2 lower, which is in much better agreement with the observations. With the temperature-dependent H2SO4–organics nucleation parameterization, the summer CCN concentrations in the lower troposphere in the Northern Hemisphere are about 10–30 % lower compared to the temperature-independent parameterization. This study highlights the importance of the temperature effect and its impacts on NPF in the global modeling of aerosol number abundance.

scholarly journals Secondary new particle formation in Northern Finland Pallas site between the years 2000 and 2010

2011 ◽  
Vol 11 (24) ◽  
pp. 12959-12972 ◽  
Author(s):  
E. Asmi ◽  
N. Kivekäs ◽  
V.-M. Kerminen ◽  
M. Komppula ◽  
A.-P. Hyvärinen ◽  
...  
Keyword(s):  
Growth Rates ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Detailed Examination ◽  
Particle Formation ◽  
New Particle Formation ◽  
Air Masses ◽  
Event Frequency ◽  
Marine Air

Abstract. Secondary new particle formation affects atmospheric aerosol and cloud droplet numbers and thereby, the aerosol effects on climate. In this paper, the frequency of nucleation events and the associated particle formation and growth rates, along with their seasonal variation, was analysed based on over ten years of aerosol measurements conducted at the Pallas GAW station in northern Finland. The long-term measurements also allowed a detailed examination of factors possibly favouring or suppressing particle formation. Effects of meteorological parameters and air mass properties as well as vapour sources and sinks for particle formation frequency and event parameters were inspected. In addition, the potential of secondary particle formation to increase the concentration of cloud condensation nuclei (CCN) sized particles was examined. Findings from these long-term measurements confirmed previous observations: event frequency peaked in spring and the highest growth rates were observed in summer, affiliated with increased biogenic activity. Events were almost exclusively observed in marine air masses on sunny cloud-free days. A low vapour sink by the background particle population as well as an elevated sulphuric acid concentration were found to favour particle formation. These were also conditions taking place most likely in marine air masses. Inter-annual trend showed a minimum in event frequency in 2003, when also the smallest annual median of growth rate was observed. This gives further evidence of the importance and sensitivity of particle formation for the condensing vapour concentrations at Pallas site. The particle formation was observed to increase CCN80 (>80 nm particle number) concentrations especially in summer and autumn seasons when the growth rates were the highest. When the growing mode exceeded the selected 80 nm limit, on average in those cases, 211 ± 114% increase of CCN80 concentrations was observed.

scholarly journals Spring and summer contrast in new particle formation over nine forest areas in North America

2015 ◽  
Vol 15 (24) ◽  
pp. 13993-14003 ◽  
Author(s):  
F. Yu ◽  
G. Luo ◽  
S. C. Pryor ◽  
P. R. Pillai ◽  
S. H. Lee ◽  
...  
Keyword(s):  
North America ◽  
Radiative Forcing ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Formation Rate ◽  
Ultrafine Particle ◽  
Particle Formation ◽  
New Particle Formation ◽  
Forest Sites ◽  
Chamber Studies

Abstract. Recent laboratory chamber studies indicate a significant role for highly oxidized low-volatility organics in new particle formation (NPF), but the actual role of these highly oxidized low-volatility organics in atmospheric NPF remains uncertain. Here, particle size distributions (PSDs) measured in nine forest areas in North America are used to characterize the occurrence and intensity of NPF and to evaluate model simulations using an empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low-volatility organics from alpha-pinene oxidation (Nucl-Org), and using an ion-mediated nucleation mechanism (excluding organics) (Nucl-IMN). On average, NPF occurred on ~ 70 % of days during March for the four forest sites with springtime PSD measurements, while NPF occurred on only ~ 10 % of days in July for all nine forest sites. Both Nucl-Org and Nucl-IMN schemes capture the observed high frequency of NPF in spring, but the Nucl-Org scheme significantly overpredicts while the Nucl-IMN scheme slightly underpredicts NPF and particle number concentrations in summer. Statistical analyses of observed and simulated ultrafine particle number concentrations and frequency of NPF events indicate that the scheme without organics agrees better overall with observations. The two schemes predict quite different nucleation rates (including their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America, highlighting the need to reduce NPF uncertainties in regional and global earth system models.

scholarly journals Spring and summer contrast in new particle formation over nine forest areas in North America

2015 ◽  
Vol 15 (15) ◽  
pp. 21271-21298 ◽  
Author(s):  
F. Yu ◽  
G. Luo ◽  
S. C. Pryor ◽  
P. R. Pillai ◽  
S. H. Lee ◽  
...  
Keyword(s):  
North America ◽  
Radiative Forcing ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Formation Rate ◽  
Ultrafine Particle ◽  
Particle Formation ◽  
New Particle Formation ◽  
Forest Sites ◽  
Chamber Studies

Abstract. Recent laboratory chamber studies indicate a significant role for highly oxidized low volatility organics in new particle formation (NPF) but the actual role of these highly oxidized low volatility organics in atmospheric NPF remains uncertain. Here, particle size distributions (PSDs) measured in nine forest areas in North America are used to characterize the occurrence and intensity of NPF and to evaluate model simulations using an empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low volatility organics from alpha-pinene oxidation (Nucl-Org), and using an ion-mediated nucleation mechanism (excluding organics; Nucl-IMN). On average, NPF occurred on ~ 70 % of days during March for the four forest sites with springtime PSD measurements, while NPF occurred on only ~ 10 % of days in July for all nine forest sites. Both Nucl-Org and Nucl-IMN schemes capture the observed high frequency of NPF in spring, but the Nucl-Org scheme significantly over-predicts while the Nucl-IMN scheme slightly under-predicts NPF and particle number concentrations in summer. Statistical analyses of observed and simulated ultrafine particle number concentrations and frequency of NPF events indicate that the scheme without organics agrees better overall with observations. The two schemes predict quite different nucleation rates (including their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America, highlighting the need to reduce NPF uncertainties in regional and global earth system models.

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