Comments of “Global analysis of continental boundary layer new particle formation based on long-term measurements”

2018 ◽  
Author(s):  
Anonymous
Atmosphere ◽  
2019 ◽  
Vol 10 (9) ◽  
pp. 493 ◽  
Author(s):  
Karine Sellegri ◽  
Clemence Rose ◽  
Angela Marinoni ◽  
Angelo Lupi ◽  
Alfred Wiedensohler ◽  
...  

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.


2016 ◽  
Author(s):  
Lubna Dada ◽  
Pauli Paasonen ◽  
Tuomo Nieminen ◽  
Stephany Buenrostro Mazon ◽  
Jenni Kontkanen ◽  
...  

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.


2007 ◽  
Vol 7 (3) ◽  
pp. 7535-7567
Author(s):  
J. Lauros ◽  
E. D. Nilsson ◽  
M. Dal Maso ◽  
M. Kulmala

Abstract. The connection between new particle formation and micro- and mesoscale meteorology was studied based on measurements at SMEAR II station in Southern Finland. We analyzed turbulent conditions described by sodar measurements and utilized these combined with surface layer measurements and a simple model to estimate the upper boundary layer conditions. Turbulence was significantly stronger on particle formation days and the organic vapor saturation ratio increase due to large eddies was stronger on event than nonevent days. We examined which variables could be the best indicators of new particle formation and concluded that the formation probability depended on the condensation sink and temporal temperature change at the top of the atmospheric boundary layer. Humidity and heat flux may also be good indicators for particle formation.


2016 ◽  
Author(s):  
C. Rose ◽  
K. Sellegri ◽  
I. Moreno ◽  
F. Velarde ◽  
M. Ramonet ◽  
...  

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.


Author(s):  
Lauri Laakso ◽  
T. Grönholm ◽  
S. Haapanala ◽  
Anne Hirsikko ◽  
Theo Kurtén ◽  
...  

2013 ◽  
Author(s):  
Hanna E. Manninen ◽  
Sander Mirme ◽  
Mikael Ehn ◽  
Katri Leino ◽  
Siegfried Schobesberger ◽  
...  

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>


2020 ◽  
Author(s):  
Xuemei Wang ◽  
Daniel Grosvenor ◽  
Hamish Gordon ◽  
Meinrat O. Andreae ◽  
Ken Carslaw

<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>


2000 ◽  
Vol 105 (D21) ◽  
pp. 26531-26546 ◽  
Author(s):  
Liisa Pirjola ◽  
Colin D. O'Dowd ◽  
Ian M. Brooks ◽  
Markku Kulmala

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