scholarly journals Variations in tropospheric submicron particle size distributions across the European continent 2008–2009

2014 ◽  
Vol 14 (8) ◽  
pp. 4327-4348 ◽  
Author(s):  
D. C. S. Beddows ◽  
M. Dall'Osto ◽  
R. M. Harrison ◽  
M. Kulmala ◽  
A. Asmi ◽  
...  

Abstract. Cluster~analysis of particle number size distributions from~background sites across Europe~is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze.~The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected.~These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6–0.9 nm h−1. Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. ~While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.

2013 ◽  
Vol 13 (11) ◽  
pp. 31197-31249 ◽  
Author(s):  
D. C. S. Beddows ◽  
M. Dall'Osto ◽  
Roy M. Harrison ◽  
M. Kulmala ◽  
A. Asmi ◽  
...  

Abstract. Cluster analysis of particle number size distributions from background sites across Europe is presented. This generated a total of nine clusters which could be further combined into two main groups, namely: a South to North category (four clusters) and a West to East category (five clusters). The first category was identified as most frequently being detected inside and around Northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from South-to-North arriving ultimately at the Arctic resulting in Arctic Haze. The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (West to East) at which they were most frequently detected. These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 1–3 nm h−1. Four specific air mass back trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex dataset and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.


2008 ◽  
Vol 8 (22) ◽  
pp. 6729-6738 ◽  
Author(s):  
N. Kalivitis ◽  
W. Birmili ◽  
M. Stock ◽  
B. Wehner ◽  
A. Massling ◽  
...  

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October, 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.


2008 ◽  
Vol 8 (2) ◽  
pp. 6571-6601
Author(s):  
N. Kalivitis ◽  
W. Birmili ◽  
M. Stock ◽  
B. Wehner ◽  
A. Massling ◽  
...  

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.


2020 ◽  
Vol 20 (19) ◽  
pp. 11329-11348 ◽  
Author(s):  
Jenni Kontkanen ◽  
Chenjuan Deng ◽  
Yueyun Fu ◽  
Lubna Dada ◽  
Ying Zhou ◽  
...  

Abstract. The climate and air quality effects of aerosol particles depend on the number and size of the particles. In urban environments, a large fraction of aerosol particles originates from anthropogenic emissions. To evaluate the effects of different pollution sources on air quality, knowledge of size distributions of particle number emissions is needed. Here we introduce a novel method for determining size-resolved particle number emissions, based on measured particle size distributions. We apply our method to data measured in Beijing, China, to determine the number size distribution of emitted particles in a diameter range from 2 to 1000 nm. The observed particle number emissions are dominated by emissions of particles smaller than 30 nm. Our results suggest that traffic is the major source of particle number emissions with the highest emissions observed for particles around 10 nm during rush hours. At sizes below 6 nm, clustering of atmospheric vapors contributes to calculated emissions. The comparison between our calculated emissions and those estimated with an integrated assessment model GAINS (Greenhouse Gas and Air Pollution Interactions and Synergies) shows that our method yields clearly higher particle emissions at sizes below 60 nm, but at sizes above that the two methods agree well. Overall, our method is proven to be a useful tool for gaining new knowledge of the size distributions of particle number emissions in urban environments and for validating emission inventories and models. In the future, the method will be developed by modeling the transport of particles from different sources to obtain more accurate estimates of particle number emissions.


2002 ◽  
Vol 2 (6) ◽  
pp. 2413-2448
Author(s):  
U. Uhrner ◽  
W. Birmili ◽  
F. Stratmann ◽  
M. Wilck ◽  
I. J. Ackermann ◽  
...  

Abstract. At Hohenpeissenberg (47°48'N, 11°07'E, 988 m asl), a rural site 200-300 m higher than the surrounding terrain, sulphuric acid concentrations, particle size distributions, and other trace gas concentrations were measured over a two and a half year period. Measured particle number concentrations and inferred particle surface area-concentrations were compared with box-model simulations based on a multimodal lognormal aerosol module that included a binary sulphuric acid water nucleation scheme. The calculated nucleation rates were corrected with a factor to match measured particle number concentrations. These corrections varied over a range of 10-3 - 1017. The correction factors were close to 1 for the measurements made in the winter, which represented stable thermal stratification and low wind conditions. In contrast, the correction factors were the largest for measurements made under strong convective conditions. Our comparison of measured and simulated particle size distributions suggest a distant particle-formation process under convective conditions near the interface of the mixed layer and the entrainment zone, followed by downward transport and particle growth. For stable stratification and low winds, our comparisons suggest that particles formed close to the measurement site.


2011 ◽  
Vol 11 (13) ◽  
pp. 6623-6637 ◽  
Author(s):  
M. Dall'Osto ◽  
A. Thorpe ◽  
D. C. S. Beddows ◽  
R. M. Harrison ◽  
J. F. Barlow ◽  
...  

Abstract. Nanoparticles emitted from road traffic are the largest source of respiratory exposure for the general public living in urban areas. It has been suggested that adverse health effects of airborne particles may scale with airborne particle number, which if correct, focuses attention on the nanoparticle (less than 100 nm) size range which dominates the number count in urban areas. Urban measurements of particle size distributions have tended to show a broadly similar pattern dominated by a mode centred on 20–30 nm diameter emitted by diesel engine exhaust. In this paper we report the results of measurements of particle number concentration and size distribution made in a major London park as well as on the BT Tower, 160 m aloft. These measurements taken during the REPARTEE project (Regents Park and BT Tower experiment) show a remarkable shift in particle size distributions with major losses of the smallest particle class as particles are advected away from the traffic source. In the Park, the traffic related mode at 20–30 nm diameter is much reduced with a new mode at <10 nm. Size distribution measurements also revealed higher number concentrations of sub-50 nm particles at the BT Tower during days affected by higher turbulence as determined by Doppler Lidar measurements and are indicative of loss of nanoparticles from air aged during less turbulent conditions. These results are suggestive of nanoparticle loss by evaporation, rather than coagulation processes. The results have major implications for understanding the impacts of traffic-generated particulate matter on human health.


2014 ◽  
Vol 7 (3) ◽  
pp. 1137-1157 ◽  
Author(s):  
J. C. Kaiser ◽  
J. Hendricks ◽  
M. Righi ◽  
N. Riemer ◽  
R. A. Zaveri ◽  
...  

Abstract. We introduce MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, 3rd generation; version: MADE3v2.0b), an aerosol dynamics submodel for application within the MESSy framework (Modular Earth Submodel System). MADE3 builds on the predecessor aerosol submodels MADE and MADE-in. Its main new features are the explicit representation of coarse mode particle interactions both with other particles and with condensable gases, and the inclusion of hydrochloric acid (HCl) / chloride (Cl) partitioning between the gas and condensed phases. The aerosol size distribution is represented in the new submodel as a superposition of nine lognormal modes: one for fully soluble particles, one for insoluble particles, and one for mixed particles in each of three size ranges (Aitken, accumulation, and coarse mode size ranges). In order to assess the performance of MADE3 we compare it to its predecessor MADE and to the much more detailed particle-resolved aerosol model PartMC-MOSAIC in a box model simulation of an idealised marine boundary layer test case. MADE3 and MADE results are very similar, except in the coarse mode, where the aerosol is dominated by sea spray particles. Cl is reduced in MADE3 with respect to MADE due to the HCl / Cl partitioning that leads to Cl removal from the sea spray aerosol in our test case. Additionally, the aerosol nitrate concentration is higher in MADE3 due to the condensation of nitric acid on coarse mode particles. MADE3 and PartMC-MOSAIC show substantial differences in the fine particle size distributions (sizes &amp;lesssim; 2 μm) that could be relevant when simulating climate effects on a global scale. Nevertheless, the agreement between MADE3 and PartMC-MOSAIC is very good when it comes to coarse particle size distributions (sizes &amp;gtrsim; 2 μm), and also in terms of aerosol composition. Considering these results and the well-established ability of MADE in reproducing observed aerosol loadings and composition, MADE3 seems suitable for application within a global model.


2020 ◽  
Author(s):  
Jenni Kontkanen ◽  
Chenjuan Deng ◽  
Yueyun Fu ◽  
Lubna Dada ◽  
Ying Zhou ◽  
...  

Abstract. The climate and air quality effects of aerosol particles depend on the number and size of the particles. In urban environments, a large fraction of aerosol particles originates from anthropogenic emissions. To evaluate the effects of different pollution sources on air quality, knowledge of size distributions of particle number emissions is needed. Here we introduce a novel method for determining size-resolved particle number emissions based on measured particle size distributions. We apply our method to data measured in Beijing, China, to determine the number size distribution of emitted particles in diameter range from 2 to 1000 nm. The observed particle number emissions are dominated by emissions of particles smaller than 30 nm. Our results suggest that traffic is the major source of particle number emissions with the highest emissions observed for particles around 10 nm during rush hours. At sizes below 6 nm, clustering of atmospheric vapors contributes to calculated emissions. The comparison between our calculated emissions and those estimated with an integrated assessment model GAINS shows that our method yields clearly higher particle emissions at sizes below 60 nm, but at sizes above that the two methods agree well. Overall, our method is proven to be a useful tool for gaining new knowledge of size distributions of particle number emissions in urban environments.


2020 ◽  
Vol 20 (21) ◽  
pp. 12721-12740
Author(s):  
Jing Cai ◽  
Biwu Chu ◽  
Lei Yao ◽  
Chao Yan ◽  
Liine M. Heikkinen ◽  
...  

Abstract. Although secondary particulate matter is reported to be the main contributor of PM2.5 during haze in Chinese megacities, primary particle emissions also affect particle concentrations. In order to improve estimates of the contribution of primary sources to the particle number and mass concentrations, we performed source apportionment analyses using both chemical fingerprints and particle size distributions measured at the same site in urban Beijing from April to July 2018. Both methods resolved factors related to primary emissions, including vehicular emissions and cooking emissions, which together make up 76 % and 24 % of total particle number and organic aerosol (OA) mass, respectively. Similar source types, including particles related to vehicular emissions (1.6±1.1 µg m−3; 2.4±1.8×103 cm−3 and 5.5±2.8×103 cm−3 for two traffic-related components), cooking emissions (2.6±1.9 µg m−3 and 5.5±3.3×103 cm−3) and secondary aerosols (51±41 µg m−3 and 4.2±3.0×103 cm−3), were resolved by both methods. Converted mass concentrations from particle size distributions components were comparable with those from chemical fingerprints. Size distribution source apportionment separated vehicular emissions into a component with a mode diameter of 20 nm (“traffic-ultrafine”) and a component with a mode diameter of 100 nm (“traffic-fine”). Consistent with similar day- and nighttime diesel vehicle PM2.5 emissions estimated for the Beijing area, traffic-fine particles, hydrocarbon-like OA (HOA, traffic-related factor resulting from source apportionment using chemical fingerprints) and black carbon (BC) showed similar diurnal patterns, with higher concentrations during the night and morning than during the afternoon when the boundary layer is higher. Traffic-ultrafine particles showed the highest concentrations during the rush-hour period, suggesting a prominent role of local gasoline vehicle emissions. In the absence of new particle formation, our results show that vehicular-related emissions (14 % and 30 % for ultrafine and fine particles, respectively) and cooking-activity-related emissions (32 %) dominate the particle number concentration, while secondary particulate matter (over 80 %) governs PM2.5 mass during the non-heating season in Beijing.


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