scholarly journals Long-term observations of aerosol size distributions in semi-clean and polluted savannah in South Africa

2013 ◽  
Vol 13 (4) ◽  
pp. 1751-1770 ◽  
Author(s):  
V. Vakkari ◽  
J. P. Beukes ◽  
H. Laakso ◽  
D. Mabaso ◽  
J. J. Pienaar ◽  
...  

Abstract. This study presents a total of four years of sub-micron aerosol particle size distribution measurements in the southern African savannah, an environment with few previous observations covering a full seasonal cycle and the size range below 100 nm. During the first 19 months, July 2006–January 2008, the measurements were carried out at Botsalano, a semi-clean location, whereas during the latter part, February 2008–May 2010, the measurements were carried out at Marikana (approximately 150 km east of Botsalano), which is a more polluted location with both pyrometallurgical industries and informal settlements nearby. The median total concentration of aerosol particles was more than four times as high at Marikana than at Botsalano. In the size ranges of 12–840 nm, 50–840 nm and 100–840 nm the median concentrations were 1856, 1278 and 698 particles cm−3 at Botsalano and 7805, 3843 and 1634 particles cm−3 at Marikana, respectively. The diurnal variation of the size distribution for Botsalano arose as a result of frequent regional new particle formation. However, for Marikana the diurnal variation was dominated by the morning and evening household burning in the informal settlements, although regional new particle formation was even more frequent than at Botsalano. The effect of the industrial emissions was not discernible in the size distribution at Marikana although it was clear in the sulphur dioxide diurnal pattern, indicating the emissions to be mostly gaseous. Seasonal variation was strongest in the concentration of particles larger than 100 nm, which was clearly elevated at both locations during the dry season from May to September. In the absence of wet removal during the dry season, the concentration of particles larger than 100 nm had a correlation above 0.7 with CO for both locations, which implies incomplete burning to be an important source of aerosol particles during the dry season. However, the sources of burning differ: at Botsalano the rise in concentration originates from regional wild fires, while at Marikana domestic heating in the informal settlements is the main source. Air mass history analysis for Botsalano identified four regional scale source areas in southern Africa and enabled the differentiation between fresh and aged rural background aerosol originating from the clean sector, i.e., western sector with very few large anthropogenic sources. Comparison to size distributions published for other comparable environments in Northern Hemisphere shows southern African savannah to have a unique combination of sources and meteorological parameters. The observed strong link between combustion and seasonal variation is comparable only to the Amazon basin; however, the lack of long-term observations in the Amazonas does not allow a quantitative comparison. All the data presented in the figures, as well as the time series of monthly mean and median size distributions are included in numeric form as a Supplement to provide a reference point for the aerosol modelling community.

2012 ◽  
Vol 12 (9) ◽  
pp. 24043-24093
Author(s):  
V. Vakkari ◽  
J. P. Beukes ◽  
H. Laakso ◽  
D. Mabaso ◽  
J. J. Pienaar ◽  
...  

Abstract. This study presents a total of four years of sub-micron aerosol particle size distribution measurements in the Southern African savannah, an environment with few previous observations covering a full seasonal cycle and the size range below 100 nm. During the first 19 months, July 2006–January 2008, the measurements were carried out at Botsalano, a semi-clean location, whereas during the latter part, February 2008–May 2010, the measurements were carried out at Marikana (approximately 150 km east of Botsalano), which is a more polluted location with both pyrometallurgical industries and informal settlements nearby. The median total concentration of aerosol particles was more than four times as high at Marikana than at Botsalano. In the size ranges of 12–840 nm, 50–840 nm and 100–840 nm the median concentrations were 1850, 1280 and 700 particles cm−3 at Botsalano and 7800, 3800 and 1600 particles cm−3 at Marikana, respectively. The diurnal variation of the size distribution for Botsalano arose as a result of frequent regional new particle formation. However, for Marikana the diurnal variation was dominated by the morning and evening household burning in the informal settlements, although regional new particle formation was even more frequent than at Botsalano. The effect of the industrial emissions was not discernible in the size distribution at Marikana although it was clear in the sulphur dioxide diurnal pattern, indicating the emissions to be mostly gaseous. Seasonal variation was strongest in the concentration of particles larger than 100 nm, which was clearly elevated at both locations during the dry season from May to September. In the absence of wet removal during the dry season the concentration of particles larger than 100 nm had a correlation above 0.7 with CO for both locations, which implies incomplete burning to be an important source of aerosol particles during the dry season. However, the sources of burning differ: at Botsalano the rise in concentration originates from regional wild fires, while at Marikana domestic heating in the informal settlements is the main source. Air mass history analysis for Botsalano identified four regional scale source areas in Southern Africa and enabled the differentiation between fresh and aged rural background aerosol originating from the clean sector, i.e., western sector with very few large anthropogenic sources. Comparison to size distributions published for other comparable environments in Northern Hemisphere shows Southern African savannah to have a unique combination of sources and meteorological parameters. The observed strong link between combustion and seasonal variation is comparable only to the Amazon basin; however the lack of long-term observations in the Amazonas does not allow a quantitative comparison. All the data presented in the figures, as well as the time series of monthly mean and median size distributions are included in numeric form as a Supplement to provide a reference point for the aerosol modelling community.


2007 ◽  
Vol 7 (1) ◽  
pp. 211-222 ◽  
Author(s):  
M. Ehn ◽  
T. Petäjä ◽  
H. Aufmhoff ◽  
P. Aalto ◽  
K. Hämeri ◽  
...  

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.


2019 ◽  
Vol 19 (18) ◽  
pp. 11985-12006 ◽  
Author(s):  
Peter J. Marinescu ◽  
Ezra J. T. Levin ◽  
Don Collins ◽  
Sonia M. Kreidenweis ◽  
Susan C. van den Heever

Abstract. A quality-controlled, 5-year dataset of aerosol number size distributions (particles with diameters (Dp) from 7 nm through 14 µm) was developed using observations from a scanning mobility particle sizer, aerodynamic particle sizer, and a condensation particle counter at the Department of Energy's Southern Great Plains (SGP) site. This dataset was used for two purposes. First, typical characteristics of the aerosol size distribution (number, surface area, and volume) were calculated for the SGP site, both for the entire dataset and on a seasonal basis, and size distribution lognormal fit parameters are provided. While the median size distributions generally had similar shapes (four lognormal modes) in all the seasons, there were some significant differences between seasons. These differences were most significant in the smallest particles (Dp<30 nm) and largest particles (Dp>800 nm). Second, power spectral analysis was conducted on this long-term dataset to determine key temporal cycles of total aerosol concentrations, as well as aerosol concentrations in specified size ranges. The strongest cyclic signal was associated with a diurnal cycle in total aerosol number concentrations that was driven by the number concentrations of the smallest particles (Dp<30 nm). This diurnal cycle in the smallest particles occurred in all seasons in ∼50 % of the observations, suggesting a persistent influence of new particle formation events on the number concentrations observed at the SGP site. This finding is in contrast with earlier studies that suggest new particle formation is observed primarily in the springtime at this site. The timing of peak concentrations associated with this diurnal cycle was shifted by several hours depending on the season, which was consistent with seasonal differences in insolation and boundary layer processes. Significant diurnal cycles in number concentrations were also found for particles with Dp between 140 and 800 nm, with peak concentrations occurring in the overnight hours, which were primarily associated with both nitrate and organic aerosol cycles. Weaker cyclic signals were observed for longer timescales (days to weeks) and are hypothesized to be related to the timescales of synoptic weather variability. The strongest periodic signals (3.5–5 and 7 d cycles) for these longer timescales varied depending on the season, with no cyclic signals and the lowest variability in the summer.


2021 ◽  
Author(s):  
Tuija Jokinen ◽  
Katrianne Lehtipalo ◽  
Kimmo Neitola ◽  
Nina Sarnela ◽  
Totti Laitinen ◽  
...  

&lt;p&gt;One way to form aerosol particles is the condensation of oxidized atmospheric trace gases, such as sulfuric acid (SA) into small molecular clusters. After growing to larger particles by condensation of low volatile gases, they can affect the planets climate directly by scattering light and indirectly by acting as cloud condensation nuclei. Observations of low-volatility aerosol precursor gases have been reported around the world but long-term measurement series and Arctic data sets showing seasonal variation are close to non-existent. In here, we present ~7 months of aerosol precursor gas measurements performed with the nitrate based chemical ionization mass spectrometer (CI-APi-TOF). We deployed our measurements ~250 km above the Arctic Circle at the Finnish sub-Arctic field station, SMEAR I in V&amp;#228;rri&amp;#246;. We report concentration measurements of the most common new particle formation related compounds; sulfuric acid, methanesulfonic acid (MSA), iodic acid (IA) and highly oxygenated organic compounds, HOMs. At this remote measurement site, surrounded by a strict nature preserve, that gets occasional pollution from a Russian city of Murmansk, SA is originated both from anthropogenic and biological sources and has a clear diurnal cycle but no significant seasonal variation, while MSA as an oxidation product of purely biogenic sources is showing a more distinct seasonal cycle. Iodic acid concentrations are the most stable throughout the measurement period, showing almost identical peak concentrations for spring, summer and autumn. HOMs are abundant during the summer months and due to their high correlation with ambient air temperature, we suggest that most of HOMs are products of monoterpene oxidation. New particle formation events at SMEAR I happen under relatively low temperatures, low relative humidity, high ozone concentration, high SA concentration in the morning and high MSA concentrations in the afternoon. The role of HOMs in aerosol formation will be discussed. All together, these are the first long term measurements of aerosol forming precursor from the sub-arctic region helping us to understand atmospheric chemical processes and aerosol formation in the rapidly changing Arctic.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;


2021 ◽  
Author(s):  
Anastasiia Demakova ◽  
Olga Garmash ◽  
Ekaterina Ezhova ◽  
Mikhail Arshinov ◽  
Denis Davydov ◽  
...  

&lt;p&gt;New Particle Formation (NPF) is a process in which a large number of particles is formed in the atmosphere via gas-to-particle conversion. Previous research shows the important role of formation of new particles for atmosphere, clouds and climate (Kerminen, V.-M. et al. 2018).&lt;/p&gt;&lt;p&gt;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; There exist measurements from different parts of the world which show that NPF is happening worldwide (Kerminen, V.-M. et al. 2018). Measurements at SMEAR II station in Hyyti&amp;#228;l&amp;#228;, Finland (Hari P. and Kulmala M., 2005), show that NPF is a common process in Finland&amp;#8217;s boreal forests. However, measurements at Zotto station in Siberia, Russia, show that NPF events are very rare in that area (Wiedensohler A. et al., 2018). Measurements in Siberian boreal forests are sparse. We have conducted new measurements at Fonovaya station near Tomsk (Siberia, Russia) using Neutral cluster Air Ion Spectrometer (NAIS), Particle Size Magnifier (PSM), Differential Mobility Particle Sizer (DMPS) and the Atmospheric Pressure interface Time-Of-Flight mass spectrometer (APi-TOF). Those instruments measure aerosol particle number size distribution (NAIS, DMPS), ion number size distribution (NAIS), size distribution of small particles (PSM) and chemical composition of aerosol particles (APi-TOF). The novelty of this work is that such complex measurements have not been done in Siberia before.&lt;/p&gt;&lt;p&gt;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; Here we report the first results of our research on NPF phenomenon in Siberian boreal forest. We present detailed statistics of NPF events, as well as formation rates (J) and growth rates (GR) of aerosol particles. The results from Fonovaya station are compared with those from SMEAR II station and from SMEAR Estonia station in J&amp;#228;rvselja, Estonia.&lt;/p&gt;&lt;p&gt;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; &amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Literature&lt;/p&gt;&lt;ul&gt;&lt;li&gt;[1] Kerminen V.-M. et al. &amp;#8220;Atmospheric new particle formation and growth: review of field observations&amp;#8221;. In: Environmental Research Letters 10 (2018), p. 103003.&lt;/li&gt; &lt;li&gt;[2] Wiedensohler A. et al. &amp;#8220;Infrequent new particle formation over the remote boreal forest of Siberia&amp;#8221;. In: Atmospheric Environment 200 (2019), pp. 167&amp;#8211;169.&lt;/li&gt; &lt;li&gt;[3] Dada L. et al. &amp;#8220;Long-term analysis of clear-sky new particle formation events and nonevents in Hyyti&amp;#228;l&amp;#228;&amp;#8221;. In: Atmospheric Chemistry and Physics 10 (2017), pp. 6227&amp;#8211;6241.&lt;/li&gt; &lt;/ul&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;


2020 ◽  
Author(s):  
Nikolay Romanov ◽  
Alexey Paley ◽  
Yuri Andreev ◽  
Sergey Dubtsov ◽  
Oleg Ozols ◽  
...  

Abstract. The paper reports on an investigation of nanometre-sized new particles formation (NPF) in aerosol-free outdoor air. This phenomenon was observed after filling of Large Aerosol Chamber (LAC) RPA Typhoon with the volume of 3200 m3 with outdoor air, passed through HEPA 13 class filter (H13). During the summer-autumn period of 2018, even in the full darkness and in presence ionizing radiation only in the shape of secondary galactic cosmic rays, new particle formation with the particle size greater than 15 nm starts 0.5–1 hour after the end of LAC filling. During the 2018–2019 winter periods the NPF event was not observed once only. Approximately one day after NPF narrow bell-shaped spectra with number concentration up to 104 cm−3 and mass concentration up to 0.6 µg per m3 are formed. During the next five or more days, these size distributions evolve due to coagulation, while their asymptotic shape remains constant with relative breadth σc ≈ 0.28, and relative asymmetry ras ≈ 2 (ras = skewness/σc). The value ras ≈ 2 defines the analytical description of the size distribution as the gamma-distribution. During additional purification of newly formed particles with the inner H13 filter, aerosol particles concentration in LAC decreases down to a few particles per cm3. This concentration remained constant for more than a week. This demonstrates that new aerosol particles are formed by homogeneous gas-to-particle conversion of gaseous precursors, which passed through the external H13 filter. The mass concentration of newly formed particles depends on the concentration of precursors. It was found that after filling LAC with outdoor unfiltered air, approximately after 10 hours the left-hand side of aerosol particle size distribution below 15 nm disappears, and after several days there forms an asymptotic bell-shaped size spectrum with σc ≈ 0.4–0.5 and ras = 2–3. The modal diameter becomes about 150 nm after five days, while the size distribution greater than 200 nm remains unchanged. This allows concluding that aerosol particles greater than 200 nm have a life-time of more than five days, while particles smaller than 15 nm, not more than five hours. The observed regularities of NPF and pre-existing aerosol spectra evolution may contribute significantly to understanding the processes of the formation of atmospheric aerosols, which are responsible for cloud and precipitation formation. They also should be considered during the design of purification methods for facilities and living spaces. During the investigation of size distribution evolution of aerosol particles generated by the spraying of tap water, it was found that this aerosol particles size distribution transforms from a power law to a bell-shaped distribution in five days with σc ≈ 0.4 and ras ≈ 2. These results may be used for the development of aerosol evolution models.


2018 ◽  
Vol 18 (13) ◽  
pp. 9597-9615 ◽  
Author(s):  
Jorma Joutsensaari ◽  
Matthew Ozon ◽  
Tuomo Nieminen ◽  
Santtu Mikkonen ◽  
Timo Lähivaara ◽  
...  

Abstract. New particle formation (NPF) in the atmosphere is globally an important source of climate relevant aerosol particles. Occurrence of NPF events is typically analyzed by researchers manually from particle size distribution data day by day, which is time consuming and the classification of event types may be inconsistent. To get more reliable and consistent results, the NPF event analysis should be automatized. We have developed an automatic analysis method based on deep learning, a subarea of machine learning, for NPF event identification. To our knowledge, this is the first time that a deep learning method, i.e., transfer learning of a convolutional neural network (CNN), has successfully been used to automatically classify NPF events into different classes directly from particle size distribution images, similarly to how the researchers carry out the manual classification. The developed method is based on image analysis of particle size distributions using a pretrained deep CNN, named AlexNet, which was transfer learned to recognize NPF event classes (six different types). In transfer learning, a partial set of particle size distribution images was used in the training stage of the CNN and the rest of the images for testing the success of the training. The method was utilized for a 15-year-long dataset measured at San Pietro Capofiume (SPC) in Italy. We studied the performance of the training with different training and testing of image number ratios as well as with different regions of interest in the images. The results show that clear event (i.e., classes 1 and 2) and nonevent days can be identified with an accuracy of ca. 80 %, when the CNN classification is compared with that of an expert, which is a good first result for automatic NPF event analysis. In the event classification, the choice between different event classes is not an easy task even for trained researchers, and thus overlapping or confusion between different classes occurs. Hence, we cross-validated the learning results of CNN with the expert-made classification. The results show that the overlapping occurs, typically between the adjacent or similar type of classes, e.g., a manually classified Class 1 is categorized mainly into classes 1 and 2 by CNN, indicating that the manual and CNN classifications are very consistent for most of the days. The classification would be more consistent, by both human and CNN, if only two different classes are used for event days instead of three classes. Thus, we recommend that in the future analysis, event days should be categorized into classes of “quantifiable” (i.e., clear events, classes 1 and 2) and “nonquantifiable” (i.e., weak events, Class  3). This would better describe the difference of those classes: both formation and growth rates can be determined for quantifiable days but not both for nonquantifiable days. Furthermore, we investigated more deeply the days that are classified as clear events by experts and recognized as nonevents by the CNN and vice versa. Clear misclassifications seem to occur more commonly in manual analysis than in the CNN categorization, which is mostly due to the inconsistency in the human-made classification or errors in the booking of the event class. In general, the automatic CNN classifier has a better reliability and repeatability in NPF event classification than human-made classification and, thus, the transfer-learned pretrained CNNs are powerful tools to analyze long-term datasets. The developed NPF event classifier can be easily utilized to analyze any long-term datasets more accurately and consistently, which helps us to understand in detail aerosol–climate interactions and the long-term effects of climate change on NPF in the atmosphere. We encourage researchers to use the model in other sites. However, we suggest that the CNN should be transfer learned again for new site data with a minimum of ca. 150 figures per class to obtain good enough classification results, especially if the size distribution evolution differs from training data. In the future, we will utilize the method for data from other sites, develop it to analyze more parameters and evaluate how successfully CNN could be trained with synthetic NPF event data.


2012 ◽  
Vol 12 (11) ◽  
pp. 29967-30019 ◽  
Author(s):  
P. Tunved ◽  
J. Ström ◽  
R. Krejci

Abstract. In this study we present a qualitative and quantitative assessment of more the 10 yr of aerosol number size distribution data observed in the Arctic environment (Mt Zeppelin (78°56' N, 11°53' E, 474 m a.s.l.), Ny Ålesund, Svalbard). We provide statistics on both seasonal and diurnal characteristics of the aerosol observations and conclude that the Arctic aerosol number size distribution and auxiliary parameters such as integral mass and surface have a very pronounced seasonal variation. This seasonal variation seems to be controlled by both dominating source as well as meteorological conditions in general. In principle, three distinctly different periods can be identified during the Arctic year: the haze period characterized by a dominating accumulation mode aerosol (March–May) followed by the sunlit summer period with low abundance of accumulation mode particles but high concentration of small particles which likely are recently and locally formed (June–August). The rest of the year is characterized by comparably low concentration of accumulation mode particles and negligible abundance of ultra fine particles (September–February). Minimum aerosol mass and number concentration is usually observed during September/October. We further show that the transition between the different regimes is fast, suggesting rapid change in conditions defining their appearance. A source climatology based on trajectory analysis is provided and it is shown that there is a strong seasonality of dominating source areas, with dominance of Eurasia during the autumn-winter period and dominance of North Atlantic air during the summer months. We also show that new particle formation events seem to be a rather common phenomenon during the Arctic summer, and this is the result of both photochemical production of nucleating/condensing species and low condensation sink. It is also suggested that wet removal play a key role in defining the Arctic aerosol year, and plays a crucial role for removal of accumulation mode size particles as well as it may play a pivotal role for facilitating the conditions favoring new particle formation events. In summary the aerosol Arctic year seems to be at least qualitatively predictable based on knowledge of seasonality of transport paths and associated source areas, meteorological conditions and removal processes.


2013 ◽  
Vol 13 (7) ◽  
pp. 3643-3660 ◽  
Author(s):  
P. Tunved ◽  
J. Ström ◽  
R. Krejci

Abstract. In this study we present a qualitative and quantitative assessment of more than 10 yr of aerosol number size distribution data observed in the Arctic environment (Mt. Zeppelin (78°56' N, 11°53' E, 474 m a.s.l.), Ny Ålesund, Svalbard). We provide statistics on both seasonal and diurnal characteristics of the aerosol observations and conclude that the Arctic aerosol number size distribution and related parameters such as integral mass and surface area exhibit a very pronounced seasonal variation. This seasonal variation seems to be controlled by both dominating source as well as meteorological conditions. Three distinctly different periods can be identified during the Arctic year: the haze period characterized by a dominating accumulation mode aerosol (March–May), followed by the sunlit summer period with low abundance of accumulation mode particles but high concentration of small particles which are likely to be recently and locally formed (June–August). The rest of the year is characterized by a comparably low concentration of accumulation mode particles and negligible abundance of ultrafine particles (September–February). A minimum in aerosol mass and number concentration is usually observed during September/October. We further show that the transition between the different regimes is fast, suggesting rapid change in the conditions defining their appearance. A source climatology based on trajectory analysis is provided, and it is shown that there is a strong seasonality of dominating source areas, with Eurasia dominating during the Autumn–Winter period and dominance of North Atlantic air during the summer months. We also show that new-particle formation events are rather common phenomena in the Arctic during summer, and this is the result of photochemical production of nucleating/condensing species in combination with low condensation sink. It is also suggested that wet removal may play a key role in defining the Arctic aerosol year, via the removal of accumulation mode size particles, which in turn have a pivotal role in facilitating the conditions favorable for new-particle formation events. In summary the aerosol Arctic year seems to be at least qualitatively predictable based on the knowledge of seasonality of transport paths and associated source areas, meteorological conditions and removal processes.


Sign in / Sign up

Export Citation Format

Share Document