scholarly journals Classification of aerosol population type and cloud condensation nuclei properties in a coastal California littoral environment using an unsupervised cluster model

2019 ◽  
Author(s):  
Samuel A. Atwood ◽  
Sonia M. Kreidenweis ◽  
Paul J. DeMott ◽  
Markus D. Petters ◽  
Gavin C. Cornwell ◽  
...  

Abstract. Aerosol particle and cloud condensation nuclei (CCN) measurements from a littoral location on the northern coast of California at Bodega Bay Marine Laboratory (BML) are presented for approximately six weeks of observations during the CalWater-2015 field campaign. A combination of aerosol microphysical and meteorological parameters was used to classify variability in the properties of the BML surface aerosol using a K-means cluster model. Eight aerosol population types were identified that were associated with a range of impacts from both marine and terrestrial sources. Average measured total particle number concentrations, size distributions, hygroscopicities, and activated fraction spectra between 0.08 % and 1.1 % supersaturation are given for each of the identified aerosol population types, along with meteorological observations and transport pathways during time periods associated with each type. Five terrestrially influenced aerosol population types represented different degrees of aging of the continental outflow from the coast and interior of California and their appearance at the BML site was often linked to changes in wind direction and transport pathway. In particular, distinct aerosol populations, associated with diurnal variations in source region induced by land/sea-breeze shifts, were classified by the clustering technique. A terrestrial type representing fresh emissions, and/or a recent new particle formation event, occurred in approximately 10 % of the observations. Over the entire study period, three marine influenced population types were identified that typically occurred when the regular diurnal land/sea-breeze cycle collapsed and BML was continuously ventilated by air masses from marine regions for multiple days. These marine types differed from each other primarily in the degree of cloud processing evident in the size distributions, and in the presence of an additional large-particle mode for the type associated with the highest wind speeds. One of the marine types was associated with a multi-day period during which an atmospheric river made landfall at BML. The generally higher total particle number concentrations but lower activated fractions of four of the terrestrial types yielded similar CCN number concentrations to two of the marine types for supersaturations below about 0.4 %. Despite quite different activated fraction spectra, the two remaining marine and terrestrial types had CCN spectral number concentrations very similar to each other, due in part to higher number concentrations associated with the terrestrial type.

2019 ◽  
Vol 19 (10) ◽  
pp. 6931-6947
Author(s):  
Samuel A. Atwood ◽  
Sonia M. Kreidenweis ◽  
Paul J. DeMott ◽  
Markus D. Petters ◽  
Gavin C. Cornwell ◽  
...  

Abstract. Aerosol particle and cloud condensation nuclei (CCN) measurements from a littoral location on the northern coast of California at Bodega Bay Marine Laboratory (BML) are presented for approximately six weeks of observations during the boreal winter–spring as part of the CalWater-2015 field campaign. The nature and variability of surface (marine boundary layer, MBL) aerosol populations were evaluated by classifying observations into periods of similar aerosol and meteorological characteristics using an unsupervised cluster model to derive distinct littoral aerosol population types and link them to source regions. Such classifications support efforts to understand the impact of changing aerosol properties on precipitation and cloud development in the region, including during important atmospheric river (AR) tropical moisture advection events. Eight aerosol population types were identified that were associated with a range of impacts from both marine and terrestrial sources. Average measured total particle number concentrations, size distributions, hygroscopicities, and activated fraction spectra between 0.08 % and 1.1 % supersaturation are given for each of the identified aerosol population types, along with meteorological observations and transport pathways during time periods associated with each type. Five terrestrially influenced aerosol population types represented different degrees of aging of the continental outflow from the coast and interior of California, and their appearance at the BML site was often linked to changes in wind direction and transport pathways. In particular, distinct aerosol populations, associated with diurnal variations in source regions induced by land- and sea-breeze shifts, were classified by the clustering technique. A terrestrial type representing fresh emissions, and/or a recent new particle formation event, occurred in approximately 10 % of the observations. Over the entire study period, three marine-influenced population types were identified that typically occurred when the regular diurnal land and sea-breeze cycle collapsed and BML was continuously ventilated by air masses from marine regions for multiple days. These marine types differed from each other primarily in the degree of cloud processing evident in the size distributions, and in the presence of an additional large-particle mode for the type associated with the highest wind speeds. One of the marine types was associated with a multi-day period during which an atmospheric river made landfall at BML. Differences between many of the terrestrial and marine population types in total CCN number concentrations active at a specific supersaturation were often not as pronounced as the associated differences in the corresponding activated fraction spectra, particularly for supersaturations below about 0.4 %. This finding was due to the generally higher number concentrations in terrestrial air masses offsetting the lower fraction of particles activating at low supersaturations. At higher supersaturations, CCN concentrations for aged terrestrial types were typically above those of the marine types due to their higher number concentrations.


2012 ◽  
Vol 12 (7) ◽  
pp. 16457-16492 ◽  
Author(s):  
M. Dall'Osto ◽  
D.C.S. Beddows ◽  
J. Pey ◽  
S. Rodriguez ◽  
A. Alastuey ◽  
...  

Abstract. Differential mobility particle sizer (DMPS) aerosol concentrations (N13–800) were collected over a one-year-period (2004) at an urban background site in Barcelona, North-Eastern Spain. Quantitative contributions to particle number concentrations of the nucleation (33–38%), Aitken (39–49%) and accumulation mode (18–22%) were estimated. We examined the source and time variability of atmospheric aerosol particles by using both K-means clustering and Positive Matrix Factorization (PMF) analysis. Performing clustering analysis on hourly size distributions, nine K-means DMPS clusters were identified and, by directional association, diurnal variation and relationship to meteorological and pollution variables, four typical aerosol size distribution scenarios were identified: traffic (69% of the time), dilution (15% of the time), summer background conditions (4% of the time) and regional pollution (12% of the time). According to the results of PMF, vehicle exhausts are estimated to contribute at least to 62–66% of the total particle number concentration, with a slightly higher proportion distributed towards the nucleation mode (34%) relative to the Aitken mode (28–32%). Photochemically induced nucleation particles make only a small contribution to the total particle number concentration (2–3% of the total), although only particles larger than 13 nm were considered in this study. Overall the combination of the two statistical methods is successful at separating components and quantifying relative contributions to the particle number population.


2013 ◽  
Vol 13 (9) ◽  
pp. 4783-4799 ◽  
Author(s):  
J. Zábori ◽  
R. Krejci ◽  
J. Ström ◽  
P. Vaattovaara ◽  
A. M. L. Ekman ◽  
...  

Abstract. Primary marine aerosols (PMAs) are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent, will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (Tw) range between −1°C and 15°C. A sharp decrease in PMA emissions for a Tw increase from −1°C to 4°C was followed by a lower rate of change in PMA emissions for Tw up to about 6°C. Near constant number concentrations for water temperatures between 6°C to 10°C and higher were recorded. Even though the total particle number concentration changes for overlapping Tw ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for a dry diameter (Dp< 0.125μm measured during winter conditions were similar (deviation of up to 3%), or lower (up to 70%) than the ones measured during summer conditions (for the same water temperature range). For Dp > 0.125μm, the particle number concentrations during winter were mostly higher than in summer (up to 50%). The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in Tw from −1°C to 10°C during winter measurements showed a decrease in the peak of relative particle number concentration at about a Dp of 0.180μm, while an increase was observed for particles with Dp > 1μm. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of Tw in the range 7–11°C. The differences in the shape of the number size distributions between winter and summer may be caused by different production of organic material in water, different local processes modifying the water masses within the fjord (for example sea ice production in winter and increased glacial meltwater inflow during summer) and different origin of the dominant sea water mass. Further research is needed regarding the contribution of these factors to the PMA production.


2012 ◽  
Vol 12 (12) ◽  
pp. 31153-31186 ◽  
Author(s):  
J. Zábori ◽  
R. Krejci ◽  
J. Ström ◽  
P. Vaattovaara ◽  
A. M. L. Ekman ◽  
...  

Abstract. Primary marine aerosols (PMA) are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (Tw) range between −1 °C and 15 °C. A sharp decrease in PMA emissions for a Tw increase from −1 °C to 4 °C was followed by a lower rate of change in PMA emissions for Tw up to about 6 °C. Near constant number concentrations for water temperatures between 6 °C to 10 °C and higher were recorded. Even though the total particle number concentrations changes for overlapping Tw ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for Dp < 0.125 μm measured during winter conditions were similar (deviation of up to 3%), or lower (up to 70%) than the ones measured during summer conditions (for the same water temperature range). For Dp > 0.125 μm, the particle number concentrations during winter were mostly higher than in summer (up to 50%). The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in Tw from −1 °C to 10 °C during winter measurements showed a decrease in the peak of relative particle number concentration at about Dp of 0.180 μm, while an increase was observed for particles with Dp > 1 μm. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of Tw in the range 7–11 °C. The differences in the shape of the number size distributions between winter and summer may be caused by different production of organic material in water, different local processes modifying the water masses within the fjord (like sea ice production in winter and increased glacial melt water inflow during summer) and different origin of the dominant sea water mass. Further research is needed regarding the contribution of these factors to the PMA production.


2003 ◽  
Vol 3 (5) ◽  
pp. 5139-5184 ◽  
Author(s):  
T. Hussein ◽  
A. Puustinen ◽  
P. P. Aalto ◽  
J. M. Mäkelä ◽  
K. Hämeri ◽  
...  

Abstract. Aerosol number size distributions were measured continuously in Helsinki, Finland from 5 May 1997 to 28 February 2003. The daily, monthly and annual patterns were investigated. The temporal variation of the particle number concentration was seen to follow the traffic density. The highest total particle number concentrations were usually observed during workdays; especially on Fridays, and the lower concentrations occurred during weekends; especially Sundays. Seasonally, the highest total number concentrations were usually observed during winter and spring and the lowest during June and July. More than 80\\% of the particle number size distributions were tri-modal: nucleation mode (Dp < 30 nm), Aitken mode (20–100 nm) and accumulation mode (Dp > 90 nm). Less than 20% of the particle number size distributions have either two modes or consisted of more than three modes. Two different measurement sites are used; in the first place (Siltavuori, 5 May 1997–5 March 2001), the overall means of the integrated particle number concentrations were 7100 cm−3, 6320 cm−3, and 960 cm−3, respectively, for nucleation, Aitken, and accumulation modes. In the second site (Kumpula, 6 March 2001–28 February 2003) they were 5670 cm−3, 4050 cm−3, and 900 cm−3. The total number concentration in nucleation and Aitken modes were usually significantly higher during weekdays than during weekends. The variations in accumulation mode were less pronounced. The smaller concentrations in Kumpula were mainly due to building construction and also slight overall decreasing trend during these years. During the site changing a period of simultaneous measurements over two weeks were performed showing nice correlation in both sites.


2018 ◽  
Author(s):  
Panayiotis Kalkavouras ◽  
Aikaterini Bougiatioti ◽  
Nikos Kalivitis ◽  
Maria Tombrou ◽  
Athanasios Nenes ◽  
...  

Abstract. A significant fraction of atmospheric particles that serve as cloud condensation nuclei (CCN), and furthermore as cloud droplets are thought to originate from the condensational growth of new particles formed from the gas phase. Here, particle number size distributions (


2012 ◽  
Vol 12 (22) ◽  
pp. 10693-10707 ◽  
Author(s):  
M. Dall'Osto ◽  
D.C.S. Beddows ◽  
J. Pey ◽  
S. Rodriguez ◽  
A. Alastuey ◽  
...  

Abstract. Differential mobility particle sizer (DMPS) aerosol concentrations (N13-800) were collected over a one-year-period (2004) at an urban background site in Barcelona, North-Eastern Spain. Quantitative contributions to particle number concentrations of the nucleation (33–39%), Aitken (39–49%) and accumulation mode (18–22%) were estimated. We examined the source and time variability of atmospheric aerosol particles by using both K-means clustering and Positive Matrix Factorization (PMF) analysis. Performing clustering analysis on hourly size distributions, nine K-means DMPS clusters were identified and, by directional association, diurnal variation and relationship to meteorological and pollution variables, four typical aerosol size distribution scenarios were identified: traffic (69% of the time), dilution (15% of the time), summer background conditions (4% of the time) and regional pollution (12% of the time). According to the results of PMF, vehicle exhausts are estimated to contribute at least to 62–66% of the total particle number concentration, with a slightly higher proportion distributed towards the nucleation mode (34%) relative to the Aitken mode (28–32%). Photochemically induced nucleation particles make only a small contribution to the total particle number concentration (2–3% of the total), although only particles larger than 13 nm were considered in this study. Overall the combination of the two statistical methods is successful at separating components and quantifying relative contributions to the particle number population.


2017 ◽  
Vol 4 (1) ◽  
Author(s):  
Julia Schmale ◽  
Silvia Henning ◽  
Bas Henzing ◽  
Helmi Keskinen ◽  
Karine Sellegri ◽  
...  

Abstract Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.


2021 ◽  
Vol 21 (10) ◽  
pp. 8023-8044
Author(s):  
Thomas Bjerring Kristensen ◽  
John Falk ◽  
Robert Lindgren ◽  
Christina Andersen ◽  
Vilhelm B. Malmborg ◽  
...  

Abstract. Residential biomass combustion is a significant source of aerosol particles on regional and global scales influencing climate and human health. The main objective of the current study was to investigate the properties of cloud condensation nuclei (CCN) emitted from biomass burning of solid fuels in different cookstoves mostly of relevance to sub-Saharan east Africa. The traditional three-stone fire and a rocket stove were used for combustion of wood logs of Sesbania and Casuarina with birch used as a reference. A natural draft and a forced-draft pellet stove were used for combustion of pelletised Sesbania and pelletised Swedish softwood alone or in mixtures with pelletised coffee husk, rice husk or water hyacinth. The CCN activity and the effective density were measured for particles with mobility diameters of ∽65, ∽100 and ∽200 nm, respectively, and occasionally for 350 nm particles. Particle number size distributions were measured online with a fast particle analyser. The chemical composition of the fuel ash was measured by application of standard protocols. The average particle number size distributions were by number typically dominated by an ultrafine mode, and in most cases a soot mode was centred around a mobility diameter of ∽150 nm. The CCN activities decreased with increasing particle size for all experiments and ranged in terms of the hygroscopicity parameter, κ, from ∽0.1 to ∽0.8 for the ultrafine mode and from ∽0.001 to ∽0.15 for the soot mode. The CCN activity (κ) of the ultrafine mode increased (i) with increasing combustion temperature for a given fuel, and (ii) it typically increased with increasing potassium concentration in the investigated fuels. The primary CCN and the estimated particulate matter (PM) emission factors were typically found to increase significantly with increasing potassium concentration in the fuel for a given stove. In order to link CCN emission factors to PM emission factors, knowledge about stove technology, stove operation and the inorganic fuel ash composition is needed. This complicates the use of ambient PM levels alone for estimation of CCN concentrations in regions dominated by biomass combustion aerosol, with the relation turning even more complex when accounting for atmospheric ageing of the aerosol.


2018 ◽  
Vol 75 (3) ◽  
pp. 787-804 ◽  
Author(s):  
Jun-Ichi Yano ◽  
Andrew J. Heymsfield ◽  
Aaron Bansemer

Abstract The possibility is suggested of estimating particle size distributions (PSD) solely based on the bulk quantities of the hydrometeors. The method, inspired by the maximum entropy principle, can be applied to any predefined general PSD form as long as the number of the free parameters is equal to or less than that of the bulk quantities available. As long as an adopted distribution is “physically based,” these bulk characterizations can recover a fairly accurate PSD estimate. This method is tested for ice particle measurements from the Tropical Composition, Cloud and Climate Coupling Experiment (TC4). The total particle number, total mass, and mean size are taken as bulk quantities. The gamma distribution and two distributions obtained under the maximum entropy principle by taking the size and the particle mass, respectively, as a restriction variable are adopted for fit. The fitting error for the two maximum entropy–based distributions is comparable to that of a standard direct fitting method with the gamma distribution. The same procedure works almost equally well when the mean size is removed from the constraint, especially for an exponential distribution. The results suggest that the total particle number and the total mass of the hydrometeors are sufficient for determining the PSD to a reasonable accuracy when a “physically based” distribution is assumed. In addition to the in situ cloud measurements, remote sensing measurements such as those from radar as well as satellite can be adopted as physical constraints. Possibilities of exploiting different types of measurements should be further pursued.


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