scholarly journals Lake spray aerosol generation: A method for producing representative particles from freshwater wave breaking

Author(s):  
Nathaniel W. May ◽  
Jessica L. Axson ◽  
Alexa Watson ◽  
Kerri A. Pratt ◽  
Andrew P. Ault

Abstract. Wave breaking action in bodies of freshwater produces atmospheric aerosols via a similar mechanism to sea spray aerosol (SSA) from seawater. The term lake spray aerosol (LSA) is proposed to describe particles formed by this mechanism, which have been observed over the Laurentian Great Lakes. Though LSA has been identified from size distribution measurements during a single measurement campaign, no measurements of LSA composition or relationship to bubble bursting dynamics have been conducted. A LSA generator utilizing a plunging jet, similar to many SSA generators, was constructed for the generation of aerosol from freshwater samples and model salt solutions. To evaluate this new generator, bubble and aerosol number size distributions were measured for salt solutions representative of freshwater (CaCO3) and seawater (NaCl) at concentrations ranging from that of freshwater to seawater (0.05–35 g L−1), synthetic seawater (inorganic), synthetic freshwater (inorganic), and a freshwater sample from Lake Michigan. Following validation of the bubble and aerosol size distributions using synthetic seawater, a range of salt concentrations was investigated. Decreasing salt concentrations from seawater to freshwater led to greater bubble coalescence and formation of larger bubbles, which generated larger particles and lower aerosol number concentrations. The systematic studies of the model salts, synthetic freshwater, and Lake Michigan sample indicate that LSA is characterized by a larger bubble size distribution, compared to seawater, with a peak near 300 μm. This resulted in a bimodal aerosol size distribution with a primary mode (180 ± 20 nm) larger than that of SSA, and a secondary mode (46 ± 6 nm) smaller than that of SSA. This new method for studying LSA under isolated conditions is needed as models, at present, utilize SSA parametrizations for freshwater systems, which are not accurate for predicting climate properties of the different size distributions observed for LSA. Given the abundance of freshwater globally, this potentially important source of aerosol needs to be thoroughly characterized, as the sizes produced are relevant to light scattering, cloud condensation nuclei (CCN), and ice nuclei (IN) concentrations over the bodies of freshwater.

2016 ◽  
Vol 9 (9) ◽  
pp. 4311-4325 ◽  
Author(s):  
Nathaniel W. May ◽  
Jessica L. Axson ◽  
Alexa Watson ◽  
Kerri A. Pratt ◽  
Andrew P. Ault

Abstract. Wave-breaking action in bodies of freshwater produces atmospheric aerosols via a similar mechanism to sea spray aerosol (SSA) from seawater. The term lake spray aerosol (LSA) is proposed to describe particles formed by this mechanism, which have been observed over the Laurentian Great Lakes. Though LSA has been identified from size distribution measurements during a single measurement campaign, no measurements of LSA composition or relationship to bubble-bursting dynamics have been conducted. An LSA generator utilizing a plunging jet, similar to many SSA generators, was constructed for the generation of aerosol from freshwater samples and model salt solutions. To evaluate this new generator, bubble and aerosol number size distributions were measured for salt solutions representative of freshwater (CaCO3) and seawater (NaCl) at concentrations ranging from that of freshwater to seawater (0.05–35 g kg−1), synthetic seawater (inorganic), synthetic freshwater (inorganic), and a freshwater sample from Lake Michigan. Following validation of the bubble and aerosol size distributions using synthetic seawater, a range of salt concentrations were investigated. The systematic studies of the model salts, synthetic freshwater, and Lake Michigan sample indicate that LSA is characterized by a larger number size distribution mode diameter of 300 nm (lognormal), compared to seawater at 110 nm. Decreasing salt concentrations from seawater to freshwater led to greater bubble coalescence and formation of larger bubbles, which generated larger particles and lower aerosol number concentrations. This resulted in a bimodal number size distribution with a primary mode (180 ± 20 nm) larger than that of SSA, as well as a secondary mode (46 ± 6 nm) smaller than that of SSA. This new method for studying LSA under isolated conditions is needed as models, at present, utilize SSA parameterizations for freshwater systems, which do not accurately predict the different size distributions observed for LSA or resulting climate properties. Given the abundance of freshwater globally, this potentially important source of aerosol needs to be thoroughly characterized, as the sizes produced are relevant to light scattering, cloud condensation nuclei (CCN), and ice nuclei (IN) concentrations over bodies of freshwater.


1982 ◽  
Vol 60 (8) ◽  
pp. 1101-1107
Author(s):  
C. V. Mathai ◽  
A. W. Harrison

As part of an ongoing general research program on the effects of atmospheric aerosols on visibility and its dependence on aerosol size distributions in Calgary, this paper presents the results of a comparative study of particle size distribution and visibility in residential (NW) and industrial (SE) sections of the city using a mobile laboratory. The study was conducted in the period October–December, 1979. An active scattering aerosol spectrometer measured the size distributions and the corresponding visibilities were deduced from scattering coefficients measured with an integrating nephelometer.The results of this transit study show significantly higher suspended particle concentrations and reduced visibilities in the SE than in the NW. The mean values of the visibilities are 44 and 97 km for the SE and the NW respectively. The exponent of R (particle radius) in the power law aerosol size distribution has a mean value of −3.36 ± 0.24 in the SE compared with the corresponding value of −3.89 ± 0.39 for the NW. These results arc in good agreement with the observations of Alberta Environment; however, they are in contradiction with a recent report published by the City of Calgary.


2017 ◽  
Vol 14 (2) ◽  
Author(s):  
Kaitlin DuPaul ◽  
Adam Whitten

A synthetic set of aerosol optical depths (AODs) generated from a standard set of aerosol size distributions was analyzed by a parameter based particle swarm optimization (PBPSO) routine in order to test the reproducibility of the results. Junge and lognormal size distributions were consistently reproduced. Gamma and bimodal distributions showed large variability in solutions. values were used to determine the best subset of possible solutions allowing quantification of parameters with uncertainties when using PBPSO. AODs measured by a sun photometer on a clear day (20160413) and a foggy day (20160508) were then processed by the PBPSO program for both bimodal and lognormal distributions. Results showed that in general the foggy day has smaller values indicating that the PBPSO algorithm is better able to match AODs when there is a larger aerosol load in the atmosphere. The bimodal distribution from the clear day best describes the aerosol size distribution since the values are lower. The lognormal distribution best describes the aerosol size distribution on the foggy day (20160508). KEYWORDS: Atmospheric Aerosols; Size Distributions; Junge; Bimodal; Gamma; Lognormal; Particle Swarm Optimization; Inverse Problem; Aerosol Optical Depth


2010 ◽  
Vol 10 (7) ◽  
pp. 3365-3383 ◽  
Author(s):  
D. Rose ◽  
A. Nowak ◽  
P. Achtert ◽  
A. Wiedensohler ◽  
M. Hu ◽  
...  

Abstract. Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1–30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20–290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≈0.1–0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity – most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1000 cm−3 at S=0.068% to 16 000 cm−3 at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of NCCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted NCCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from individual CCN efficiency spectra, the relative deviations were on average less than ~10% and hardly exceeded 20%, confirming the applicability of the κ-Köhler model approach for efficient description of the CCN activity of atmospheric aerosols. Note, however, that different types of κ-parameters must be distinguished for external mixtures of CCN-active and -inactive aerosol particles (κa, κt, κcut). Using a constant average hygroscopicity parameter (κ=0.3) and variable size distributions as measured, the deviations between observed and predicted CCN concentrations were on average less than 20%. In contrast, model calculations using variable hygroscopicity parameters as measured and constant size distributions led to much higher deviations: ~70% for the campaign average size distribution, ~80% for a generic rural size distribution, and ~140% for a generic urban size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this study should enable efficient description of the CCN activity of atmospheric aerosols in detailed process models as well as in large-scale atmospheric and climate models.


2004 ◽  
Vol 4 (4) ◽  
pp. 4507-4543 ◽  
Author(s):  
P. Tunved ◽  
J. Ström ◽  
H.-C. Hansson

Abstract. Aerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E). Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing the different stages of the aerosol lifecycle. The aerosol was interpreted as belonging to fresh, intermediate and aged type of size distribution and different magnitudes thereof. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features likely related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability. Processing by non-precipitating clouds most obviously affect aerosols in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions bearing signs of recent new particle formation (~30% of the observed size distributions) represent the first stage in the lifecycle. Aging may proceed in two directions: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area) in environments similar to the one studied.


2019 ◽  
Vol 19 (24) ◽  
pp. 15483-15502 ◽  
Author(s):  
Yicheng Shen ◽  
Aki Virkkula ◽  
Aijun Ding ◽  
Krista Luoma ◽  
Helmi Keskinen ◽  
...  

Abstract. The concentration of cloud condensation nuclei (CCN) is an essential parameter affecting aerosol–cloud interactions within warm clouds. Long-term CCN number concentration (NCCN) data are scarce; there are a lot more data on aerosol optical properties (AOPs). It is therefore valuable to derive parameterizations for estimating NCCN from AOP measurements. Such parameterizations have already been made, and in the present work a new parameterization is presented. The relationships between NCCN, AOPs, and size distributions were investigated based on in situ measurement data from six stations in very different environments around the world. The relationships were used for deriving a parameterization that depends on the scattering Ångström exponent (SAE), backscatter fraction (BSF), and total scattering coefficient (σsp) of PM10 particles. The analysis first showed that the dependence of NCCN on supersaturation (SS) can be described by a logarithmic fit in the range SS <1.1 %, without any theoretical reasoning. The relationship between NCCN and AOPs was parameterized as NCCN≈((286±46)SAE ln(SS/(0.093±0.006))(BSF − BSFmin) + (5.2±3.3))σsp, where BSFmin is the minimum BSF, in practice the 1st percentile of BSF data at a site to be analyzed. At the lowest supersaturations of each site (SS ≈0.1 %), the average bias, defined as the ratio of the AOP-derived and measured NCCN, varied from ∼0.7 to ∼1.9 at most sites except at a Himalayan site where the bias was >4. At SS >0.4 % the average bias ranged from ∼0.7 to ∼1.3 at most sites. For the marine-aerosol-dominated site Ascension Island the bias was higher, ∼1.4–1.9. In other words, at SS >0.4 % NCCN was estimated with an average uncertainty of approximately 30 % by using nephelometer data. The biases were mainly due to the biases in the parameterization related to the scattering Ångström exponent (SAE). The squared correlation coefficients between the AOP-derived and measured NCCN varied from ∼0.5 to ∼0.8. To study the physical explanation of the relationships between NCCN and AOPs, lognormal unimodal particle size distributions were generated and NCCN and AOPs were calculated. The simulation showed that the relationships of NCCN and AOPs are affected by the geometric mean diameter and width of the size distribution and the activation diameter. The relationships of NCCN and AOPs were similar to those of the observed ones.


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.


2019 ◽  
Vol 19 (11) ◽  
pp. 7839-7857
Author(s):  
Lianet Hernández Pardo ◽  
Luiz Augusto Toledo Machado ◽  
Micael Amore Cecchini ◽  
Madeleine Sánchez Gácita

Abstract. This work uses the number concentration-effective diameter phase-space to test cloud sensitivity to variations in the aerosol population characteristics, such as the aerosol size distribution, number concentration and hygroscopicity. It is based on the information from the top of a cloud simulated by a bin-microphysics single-column model, for initial conditions typical of the Amazon, using different assumptions regarding the entrainment and the aerosol size distribution. It is shown that the cloud-top evolution can be very sensitive to aerosol properties, but the relative importance of each parameter is variable. The sensitivity to each aerosol characteristic varies as a function of the parameter tested and is conditioned by the base values of the other parameters, showing a specific dependence for each configuration of the model. When both the entrainment and the bin treatment of the aerosol are allowed, the largest influence on the droplet size distribution sensitivity was obtained for the median radius of the aerosols and not for the total number concentration of aerosols. Our results reinforce that the cloud condensation nuclei activity can not be predicted solely on the basis of the w∕Na supersaturation-based regimes.


2018 ◽  
Vol 11 (6) ◽  
pp. 3491-3509 ◽  
Author(s):  
Christina Williamson ◽  
Agnieszka Kupc ◽  
James Wilson ◽  
David W. Gesler ◽  
J. Michael Reeves ◽  
...  

Abstract. Earth's radiation budget is affected by new particle formation (NPF) and the growth of these nanometre-scale particles to larger sizes where they can directly scatter light or act as cloud condensation nuclei (CCN). Large uncertainties remain in the magnitude and spatiotemporal distribution of nucleation (less than 10 nm diameter) and Aitken (10–60 nm diameter) mode particles. Acquiring size-distribution measurements of these particles over large regions of the free troposphere is most easily accomplished with research aircraft. We report on the design and performance of an airborne instrument, the nucleation mode aerosol size spectrometer (NMASS), which provides size-selected aerosol concentration measurements that can be differenced to identify aerosol properties and processes or inverted to obtain a full size distribution between 3 and 60 nm. By maintaining constant downstream pressure the instrument operates reliably over a large range of ambient pressures and during rapid changes in altitude, making it ideal for aircraft measurements from the boundary layer to the stratosphere. We describe the modifications, operating principles, extensive calibrations, and laboratory and in-flight performance of two NMASS instruments operated in parallel as a 10-channel battery of condensation particle counters (CPCs) in the NASA Atmospheric Tomography Mission (ATom) to investigate NPF and growth to cloud-active sizes in the remote free troposphere. An inversion technique to obtain size distributions from the discrete concentrations of each NMASS channel is described and evaluated. Concentrations measured by the two NMASS instruments flying in parallel are self-consistent and also consistent with measurements made with an optical particle counter. Extensive laboratory calibrations with a range of particle sizes and compositions show repeatability of the response function of the instrument to within 5–8 % and no sensitivity in sizing performance to particle composition. Particle number, surface area, and volume concentrations from the data inversion are determined to better than 20 % for typical particle size distributions. The excellent performance of the NMASS systems provides a strong analytical foundation to explore NPF around the globe in the ATom dataset.


2009 ◽  
Vol 9 (18) ◽  
pp. 7053-7066 ◽  
Author(s):  
A. Bougiatioti ◽  
C. Fountoukis ◽  
N. Kalivitis ◽  
S. N. Pandis ◽  
A. Nenes ◽  
...  

Abstract. Measurements of cloud condensation nuclei (CCN) concentrations (cm−3) between 0.2 and 1.0% supersaturation, aerosol size distribution and chemical composition were performed at a remote marine site in the eastern Mediterranean, from September to October 2007 during the FAME07 campaign. Most of the particles activate at ~0.6% supersaturation, characteristic of the aged nature of the aerosol sampled. Application of Köhler theory, using measurements of bulk composition, size distribution, and assuming that organics are insoluble resulted in agreement between predicted and measured CCN concentrations within 7±11% for all supersaturations, with a tendency for CCN underprediction (16±6%; r2=0.88) at the lowest supersaturations (0.21%). Including the effects of the water-soluble organic fraction (which represent around 70% of the total organic content) reduces the average underprediction bias at the low supersaturations, resulting in a total closure error of 0.6±6%. Using threshold droplet growth analysis, the growth kinetics of ambient CCN is consistent with NaCl calibration experiments; hence the presence of aged organics does not suppress the rate of water uptake in this environment. The knowledge of the soluble salt fraction is sufficient for the description of the CCN activity in this area.


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