Aitken Mode Particles Research Articles

Revisiting particle dry deposition and its role in radiative effect estimates

Wet and dry deposition remove aerosols from the atmosphere, and these processes control aerosol lifetime and thus impact climate and air quality. Dry deposition is a significant source of aerosol uncertainty in global chemical transport and climate models. Dry deposition parameterizations in most global models were developed when few particle deposition measurements were available. However, new measurement techniques have enabled more size-resolved particle flux observations. We combined literature measurements with data that we collected over a grassland in Oklahoma and a pine forest in Colorado to develop a dry deposition parameterization. We find that relative to observations, previous parameterizations overestimated deposition of the accumulation and Aitken mode particles, and underestimated in the coarse mode. These systematic differences in observed and modeled accumulation mode particle deposition velocities are as large as an order of magnitude over terrestrial ecosystems. As accumulation mode particles form most of the cloud condensation nuclei (CCN) that influence the indirect radiative effect, this model-measurement discrepancy in dry deposition alters modeled CCN and radiative forcing. We present a revised observationally driven parameterization for regional and global aerosol models. Using this revised dry deposition scheme in the Goddard Earth Observing System (GEOS)-Chem chemical transport model, we find that global surface accumulation-mode number concentrations increase by 62% and enhance the global combined anthropogenic and natural aerosol indirect effect by -0.63 W m-2 Our observationally constrained approach should reduce the uncertainty of particle dry deposition in global chemical transport models.

A study on the characteristics of ice nucleating particles concentration and aerosols and their relationship in spring in Beijing

In this study, Bigg cloud chamber was used to determine the concentrations of ice nucleating particles (INPs) in the temperature range from −15 to −30 °C in Beijing in the spring of 2017. The concentrations were compared with historical results observed by a similar instrument in Beijing, showing that the INP concentration in 2017 was generally lower than those obtained in 1995 and 1996. Based on air mass trajectory clustering analysis, the high INP concentration in 1995 and 1996 might be attributable mainly to the transport of sand-dust from the northwestern region. Furthermore, the aerosol number size distribution and chemical composition in PM2.5 were measured simultaneously. The number of aerosols was dominated by particles in Aitken mode and accumulation mode particles during the observation period, but coarse mode particles obviously exhibited stronger correlation with INPs. NO3−, NH4+, and SO42− were the major ions and existed mainly in the form of NH4NO3 and (NH4)2SO4 in PM2.5. Ratio analysis indicated that air pollution originated mainly from mobile sources in Beijing and had serious secondary pollution process. The high ratio of organic carbon (OC) to elemental carbon (EC) implies existing severe secondary organic carbon pollution. In addition, we investigated the relationship between INPs and aerosols with different sizes and compositions in spring in Beijing, the results indicated that for aerosols with a diameter above 0.5 μm, the correlation between INPs and aerosols increased clearly with increasing particle size, but for aerosols with sizes below 0.5 μm, the correlation coefficient displayed a clear trend of increasing first and then decreasing with increasing aerosol size. An INP parameterization depending on aerosol particles and the activation temperature was also established. A comparison of the correlations between the INPs and compositions in PM2.5 shows that NaCl, NH4NO3 and (NH4)2SO4 were more correlated with INPs than other ionic compounds, but a strong correlation existed only at −30 °C, there was no correlation at −20 °C and above. Additionally, OC was more relevant to INP than EC, but the correlation was observed only at low temperature region.

Linkage between Particulate Matter Properties and Lung Function in Schoolchildren: A Panel Study in Southern China.

While several scientific studies have linked PM2.5 to decreased lung function, there is still some degree of uncertainty regarding which particulate physicochemical properties are most harmful. We followed a panel of 57 healthy schoolchildren (857 person-days) to investigate the associations between a wide variety of PM2.5 and lung function in Heshan, China in 2016 for three periods. We monitored the daily concentrations of mass, chemical composition, size, number, surface area, and volume of particulate mixture. Associations of lung function with various particle metrics were estimated using generalized estimating equations and unconstrained distributed lag models. Random forest model was used to compare the relative importance of exposure metrics. Immediate (lag 0) associations of PM2.5 and carbonaceous aerosols with reduced FEV1 and MMEF, and accumulation-mode particles with FEV1 were found. Slightly delayed (lag 1, 2) effects on PEF were particularly prominent for Aitken-mode particles. Possible cumulative (lags 0-2) effects of PM2.5 and carbonaceous aerosols on PEF and Aitken-mode particles on FEV1, MMEF, and PEF were observed. This study provides comprehensive evidence that the physicochemical properties of particulate mixtures are associated with reduced lung function in children. Organic carbon (OC) may be an important risk factor for the decreased lung function related to PM exposure.

Spatial-temporal variability of aerosol sources based on chemical composition and particle number size distributions in an urban settlement influenced by metallurgical industry.

The Moravian-Silesian region of the Czech Republic with its capital city Ostrava is a European air pollution hot spot for airborne particulate matter (PM). Therefore, the spatiotemporal variability assessment of source contributions to aerosol particles is essential for the successful abatement strategies implementation. Positive Matrix Factorization (PMF) was applied to highly-time resolved PM0.15-1.15 chemical composition (1h resolution) and particle number size distribution (PNSD, 14nm - 10μm) data measured at the suburban (Ostrava-Plesná) and urban (Ostrava-Radvanice) residential receptor sites in parallel during an intensive winter campaign. Diel patterns, meteorological variables, inorganic and organic markers, and associations between the chemical composition factors and PNSD factors were used to identify the pollution sources and their origins (local, urban agglomeration and regional). The source apportionment analysis resolved six and four PM0.15-1.15 sources in Plesná and Radvanice, respectively. In Plesná, local residential combustion sources (coal and biomass combustion) followed by regional combustion sources (residential heating, metallurgical industry) were the main contributors to PM0.15-1.15. In Radvanice, local residential combustion and the metallurgical industry were the most important PM0.15-1.15 sources. Aitken and accumulation mode particles emitted by local residential combustion sources along with common urban sources (residential heating, industry and traffic) were the main contributors to the particle number concentration (PNC) in Plesná. Additionally, accumulation mode particles from local residential combustion sources and regional pollution dominated the particle volume concentration (PVC). In Radvanice, local industrial sources were the major contributors to PNC and local coal combustion was the main contributor to PVC. The source apportionment results from the complementary datasets elucidated the relevance of highly time-resolved parallel measurements at both receptor sites given the specific meteorological conditions produced by the regional orography. These results are in agreement with our previous studies conducted at this site. Graphical abstract.

Identifying a regional aerosol baseline in the eastern North Atlantic using collocated measurements and a mathematical algorithm to mask high-submicron-number-concentration aerosol events

Abstract. High-time-resolution measurements of in situ aerosol and cloud properties provide the ability to study regional atmospheric processes that occur on timescales of minutes to hours. However, one limitation to this approach is that continuous measurements often include periods when the data collected are not representative of the regional aerosol. Even at remote locations, submicron aerosols are pervasive in the ambient atmosphere with many sources. Therefore, periods dominated by local aerosol should be identified before conducting subsequent analyses to understand aerosol regional processes and aerosol–cloud interactions. Here, we present a novel method to validate the identification of regional baseline aerosol data by applying a mathematical algorithm to the data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility in the eastern North Atlantic (ENA). The ENA central facility (C1) includes an aerosol observing system (AOS) for the measurement of aerosol physical, optical, and chemical properties at time resolutions from seconds to minutes. A second temporary supplementary facility (S1), located ∼0.75 km from C1, was deployed for ∼1 year during the Aerosol and Cloud Experiments (ACE-ENA) campaign in 2017. First, we investigate the local aerosol at both locations. We associate periods of high submicron number concentration (Ntot) in the fine-mode condensation particle counter (CPC) and size distributions from the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) as a function of wind direction using a meteorology sensor with local sources. Elevated concentrations of Aitken-mode (< 100 nm diameter) particles were observed in correspondence with the wind directions associated with airport operations. At ENA, the Graciosa Airport and its associated activities were found to be the main sources of high-concentration aerosol events at ENA, causing peaks in 1 min Ntot that exceeded 8000 and 10 000 cm−3 at C1, in summer and winter, respectively, and 5000 cm−3 at S1 in summer. Periods with high Ntot not associated with these wind directions were also observed. As a result, the diverse local sources at ENA yielded a poor relationship between Ntot measurements collected at C1 and S1 (R2=0.03 with a slope =0.05±0.001). As a first approach to mask these events, the time periods when the wind direction was associated with the airport operations (west to northwest and southeast to south at C1 and east to south at S1) were applied. The meteorological masks removed 38.9 % of the data at C1 and 43.4 % at S1, and they did not significantly improve the relationship between the two sites (R2=0.18 with a slope =0.06±0.001). Due to the complexity of high-Ntot events observed at ENA, we develop and validate a mathematical ENA Aerosol Mask (ENA-AM) to identify high-Ntot events using 1 min resolution data from the AOS CPC at C1 and S1. After its parameterization and application, ENA-AM generated a high correlation between Ntot in the summer at C1 and S1 (R2=0.87 with a slope =0.84±0.001). We identified the regional baseline at ENA to be 428±228 cm−3 in the summer and 346±223 cm−3 in the winter. Lastly, we compared masked measurements from the AOS with the ARM Aerial Facility (AAF) during flights over C1 in the summer to understand submicron aerosol vertical mixing over C1. The high correlation (R2=0.71 with a slope of 1.04±0.01) observed between C1 and the AAF Ntot collected within an area of 10 km surrounding ENA and at altitudes < 500 m indicated that the submicron aerosol at ENA was well mixed within the first 500 m of the marine boundary layer during the month of July during ACE-ENA. Our novel method for determining a regional aerosol baseline at ENA can be applied to other time periods and at other locations with validation by a secondary site or additional collocated measurements.

Changes in the elemental composition of particulate matter in a speleotherapeutic cave

Atmosphere inside caves used for speleotherapy are microenvironments influenced by ventilation and human activities inside. In this context, particulate matter with an aerodynamic diameter from 15 nm to 10 μm was collected with an electrical low-pressure impactor ELPI+ in the Císařská Cave in the northern part of the Moravian Karst (Czech Republic) and 33 elements were determined with inductively coupled plasma tandem mass spectrometry (ICPMS/MS). To see the effect of ventilation, samples were collected with closed and opened entrances.Nucleation mode particles (particles with aerodynamic diameter less than 10 nm) were dominant in particle number concentrations at both cave ventilation regimes. Aitken mode particles (10–100 nm) differed in the content of sulphur, calcium, iron, chromium, magnesium and nickel for different ventilation regimes. Accumulation mode particles (100–1000 nm) consisted predominantly of sulphur and calcium, also chromium, copper, arsenic, molybdenum, selenium, cadmium and lead were mainly present in this particle size range. Coarse mode particles (larger than 1000 nm) contained predominantly calcium, in addition to common earth crust elements, originating by mechanical abrasion of cave floor.It is suggested that ventilation as well as children activities in the cave influence the elemental composition of particulate matter, which might have an impact on speleotherapy.

Application of SERS on the chemical speciation of individual Aitken mode particles after condensational growth

The chemical speciation of nanoparticles is technically challenging because of the minute mass of the particles. There is a constant need for more sensitive collection methods and chemical analyses...

Improved representation of particle size and solubility in model simulations of atmospheric dispersion and wet-deposition from Fukushima

Radionuclides released into the atmosphere following the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident were detected by ground-based monitoring stations worldwide. The inter-continental dispersion of radionuclides provides a unique opportunity to evaluate the ability of atmospheric dispersion models to represent the processes controlling their transport and deposition in the atmosphere. Co-located measurements of radioxenon (133Xe) and caesium (137Cs) concentrations enable individual physical processes (dispersion, dry and wet deposition) to be isolated. In this paper we focus on errors in the prediction of 137Cs attributed to the representation of particle size and solubility, in the process of modelling wet deposition. Simulations of 133Xe and 137Cs concentrations using the UK Met Office NAME (Numerical Atmospheric-dispersion Modelling Environment) model are compared with CTBTO (Comprehensive Nuclear-Test-Ban Treaty Organisation) surface station measurements. NAME predictions of 137Cs using a bulk wet deposition parameterisation (which does not account for particle size dependent scavenging or solubility) significantly underestimate observed 137Cs. When a binned wet deposition parameterisation is implemented (which accounts for particle size dependent scavenging) the correlations between modelled and observed air concentrations improve at all 9 of the Northern Hemisphere sites studied and the respective RMSLE (root-mean-square-log-error) decreases by a factor of 7 due to a decrease in the wet-deposition of Aitken and Accumulation mode particles. Finally, NAME simulations were performed in which insoluble submicron particles are represented. Representing insoluble particles in the NAME simulations improves the RMSLE at all sites further by a factor of 7. Thus NAME is able to predict 137Cs with good accuracy (within a factor of 10 of observed 137Cs values) at distances greater than 10,000 km from FDNPP only if insoluble submicron particles are considered in the description of the source. This result provides further evidence of the presence of insoluble Cs-rich microparticles in the release following the accident at FDNPP and suggests that these small particles travelled across the Pacific Ocean to the US and further across the North Atlantic Ocean towards Europe.

Characterization of aerosol particles at Cabo Verde close to sea level and at the cloud level – Part 1: Particle number size distribution, cloud condensation nuclei and their origins

Abstract. In the framework of the MarParCloud (Marine biological production, organic aerosol particles and marine clouds: a Process Chain) project, measurements were carried out on the islands of Cabo Verde (a.k.a. Cape Verde) to investigate the abundance, properties and sources of aerosol particles in general, and cloud condensation nuclei (CCN) in particular, both close to sea level and at the cloud level. A thorough comparison of particle number concentration (PNC), particle number size distribution (PNSD) and CCN number concentration (NCCN) at the Cape Verde Atmospheric Observatory (CVAO, sea-level station) and Monte Verde (MV, cloud-level station) reveals that during times without clouds the aerosols at CVAO and MV are similar and the boundary layer is generally well mixed. Therefore, data obtained at CVAO can be used to describe the aerosol particles at cloud level. Cloud events were observed at MV during roughly 58 % of the time, and during these events a large fraction of particles was activated to cloud droplets. A trimodal parameterization method was deployed to characterize PNC at CVAO. Based on number concentrations in different aerosol modes, four well-separable types of PNSDs were found, which were named the marine type, mixture type, dust type1 and dust type2. Aerosol particles differ depending on their origins. When the air masses came from the Atlantic Ocean, sea spray can be assumed to be one source for particles besides new particle formation. For these air masses, PNSDs featured the lowest number concentration in Aitken, accumulation and coarse modes. Particle number concentrations for sea spray aerosol (SSA, i.e., the coarse mode for these air masses) accounted for about 3.7 % of NCCN,0.30 % (CCN number concentration at 0.30 % supersaturation) and about 1.1 % to 4.4 % of Ntotal (total particle number concentration). When the air masses came from the Sahara, we observed enhanced Aitken, accumulation and coarse mode particle number concentrations and overall increased NCCN; NCCN,0.30 % during the strongest observed dust periods is about 2.5 times higher than that during marine periods. However, the particle hygroscopicity parameter κ for these two most different periods shows no significant difference and is generally similar, independent of air mass. Overall, κ averaged 0.28, suggesting the presence of organic material in particles. This is consistent with previous model work and field measurements. There is a slight increase in κ with increasing particle size, indicating the addition of soluble, likely inorganic, material during cloud processing.

Chemical characterization and source identification of particulate matter at Ballari (15.15°N, 76.93°E), Karnataka over Southern Indian region

The present study reports the chemical composition and source identification of the total suspended particulate matter in the sub-urban environment, Ballari. There were 28 particulate matter aerosol sampled between February 2017–July 2018. The surface mass concentration ranged from 103 μg m−3 to 367 μg m−3 with an average value of ~225 ± 65 μg m−3 during the study period. The morphology and elemental composition of aerosol particles were analyzed by using a scanning electron microscope (SEM) coupled with an energy dispersive X-ray system (EDX). From the EDX results aluminosilicate group (Al, Si, K, Fe, Na, Mg, Ti and Ca) contains about ~31% of the total particles, which mainly due to mineral particulate aerosol originate from crustal origin through windblown dust. Further, we also investigated the morphology and chemical composition of total mass concentration during haze (27-03-2018) and clear days (23-02-2018). The SEM pictures show the most notable deposition of spherical particles with smooth surfaces on a hazy day suggesting that the carbon aerosols on haze day were favourable to coagulation of Aitken mode particles, which is consistent with their respective aerosol subtypes captured from Cloud-Aerosol Lidar with Orthogonal Polarization (CALIPSO) satellite over the study region. Inductively coupled plasma optical emission spectrometer (ICP-OES) analysis showed the relative contribution of inorganic ions (SO42−, NO3−, Na+, Ca2+, Cl−, NH4+, K+) is higher than others on 1-05-2017 and 01-01-2018 days over the observational site. The relative contribution of non-sea salt SO42− was abundance (~35%) on both days, indicating the significant anthropogenic influence at this location. The concentration weighted trajectory (CWTs) analysis showed the major sources of particulate matter were soil particles, vehicular emissions, and mining activities surroundings the vicinity of the sampling site.

Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol.

The diffusivity of semivolatile organic compounds (SVOCs) in the bulk particle phase of a viscous atmospheric secondary organic aerosol (SOA) can have a profound impact on aerosol growth and size distribution dynamics. Here, we investigate the bulk diffusivity of SVOCs formed from photo-oxidation of isoprene as they partition to a bimodal aerosol consisting of an Aitken (potassium sulfate) and accumulation mode (aged α-pinene SOA) particles as a function of relative humidity (RH). The model analysis of the observed size distribution evolution shows that liquid-like diffusion coefficient values of Db > 10-10 cm2 s-1 fail to explain the growth of the Aitken mode. Instead, much lower values of Db between2.5 × 10-15 cm2 s-1 at 32% RH and 8 × 10-15 cm2 s-1 at 82% RH were needed to successfully reproduce the growth of both modes. The diffusivity within the aged α-pinene SOA remains appreciably slow even at 80% RH, resulting in hindered partitioning of SVOCs to large viscous particles and allowing smaller and relatively less viscous particles to effectively absorb the available SVOCs and grow much faster than would be possible otherwise. These results have important implications for modeling SOA formation and growth in the ambient atmosphere.

Transient Characterization of Automotive Exhaust Emission from Different Vehicle Types Based on On-Road Measurements

Previous works on real-world vehicle emission characteristics have mainly focused on the influences of fuel, speed, vehicle type, elevation, and other factors on vehicle emission quantity and components. However, few studies have investigated the transient trend of automotive exhaust emissions through on-road measurements. The key objective of the present paper was to examine the transient characteristics of exhaust emissions from different vehicle types on the roads of Tianjin. To achieve the goal, a portable emission measurement system (PEMS) was employed to monitor emissions from selected test vehicles—private cars, passenger vehicles, and cargo vehicles. It was found that the high-emission points of test vehicles were mainly distributed in two regions: the high-speed region (speed > 70–90 km/h, vehicle-specific power (VSP) > 0 kW/t) and the medium-speed–acceleration region (20–30 km/h < speed < 60–90 km/h, 0 kW/t <VSP < 12 kW/t). The CO, hydrocarbon (HC), NOx, and particulate number (PN) average emission rates in the high-emission points could be 3.15–14.93 times, 1.93–24.89 times, 3.23–6.03 times, and 3.22–30.27 times of those of average emission rates. The HC, NOx, and PN average emission rates of China IV vehicles in the high-emission points were 2.46–4.92 times, 3.56–6.03 times, and 3.22–13.21 times of those of average emission rates, not less than those of China III (1.93–2.52 times, 2.75–3.90 times, and 9.98–22.34 times). Test vehicles mainly emitted nucleation-mode and Aitken-mode particles, and the increase of the PN concentration emission rate in low-speed and high-speed regions was higher than that in the medium-speed region. The exhaust gas recirculation (EGR) + diesel particulate filter (DPF) could effectively inhibit the Aitken output caused by turbocharged intercooler (CIC). The selective catalytic reduction (SCR) might cause more nucleation-mode particles.

Analytical Relationships Between Bulk Microphysical Parameters of Nucleation, Aitken, Accumulation and Coarse Mode Particles and Extinction and Backscatter Coefficients Measured with Lidar

We derive analytical relationships between bulk microphysical parameters of nucleation, Aitken, accumulation and coarse mode particles and extinction and backscatter coefficients measured at wavelengths 355, 532 and 1064 nm. The bulk parameters are represented by number concentration, mean (effective) radius, variance and complex refractive index. Analytical relationships hold true for arbitrarily shaped particles and complex refractive indices m=mR-imI, where mR>>mI. The accuracy is above 60%.

Chemical Characterization of Sub-micron Aerosols during New Particle Formation in an Urban Atmosphere

ABSTRACT While high concentrations of pre-existing particles tend to inhibit new particle formation (NPF) in the atmosphere, severely polluted megacities around the world are becoming hot spots for the latter. We measured the particle number-size distributions with a Scanning Mobility Particle Sizer (SMPS) in the urban environment of Kanpur, India, and discovered that particle bursts occurred on 82% of the observation days, indicating that new particles frequently formed from gaseous precursors despite the relatively high concentrations of pre-existing particles. During such events, Aitken-mode particles contributed more than 50% of the total particle mass. Additionally, we used a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) to assess chemical changes in the sub-micron particles during NPF events. Because the HR-ToF-AMS can not detect particles smaller than 40 nm in diameter, however, it was not possible to investigate the chemistry driving the NPF. Our results indicated that oxygenated organic aerosols (OAs) constituted almost 77%—the largest fraction—of the sub-micron particles. The m/z 57 ion (C4H9+), a tracer of hydrocarbon-like OA (HOA), displayed significantly enhanced signal intensity during all of the NPF event days. Moreover, the increased proportion of organic ions, m/z 44 (CO2+), on these days suggested the presence of less volatile, highly oxidized OAs (LV-OOAs), revealing that the growth of new particles was mainly due to the condensation of low-volatility organic species. The substantially elevated signal intensity of amines (viz., CHN+, CH4N+, C2H4N+, C3H8N+, and C5H12N+) in the sub-micron aerosols during NPF further demonstrated that these nitrogen-containing organic compounds may have played a critical role in these events. Thus, our findings emphasize the relevance of amines to secondary aerosol formation in severely polluted urban environments.

New particle formation and its effect on cloud condensation nuclei abundance in the summer Arctic: a case study in the Fram Strait and Barents Sea

Abstract. In a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol–cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10–50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm−3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s−1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15–50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation.

Characterization of aerosol properties at Cyprus, focusing on cloud condensation nuclei and ice-nucleating particles

Abstract. As part of the A-LIFE (Absorbing aerosol layers in a changing climate: aging, LIFEtime and dynamics) campaign, ground-based measurements were carried out in Paphos, Cyprus, to characterize the abundance, properties, and sources of aerosol particles in general and cloud condensation nuclei (CCN) and ice-nucleating particles (INP) in particular. New particle formation (NPF) events with subsequent growth of the particles into the CCN size range were observed. Aitken mode particles featured κ values of 0.21 to 0.29, indicating the presence of organic materials. Accumulation mode particles featured a higher hygroscopicity parameter, with a median κ value of 0.57, suggesting the presence of sulfate and maybe sea salt particles mixed with organic carbon. A clear downward trend of κ with increasing supersaturation and decreasing dcrit was found. Super-micron particles originated mainly from sea-spray aerosol (SSA) and partly from mineral dust. INP concentrations (NINP) were measured in the temperature range from −6.5 to −26.5 ∘C, using two freezing array-type instruments. NINP at a particular temperature span around 1 order of magnitude below −20 ∘C and about 2 orders of magnitude at warmer temperatures (T>-18 ∘C). Few samples showed elevated concentrations at temperatures >-15 ∘C, which suggests a significant contribution of biological particles to the INP population, which possibly could originate from Cyprus. Both measured temperature spectra and NINP probability density functions (PDFs) indicate that the observed INP (ice active in the temperature range between −15 and −20 ∘C) mainly originate from long-range transport. There was no correlation between NINP and particle number concentration in the size range >500 nm (N>500 nm). Parameterizations based on N>500 nm were found to overestimate NINP by about 1 to 2 orders of magnitude. There was also no correlation between NINP and particle surface area concentration. The ice active surface site density (ns) for the polluted aerosol encountered in the eastern Mediterranean in this study is about 1 to 3 orders of magnitude lower than the ns found for dust aerosol particles in previous studies. This suggests that observed NINP PDFs such as those derived here could be a better choice for modeling NINP if the aerosol particle composition is unknown or uncertain.

Investigation of Atmospheric Aerosol Size Distributions from Ground-Based Solar Spectrometer Measurements Synthesized with Satellite Data

Data collected by a ground-based solar spectrometer at Collegeville, MN, was used to generate Aerosol Optical Depths (AODs) throughout the 2017 calendar year. The AOD data was then visualized at 13 selected wavelengths throughout the year and analyzed in comparison to satellite imagery, upper air charts and backwards trajectories of air masses moving towards Central Minnesota in order to determine key dates of interest that correspond to times before (20170615), during (20170729), and at the conclusion of (20170914) forest fires that burned in British Columbia (BC) during the summer of 2017. The data from these specific days were analyzed further by inputting the maximum and minimum AODs for each day into a Parameter Based Particle Swarm Optimization (PBPSO) algorithm in order to generate bimodal lognormal particle size distributions. The bimodal distributions were chosen because they carry more information about the aerosol loads across the entire spectrum of particle radii. The resulting distributions show an increase in number density and decrease in median radius in the Aitken mode during the BC forest fires and a relatively constant (within uncertainty) number density of accumulation mode particles at daily maximum AODs. Comparing the resulting bimodal lognormal distribution for daily minimum AODs (where evaporation and other diurnal effects are at a minimum) shows an increased number density of Aitken mode particles by two orders of magnitude from pre- to post-forest fires. This measured increase in the number density of smaller radii particles due to forest fires illustrates the PBPSO’s capability of distinguishing variations in atmospheric aerosol particle number size distributions in the Aitken mode based on data collected by the Kipp-Zonen PGS-100 solar spectrometer. KEYWORDS: Atmospheric Aerosol; Particle Swarm Optimization; Aerosol Optical Depth; Solar Spectrometer; Size Distributions; Forest Fire; Satellite Imagery; Upper Air Charts; Backward Trajectory

Effects of Continental Clouds on Surface Aitken and Accumulation Modes

AbstractRelationships between clouds and surface aerosol are investigated at the Oklahoma Atmospheric Radiation Measurements Southern Great Plains site. Cloud chemical transformations, coalescence, and Brownian capture increase material within cloud droplets. Then when cloud droplets evaporate, as they often do, their residuals are larger than unnucleated particles. This creates a bimodal particle size distribution by moving some Aitken mode (25‐ to 100‐nm diameter) particles to the accumulation mode (100‐ to 825‐nm diameter). Clouds also block solar radiation that causes photochemical reactions that produce small particles that grow by coagulation and condensation into the Aitken mode. Highly significant positive correlations of remotely sensed cloud fraction (cf) with time‐lagged Aitken and accumulation mode mean particle diameter (mpd) isolated the effects of cloud processing on both modes. Positive correlations of cf with accumulation concentrations and negative correlations of cf with Aitken concentrations also provided evidence of cloud processing. Photochemical production of very small particles under clear daylight skies worked together with cloud processing to enhance Aitken mpd and concentration correlations with cf. Cloud‐processed aerosol was evident only during daylight and when the boundary layer mixing height exceeded the remotely sensed cloud base altitude. Greater cf, especially consecutive high cf hours increased accumulation and Aitken mpd and accumulation concentrations while it decreased Aitken concentrations. Lower cf, especially consecutive hours of no clouds, decreased overall mpd and did not enhance the accumulation mode. All of these results implicated clouds as a source of the accumulation mode, and thus, clouds seemed to explain bimodal aerosol over the mid‐North American continent.

PM2.5 vertical variation during a fog episode in a rural area of the Yangtze River Delta, China

A dense radiation fog event occurred at the Shouxian site, Anhui Province, China, from the evening of January 2 to noon on January 3, 2017. During this event, vertical profiles of particulate matter (PM) and meteorological parameters within the lower troposphere (0–1000 m) were collected using a tethered balloon. This study assessed the evolution of the PM2.5 profile with the planetary boundary layer (PBL) structure and the effects of fog on the PM2.5 concentration. The results showed the following: (1) At the surface, the average diurnal variation in Aitken mode, accumulation mode and coarse mode particles had bimodal patterns before fog formation and was mainly influenced by diurnal variation in the mixing level depth (MLD). The aerosol number concentrations decreased remarkably, and the PM2.5 was strongly scavenged from 150 μg/m3 to 45 μg/m3 during the fog process. (2) In the vertical direction, the PM2.5 distribution was affected by the PBL height and the vertical fog structure. At 05:00 LT (local time) (i.e., early morning before the fog event), the PM2.5 concentration was slightly higher in the stable layer (260 μg/m3) than in the residual layer (200 μg/m3). At 14:00 LT (haze period), PM2.5 was well mixed below 500 m, with a concentration of 310 μg/m3. After 20:00 LT, when fog formed, PM2.5 was scavenged from the surface to the upper layers, and the scavenging height was controlled by the fog top height. (3) The vertical development of fog was promoted by turbulent mixing and radiation cooling at the fog top. Turbulent mixing enhanced the particle scavenging efficiency of fog droplets by the collision-coalescence process. The PM2.5 scavenging height was corresponded to the turbulence height. Therefore, turbulence development in the fog was the essential dynamic factor driving PM2.5 reduction.

Growth of Aitken mode ammonium sulfate particles by α-pinene ozonolysis

The fraction of Aitken mode particles that grow sufficiently large to act as cloud condensation nuclei is an important factor in understanding the climate impact of atmospheric particles. Elucidati...