Aerosol Size Distribution Measurements Research Articles

Morphochemical characteristics and mixing state of long range transported wildfire particles at Ny-Ålesund (Svalbard Islands)

A prolonged and exceptionally intense air mass advection event transporting biomass burning aerosols generated in Alaska affected Ny-Ålesund in the mid of July 2015. This paper reports the morphochemical characteristics and mixing state of individual aerosol particles collected during the event. To this aim aerosol samples were collected on nucleopore polycarbonate membrane filters using a DEKATI 12-stage low volume impactor and analyzed by scanning electron microscopy (SEM) techniques. Results of SEM investigations depict a complex aerosol characterized by an external mixing between a main part of carbonaceous organic particles (tar balls and organic particles), lower ammonium sulfate and minor potassium chloride and mineral dust amounts. The carbonaceous particles are spherical to slightly elongated and the organic particles show an internal mixing of low density organics and/or ammonium sulfate upon denser nuclei. Most particles are in the accumulation mode size range although the size and the morphology of the chloride and the sulfate salts evidence the growth of these species both in the air and upon the sampling membranes. Individual particle analyses were complemented by aerosol size distribution (Aerodynamic Particle Sizer, Scanning Mobility Particle Sizer) and optical (Particle Soot Absorption Photometer, nephelometer) measurements at ground level in order to retrieve the optical and radiative properties of the aerosol in the atmosphere and to predict the fate and behaviour of particles upon deposition at ground level. Individual particle analyses were also compared with bulk chemical analyses on daily sampling filters and back-trajectory analyses of the air mass movement in order to enucleate distinct sources of the aerosol during the long range transport.

A fast integrated mobility spectrometer for rapid measurement of sub-micrometer aerosol size distribution, Part I: Design and model evaluation

A fast integrated mobility spectrometer (FIMS) was previously developed to characterize submicron aerosol size distributions at a frequency of 1Hz and with high size resolution and counting statistics (Kulkarni & Wang, 2006a, 2006b; Olfert, Kulkarni, & Wang, 2008). However, the dynamic size range of the FIMS was limited to one decade in particle electrical mobility. It was proposed that the FIMS dynamic size range can be greatly increased by using a spatially varying electric field (Wang, 2009). This electric field creates regions with drastically different field strengths in the separator, such that particles of a wide diameter range can be simultaneously classified and subsequently measured. A FIMS incorporating this spatially varying electric field is developed. This paper describes the theoretical frame work and numerical simulations of the FIMS with extended dynamic size range, including the spatially varying electric field, particle trajectories, activation of separated particles in the condenser, and the transfer function, transmission efficiency, and mobility resolution. The influences of the particle Brownian motion on FIMS transfer function and mobility resolution are examined. The simulation results indicate that the FIMS incorporating the spatially varying electric field is capable of measuring aerosol size distribution from 8 to 600nm with high time resolution. The experimental characterization of the FIMS is presented in an accompanying paper.

Measurement of an electronic cigarette aerosol size distribution during a puff

Electronic cigarettes (e-cigarettes) have become very popular recently because they are marketed as a healthier alternative to tobacco smoking and as a useful tool to smoking cessation. E-cigarettes use a heating element to create an aerosol from a solution usually consisting of propylene glycol, glycerol, and nicotine. Despite the wide spread of e-cigarettes, information about aerosol size distributions is rather sparse. This can be caused by the relative newness of e-cigarettes and by the difficulty of the measurements, in which one has to deal with high concentration aerosol containing volatile compounds. Therefore, we assembled an experimental setup for size measurements of e-cigarette aerosol in conjunction with a piston based machine in order to simulate a typical puff. A TSI scanning mobility particle sizer 3936 was employed to provide information about particle concentrations and sizes. An e-cigarette commercially available on the Czech Republic market was tested and the results were compared with a conventional tobacco cigarette. The particles emitted from the e-cigarette were smaller than those of the conventional cigarette having a CMD of 150 and 200 nm. However, the total concentration of particles from e-cigarette was higher.

Novel aerosol analysis approach for characterization of nanoparticulate matter in snow.

Tropospheric aerosols are involved in several key atmospheric processes: from ice nucleation, cloud formation, and precipitation to weather and climate. The impact of aerosols on these atmospheric processes depends on the chemical and physical characteristics of aerosol particles, and these characteristics are still largely uncertain. In this study, we developed a system for processing and aerosolization of melted snow in particle-free air, coupled with a real-time measurement of aerosol size distributions. The newly developed technique involves bringing snow-borne particles into an airborne state, which enables application of high-resolution aerosol analysis and sampling techniques. This novel analytical approach was compared to a variety of complementary existing analytical methods as applied for characterization of snow samples from remote sites in Alert (Canada) and Barrow (USA), as well as urban Montreal (Canada). The dry aerosol measurements indicated a higher abundance of particles of all sizes, and the 30nm size dominated in aerosol size distributions for the Montreal samples, closely followed by Barrow, with about 30% fewer 30nm particles, and about four times lower 30nm particle abundance in Alert samples, where 15nm particles were most abundant instead. The aerosolization technique, used together with nanoparticle tracking analysis and electron microscopy, allowed measurement of a wide size range of snow-borne particles in various environmental snow samples. Here, we discuss the application of the new technique to achieve better physicochemical understanding of atmospheric and snow processes. The results showed high sensitivity and reduction of particle aggregation, as well as the ability to measure a high-resolution snow-borne particle size distribution, including nanoparticulate matter in the range of 10 to 100nm.

Physical and optical properties of aged biomass burning aerosol from wildfires in Siberia and the Western USA at the Mt. Bachelor Observatory

Abstract. The summer of 2015 was an extreme forest fire year in the Pacific Northwest. Our sample site at the Mt. Bachelor Observatory (MBO, 2.7 km a.s.l.) in central Oregon observed biomass burning (BB) events more than 50 % of the time during August. In this paper we characterize the aerosol physical and optical properties of 19 aged BB events during August 2015. Six of the 19 events were influenced by Siberian fires originating near Lake Baikal that were transported to MBO over 4–10 days. The remainder of the events resulted from wildfires in Northern California and Southwestern Oregon with transport times to MBO ranging from 3 to 35 h. Fine particulate matter (PM1), carbon monoxide (CO), aerosol light scattering coefficients (σscat), aerosol light absorption coefficients (σabs), and aerosol number size distributions were measured throughout the campaign. We found that the Siberian events had a significantly higher Δσabs∕ΔCO enhancement ratio, higher mass absorption efficiency (MAE; Δσabs∕ΔPM1), lower single scattering albedo (ω), and lower absorption Ångström exponent (AAE) when compared with the regional events. We suggest that the observed Siberian events represent that portion of the plume that has hotter flaming fire conditions and thus enabled strong pyroconvective lofting and long-range transport to MBO. The Siberian events observed at MBO therefore represent a selected portion of the original plume that would then have preferentially higher black carbon emissions and thus an enhancement in absorption. The lower AAE values in the Siberian events compared to regional events indicate a lack of brown carbon (BrC) production by the Siberian fires or a loss of BrC during transport. We found that mass scattering efficiencies (MSE) for the BB events ranged from 2.50 to 4.76 m2 g−1. We measured aerosol size distributions with a scanning mobility particle sizer (SMPS). Number size distributions ranged from unimodal to bimodal and had geometric mean diameters (Dpm) ranging from 138 to 229 nm and geometric standard deviations (σg) ranging from 1.53 to 1.89. We found MSEs for BB events to be positively correlated with the geometric mean of the aerosol size distributions (R2 = 0.73), which agrees with Mie theory. We did not find any dependence on event size distribution to transport time or fire source location.

OBSERVAÇÕES POR AVIÃO DA INTERAÇÃO DA PLUMA DE MANAUS COM OS AEROSSÓIS DA FLORESTA DURANTE A ESTAÇÃO CHUVOSA: UM ESTUDO DE CASO

Measurements of aerosol size distribution and cloud condensation nuclei (CCN) efficiency over the Amazon Region close to the city of Manaus, Brazil, were taken during an airborne experiment in February – March (rainy season) 2014 as part of the Green Ocean Amazon Experiment (GOAmazon). A variety of aerosols were observed following the aging along the downwind Manaus plume, in a relatively well preserved portion of Amazon basin. At this work we evaluate how those aerosols interact with the Amazonian environment for the situation observed during 13th march 2014. The aerosols size distribution is studied considering its aging downwind the Manaus plume. The concentration of CCN inside the plume is evaluated and a large enhancement is observed.

Aerosol optical properties in the southeastern United States in summer – Part 1: Hygroscopic growth

Abstract. Aircraft observations of meteorological, trace gas, and aerosol properties were made during May–September 2013 in the southeastern United States (US) under fair-weather, afternoon conditions with well-defined planetary boundary layer structure. Optical extinction at 532 nm was directly measured at relative humidities (RHs) of ∼ 15, ∼ 70, and ∼ 90 % and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. The calculated enhancement in hydrated aerosol extinction with relative humidity, f(RH), calculated by this method agreed well with the observed f(RH) at ∼ 90 % RH. The dominance of organic aerosol, which comprised 65 ± 10 % of particulate matter with aerodynamic diameter < 1 µm in the planetary boundary layer, resulted in relatively low f(RH) values of 1.43 ± 0.67 at 70 % RH and 2.28 ± 1.05 at 90 % RH. The subsaturated κ-Köhler hygroscopicity parameter κ for the organic fraction of the aerosol must have been < 0.10 to be consistent with 75 % of the observations within uncertainties, with a best estimate of κ = 0.05. This subsaturated κ value for the organic aerosol in the southeastern US is broadly consistent with field studies in rural environments. A new, physically based, single-parameter representation was developed that better described f(RH) than did the widely used gamma power-law approximation.

Comparison of atmospheric particle concentration measurements using different optical detectors: Potentiality and limits for air quality applications

Optical detectors for atmospheric aerosol concentration measurements are often used in air quality applications given their potentialities for online measurements of air quality parameters at high temporal resolution. In this work the performances of different optical aerosol detectors used in air quality applications have been tested and compared for urban background aerosol conditions. Simultaneous measurements of aerosol number concentrations, size distributions and mass concentrations were taken in two different periods: November 2013 – February 2014 and May–June 2014 at an urban background site in Lecce (Southeastern Italy). Measurements were carried out using an OPC Grimm (mod. 1.109), an OPC FAI (Multichannel Monitor) and an optical photometer Mie pDR-1200. Good correlation, with determination coefficients R2 larger than 0.93 were found between particle number concentrations measured by the two OPCs both in accumulation (0.28–0.90μm for FAI and 0.29–0.90μm for Grimm) and coarse modes (1.10–10μm for FAI and 1.15–11.25μm for Grimm). Absolute counting for the accumulation fraction shows that Grimm OPC detects more particles (about 10%) than FAI OPC at concentration higher than 200,000particles/L in condition of high RH. This could be due to the changes of the optical properties of particles in high RH conditions visible even if the inlets of the two instruments are conditioned for lowering RH in sampled air. The differences in the absolute counting of the coarse fraction does not seems to be related to RH effects. The performances in evaluating mass concentrations PM10, and PM2.5 were evaluated comparing OPCs and pDR-1200 outputs with reference gravimetric and β-ray methods (that appeared to be essentially equivalent). Good agreement between Grimm OPC and SWAM is found both in PM10 and PM2.5 fractions while FAI OPC revealed greater discrepancy and scatter with respect to reference measurements. The performances of the pDR-1200 photometer were lower with respect to the OPCs with a larger influence of RH and optical properties of particles. The analysis of diurnal average trends in number and mass concentrations as well as the high temporal resolution responses of the instruments showed that optical detectors could be very useful to investigate atmospheric aerosol for air quality applications and to individuate and investigate specific pollution events. However, especially if they are used for evaluating mass concentrations (PM1, PM2.5 or PM10), it is necessary to take into account RH effects (even if the inlet are conditioned) and, possibly, use optical detectors together with reference gravimetric or β-ray methods to check their response in the effective operative conditions.

A light-weight, high-sensitivity particle spectrometer for PM2.5 aerosol measurements

ABSTRACTA light-weight, low-cost optical particle spectrometer for measurements of aerosol number concentrations and size distributions has been designed, constructed, and demonstrated. The spectrometer is suitable for use on small, unmanned aerial vehicles (UAVs) and in balloon sondes. The spectrometer uses a 405 nm diode laser to count and size individual particles in the size range 140–3000 nm. A compact data system combines custom electronics with a single-board commercial computer. Power consumption is 7W at 9–15 V. 3D printing technology was used in the construction of the instrument to reduce cost, manufacturing complexity, and weight. The resulting Printed Optical Particle Spectrometer (POPS) instrument weighs about 800 g with an approximate materials cost of 2500 USD. Several POPS units have been constructed, tested in the laboratory, and deployed on UAVs. Here we present an overview of the instrument design and construction, laboratory validation data, and field engineering data for POPS.

Analysis of long‐term aerosol size distribution data from Jungfraujoch with emphasis on free tropospheric conditions, cloud influence, and air mass transport

AbstractSix years of aerosol size distribution measurements between 20 and 600 nm diameters and total aerosol concentration above 10 nm from March 2008 to February 2014 at the high‐alpine site Jungfraujoch are presented. The size distribution was found to be typically bimodal with mode diameters and widths relatively stable throughout the year and the observation period. New particle formation was observed on 14.5% of all days without a seasonal preference. Particles typically grew only into the Aitken mode and did not reach cloud condensation nucleus (CCN) sizes on the time scale of several days. Growth of preexisting particles in the Aitken mode, on average, contributed very few CCN. We concluded that the dominant fraction of CCN at Jungfraujoch originated in the boundary layer. A number of approaches were used to distinguish free tropospheric (FT) conditions and episodes with planetary boundary layer (PBL) influence. In the absence of PBL injections, the concentration of particles larger than 90 nm (N90, roughly corresponding to the CCN concentration) reached a value ~40 cm−3 while PBL influence caused N90 concentrations of several hundred or even 1000 cm−3. Comparing three criteria for free tropospheric conditions, we found FT prevalence for 39% of the time with over 60% during winter and below 20% during summer. It is noteworthy that a simple criterion based on standard trace gas measurements appeared to outperform alternative approaches.

Intercomparisons of Mobility Size Spectrometers and Condensation Particle Counters in the Frame of the Spanish Atmospheric Observational Aerosol Network

Red Espanola de DMAs Ambientales (REDMAAS), the Spanish network of environmental differential mobility analyzers (DMAs), currently comprises six research groups involved in the measurement of atmospheric aerosol size distributions by means of DMAs. The aim of this network is to guarantee the good quality and comparability of the routine measurements carried out at each location and in diverse environments across Spain. In order to achieve this objective, one of its main activities is the annual intercomparison of mobility size spectrometers used within the network (five units of scanning mobility particle sizers [SMPS] and one ultrafine particle monitor [UFPM]). Here we report the 2main results obtained during the 2010–2012 campaigns, including a study on particle deposition in dryers used in ambient air sampling systems. In general, all instruments showed good performance with deviations in accepted tolerance. The intercomparisons have been proved to be a useful exercise to detect instrument problems, su...

RACORO continental boundary layer cloud investigations: 1. Case study development and ensemble large‐scale forcings

AbstractObservation‐based modeling case studies of continental boundary layer clouds have been developed to study cloudy boundary layers, aerosol influences upon them, and their representation in cloud‐ and global‐scale models. Three 60 h case study periods span the temporal evolution of cumulus, stratiform, and drizzling boundary layer cloud systems, representing mixed and transitional states rather than idealized or canonical cases. Based on in situ measurements from the Routine AAF (Atmospheric Radiation Measurement (ARM) Aerial Facility) CLOWD (Clouds with Low Optical Water Depth) Optical Radiative Observations (RACORO) field campaign and remote sensing observations, the cases are designed with a modular configuration to simplify use in large‐eddy simulations (LES) and single‐column models. Aircraft measurements of aerosol number size distribution are fit to lognormal functions for concise representation in models. Values of the aerosol hygroscopicity parameter, κ, are derived from observations to be ~0.10, which are lower than the 0.3 typical over continents and suggestive of a large aerosol organic fraction. Ensemble large‐scale forcing data sets are derived from the ARM variational analysis, European Centre for Medium‐Range Weather Forecasts, and a multiscale data assimilation system. The forcings are assessed through comparison of measured bulk atmospheric and cloud properties to those computed in “trial” large‐eddy simulations, where more efficient run times are enabled through modest reductions in grid resolution and domain size compared to the full‐sized LES grid. Simulations capture many of the general features observed, but the state‐of‐the‐art forcings were limited at representing details of cloud onset, and tight gradients and high‐resolution transients of importance. Methods for improving the initial conditions and forcings are discussed. The cases developed are available to the general modeling community for studying continental boundary clouds.

Altitude‐resolved shortwave and longwave radiative effects of desert dust in the Mediterranean during the GAMARF campaign: Indications of a net daily cooling in the dust layer

AbstractDesert dust interacts with shortwave (SW) and longwave (LW) radiation, influencing the Earth radiation budget and the atmospheric vertical structure. Uncertainties on the dust role are large in the LW spectral range, where few measurements are available and the dust optical properties are not well constrained. The first airborne measurements of LW irradiance vertical profiles over the Mediterranean were carried out during the Ground‐based and Airborne Measurements of Aerosol Radiative Forcing (GAMARF) campaign, which took place in spring 2008 at the island of Lampedusa. The experiment was aimed at estimating the vertical profiles of the SW and LW aerosol direct radiative forcing (ADRF) and heating rates (AHR), taking advantage of vertically resolved measurements of irradiances, meteorological parameters, and aerosol microphysical and optical properties. Two cases, characterized respectively by the presence of a homogeneous dust layer (3 May, with aerosol optical depth, AOD, at 500 nm of 0.59) and by a low aerosol burden (5 May, with AOD of 0.14), are discussed. A radiative transfer model was initialized with the measured vertical profiles and with different aerosol properties, derived from measurements or from the literature. The simulation of the irradiance vertical profiles, in particular, provides the opportunity to constrain model‐derived estimates of the AHR. The measured SW and LW irradiances were reproduced when the model was initialized with the measured aerosol size distributions and refractive indices. For the dust case, the instantaneous (solar zenith angle, SZA, of 55.1°) LW‐to‐SW ADRF ratio was 23% at the surface and 11% at the top of the atmosphere (TOA), with a more significant LW contribution on a daily basis (52% at the surface and 26% at TOA), indicating a relevant reduction of the SW radiative effects. The AHR profiles followed the aerosol extinction profile, with comparable peaks in the SW (0.72 ± 0.11 K d−1) and in the LW (−0.52 ± 0.12 K d−1) for the considered SZA. On a daily basis, the absolute value of the heating rate was larger in the LW than in the SW, producing a net cooling effect at specific levels. These are quite unexpected results, emphasizing the important role of LW radiation.

Near‐cloud aerosols in monsoon environment and its impact on radiative forcing

AbstractIn order to understand the near‐cloud aerosol properties and their impact on radiative forcing, we utilized in situ aircraft measurements of aerosol particles and cloud droplets during the Cloud Aerosol Interaction and Precipitation Enhancement Experiment carried out over the Indian subcontinent in the monsoon season. From the measurement of aerosol size distribution of diameter range from 0.1 to 50 µm, we reported that aerosol concentrations could be enhanced by 81% and the effective diameter (deff, µm) by a factor of 2 near the cloud edges when compared with regions far from the cloud. These enhanced aerosol concentrations are a function of the relative humidity (RH) in the cloud‐free zone, attributed to mixing and entrainment processes in the cloud edges. It is also found that for warm clouds, RH increases exponentially in the near‐cloud regions. In addition, deff was increased linearly with RH. Through model simulations, we found that aerosol optical depth decreases with distance from the cloud edge. Further, aerosols in cloud edges were found to increase the reflected flux by 20% compared to cloud‐free regions, thus brightening the near‐cloud areas.

Characteristics of Aerosol Extinction Coefficient in Taipei Metropolitan Atmosphere

The object of this study investigated the correlation of visibility with aerosol physical properties in the urban atmosphere. The field experiments were conducted in four seasons from August 2010 to March 2011 in National Taipei University of Technology (NTUT), located in the downtown of Taipei city. Integrating nephelometer was used to measure the aerosol optical properties and compared with the calculated values based upon the measurements of aerosol concentration and size distribution. The characterization of visibility was influenced by aerosol concentrations and relative humidity. When the relative humidity was above 70%, the particles usually grew into larger size range and changed their optical characteristics. The results showed that the surface area concentration had a great relationship with extinction coefficient, especially for PM2.5. The correlation between particle number or volume concentration and extinction coefficient was complicated. Hence, visibility could be estimated by particle surface area concentration. The conclusions suggested that particle surface area concentration obtained from number concentration combined with size distribution could be used to estimate visibility.

A spectrometer for measuring particle size distributions in the range of 3 nm to 10 μm

A spectrometer combining electrical mobility sizing and aerodynamic sizing was developed to measure aerosol size distributions in the range of 3 nm to 10 μm. It includes three instruments which cover different size ranges (a nano scanning mobility particle sizer (NSMPS, 3–60 nm), a regular scanning mobility particle sizer (RSMPS, 40–700 nm), and an aerodynamic particle sizer (APS, 550 nm–10 μm)). High voltage and sheath flow of the NSMPS and RSMPS were supplied using two home-built control boxes. A LabVIEW program was developed for spectrometer automatic operation. A linear inversion method was applied to correct particle multiple charging effects and to integrate data from the three instruments into a wide-range size distribution. Experiments were conducted to compare distributions in the overlap size ranges measured by three instruments. Good agreement between the NSMPS and RSMPS was achieved after correcting for the difference in counting efficiencies of the two particle counters. Aerodynamic size distributions reported by the APS were converted to mobility size distributions by applying an effective density method. Distributions measured by the RSMPS and APS were consistent in the overlap size range of 550–700 nm. A full spectrum in the size range of 3 nm to 10 μm was demonstrated by measuring aerosol generated using a mixture of different sized polystyrene latex spheres.

Temperature influence on the natural aerosol budget over boreal forests

Abstract. We investigated the natural aerosol evolution of biogenic monoterpene emissions over the northern boreal forest area as a function of temperature using long-term field measurements of aerosol size distributions and back trajectories at two SMEAR (Station for Measuring Ecosystem–Atmosphere Relations) stations, SMEAR I and SMEAR II, in Finland. Similar to earlier studies, we found that new particles were formed via nucleation when originally clean air from the ocean entered the land, after which these particles continuously grew to larger sizes during the air mass transport. Both the travelling hour over land and temperature influenced the evolution of the particle number size distribution and aerosol mass yield from biogenic emissions. Average concentrations of nucleation mode particles were higher at lower temperatures, whereas the opposite was true for accumulation mode particles. Thus, more cloud condensation nuclei (CCN) may be formed at higher temperatures. The overall apparent aerosol yield, derived from the aerosol masses against accumulated monoterpene emissions, ranges from 13 to 37% with a minor, yet complicating, temperature dependence.

Effect of Aerosol Volatility on the Sizing Accuracy of Differential Mobility Analyzers

Differential mobility analyzers (DMAs) are widely used for calibrating other instruments and measuring aerosol size distributions. DMAs classify aerosol particles according to their electrical mobility, which is assumed to be constant during the classification process. However, particles containing semivolatile substances can change their size in the DMA, leading to sizing errors. In this article, the effect of particle size changes during the classification process on the sizing accuracy of DMAs is discussed. It is shown that DMAs select particles whose time-of-flight-averaged electrical mobility is equal to that of stable particles that are selected under given operating conditions. For evaporating particles, this implies that DMAs select particles that are originally larger than the reported size. At the exit of the DMA, selected particles are smaller than the reported size. Particle evaporation and growth inside DMAs was modeled to study the effect of particle size changes on the sizing accuracy and the transfer function of DMAs in constant- and scanning-voltage modes of operation. Modeling predictions were found to agree well with the results of experiments with ammonium nitrate aerosol. The model was used to estimate sizing errors when measuring hygroscopic and other volatile aerosols. Errors were found to be larger at smaller sizes and low sheath flow rates. Errors, however, are fairly small when saturation concentration is below 10 μg/m3, assuming an evaporation coefficient of 0.1. Particles size changes during classification lead to distortion of the DMA transfer function. In voltage scanning mode, errors are generally larger, especially at high scan rates.Copyright 2014 American Association for Aerosol Research

Aerosol Measurements in the Atmospheric Surface Layer at L’Aquila, Italy: Focus on Biogenic Primary Particles

Two year measurements of aerosol concentration and size distribution (0.25 μm < d < 30 μm) in the atmospheric surface layer, collected in L’Aquila (Italy) with an optical particle counter, are reported and analysed for the different modes of the particle size distribution. A different seasonal behaviour is shown for fine mode aerosols (largely produced by anthropogenic combustion), coarse mode and large-sized aerosols, whose abundance is regulated not only by anthropogenic local production, but also by remote natural sources (via large scale atmospheric transport) and by local sources of primary biogenic aerosols. The observed total abundance of large particles with diameter larger than 10 μm is compared with a statistical counting of primary biogenic particles, made with an independent technique. Results of these two observational approaches are analysed and compared to each other, with the help of a box model driven by observed meteorological parameters and validated with measurements of fine and coarse mode aerosols and of an atmospheric primary pollutant of anthropogenic origin (NOx). Except in winter months, primary biogenic particles in the L’Aquila measurement site are shown to dominate the atmospheric boundary layer population of large aerosol particles with diameter larger than 10 μm (about 80 % of the total during summer months), with a pronounced seasonal cycle, contrary to fine mode aerosols of anthropogenic origin. In order to explain these findings, the main mechanisms controlling the abundance and variability of particulate matter tracers in the atmospheric surface layer are analysed with the numerical box-model.

Application of Half Mini DMA for sub 2 nm particle size distribution measurement in an electrospray and a flame aerosol reactor

Conventional Differential Mobility Analyzers (DMA) have had limited success in classifying sub 2nm particles with high resolution, primarily due to diffusion broadening. High flow DMAs have been able to overcome this limitation and achieve high-resolution classification of sub 2nm particles, by maintaining laminar flow at high Reynolds numbers. A Half Mini DMA was compared with a Nano DMA (TSI model 3085) for sub 2nm size distribution measurements of organic ions generated by electrospray of tetra-heptyl ammonium bromide (THAB) solution and aerosols generated by a premixed flat flame reactor. Obscurities in ion peak measurements with the Nano DMA indicated a higher diffusion effect. Calculations of the diffusing transfer functions indicated that the Half Mini DMA deviated significantly from ideal conditions, possibly due to the higher demands for a more precise electrode placement and a smaller surface roughness, since it is operated at a high sheath flow rate.The Half Mini DMA was then applied to study the formation of flame-generated aerosols in the sub 2nm range. This is the first reported measurement of these clusters in an aerosol reactor. The effects of the flame synthesis precursor (titanium (IV) isopropoxide), the Kr-85 radioactive neutralizer, and the tubing materials on the flame aerosol size distribution measurements were investigated. After the introduction of titanium (IV) isopropoxide, several discrete peaks were detected, suggesting discrete cluster formation during the initial stages of TiO2 particle synthesis. The addition of a radioactive neutralizer balanced the size distribution of flame aerosols by changing the charging mechanisms. Compared with copper tubing, silicone conductive tubing generated extremely high positive ion contamination after neutralization.