Differential Mobility Particle Sizer Research Articles

Cloud activation properties of aerosol particles in a continental Central European urban environment

Abstract. Collocated measurements using a condensation particle counter, differential mobility particle sizer and cloud condensation nuclei counter were realised in parallel in central Budapest from 15 April 2019 to 14 April 2020 to gain insight into the cloud activation properties of urban aerosol particles. The median total particle number concentration was 10.1 × 103 cm−3. The median concentrations of cloud condensation nuclei (CCN) at water vapour supersaturation (S) values of 0.1 %, 0.2 %, 0.3 %, 0.5 % and 1.0 % were 0.59, 1.09, 1.39, 1.80 and 2.5 × 103 cm−3, respectively. The CCN concentrations represented 7–27 % of all particles. The CCN concentrations were considerably larger but the activation fractions were systematically substantially smaller than observed in regional or remote locations. The effective critical dry particle diameters (dc,eff) were derived utilising the CCN concentrations and particle number size distributions. Their median values at the five supersaturation values considered were 207, 149, 126, 105 and 80 nm, respectively; all of these diameters were positioned within the accumulation mode of the typical particle number size distribution. Their frequency distributions revealed a single peak for which the geometric standard deviation increased monotonically with S. This broadening indicated high time variability in the activating properties of smaller particles. The frequency distributions also showed fine structure, with several compositional elements that seemed to reveal a consistent or monotonical tendency with S. The relationships between the critical S and dc,eff suggest that urban aerosol particles in Budapest with diameters larger than approximately 130 nm showed similar hydroscopicity to corresponding continental aerosol particles, whereas smaller particles in Budapest were less hygroscopic than corresponding continental aerosol particles. Only modest seasonal cycling in CCN concentrations and activation fractions was seen, and only for large S values. This cycling likely reflects changes in the number concentration, chemical composition and mixing state of the particles. The seasonal dependencies of dc,eff were featureless, indicating that the droplet activation properties of the urban particles remained more or less the same throughout the year. This is again different from what is seen in non-urban locations. Hygroscopicity parameters (κ values) were computed without determining the time-dependent chemical composition of the particles. The median values for κ were 0.15, 0.10, 0.07, 0.04 and 0.02, respectively, at the five supersaturation values considered. The averages suggested that the larger particles were considerably more hygroscopic than the smaller particles. We found that the κ values for the urban aerosol were substantially smaller than those previously reported for aerosols in regional or remote locations. All of these characteristics can be linked to the specific source composition of particles in cities. The relatively large variability in the hygroscopicity parameters for a given S emphasises that the individual values represent the CCN population in ambient air while the average hygroscopicity parameter mainly corresponds to particles with sizes close to the effective critical dry particle diameter.

Mediterranean nascent sea spray organic aerosol and relationships with seawater biogeochemistry

Abstract. The organic mass fraction from sea spray aerosol (SSA) is currently a subject of intense research. The majority of this research is dedicated to measurements in ambient air. However a number of studies have recently started to focus on nascent sea spray aerosol. This work presents measurements collected during a 5-week cruise in May and June 2017 in the central and western Mediterranean Sea, an oligotrophic marine region with low phytoplankton biomass. Surface seawater was continuously pumped into a bubble-bursting apparatus to generate nascent sea spray aerosol. Size distributions were measured with a differential mobility particle sizer (DMPS). Chemical characterization of the submicron aerosol was performed with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) operating with 10 min time resolution and with filter-based chemical analysis on a daily basis. Using positive matrix factorization analysis, the ToF-ACSM non-refractory organic matter (OMNR) was separated into four different organic aerosol types, identified as primary OA (POANR), oxidized OA (OOANR), methanesulfonic acid type OA (MSA-OANR), and mixed OA (MOANR). In parallel, surface seawater biogeochemical properties were monitored providing information on phytoplankton cell abundance and seawater particulate organic carbon (1 h time resolution) and seawater surface microlayer (SML) dissolved organic carbon (DOC) (on a daily basis). Statistically robust correlations (for n>500) were found between MOANR and nanophytoplankton cell abundance, as well as between POANR, OOANR, and particulate organic carbon (POC). Parameterizations of the contributions of different types of organics to the submicron nascent sea spray aerosol are proposed as a function of the seawater biogeochemical properties for use in models.

Ultrafine Aerosol Particle Sizer Based on Piezoresistive Microcantilever Resonators with Integrated Air-Flow Channel.

To monitor airborne nano-sized particles (NPs), a single-chip differential mobility particle sizer (DMPS) based on resonant micro cantilevers in defined micro-fluidic channels (µFCs) is introduced. A size bin of the positive-charged fraction of particles herein is separated from the air stream by aligning their trajectories onto the cantilever under the action of a perpendicular electrostatic field of variable strength. We use previously described µFCs and piezoresistive micro cantilevers (PMCs) of 16 ng mass fabricated using micro electro mechanical system (MEMS) technology, which offer a limit of detection of captured particle mass of 0.26 pg and a minimum detectable particulate mass concentration in air of 0.75 µg/m3. Mobility sizing in 4 bins of a nebulized carbon aerosol NPs is demonstrated based on finite element modelling (FEM) combined with a-priori knowledge of particle charge state. Good agreement of better than 14% of mass concentration is observed in a chamber test for the novel MEMS-DMPS vs. a simultaneously operated standard fast mobility particle sizer (FMPS) as reference instrument. Refreshing of polluted cantilevers is feasible without de-mounting the sensor chip from its package by multiply purging them alternately in acetone steam and clean air.

High-performance and sustainable aerosol filters based on hierarchical and crosslinked nanofoams of cellulose nanofibers

Nano-structured and porous foams derived from crosslinked cellulose nanofibers (CNF) were designed and tailored as highly efficient aerosol filters. The lignin-containing CNF was prepared from a recycled milk-container board using deep eutectic solvent pretreatment and mechanical grinding. The nanofoams or aerogels were formed in different densities (initial CNF concentration of 0.2–1.0 wt%) with a freeze-drying process using two silane compounds for strengthening the structure. The filtration performance of nanofoams was studied with a Differential Mobility Particle Sizer (DMPS) setup using 10–500 nm NaCl aerosol particles. DMPS determines particle number size distribution of particles passing through nanofoams which is used to calculate the filtration performance. All nanofoams, which possessed porosity from 99.1% to 99.8% and specific surface area from 5.9 m2 g−1 to 18.6 m2 g−1, achieved good filtration performance (>96%) in the measured particle size range. Very high filtration efficiency (>99.5%) was achieved with the 0.7 wt% nanofoam sample for particles smaller than 360 nm. Based on the quality factors (QF), 0.3 wt% nanofoam produced the lowest pressure drop yet with relatively high filtration efficiency and resulted in the highest QF value that met the N95 standard requirements of respirator face masks. The structure and thickness of the nanofoam filter makes possible high particle bearing without loss on its performance.

In-depth characterization of submicron particulate matter inter-annual variations at a street canyon site in northern Europe

Abstract. Atmospheric aerosols play an important role in air pollution. Aerosol particle chemical composition is highly variable depending on the season, hour of the day, day of the week, meteorology, and location of the measurement site. Long measurement periods and highly time-resolved data are required in order to achieve a statistically relevant amount of data for assessing those variations and evaluating pollution episodes. In this study, we present continuous atmospheric PM1 (particulate matter < 1 µm) concentration and composition measurements at an urban street canyon site located in Helsinki, Finland. The study was performed for 4.5 years (2015–2019) and involved highly time-resolved measurements by taking advantage of a suite of online state-of-the-art instruments such as an aerosol chemical speciation monitor (ACSM), a multi-angle absorption photometer (MAAP), a differential mobility particle sizer (DMPS), and an Aethalometer (AE). PM1 consisted mostly of organics, with mean mass concentrations of 2.89 µg m−3 (53 % of PM1) followed by inorganic species (1.56 µg m−3, 29 %) and equivalent black carbon (eBC, 0.97 µg m−3, 18 %). A trend analysis revealed a decrease in BC from fossil fuel (BCFF), organics, and nitrate over the studied years. Clear seasonal and/or diurnal variations were found for the measured atmospheric PM1 constituents. Particle number and mass size distributions over different seasons revealed the possible influence of secondary organic aerosols (SOAs) during summer and the dominance of ultrafine traffic aerosols during winter. The seasonality of measured constituents also impacted the particle's coating and absorptive properties. The investigation of pollution episodes observed at the site showed that a large fraction of aerosol particle mass was comprised of inorganic species during long-range transport, while during local episodes eBC and organics prevailed together with elevated particle number concentration. Overall, the results increased knowledge of the variability of PM1 concentration and composition in a Nordic traffic site and its implications on urban air quality. Considering the effects of PM mitigation policies in northern Europe in the last decades, the results obtained in this study may be considered illustrative of probable future air quality challenges in countries currently adopting similar environmental regulations.

Physical and chemical properties of aerosol particles and cloud residuals on Mt. Åreskutan in Central Sweden during summer 2014

The size distribution, volatility and hygroscopicity of ambient aerosols and cloud residuals were measured with a differential mobility particle sizer (DMPS) and a volatility–hygroscopicity tandem differential mobility analyser (VHTDMA) coupled to a counterflow virtual impactor (CVI) inlet during the Cloud and Aerosol Experiment at Åre (CAEsAR) campaign at Mt. Åreskutan during summer 2014. The chemical composition of particulate matter (PM) and cloud water were analysed offline using thermo-optical OC/EC analysis and ion chromatography. The importance of aerosol particle size for cloud droplet activation and subsequent particle scavenging was clearly visible in the measured size distributions. Cloud residuals were shifted towards larger sizes compared to ambient aerosol, and the cloud events were followed by a size distribution dominated by smaller particles. Organics dominated both PM (62% organic mass fraction) and cloud water (63% organic mass fraction) composition. The volatility and hygroscopicity of the ambient aerosols were representative of homogeneous aged aerosol with contributions from biogenic secondary organics, with median volume fraction remaining (VFR) of 0.04–0.05, and median hygroscopicity parameter κ of 0.16–0.24 for 100–300 nm particles. The corresponding VFR and κ for the cloud residuals were 0.03–0.04 and 0.18–0.20. The chemical composition, hygroscopicity and volatility measurements thus showed no major differences between the ambient aerosol particles and cloud residuals. The VFR and κ values predicted based on the chemical composition measurements agreed well with the VHTDMA measurements, indicating the bulk chemical composition to be a reasonable approximation throughout the size distribution. There were indications, however, of some more subtle changes in time scales not achievable by the offline chemical analysis applied here. Further, online observations of aerosol and cloud residual chemical composition are therefore warranted.

In-situ aerosol nanoparticle characterization by small angle X-ray scattering at ultra-low volume fraction

State-of-the-art aerosol nanoparticle techniques all have one feature in common: for analysis they remove the nanoparticles from their original environment. Therefore, physical and chemical properties of the particles might be changed or cannot be measured correctly. To overcome these shortcomings, we apply synchrotron based small angle X-ray scattering (SAXS) as an in-situ measurement technique. Contrasting other aerosol studies using SAXS, we focus on particle concentrations which allow direct comparison to common aerosol nanoparticle analyzers. To this end, we analyze aerosol nanoparticles at ambient pressure and concentrations of slightly above ~106 cm−3. A differential mobility particle sizer (DMPS) is operated in parallel. We find that SAXS enables measurement of the primary particles and the aggregates, whereas the DMPS detects only aggregates. We conclude that in-situ nanoparticle characterization with ultra-low volume fractions of ~10–10 is feasible with SAXS. Our technique opens up a doorway to the in-situ analysis of aerosol nanoparticles under atmospheric conditions.

Development and qualification of a VH-TDMA for the study of pure aerosols

We create and qualify a Volatility and Hygroscopicity Tandem Differential Mobility Analyzer (VH-TDMA) for the study of aerosols. This VH-TDMA measures size distributions, volatility, and hygroscopicity and includes an auxiliary conditioner that allows quick connection to other external aerosol conditioners. The differential mobility analyzers are not temperature controlled, allowing the surrounding environment to influence the measurement conditions, and this is fully accounted for when measuring aerosol volatility and hygroscopicity. For the volatility conditioner, the VH-TDMA uses a 15 m coil of tubing in an oven to evaporate aerosol samples at elevated temperatures. We measured several single component model aerosols to qualify the differential mobility particle sizer (DMPS) channel and each of the conditioners: hygroscopicity and volatility. Due to insufficient power supply calibration in this study, the TDMA channel is limited to particle sizes greater than 70 nm. The DMPS channel was able to...

Applicability of Optical and Diffusion Charging-Based Particulate Matter Sensors to Urban Air Quality Measurements

ABSTRACT High spatial resolution particulate matter measurements are necessary to accurately characterize urban air quality issues. This study investigates how sensors can be used in an urban area to complement existing air quality measurements. A measurement campaign was conducted during winter in Helsinki, Finland, where the performance of a custom-built optical instrument—the Prototype Aerosol Sensor (PAS; uses Shinyei PPD60PV and PPD42NS sensor modules)—and three commercial diffusion charging-based sensors (Pegasor AQ Urban, DiSCmini and Partector) was evaluated against reference instruments. The results showed that the PAS was able to measure the coarse (PM2.5-10; range: 0–400 µg m–3) and fine (PM2.5; range: 0–50 µg m–3) fractions with reasonably high correlations (R2 = 0.87 and 0.77) when compared to a gravimetric monitor. Likewise, the lung deposited surface area (LDSA) concentrations delivered by the three diffusion charging sensors indicated good performance (R2: 0.92–0.97) when compared to LDSA concentrations calculated from the size distribution data of the differential mobility particle sizer. A clear correlation (R2 = 0.77) between the black carbon and Pegasor-measured LDSA concentrations, as well as similar diurnal cycles, was observed, suggesting a common source. The optical sensors were useful for measuring the mass concentrations of coarse local particles. By contrast, the diffusion charging sensors were applicable in urban environments, where ultrafine particles from traffic or other local combustion sources affect air quality.

Driving parameters of biogenic volatile organic compounds and consequences on new particle formation observed at an eastern Mediterranean background site

Abstract. As a part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) and Cyprus Aerosols and Gas Precursors (ENVI-Med CyAr) programs, this study aims primarily to provide an improved understanding of the sources and the fate of volatile organic compounds (VOCs) in the eastern Mediterranean. More than 60 VOCs, including biogenic species (isoprene and eight monoterpenes) and oxygenated VOCs, were measured during a 1-month intensive field campaign performed in March 2015 at the Cyprus Atmospheric Observatory (CAO), a regional background site in Cyprus. VOC measurements were conducted using complementary online and offline techniques. Biogenic VOCs (BVOCs) were principally imputed to local sources and characterized by compound-specific daily cycles such as diurnal maximum for isoprene and nocturnal maximum for α- and β-pinenes, in connection with the variability of emission sources. The simultaneous study of pinene and isoprene temporal evolution and meteorological parameters has shown that BVOC emissions were mainly controlled by ambient temperature, precipitation and relative humidity. It was found that isoprene daytime emissions at CAO depended on temperature and solar radiation changes, whereas nocturnal BVOC concentrations (e.g., from oak and pine forests) were more prone to the relative humidity and temperature changes. Significant changes in monoterpene mixing ratios occurred during and after rainfall. The second part of the study focused on new particle formation (NPF) events at CAO. BVOCs are known to potentially play a role in the growth as well as in the early stages of formation of new atmospheric particles. Based on observations of the particle size distribution performed with a differential mobility particle sizer (DMPS) and the total number concentrations of particles larger than 1 nm diameter measured by particle size magnifier (PSM), NPF events were found on 14 out of 20 days of the field campaign. For all possible proxy parameters (meteorological parameters, calculated H2SO4 and measured gaseous compounds) having a role in NPF, we present daily variations of different classes during nucleation event and non-event days. NPF can occur at various condensational sink (CS) values and both under polluted and clean atmospheric conditions. High H2SO4 concentrations coupled with high BVOC concentrations seemed to be one of the most favorable conditions to observe NPF at CAO in March 2015. NPF event days were characterized by either (1) a predominant anthropogenic influence (high concentrations of anthropogenic source tracers observed), (2) a predominant biogenic influence (high BVOC concentrations coupled with low anthropogenic tracer concentrations), (3) a mixed influence (high BVOC concentrations coupled with high anthropogenic tracer concentrations) and (4) a marine influence (both low BVOC and anthropogenic tracer concentrations). More pronounced NPF events were identified during mixed anthropogenic–biogenic conditions compared to the pure anthropogenic or biogenic ones, for the same levels of precursors. Analysis of a specific NPF period of the mixed influence type highlighted that BVOC interactions with anthropogenic compounds enhanced nucleation formation and growth of newly formed particles. During this period, the nucleation-mode particles may be formed by the combination of high H2SO4 and isoprene amounts, under favorable meteorological conditions (high temperature and solar radiation and low relative humidity) along with low CS. During the daytime, growth of the newly formed particles, not only sulfate but also oxygen-like organic aerosol (OOA) mass contributions, increased in the particle phase. High BVOC concentrations were observed during the night following NPF events, accompanied by an increase in CS and in semi-volatile OOA contributions, suggesting further BVOC contribution to aerosol nighttime growth by condensing onto pre-existing aerosols.

High occurrence of new particle formation events at the Maïdo high-altitude observatory (2150 m), Réunion (Indian Ocean)

Abstract. This study aims to report and characterise the frequent new particle formation (NPF) events observed at the Maïdo observatory, Réunion, a Southern Hemisphere site located at 2150 m (a.s.l.) and surrounded by the Indian Ocean. From May 2014 to December 2015, continuous aerosol measurements were made using both a differential mobility particle sizer (DMPS) and an air ion spectrometer (AIS) to characterise the NPF events down to the lowest particle-size scale. Carbon monoxide (CO) and black carbon (BC) concentrations were monitored, as well as meteorological parameters, in order to identify the conditions that were favourable to the occurrence of nucleation in this specific environment. We point out that the annual NPF frequency average (65 %) is one of the highest reported so far. Monthly averages show a bimodal variation in the NPF frequency, with a maximum observed during transition periods (autumn and spring). A high yearly median particle growth rate (GR) of 15.16 nm h−1 is also measured showing a bimodal seasonal variation with maxima observed in July and November. Yearly medians of 2 and 12 nm particle formation rates (J2 and J12) are 0.858 and 0.508 cm−3 s−1, respectively, with a seasonal variation showing a maximum during winter, that correspond to low temperature and RH typical of the dry season, but also to high BC concentrations. We show that the condensation sink exceeds a threshold value (1.04×10−3 s−1) with a similar seasonal variation than the one of the NPF event frequency, suggesting that the occurrence of the NPF process might be determined by the availability of condensable vapours, which are likely to be transported together with pre-existing particles from lower altitudes.

Laboratory verification of a new high flow differential mobility particle sizer, and field measurements in Hyytiälä

Measurement of atmospheric sub-10 nm nanoparticle number concentrations has been of substantial interest recently, which, however, is subject to considerable uncertainty. We report a laboratory characterization of a high flow differential mobility particle sizer (HFDMPS), which is based on the Half-mini type differential mobility analyzer (DMA) and nano condensation nuclei counter (A11), and show the first results from atmospheric observations. The HFDMPS utilizes the state-of-the-art aerosol technology, and is optimized for sub-10 nm particle size distribution measurements by a moderate resolution DMA, optimized and characterized low-loss particle sampling line and minimal dilution in the detector. We present an exhaustive laboratory calibration to the HFDMPS and compare the measured size data to the Hyytiälä long-term DMPS and Neutral cluster and ion spectrometer. The HFDMPS detects about two times higher 3–10 nm particle concentrations than the long-term DMPS, and the counting uncertainties are halved as compared to the long-term DMPS. The HFDMPS did not observe any sub-2.5 nm particles in Hyytiälä, and the reason for that was shown to be the inability of diethylene glycol to condense on such small biogenic particles. Last, we discuss the general implications of our results to the sub-10 nm DMPS based measurements.

Laboratory verification of Aerosol Diffusion Spectrometer and the application to ambient measurements of new particle formation

Information on the ambient aerosol number size distribution is essential to address various scientific questions related to aerosol particles in the atmosphere. However, due to the wide size and concentrations ranges of ambient aerosol particles, no single instrument alone is capable of measuring them all. Instruments based on different measurement principles are engaged in the measurement of atmospheric aerosols. Intercomparison of such instruments is necessary to cross-validate the reliability of obtained data. In this study, a verification of a Novosibirsk Aerosol Diffusion Spectrometer (ADS) in the size classification of aerosol particles was carried out in laboratory and via a field intercomparison with a Differential Mobility Particle Sizer (DMPS) and a Neutral cluster and Air Ion Spectrometer (NAIS). The laboratory experiments affirmed the good accuracy of the ADS on sizing and concentration measurement. The ADS was satisfactorily comparable with the DMPS and the NAIS for the measurement of ambient aerosols within the size range 3–200nm. The differences between condensation sinks derived from the ADS and DMPS measurements were smaller on days with new particle formation (NPF) than on non-NPF days. Similar formation rates and growth rates were acquired based on the DMPS, NAIS and ADS measurements, proving a reasonable ability of the ADS in measuring the concentrations and size distribution of nucleation-mode particles.

Submicrometer aerosols and excess CO as tracers for biomass burning air mass transport over southern Africa

This paper links surface measurements of biomass burning aerosols and trace gases with trajectory analysis to determine transport pathways for air masses with high and low concentrations. We interpret the long-term atmospheric monitoring record from a remote monitoring station in central southern Africa (North West Province, South Africa). Trace gas analyzers and a Differential Mobility Particle Sizer were used to measure ground level trace gas and submicron aerosol concentrations. Fire signatures were identified based on excess CO above average tropospheric levels, and episodes of enhanced particulate matter concentrations in the 10 to 840 nm size range. Thirty-six biomass burning plumes were reported; 7 had strong signals of excess CO, with ratios between 0.41 and 0.64, while 29 had weak signals ranging between 0.07 and 0.32. Pathways identified for the long-range transport of biomass burning aerosols were as follows: easterly (39% frequency), southwesterly (31%), recirculation (22%), and northerly (8%) flow patterns. CO and Aitken-mode aerosol number strengths were larger for fire emissions arriving in the easterly and southwesterly air masses than for recirculation and northerly air masses. Easterly and southwesterly flows were dominated by Aitken-mode aerosol, whereas accumulation-mode particles dominated in the recirculation and northerly flows. Findings identify biomass burning as a major source of Aitken-mode aerosols. Enhanced CO concentrations, combined with Aitken- and accumulation-mode particle number size distributions, are shown to provide a useful signature of plumes originating over regional biomass combustion events.

Measurement, growth types and shrinkage of newly formed aerosol particles at an urban research platform

Abstract. Budapest platform for Aerosol Research and Training (BpART) was created for advancing long-term on-line atmospheric measurements and intensive aerosol sample collection campaigns in Budapest. A joint study including atmospheric chemistry or physics, meteorology, and fluid dynamics on several-year-long data sets obtained at the platform confirmed that the location represents a well-mixed, average atmospheric environment for the city centre. The air streamlines indicated that the host and neighbouring buildings together with the natural orography play an important role in the near-field dispersion processes. Details and features of the airflow structure were derived, and they can be readily utilised for further interpretations. An experimental method to determine particle diffusion losses in the differential mobility particle sizer (DMPS) system of the BpART facility was proposed. It is based on CPC–CPC (condensation particle counter) and DMPS–CPC comparisons. Growth types of nucleated particles observed in 4 years of measurements were presented and discussed specifically for cities. Arch-shaped size distribution surface plots consisting of a growth phase followed by a shrinkage phase were characterised separately since they supply information on nucleated particles. They were observed in 4.5 % of quantifiable nucleation events. The shrinkage phase took 1 h 34 min in general, and the mean shrinkage rate with standard deviation was −3.8 ± 1.0 nm h−1. The shrinkage of particles was mostly linked to changes in local atmospheric conditions, especially in global radiation and the gas-phase H2SO4 concentration through its proxy, or to atmospheric mixing in few cases. Some indirect results indicate that variations in the formation and growth rates of nucleated particles during their atmospheric transport could be a driving force of shrinkage for particles of very small sizes and on specific occasions.

Multi-seasonal ultrafine aerosol particle number concentration measurements at the Gruvebadet observatory, Ny-Ålesund, Svalbard Islands

The object of this study was to investigate the different modal behavior of ultrafine aerosol particles collected at the Gruvebadet observatory located in Ny-Alesund (Svalbard Islands, 78°55′N, 11°56′E). Aerosol particle size distribution was measured in the size range from 10 to 470 nm typically from the beginning of spring to the beginning of fall during four (non-consecutive) years (2010, 2011, 2013 and 2014). The median concentration for the whole period taken into account was 214 particles cm−3, oscillating between the median maximum in July with a concentration of 257 particles cm−3 and a median minimum in April with 197 particles cm−3. The median total number concentration did not present a well-defined seasonal behavior, as shown by contrast looking at the sub/modal number concentration, where distinct trends appeared in the predominant accumulation concentration recorded during April/May and the preponderant concentration of Aitken particles during the summer months. Lastly, the short side-by-side spring 2013 campaign performed at the Zeppelin observatory with a differential mobility particle sizer was characterized by an aerosol concentration mean steady difference between the two instruments of around 14 %, thereby supporting the reliability of the device located at Gruvebadet.

Notably improved inversion of differential mobility particle sizer data obtained under conditions of fluctuating particle number concentrations

Abstract. The differential mobility particle sizer (DMPS) is designed for measurements of particle number size distributions. It performs a number of measurements while scanning over different particle sizes. A standard assumption in the data-processing (inversion) algorithm is that the size distribution remains the same throughout each scan. For a DMPS deployed in an urban area this assumption is likely to be violated most of the time, and the resulting size distribution data are unreliable. To improve the reliability, we developed a new algorithm using a statistical model in which the problematic assumption was replaced with more realistic smoothness assumptions, which were expressed through Gaussian process prior probabilities. We tested the model with data from a twin DMPS located at an urban background site in Helsinki and found that it provides size distribution data which are much more realistic. Furthermore, particle number concentrations extracted from the DMPS data were compared with data from a condensation particle counter. At 10 min resolution, the correlation for a period of 10 days was 0.984 with the new algorithm and 0.967 with the old one. Moreover, the time resolution was improved, and at 30 s resolution we obtained positive correlations for 89 % of the scans. Thus, the quality of the inverted data was clearly improved.

Aerosol size distribution seasonal characteristics measured in Tiksi, Russian Arctic

Abstract. Four years of continuous aerosol number size distribution measurements from the Arctic Climate Observatory in Tiksi, Russia, are analyzed. Tiksi is located in a region where in situ information on aerosol particle properties has not been previously available. Particle size distributions were measured with a differential mobility particle sizer (in the diameter range of 7–500 nm) and with an aerodynamic particle sizer (in the diameter range of 0.5–10 μm). Source region effects on particle modal features and number, and mass concentrations are presented for different seasons. The monthly median total aerosol number concentration in Tiksi ranges from 184 cm−3 in November to 724 cm−3 in July, with a local maximum in March of 481 cm−3. The total mass concentration has a distinct maximum in February–March of 1.72–2.38 μg m−3 and two minimums in June (0.42 μg m−3) and in September–October (0.36–0.57 μg m−3). These seasonal cycles in number and mass concentrations are related to isolated processes and phenomena such as Arctic haze in early spring, which increases accumulation and coarse-mode numbers, and secondary particle formation in spring and summer, which affects the nucleation and Aitken mode particle concentrations. Secondary particle formation was frequently observed in Tiksi and was shown to be slightly more common in marine, in comparison to continental, air flows. Particle formation rates were the highest in spring, while the particle growth rates peaked in summer. These results suggest two different origins for secondary particles, anthropogenic pollution being the important source in spring and biogenic emissions being significant in summer. The impact of temperature-dependent natural emissions on aerosol and cloud condensation nuclei numbers was significant: the increase in both the particle mass and the CCN (cloud condensation nuclei) number with temperature was found to be higher than in any previous study done over the boreal forest region. In addition to the precursor emissions of biogenic volatile organic compounds, the frequent Siberian forest fires, although far away, are suggested to play a role in Arctic aerosol composition during the warmest months. Five fire events were isolated based on clustering analysis, and the particle mass and cloud condensation nuclei number were shown to be somewhat affected by these events. In addition, during calm and cold months, aerosol concentrations were occasionally increased by local aerosol sources in trapping inversions. These results provide valuable information on interannual cycles and sources of Arctic aerosols.

Variability of air ion concentrations in urban Paris

Abstract. Air ion concentrations influence new particle formation and consequently the global aerosol as potential cloud condensation nuclei. We aimed to evaluate air ion concentrations and characteristics of new particle formation events (NPF) in the megacity of Paris, France, within the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric Pollution and climate effects, and Integrated tools for assessment and mitigation) project. We measured air ion number size distributions (0.8–42 nm) with an air ion spectrometer and fine particle number concentrations (> 6 nm) with a twin differential mobility particle sizer in an urban site of Paris between 26 June 2009 and 4 October 2010. Air ions were size classified as small (0.8–2 nm), intermediate (2–7 nm), and large (7–20 nm). The median concentrations of small and large ions were 670 and 680 cm−3, respectively, (sum of positive and negative polarities), whereas the median concentration of intermediate ions was only 20 cm−3, as these ions were mostly present during new particle formation bursts, i.e. when gas-to-particle conversion produced fresh aerosol particles from gas phase precursors. During peaks in traffic-related particle number, the concentrations of small and intermediate ions decreased, whereas the concentrations of large ions increased. Seasonal variations affected the ion population differently, with respect to their size and polarity. NPF was observed in 13 % of the days, being most frequent in spring and late summer (April, May, July, and August). The results also suggest that NPF was favoured on the weekends in comparison to workdays, likely due to the lower levels of condensation sinks in the mornings of weekends (CS weekdays 09:00: 18 × 10−3 s−1; CS weekend 09:00: 8 × 10−3 s−1). The median growth rates (GR) of ions during the NPF events varied between 3 and 7 nm h−1, increasing with the ion size and being higher on workdays than on weekends for intermediate and large ions. The median GR of small ions on the other hand were rather similar on workdays and weekends. In general, NPF bursts changed the diurnal cycle of particle number as well as intermediate and large ions by causing an extra peak between 09:00 and 14:00. On average, during the NPF bursts the concentrations of intermediate ions were 8.5–10 times higher than on NPF non-event days, depending on the polarity, and the concentrations of large ions and particles were 1.5–1.8 and 1.2 times higher, respectively. Because the median concentrations of intermediate ions were considerably higher on NPF event days in comparison to NPF non-event days, the results indicate that intermediate ion concentrations could be used as an indication for NPF in Paris. The results suggest that NPF was a source of ions and aerosol particles in Paris and therefore contributed to both air quality degradation and climatic effects, especially in the spring and summer.

Lung burden and deposition distribution of inhaled atmospheric urban ultrafine particles as the first step in their health risk assessment

Realistic median particle number size distributions were derived by a differential mobility particle sizer in a diameter range of 6–1000 nm for near-city background, city centre, street canyon and road tunnel environments in Budapest. Deposition of inhaled particles within airway generations of an adult woman was determined by a stochastic lung deposition model for sleeping, sitting, light and heavy exercise breathing conditions. Deposition fractions in the respiratory tract were considerable and constant for all physical activities with a mean of 56%. Mean deposition fraction in the extra-thoracic region averaged for the urban environments was decreasing monotonically from 26% for sleeping to 9.4% for heavy exercise. The mean deposition fractions in the tracheobronchial region were constant for the physical activities and urban environments with an overall mean of 12.5%, while the mean deposition fraction in the acinar region averaged for the urban locations increased monotonically with physical activity from 14.7% for sleeping to 34% for heavy exercise. The largest contribution of the acinar deposition to the lung deposition was 75%. The deposition rates in the lung were larger than in the extra-thoracic region, and the deposition rate in the lung was increasingly realised in the AC region by physical activity. It was the extra-thoracic region that received the largest surface density deposition rates; its loading was higher by 3 orders of magnitude than for the lung. Deposition fractions in the airway generations exhibited a distinct peak in the acinar region. The maximum of the curves was shifted to peripheral airway generations with physical activity. The shapes of the surface density deposition rate curves were completely different from those for the deposition rates, indicating that the first few airway generations received the highest surface loading in the lung.