Estimating the contribution of photochemical particle formation to ultrafine particle number averages in an urban atmosphere

Ultrafine particles (UFPs, diameter < 100 nm) have gained major attention in the environmental health discussion due to a number of suspected health effects. Observations of UFPs in urban air reveal the presence of several, time-dependent particle sources. In order to attribute measured UFP number concentrations to different source type contributions, we analyzed observations collected at a triplet of observation sites (roadside, urban background, rural) in the city of Leipzig, Germany. Photochemical new particle formation (NPF) events can be the overwhelming source of UFP particles on particular days, and were identified on the basis of characteristic patterns in the particle number size distribution data. A subsequent segmentation of the diurnal cycles of UFP concentration yielded a quantitative contribution of NPF events to daily, monthly, and annual mean values. At roadside, we obtained source contributions to the annual mean UFP number concentration (diameter range 5–100 nm) for photochemical NPF events (7%), local traffic (52%), diffuse urban sources (20%), and regional background (21%). The relative contribution of NPF events rises when moving away from roadside to the urban background and rural sites (14 and 30%, respectively). Their contribution also increases when considering only fresh UFPs (5–20 nm) (21% at the urban background site), and conversely decreases when considering UFPs at bigger sizes (20–100 nm) (8%). A seasonal analysis showed that NPF events have their greatest importance on UFP number concentration in the months May–August, accounting for roughly half of the fresh UFPs (5–20 nm) at the urban background location. The simplistic source apportionment presented here might serve to better characterize exposure to ambient UFPs in future epidemiological studies

Non-volatile residuals of newly formed atmospheric particles in the boreal forest

The volatility of sub-micrometer atmospheric aerosol particles was studied in a rural background environment in Finland using a combination of a heating tube and a scanning mobility particle sizer. The analysis focused on nanoparticles formed through nucleation which were subsequently observed during their growth in the diameter range between 5 and 60 nm. During the 6 days of new particle formation shown in detail, the concentrations of newly formed particles increased up to 10 000 cm−3. The number of nucleation mode particles measured after volatilization in the heating tube at 280°C was up to 90% of the total number under ambient conditions. Taking into account the absolute accuracy of the size distribution measurements, all ambient particles found in the rural atmosphere could have a non-volatile core after volatilization at 280°C. As the regional new particle formation events developed over time as a result of further vapor condensation, the newly formed particles grew at an average growth rate of 2.4±0.3 nm h−1. Importantly, the non-volatile cores of nucleation mode particles were also observed to grow over time, however, at a lower average growth rate of 0.6±0.3 nm h−1. One implication of the volatility analysis is that the newly formed particles, which have reached ambient diameters of 15 nm, are unlikely to consist of sulfuric acid, ammonium sulfate, and water alone. A relatively constant ratio between the growth rate of the ambient particles as well as their non-volatile cores indicates that non-volatile matter is formed only gradually in the growing particles. The non-volatile fraction of the particles showed some correlation with the ambient temperature. The composition and formation mechanism of this non-volatile material in nucleation mode particles are, to date, not known

The atmospheric aerosol over Siberia, as seen from the 300 m ZOTTO tower

This report describes a unique setup for aerosol measurements at the new long-term Tall Tower monitoring facility near Zotino, Siberia (ZOTTO). Through two inlets at 50 and 300 m aerosol particle number size distributions are measured since September 2006 in the size range 15–835 nanometer dry diameter. Until the end of May 2007 total number (N300) concentrations at 300 m height ranged between 400 cm-3 (5%) and 4000 cm-3 (95%) with a median of 1200 cm-3, which is rather high for a nearly uninhabited boreal forest region during the low productivity period of the year. Fitting 1-h average distributions with a maximum of four lognormal functions yielded frequent ultrafine modes below 20 nm at 50 m height than at 300 m, whereas the latter height more frequently showed an aged nucleation mode near 30 nm. The positions of Aitken (≈80 nm) and accumulation modes (≈210 nm) were very similar at both inlet heights, the very sharp latter one being the most frequent of all modes. The encouraging first results let us expect exciting newfindings during the summer period with frequent forest fires and secondary particle sources from vegetation emissions

Correlation between traffic density and particle size distribution in a street canyon and the dependence on wind direction

Combustion of fossil fuel in gasoline and diesel powered vehicles is a major source of aerosol particles in a city. In a street canyon, the number concentration of particles smaller than 300 nm in diameter, which can be inhaled and cause serious health effects, is dominated by particles originating from this source. In this study we measured both, particle number size distribution and traffic density continuously in a characteristic street canyon in Germany for a time period of 6 months. The street canyon with multistory buildings and 4 traffic lanes is very typical for larger cities. Thus, the measurements also are representative for many other street canyons in Europe. In contrast to previous studies, we measured and analyzed the particle number size distribution with high size resolution using a Twin Differential Mobility Analyzer (TDMPS). The measured size range was from 3 to 800 nm, separated into 40 size channels. Correlation coefficients between particle number concentration for integrated size ranges and traffic counts of 0.5 were determined. Correlations were also calculated for each of the 40 size channels of the DMPS system, respectively. We found a maximum of the correlation coefficients for nucleation mode particles in the size range between 10 and 20 nm in diameter. Furthermore, correlations between traffic and particles in dependence of meteorological data were calculated. Relevant parameters were identified by a multiple regression method. In our experiment only wind parameters have influenced the particle number concentration significantly. High correlation coefficients (up to 0.8) could be observed in the lee side of the street canyon for particles in the range between 10 and 100 nm in diameter. These values are significantly higher than correlation coefficients for other wind directions and other particle sizes. A minimum was found in the luff side of the street. These findings are in good agreement with theory of fluid dynamics in street canyons

Analysis of exceedances in the daily PM10 mass concentration (50 μg m−3) at a roadside station in Leipzig, Germany

Five years of PM10 and PM2.5 ambient air measurements at a roadside, an urban, and a regional background site in Leipzig (Germany) were analyzed for violations of the legal PM10 limit value (EC, 1999). The annual mean PM10 concentrations at the three sites were well below the legal threshold of 40 μg m−3 (32.6, 22.0 and 21.7 μg m−3, respectively). At roadside, the daily maximum value of 50 μg m−3 was exceeded on 232 days (13% of all days) in 2005–2009, which led to a violation of the EC directive in three out of five years. We analysed the meteorological factors and local source contributions that eventually led to the exceedances of the daily limit value. As noted in other urban environments before, most exceedance days were observed in the cold season. Exceedance days were most probable under synoptic situations characterised by stagnant winds, low temperatures and strong temperature inversions in winter time. However, these extreme situations accounted for only less than half of the exeedance days. We also noticed a significant number of exceedance days that occurred in the cold season under south-westerly winds, and in the warm season in the presence of easterly winds. Our analysis suggests that local as well as regional sources of PM are equally responsible for exceedances days at the roadside site. The conclusion is that a combined effort of local, national and international reduction measures appears most likely to avoid systematic exceedances of the daily limit value in the future

Correlation between traffic density and particle size distribution in a street canyon and the dependence on wind direction

International audienceCombustion of fossil fuel in gasoline and diesel powered vehicles is a major source of aerosol particles in a city. In a street canyon, the number concentration of particles smaller than 300 nm in diameter, which can be inhaled and cause serious health effects, is dominated by particles originating from this source. In this study we measured both, particle number size distribution and traffic density continuously in a characteristic street canyon in Germany for a time period of 6 months. The street canyon with multistory buildings and 4 traffic lanes is very typical for larger cities. Thus, the measurements also are representative for many other street canyons in Europe. In contrast to previous studies, we measured and analyzed the particle number size distribution with high size resolution using a Twin Differential Mobility Analyzer (TDMPS). The measured size range was from 3 to 800 nm, separated into 40 size channels. Correlation coefficients between particle number concentration for integrated size ranges and traffic counts of 0.5 were determined. Correlations were also calculated for each of the 40 size channels of the DMPS system, respectively. We found a maximum of the correlation coefficients for nucleation mode particles in the size range between 10 and 20 nm in diameter. Furthermore, correlations between traffic and particles in dependence of meteorological data were calculated. Relevant parameters were identified by a multiple regression method. In our experiment only wind parameters have influenced the particle number concentration significantly. High correlation coefficients (up to 0.8) could be observed in the lee side of the street canyon for particles in the range between 10 and 100 nm in diameter. These values are significantly higher than correlation coefficients for other wind directions and other particle sizes. A minimum was found in the luff side of the street. These findings are in good agreement with theory of fluid dynamics in street canyons

Particle number emission rates of aerosol sources in 40 German households and their contributions to ultrafine and fine particle exposure

More representative data on source-specific particle number emission rates and associated exposure in European households are needed. In this study, indoor and outdoor particle number size distributions (10–800 nm) were measured in 40 German households under real-use conditions in over 500 days. Particle number emission rates were derived for around 800 reported indoor source events. The highest emission rate was caused by burning candles (5.3 × 1013 h−1). Data were analyzed by the single-parameter approach (SPA) and the indoor aerosol dynamics model approach (IAM). Due to the consideration of particle deposition, coagulation, and time-dependent ventilation rates, the emission rates of the IAM approach were about twice as high as those of the SPA. Correction factors are proposed to convert the emission rates obtained from the SPA approach into more realistic values. Overall, indoor sources contributed ~ 56% of the daily-integrated particle number exposure in households under study. Burning candles and opening the window leads to seasonal differences in the contributions of indoor sources to residential exposure (70% and 40% in the cold and warm season, respectively). Application of the IAM approach allowed to attribute the contributions of outdoor particles to the penetration through building shell and entry through open windows (26% and 15%, respectively). © 2020 John Wiley & Sons A/S. Published by John Wiley & Sons Lt

A fast and easy-to-implement inversion algorithm for mobility particle size spectrometers considering particle number size distribution information outside of the detection range

Multiple-charge inversion is an essential procedure to convert the raw mobility distributions recorded by mobility particle size spectrometers, such as the DMPS or SMPS (differential or scanning mobility particle sizers), into true particle number size distributions. In this work, we present a fast and easy-to-implement multiple-charge inversion algorithm with sufficient precision for atmospheric conditions, but extended functionality. The algorithm can incorporate size distribution information from sensors that measure beyond the upper sizing limit of the mobility spectrometer, such as an aerodynamic particle sizer (APS) or an optical particle counter (OPC). This feature can considerably improve the multiple-charge inversion result in the upper size range of the mobility spectrometer, for example, when substantial numbers of coarse particles are present. The program also yields a continuous size distribution from both sensors as an output. The algorithm is able to calculate the propagation of measurement errors, such as those based on counting statistics, into on the final particle number size distribution. As an additional aspect, the algorithm can perform all inversion steps under the assumption of non-spherical particle shape, including constant or size-dependent shape factors

Size-segregated chemical, gravimetric and number distribution-derived mass closure of the aerosol in Sagres, Portugal during ACE-2

During the ACE-2 field campaign in the summer of 1997 an intensive, ground-based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3-way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically-determined mass with both number distribution-derived (slope=1.23/1.09; R2>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R2=0.79) for particles smaller than 3 mm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R2=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size-segregated mass fractions can be explained by the measurement uncertainties. However, the number distributionderived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS