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Properties of atmospheric black carbon (BC) particles were characterized during a field experiment at a rural background site (Melpitz, Germany) in February 2017. BC absorption at a wavelength of 870 nm was measured by a photoacoustic extinctiometer, and BC physical properties (BC mass concentration, core size distribution and coating thickness) were measured by a single-particle soot photometer (SP2). Additionally, a catalytic stripper was used to intermittently remove BC coatings by alternating between ambient and thermo-denuded conditions. From these data the mass absorption cross section of BC (MACBC) and its enhancement factor (EMAC) were inferred for essentially water-free aerosol as present after drying to low relative humidity (RH). Two methods were applied independently to investigate the coating effect on EMAC: a correlation method (MACBC, ambient vs. BC coating thickness) and a denuding method (MACBC, ambient vs. MACBC, denuded). Observed EMAC values varied from 1.0 to 1.6 (lower limit from denuding method) or ∼1.2 to 1.9 (higher limit from correlation method), with the mean coating volume fraction ranging from 54 % to 78 % in the dominating mass equivalent BC core diameter range of 200–220 nm. MACBC and EMAC were strongly correlated with coating thickness of BC. By contrast, other potential drivers of EMAC variability, such as different BC sources (air mass origin and absorption Ångström exponent), coating composition (ratio of inorganics to organics) and BC core size distribution, had only minor effects. These results for ambient BC measured at Melpitz during winter show that the lensing effect caused by coatings on BC is the main driver of the variations in MACBC and EMAC, while changes in other BC particle properties such as source, BC core size or coating composition play only minor roles at this rural background site with a large fraction of aged particles. Indirect evidence suggests that potential dampening of the lensing effect due to unfavorable morphology was most likely small or even negligible.

To characterize the role of dew water for the ground surface HONO distribution, nitrous acid (HONO) measurements with a Monitor for AeRosols and Gases in ambient Air (MARGA) and a LOng Path Absorption Photometer (LOPAP) instrument were performed at the Leibniz Institute for Tropospheric Research (TROPOS) research site in Melpitz, Germany, from 19 to 29 April 2018. The dew water was also collected and analyzed from 8 to 14 May 2019 using a glass sampler. The high time resolution of HONO measurements showed characteristic diurnal variations that revealed that (i) vehicle emissions are a minor source of HONO at Melpitz station; (ii) the heterogeneous conversion of NO2 to HONO on the ground surface dominates HONO production at night; (iii) there is significant nighttime loss of HONO with a sink strength of 0.16±0.12 ppbv h−1; and (iv) dew water with mean NO2- of 7.91±2.14 µg m−2 could serve as a temporary HONO source in the morning when the dew droplets evaporate. The nocturnal observations of HONO and NO2 allowed the direct evaluation of the ground uptake coefficients for these species at night: γNO2→HONO=2.4×10-7 to 3.5×10-6, γHONO,ground=1.7×10-5 to 2.8×10-4. A chemical model demonstrated that HONO deposition to the ground surface at night was 90 %–100 % of the calculated unknown HONO source in the morning. These results suggest that dew water on the ground surface was controlling the temporal HONO distribution rather than straightforward NO2–HONO conversion. This can strongly enhance the OH reactivity throughout the morning time or in other planted areas that provide a large amount of ground surface based on the OH production rate calculation.

A unique data set derived from remote sensing, airborne, and ground-based in situ measurements is presented. This measurement report highlights the known complexity of comparing multiple aerosol optical parameters examined with different approaches considering different states of humidification and atmospheric aerosol concentrations. Mie-theory-based modeled aerosol optical properties are compared with the respective results of airborne and ground-based in situ measurements and remote sensing (lidar and photometer) performed at the rural central European observatory at Melpitz, Germany. Calculated extinction-to-backscatter ratios (lidar ratios) were in the range of previously reported values. However, the lidar ratio is a function of the aerosol type and the relative humidity. The particle lidar ratio (LR) dependence on relative humidity was quantified and followed the trend found in previous studies. We present a fit function for the lidar wavelengths of 355, 532, and 1064 nm with an underlying equation of fLR(RH, γ(λ))=fLR (RH=0, λ) x (1-RH)⁻γ⁽λ⁾, with the derived estimates of γ(355 nm) = 0.29 (±0.01), γ(532 nm) = 0.48 (±0.01), and γ(1064 nm) = 0.31 (±0.01) for central European aerosol. This parameterization might be used in the data analysis of elastic-backscatter lidar observations or lidar-ratio-based aerosol typing efforts. Our study shows that the used aerosol model could reproduce the in situ measurements of the aerosol particle light extinction coefficients (measured at dry conditions) within 13 %. Although the model reproduced the in situ measured aerosol particle light absorption coefficients within a reasonable range, we identified many sources for significant uncertainties in the simulations, such as the unknown aerosol mixing state, brown carbon (organic material) fraction, and the unknown aerosol mixing state wavelength-dependent refractive index. The modeled ambient-state aerosol particle light extinction and backscatter coefficients were smaller than the measured ones. However, depending on the prevailing aerosol conditions, an overlap of the uncertainty ranges of both approaches was achieved.

The mass concentration of black carbon (BC) particles in the atmosphere has traditionally been quantified with two methods: as elemental carbon (EC) concentrations measured by thermal–optical analysis and as equivalent black carbon (eBC) concentrations when BC mass is derived from particle light absorption coefficient measurements. Over the last decade, ambient measurements of refractory black carbon (rBC) mass concentrations based on laser-induced incandescence (LII) have become more common, mostly due to the development of the Single Particle Soot Photometer (SP2) instrument. In this work, EC and rBC mass concentration measurements from field campaigns across several background European sites (Palaiseau, Bologna, Cabauw and Melpitz) have been collated and examined to identify the similarities and differences between BC mass concentrations measured by the two techniques. All EC concentration measurements in PM2.5 were performed with the EUSAAR-2 thermal–optical protocol. All rBC concentration measurements were performed with SP2 instruments calibrated with the same calibration material as recommended in the literature. The observed values of median rBC-to-EC mass concentration ratios on the single-campaign level were 0.53, 0.65, 0.97, 1.20 and 1.29, respectively, and the geometric standard deviation (GSD) was 1.5 when considering all data points from all five campaigns. This shows that substantial systematic bias between these two quantities occurred during some campaigns, which also contributes to the large overall GSD. Despite considerable variability in BC properties and sources across the whole dataset, it was not possible to clearly assign reasons for discrepancies to one or the other method, both known to have their own specific limitations and uncertainties. However, differences in the particle size range covered by these two methods were identified as one likely reason for discrepancies. Overall, the observed correlation between rBC and EC mass reveals a linear relationship with a constant ratio, thus providing clear evidence that both methods essentially quantify the same property of atmospheric aerosols, whereas systematic differences in measured absolute values by up to a factor of 2 can occur. This finding for the level of agreement between two current state-of-the-art techniques has important implications for studies based on BC mass concentration measurements, for example for the interpretation of uncertainties in inferred BC mass absorption coefficient values, which are required for modeling the radiative forcing of BC. Homogeneity between BC mass determination techniques is also very important for moving towards a routine BC mass measurement for air quality regulations.

Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiaġvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13–4 µm projected area diameter) and real-time single-particle mass spectrometry (0.2–1.5 µm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 % of the study), our results show that fresh sea spray aerosol contributed  ∼ 20 %, by number, of particles between 0.13 and 0.4 µm, 40–70 % between 0.4 and 1 µm, and 80–100 % between 1 and 4 µm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13–1 µm) combustion-derived particles (20–50 % organic carbon, by number; 5–10 % soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 µm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm−3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations.

Black carbon (BC) is one of the most harmful substances within traffic emissions, contributing considerably to urban pollution. Nevertheless, it is not explicitly regulated and the official laboratory derived emission factors are barely consistent with real world emissions. However, realistic emission factors (EFs) are crucial for emission, exposure, and climate modelling. A unique dataset of 10 years (2009–2018) of roadside and background measurements of equivalent black carbon (eBC) concentration made it possible to estimate real world traffic EFs and observe their change over time. The pollutant dispersion was modelled using the Operational Street Pollution Model (OSPM). The EFs for eBC are derived for this specific measurement site in a narrow but densely trafficked street canyon in Leipzig, Germany. The local conditions and fleet composition can be considered as typical for an inner-city traffic scenario in a Western European city. The fleet is composed of 22% diesel and 77% petrol cars in the passenger car segment, with an unknown proportion of direct injection engines. For the mixed fleet the eBC EF was found to be 48 mg km−1 in the long-term average. Accelerated by the introduction of a low emission zone, the EFs decreased over the available time period from around 70 mg km−1 to 30–40 mg km−1. Segregation into light (<3.5 t) and heavy (>3.5 t) vehicles resulted in slightly lower estimates for the light vehicles than for the mixed fleet, and one order of magnitude higher values for the heavy vehicles. The found values are considerably higher than comparable emission standards for particulate matter and even the calculations of the Handbook Emission Factors for Road Transport (HBEFA), which is often used as emission model input.

Anthropogenic emissions are dominant contributors to air pollution. Consequently, mitigation policies have been attempted since the 1990s in Europe to reduce pollution by anthropogenic emissions. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon (BC) and sub-micrometre aerosol particles. In this study, long-term trends of atmospheric particle number concentrations (PNCs) and equivalent BC (eBC) mass concentration over a 10-year period (2009–2018) were determined for 16 GUAN sites ranging from roadside to high Alpine environments. Overall, statistically significant decreasing trends are found for most of these parameters and environments in Germany. The annual relative slope of eBC mass concentration varies between −13.1 % and −1.7 % per year. The slopes of the PNCs vary from −17.2 % to −1.7 %, −7.8 % to −1.1 %, and −11.1 % to −1.2 % per year for 10–30, 30–200, and 200–800 nm size ranges, respectively. The reductions in various anthropogenic emissions are found to be the dominant factors responsible for the decreasing trends of eBC mass concentration and PNCs. The diurnal and seasonal variations in the trends clearly show the effects of the mitigation policies for road transport and residential emissions. The influences of other factors such as air masses, precipitation, and temperature were also examined and found to be less important or negligible. This study proves that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales. It also suggests that a long-term aerosol measurement network at multi-type sites is an efficient and necessary tool for evaluating emission mitigation policies.

Ambient aerosol has been identified as a major pollutant affecting human health. Standards to reduce particles mass concentrations have therefore been established in many countries. Recent studies suggest that the number concentration of aerosol particles, which is dominated by the ultrafine size range smaller than 100 nm in diameter, may be independently associated with health effects. Currently, epidemiological evidence for such effects is conflicting. We have measured aerosol size distributions at two stations (urban background, street canyon) located at a distance of 1.5 km for a time period of 1 year. Number concentrations and particle size distributions at both sites were significantly different. Short-term correlation between the two sites was weak for individual measurements of number concentrations and size bins of ultrafine particles (0.19–0.46). Correlation coefficients for hourly and daily averages in selected size ranges ranged from 0.35 to 0.46. On the other hand, the correlation coefficient for daily average particle volume concentrations was found to be 0.67. About 10% to 20% of the population of European cities lives close to roads with traffic densities comparable to our site. The underestimation of the exposure of a considerable part of a study population may therefore severely influence the outcome of epidemiological studies focused on health effects associated with ultrafine particles. A single background measurement site may not be sufficient for exposure assessment in these studies without taking spatial and temporal variability into account.

Few studies investigated residential particle concentration levels with a full picture of aerosol particles from 10 nm to 10 µm size range with size-resolved information, and none was performed in central Europe in the long-term in multiple homes. To capture representative diurnal and seasonal patterns of exposure to particles, and investigate the driving factors to their variations, measurements were performed in 40 homes for around two weeks each in Leipzig and Berlin, Germany. These over 500 days’ measurements combined PM 10 and PM 2.5 mass concentrations, particle number concentration and size distribution (PNC and PNSD, 10–800 nm), CO 2 concentration, and residential activities diary into a unique dataset. Natural ventilation was dominated, the mean ventilation rate calculated from CO 2 measurements was 0.2 h –1 and 3.7 h –1 with closed and opened windows, respectively. The main findings of this study showed that, the residents in German homes were exposed to a significantly higher mass concentration of coarse particles than outdoors, thus indoor exposure to coarse particles cannot be described by outdoors. The median indoor PNC diurnal cycles were generally lower than outdoors (median I/O ratio 0.69). However, indoor exposure to particles was different in the cold and warm season. In the warm season, due to longer opening window periods, indoor sources’ contribution was weakened, which also resulted in the indoor PNC and PNSD being very similar to the outdoors. In the cold season, indoor sources caused strong peaks of indoor PNC that exceeded outdoors, along with the relatively low penetration factor - 0.5 for all size ranges, and indoor particle losses, which was particularly effective in reducing the ultrafine PNC, resulting in a different particle exposure load than outdoors. This study provides a detailed understanding of residential particle exposure in multiple homes, facilitating future studies to assess health effects in residential environments.

Although new particle formation (NPF) events have been studied extensively for some decades, the mechanisms that drive their occurrence and development are yet to be fully elucidated. Laboratory studies have done much to elucidate the molecular processes involved in nucleation, but this knowledge has yet to be conclusively linked to NPF events in the atmosphere. There is great difficulty in successful application of the results from laboratory studies to real atmospheric conditions due to the diversity of atmospheric conditions and observations found, as NPF events occur almost everywhere in the world without always following a clearly defined trend of frequency, seasonality, atmospheric conditions, or event development. The present study seeks common features in nucleation events by applying a binned linear regression over an extensive dataset from 16 sites of various types (combined dataset of 85 years from rural and urban backgrounds as well as roadside sites) in Europe. At most sites, a clear positive relation with the frequency of NPF events is found between the solar radiation intensity (up to R2=0.98), temperature (up to R2=0.98), and atmospheric pressure (up to R2=0.97), while relative humidity (RH) presents a negative relation (up to R2=0.95) with NPF event frequency, though exceptions were found among the sites for all the variables studied. Wind speed presents a less consistent relationship, which appears to be heavily affected by local conditions. While some meteorological variables (such as the solar radiation intensity and RH) appear to have a crucial effect on the occurrence and characteristics of NPF events, especially at rural sites, it appears that their role becomes less marked at higher average values. The analysis of chemical composition data presents interesting results. Concentrations of almost all chemical compounds studied (apart from O3) and the condensation sink (CS) have a negative relationship with NPF event frequency, though areas with higher average concentrations of SO2 had higher NPF event frequency. Particulate organic carbon (OC), volatile organic compounds (VOCs), and particulate-phase sulfate consistently had a positive relation with the growth rate of the newly formed particles. As with some meteorological variables, it appears that at increased concentrations of pollutants or the CS, their influence upon NPF frequency is reduced.