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Abstract: A new method based on the combination of a differential mobility analyser (DMA) and aerodynamic particle sizer (APS) is presented, to measure the aerodynamic hygroscopic growth factor of aerosol particles around one micrometer in size. The DMA is used as a filter, selecting a size fraction of the ambient aerosol. One half of the selected monodisperse aerosol is sized in dry state in a first APS, while the second half of the aerosol is humidified, and then sized in a second APS. By comparing the particle size distributions measured in the first and second APS, the hygroscopic growth factor can be derived as a function of relative humidity (RH). Hygroscopic growth factors can be measured at RHs up to 90%. Particle modes of different hygroscopicity can be distinguished, giving information on the mixing state and the fraction of more and less hygroscopic particles. The system was tested and characterised in the laboratory, using inorganic salt particles of known hygroscopic growth behaviour. It agreed with growth curves given in the literature, within the measurement uncertainty. [Copyright &y& Elsevier]

Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs , single-scattering albedo SSA, and mass absorption cross-section MAC BC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100 nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25 % uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10 % for particles with dp,V between 60–160 nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14 nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC. [ABSTRACT FROM AUTHOR]

The oceanic emission of dimethyl sulfide (DMS) plays a vital role in the Earth's climate system and constitutes a substantial source of uncertainty when evaluating aerosol radiative forcing. Currently, the widely used monthly climatology of sea surface DMS concentration falls short of meeting the requirement for accurately simulating DMS-derived aerosols with chemical transport models. Hence, there is an urgent need for a high-resolution, multi-year global sea surface DMS dataset. Here we develop an artificial neural network ensemble model that uses nine environmental factors as input features and captures the variability of the DMS concentration across different oceanic regions well. Subsequently, a global sea surface DMS concentration and flux dataset (1° × 1°) with daily resolution spanning from 1998 to 2017 is established. According to this dataset, the global annual average concentration was ∼ 1.71 nM, and the annual total emissions were ∼ 17.2 Tg S yr -1 , with ∼ 60 % originating from the Southern Hemisphere. While overall seasonal variations are consistent with previous DMS climatologies, notable differences exist in regional-scale spatial distributions. The new dataset enables further investigations into daily and decadal variations. Throughout the period 1998–2017, the global annual average concentration exhibited a slight decrease, while total emissions showed no significant trend. The DMS flux from our dataset showed a stronger correlation with the observed atmospheric methanesulfonic acid concentration compared to those from previous monthly climatologies. Therefore, it can serve as an improved emission inventory of oceanic DMS and has the potential to enhance the simulation of DMS-derived aerosols and associated radiative effects. The new DMS gridded products are available at https://doi.org/10.5281/zenodo.11879900 (Zhou et al., 2024). [ABSTRACT FROM AUTHOR]

Ultrafine particles (UFP) pose a risk to human health, but due to the multitude of sources and fast transformation in the urban atmosphere, quantifying the exposure is challenging. Furthermore, physical properties of aerosol particles depend on the particle size. Statistical models are used to quantify spatial and temporal variation of UFP, but rarely used for particle number size distribution (PNSD). The aim of the study was to establish an interpretable statistical model capturing spatial and temporal variation of urban PNSDs using generalized additive models (GAM) and multivariate adaptive regression spline models (MARS). These algorithms automatically fit interpretable, non-linear marginal function to represent relationships between explanatory and response variables. Three different approaches were evaluated to cope with the multidimensionality of the PNSD data (20–800 nm, 34 size bins): a generalized additive model for the particle number concentration (PNC) of every individual size bin (GAM bins), a generalized additive model for the parameters of the PNSD function (GAM pams) and a multivariate adaptive regression spline model for the PNC of every size bin (MARS bins). Reanalysis data of meteorological quantities, urban geometry parameters and approximated traffic counts were used as explanatory variables. Marginal functions of the final models could be attributed to major processes that contribute to spatial and temporal variation of the PNSD, i.e. emissions from vehicle traffic, transport, dilution, accumulation, deposition and new particle formation. Cross-validation coefficients of determination ranged between 0.27 and 0.48 for most size bins. Nonetheless, the modelling approaches resulted in similar root mean square errors (RMSE) and mean absolute error (MAE). Though direct spatial transferability of the models is limited, the presented approaches may be useful for estimating ambient exposure to particles. Image 1 • GAM and MARS algorithms were used on urban particle number size distributions (PNSD). • Three approaches were evaluated to cope with the multidimensionality of PNSD data. • Reanalysis data, urban geometry and traffic were used as explanatory variables. • The models capture important processes involving spatio-temporal PNSD variation. • Cross-validation R2 ranged between 0.27 and 0.48 for most size bins. [ABSTRACT FROM AUTHOR]

Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parametrization schemes for the optical properties of BC using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. In the first step, the modeling techniques were examined for bare BC particles, and in the second step, for BC particles with organic material. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. The BC fractal aggregate is usually modelled using monodispersed particles since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the discrepancy between modelled and measured particle light absorption coefficient to 10%, for particles with volume mean mobility diameters between 60-160 nm. However, for particles larger than 100 nm, the Absorption Ångström Exponent (AAE) calculated by using a spherical morphology was more consistent with measured value. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 to 2; mim between 0.50 to 1; Df from 1.7 to 1.9, and app between 10 to 14 nm. Overall, this study provides experimental support for emphasizing the use of an appropriate size representation (polydisperse size method) and an appropriate morphological representation (aggregate morphology) for optical modelling and parametrization scheme development of BC. [ABSTRACT FROM AUTHOR]

Fabricates nanometer sized columns of indium phosphide (InP) by applying aerosol and plasma etching techniques. Deposition of well-defined particles of silver; Production of silver particles through homogeneous nucleation out of silver vapor saturated nitrogen gas; Transfer of the silver particles into the InP material.

There is a gap between the need for city-wide air-quality simulations considering the intra-urban variability and mircoscale dispersion features and the computational capacities that conventional urban microscale models require. This gap can be bridged by targeting model applications on the gray zone situated between the mesoscale and large-eddy scale. The urban dispersion model CAIRDIO is a new contribution to the class of computational-fluid dynamics models operating in this scale range. It uses a diffuse-obstacle boundary method to represent buildings as physical obstacles at gray-zone resolutions in the order of tens of meters. The main objective of this approach is to find an acceptable compromise between computationally inexpensive grid sizes for spatially comprehensive applications and the required accuracy in the description of building and boundary-layer effects. For this purpose, CAIRDIO is applied in dispersion simulation of black carbon and particulate matter for an entire mid-size city using an uniform horizontal resolution of 40 m in this paper. For evaluation, the simulation results are compared with measurements from 5 operational air monitoring stations, which are representative for the urban background and high-traffic roads, respectively. Moreover, the comparison includes the mesoscale host simulation, which provides the boundary conditions. The temporal variability of the concentration measurements at the background sites was largely influenced only by the characteristics of the mixing layer. As a consequence, the model results were not significantly dependent on spatial resolution, so that the mesoscale simulation also performed reasonably well. At the traffic sites, however, concentrations were in addition markedly influenced by the proximity to road-traffic sources and the surrounding building environment. Here, the mesoscale simulation indiscriminately reproduced almost the same urban-background profiles, which resulted in a large positive model bias. On the other hand, the CAIRDIO simulation was able to respond to the significantly amplified diurnal variability with its pronounced rush-hour peaks. This resulted in a consistent improvement of the model deviation to mea- surements compared to the mesoscale simulation. Nevertheless, discrepancies to measurements remain in the 40 m-CAIRDIO simulation, e.g., an underestimation of peak concentrations at two traffic sites inside narrow street canyons. To further research resolution sensitivity, the horizontal grid spacing of locally nested CAIRDIO domains is refined down to 5 m. While for the street canyons the representation of peak concentrations can be improved using horizontal grid spacings of up to 10 m, no further improvements beyond this resolution can be observed. This suggests that the too low peak concentrations with the default grid spacing of 40 m result from an inadequate representation of the traffic emissions inside narrow street canyons. If the total gain in accuracy due to the grid refinements is put in relation to the remaining model error, the improvements are only modest. In conclusion, the proposed gray-scale modeling is a promising downscaling approach for urban air-quality applications. Nevertheless, the results also show that aspects other than the actual resolution of flow patterns and numerical effects can determine the simulations at the urban microscale. [ABSTRACT FROM AUTHOR]

The oceanic emission of dimethyl sulfide (DMS) plays a vital role in the Earth's climate system and is a significant source of uncertainty in aerosol radiative forcing. Currently, the widely used monthly climatology of sea surface DMS concentration cannot meet the requirement for accurately simulating DMS-derived aerosols by chemical transport models. Thus, there is an urgent need to construct a global sea surface DMS dataset with high time resolution spanning multiple years. Here we develop an artificial neural network ensemble model based on 9 environmental factors, which demonstrate high accuracy and generalization in predicting DMS concentrations. Subsequently, a global sea surface DMS concentration and flux dataset (1°×1°) with daily resolution covering the period from 1998 to 2017 is established. According to this dataset, the global annual average concentration was ~1.82 nM, and the annual total emission was ~17.9 TgS yr–1, with ~60 % originating from the southern hemisphere. While overall seasonal variations are consistent with previous DMS climatologies, notable differences exist in regional-scale spatial distributions. The new dataset enables further investigation of daily and decadal variations. During 1998–2017, the global annual average concentration exhibited a slight decrease, while total emissions showed no significant trend. Benefiting from the incorporation of daily and interannual variation information, the DMS flux from our dataset showed a much stronger correlation with observed atmospheric methanesulfonic acid concentration compared to those from previous monthly climatologies. As a result, it can serve as an improved emission inventory of oceanic DMS and has the potential to enhance the simulation of DMS-derived aerosols and associated radiative effects. [ABSTRACT FROM AUTHOR]

The present study is based on hourly aerosol particle and ancillary data taken at three stations in Northeastern Germany 150–200 km apart in the years 2009 through 2015 in order to investigate systematic process related differences that might show up when connecting their data with forward and backward air mass trajectories. The analysis of changes in the atmospheric aerosol during air mass transport between the stations focused on two low-pollution-to-high-pollution pathways of similar distance around 200 km. Despite rather different initial size distributions the increases in total concentration of particle number, volume, and black carbon agreed within 15%. Systematic variations were found in the different concentration increases as a function of time of day at which an interstation air mass transport took place that could be explained with related source and transport processes. With Radar-based precipitation data at the stations and along connecting trajectories sub-cloud particle scavenging was investigated. At each station sub-cloud particle scavenging coefficients were determined as a function of particle size between 10 and 700 nm diameter, and as a function of precipitation sums. Median particle scavenging coefficients taken over the central part of the size range of the study strongly increased between 0.2 and 1 mm of precipitation and then planed out towards higher precipitation values. With the particle scavenging coefficients determined at the individual stations and precipitation data along connecting trajectories the sub-cloud particle scavenging analysis was extended to wet scavenging along the transport paths yielding median sub-cloud scavenging ratios over the range 0.2–25 mm of precipitation sums with a non-linear shape similar to that of the median particle scavenging coefficients at the individual stations. Whereas in light precipitation more than 80% of the initial particles in the considered range survived 150–200 km of transport, more than 50% was scavenged by more than 15 mm of precipitation during aerosol transport. [ABSTRACT FROM AUTHOR]

Ultrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM 10 and PM 2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm 3 . That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM 2.5 . The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authors' knowledge, no other studies reported such high number concentration of ultrafine refractory particles under ambient conditions. Inverse modeling of emission factors of refractory particle number size distributions revealed that diesel-fed public utility Jeepneys , commonly used for public transportation, are responsible for 94% of total roadside emitted refractory particle mass. The observed results showed that the majority of urban pollution in Metro Manila is dominated by carbonaceous aerosol. This suggests that PM 10 or PM 2.5 metrics do not fully describe possible health related effects in this kind of urban environments. Extremely high concentrations of ultrafine particles have been and will continue to induce adverse health related effects, because of their potential toxicity. We imply that in megacities, where the major fraction of particulates originates from the transport sector, PM 10 or PM 2.5 mass concentration should be complemented by legislative measurements of equivalent black carbon mass concentration. [ABSTRACT FROM AUTHOR]

There exists a lack of aerosol absorption measurement techniques with low uncertainties and without artefacts. We have developed the two-wavelength Photothermal Aerosol Absorption Monitor (PTAAM- 2λ) , which measures the aerosol absorption coefficient at 532 and 1064 nm. Here we describe its design, calibration and mode of operation and evaluate its applicability, limits and uncertainties. The 532 nm channel was calibrated with ∼ 1 µmol mol -1 NO 2 , whereas the 1064 nm channel was calibrated using measured size distribution spectra of nigrosin particles and a Mie calculation. Since the aerosolized nigrosin used for calibration was dry, we determined the imaginary part of the refractive index of nigrosin from the absorbance measurements on solid thin film samples. The obtained refractive index differed considerably from the one determined using aqueous nigrosin solution. PTAAM-2 λ has no scattering artefact and features very low uncertainties: 4 % and 6 % for the absorption coefficient at 532 and 1064 nm, respectively, and 9 % for the absorption Ångström exponent. The artefact-free nature of the measurement method allowed us to investigate the artefacts of filter photometers. Both the Aethalometer AE33 and CLAP suffer from cross-sensitivity to scattering – this scattering artefact is most pronounced for particles smaller than 70 nm. We observed a strong dependence of the filter multiple scattering parameter on the particle size in the 100–500 nm range. The results from the winter ambient campaign in Ljubljana showed similar multiple scattering parameter values for ambient aerosols and laboratory experiments. The spectral dependence of this parameter resulted in AE33 reporting the absorption Ångström exponent for different soot samples with values biased 0.23–0.35 higher than the PTAAM-2 λ measurement. Photothermal interferometry is a promising method for reference aerosol absorption measurements. [ABSTRACT FROM AUTHOR]

There is a gap between the need for city-wide air-quality simulations considering the intra-urban variability and mircoscale dispersion features and the computational capacities that conventional urban microscale models require. This gap can be bridged by targeting model applications on the gray zone situated between the mesoscale and large-eddy scale. The urban dispersion model CAIRDIO is a new contribution to the class of computational-fluid dynamics models operating in this scale range. It uses a diffuse-obstacle boundary method to represent buildings as physical obstacles at gray-zone resolutions in the order of tens of meters. The main objective of this approach is to find an acceptable compromise between computationally inexpensive grid sizes for spatially comprehensive applications and the required accuracy in the description of building and boundary-layer effects. In this paper, CAIRDIO is applied on the simulation of black carbon and particulate matter dispersion for an entire mid-size city using a uniform horizontal grid spacing of 40 m. For model evaluation, measurements from five operational air monitoring stations representative for the urban background and high-traffic roads are used. The comparison also includes the mesoscale host simulation, which provides the boundary conditions. The measurements show a dominant influence of the mixing layer evolution at background sites, and therefore both the mesoscale and large-eddy simulation (LES) results are in good agreement with the observed air pollution levels. In contrast, at the high-traffic sites the proximity to emissions and the interactions with the building environment lead to a significantly amplified diurnal variability in pollutant concentrations. These urban road conditions can only be reasonably well represented by CAIRDIO while the meosocale simulation indiscriminately reproduces a typical urban-background profile, resulting in a large positive model bias. Remaining model discrepancies are further addressed by a grid-spacing sensitivity study using offline-nested refined domains. The results show that modeled peak concentrations within street canyons can be further improved by decreasing the horizontal grid spacing down to 10 m , but not beyond. Obviously, the default grid spacing of 40 m is too coarse to represent the specific environment within narrow street canyons. The accuracy gains from the grid refinements are still only modest compared to the remaining model error, which to a large extent can be attributed to uncertainties in the emissions. Finally, the study shows that the proposed gray-scale modeling is a promising downscaling approach for urban air-quality applications. The results, however, also show that aspects other than the actual resolution of flow patterns and numerical effects can determine the simulations at the urban microscale. [ABSTRACT FROM AUTHOR]

The airborne transmission of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has been identified as a potential pandemic challenge, especially in poorly ventilated indoor environments, such as certain hospitals, schools, public buildings, and transports. The impacts of meteorological parameters (temperature and humidity) and physical property (droplet size) on the airborne transmission of coronavirus in indoor settings have been previously investigated. However, the impacts of chemical properties of viral droplets and aerosol particles (i.e., chemical composition and acidity (pH)) on viability and indoor transmission of coronavirus remain largely unknown. Recent studies suggest high organic content (proteins) in viral droplets and aerosol particles supports prolonged survival of the virus by forming a glassy gel-type structure that restricts the virus inactivation process under low relative humidity (RH). In addition, the virus survival was found at neutral pH, and inactivation was observed to be best at low (<5) and high pH (>10) values (enveloped bacteriophage Phi6). Due to limited available information, this article illustrates an urgent need to research the impact of chemical properties of exhaled viral particles on virus viability. This will improve our fundamental understanding of indoor viral airborne transmission mechanisms. [ABSTRACT FROM AUTHOR]

New aerosol particle formation (NPF) events play a significant role in altering aerosol concentrations and dispersion within the atmosphere, making them vital for both climate and air quality research. The primary objective of investigating NPF events is to precisely determine their occurrence dates. In this study, we introduced the ConvNeXt model for the first time to identify NPF events, and compared its performance with two other deep learning models, EfficientNet and Swin Transformer. Our main aim was to automate an objective identification and classification of NPF events accurately. All three models employed transfer learning to effectively capture critical features associated with NPF. Our results demonstrated that the ConvNeXt model significantly outperformed the other models, achieving an impressive accuracy rate of 95.3% on event days, surpassing EfficientNet (92.8%) and Swin Transformer (94.9%). Furthermore, we performed tests using different ConvNeXt variants (ConvNeXt-T/S/B/L/XL) and different pre-training weights, revealing that different configurations of ConvNeXt models exhibited improved NPF event recognition capabilities. Finally, we conducted generalizability experiments using the ConvNeXt-XL model, achieving the highest accuracy of 96.4% on event days. This study not only underscores the recognition prowess of ConvNeXt models but also highlights their practical utility in accurately detecting NPF events in real-world scenarios. This contribution aids in advancing our comprehension of aerosol dynamics in atmospheric environments, providing valuable insights for climate and air quality research. • Employed ConvNeXt model, used transfer learning to identify NPF events. • Comparative analysis showed ConvNeXt's outstanding 95.3% accuracy. • Tests with different ConvNeXt variants demonstrated enhanced capabilities. • ConvNeXt-XL excelled, achieving 96.4% accuracy in generalization experiments. [ABSTRACT FROM AUTHOR]

Abstract: Background: Previous studies observed associations between airborne particles and cardio-vascular disease. Questions, however, remain as to which size of the inhalable particles (coarse, fine, or ultrafine) exerts the most significant impact on health. Methods: For this retrospective study, data of the total number of 23,741 emergency service calls, registered between February 2002 and January 2003 in the City of Leipzig, were analysed, identifying 5326 as being related to cardiovascular incidences. Simultaneous particle exposure was determined for the particle sizes classes <100nm (UFP), <2.5μm (PM2.5) and <10μm (PM10). We used a time resolution of 1day for both parameters, emergency calls and exposure. Results: Within the group of cardiovascular diseases, the diagnostic category of hypertensive crisis showed a significant association with particle exposure. The significant effect on hypertensive crisis was found for particles with a size of <100nm in diameter and starting with a lag of 2days after exposure. No consistent influence could be observed for PM2.5 and PM10. The Odds Ratios on hypertensive crisis were significant for the particle size <100nm in diameter from day 2 post exposure OR=1.06 (95%CI: 1.02–1.10, p=0.002) up to day 7 OR=1.05 (95%CI 1.02–1.09, p=0.005). Conclusion: Ultrafine particles affect cardiovascular disease adversely, particularly hypertensive crises. Their effect is significant compared with PM2.5 and PM10. It appears necessary, from a public health point of view, to consider regulating this type of particles using appropriate measurands as particle number. [Copyright &y& Elsevier]

Abstract: Direct measurements of turbulent particle number fluxes above a Norway spruce forest are compared with a size-resolved particle deposition model in combination with particle size distribution measurements. In most cases, the model output is in reasonable agreement with the eddy covariance measurements. The combination of deposition model and size distribution measurements allows the evaluation of size-resolved particle number and mass fluxes. While turbulent particle number fluxes are dominated by ultrafine particles below 50nm diameter, submicron particle mass fluxes are established mainly in the accumulation mode. The effective deposition diameter is introduced as a new parameter to describe the effect of the size distribution of a polydisperse particle population on the integral particle transfer velocity. [Copyright &y& Elsevier]

There exists a lack of aerosol absorption measurement techniques with low uncertainties and without artefacts. We have developed a two-wavelength Photothermal Aerosol Absorption Monitor (PTAAM-2λ), which measures the aerosol absorption coefficient at 532 and 1064 nm. Here we describe its design, calibration and mode of operation and evaluate its applicability, limits and uncertainties. The 532 nm channel was calibrated with ~1 µmol/mol NO2, whereas the 1064 nm channel was calibrated using measured size distribution spectra of nigrosin particles and a Mie calculation. Since the aerosolized nigrosin used for calibration was dry, we determined the imaginary part of the refractive index of nigrosin from the absorbance measurements on solid thin film samples. The obtained refractive index differed considerably from the one determined using aqueous nigrosin solution. PTAAM-2λ has no scattering artefact and features very low uncertainties: 4 % and 6 % for the absorption coefficient at 532 nm and 1064 respectively; and 9 % for the absorption Ångström exponent. The artefact-free nature of the measurement method allowed us to investigate the artefacts of filter photometers. Both the Aethalometer AE33 and the CLAP suffer from the cross-sensitivity to scattering - this scattering artefact is most pronounced for particles smaller than 70 nm. We observed a strong dependence of the filter multiple scattering parameter on the particle size in the 100-500 nm range. The results from the winter ambient campaign in Ljubljana showed similar multiple scattering parameter values for ambient aerosols and laboratory experiments. The spectral dependence of this parameter resulted in AE33 reporting the absorption Ångström exponent for different soot samples with values biased 0.17-0.3 higher than the PTAAM-2λ measurement. Photothermal interferometry is a promising method for reference aerosol absorption measurements. [ABSTRACT FROM AUTHOR]

Emissions from vehicular traffic are considered to be a major source of anthropogenic submicrometer particles in the urban environment. In this study, volatile and non-volatile number and volume fractions were distinguished in particles sampled for three consecutive days (Friday, Saturday, and Sunday) close to a highway (HW) (A4) in Germany and for one day in the urban area of Aachen, Germany. A volatility tandem differential mobility analyzer (VTDMA) and a thermodenuder (TD) combined with two scanning mobility particle sizers (SMPS) were used to get insight into a size-resolved mixing state of volatile and non-volatile particle fractions. Operating the VTDMA at 280°C, the number size distribution of non-volatile particle cores was determined for initial particle sizes of 30, 50, 80, and 150nm. The number size distributions from 10 to 400nm of ambient and non-volatile aerosol particles were measured by using parallel a SMPS and TD/SMPS combination, respectively. Number size distributions measured near the HW showed a bimodal size distribution with a maximum number concentration at particle sizes between 10 and 20nm. The TD/SMPS results for the HW site revealed that the nucleation mode disappeared after heating (completely volatile) and in total 10–20% by number of traffic-related particles were non-volatile. The VTDMA results revealed that only 22% of the 30nm particles had a non-volatile core above the instrument detection limit of 10nm. With increasing particle diameter, this non-volatile number fraction increased to ca. 60% for 50nm particles and to approximately 100% for 80 and 150nm particles. These findings mean that each particle in the upper Aitken and lower accumulation mode range contains a non-volatile core. With increasing traffic influence the number fraction of less-volatile particles representing mainly primary soot emissions increases to 62% for 50nm particles and 71% for 80nm particles. [Copyright &y& Elsevier]

Past studies have indicated that long-term averages of the aerosol number to volume ratios (defined as the number of particles larger than a certain diameter divided by the particle volume over some range less than 1μm) show little variability over the Atlantic. This work presents number to volume ratios (R) measured during the ACE-2 experiment on the land-based Sagres field site located in Southwest Portugal. The values ofRmeasured in Sagres compare reasonably well with previous measurements over the Atlantic. The main emphasis of this work is therefore to investigate more closely possible reasons for the observed stability of the number to volume ratio. Aerosol number size distributions measured in Sagres are parametrized by the sum of two log-normal distributions fitted to the accumulation and to the Aitken mode. The main factor that limits the variability ofRis that the parameters of these log-normal distributions are not always independent but show some covariance. In polluted air mass types correlations between parameters of the Aitken and accumulation mode are mostly responsible for stabilizingR. In marine air mass types the variability ofRis reduced by an inverse relationship between the accumulation-mode mean diameter and standard deviation, consistent with condensational processes and cloud processing working on the aerosol. However, despite this reduction, the variability ofRin marine air mass types is still considerable andRis linearly dependent on the number concentration of particles larger than 90 nm. This partly due to a tail of Aitken-mode particles extending to sizes larger than 90 nm. [ABSTRACT FROM AUTHOR]

Submicrometre dry number size distributions from four marine and one continental aerosol experiment were evaluated jointly in the present study. In the marine experiments only data with back trajectories of at least 120 h without land contact were used to minimize continental contamination. Log-normal functions were fitted to the size distributions. Basic statistics of the marine aerosol indicate a closed character of the size distribution at the lower size limit as opposed to an open character for corresponding continental data. Together with the infrequent occurrences of marine particles below 20 nm this finding supports hypotheses and model results suggesting low probabilities of homogeneous nucleation in the marine boundary layer. The variability of submicrometre marine number concentrations was parametrized with a bimodal log-normal function that quantifies the probability of finding different number concentrations about a given median value. Together with a four-modal log-normal approximation of the submicrometre marine size distribution itself, this model allows a statistical representation of the marine aerosol that facilitates comparison of experiments and validation of aerosol models. Autocorrelation at the one fixed marine site with a minimum of interruptions in times-series revealed a strong size dependency of persistence in particle number concentration with the shortest persistence at the smallest sizes. Interestingly, in the marine aerosol (at Cape Grim) persistence exhibits a size dependency that largely matches the modes in dg0, i.e. near the most frequent geometric mean diameters number concentrations are most persistent. Over the continent, persistence of particle numbers is strongly constrained by diurnal meteorological processes and aerosol dynamics. Thus, no strong modal structure appears in the size-dependent persistence at Melpitz. As with the aerosol variability, marine aerosol processes in models of aerosol dynamics can be tested with these findings. [ABSTRACT FROM AUTHOR]

Presents a study that proposed and tested a method to calculate cloud condensation nuclei (CCN) spectra based on aerosol number size distributions and hygroscopic growth factors. Crucial step in the calculation; Basis for the calculation of CCN spectra; Factor which enhanced the CCN concentrations.

• Studying MAC variability impact on eBC estimation. • Presenting spatial, seasonal and temporal MAC variability in Europe. • Proposing the site-specific MAC as the most effective approach to estimate eBC. • Long-term trend analysis links decreasing EC trends with method-dependent corrected eBC trends. A reliable determination of equivalent black carbon (eBC) mass concentrations derived from filter absorption photometers (FAPs) measurements depends on the appropriate quantification of the mass absorption cross-section (MAC) for converting the absorption coefficient (b abs) to eBC. This study investigates the spatial–temporal variability of the MAC obtained from simultaneous elemental carbon (EC) and b abs measurements performed at 22 sites. We compared different methodologies for retrieving eBC integrating different options for calculating MAC including: locally derived, median value calculated from 22 sites, and site-specific rolling MAC. The eBC concentrations that underwent correction using these methods were identified as LeBC (local MAC), MeBC (median MAC), and ReBC (Rolling MAC) respectively. Pronounced differences (up to more than 50 %) were observed between eBC as directly provided by FAPs (NeBC ; Nominal instrumental MAC) and ReBC due to the differences observed between the experimental and nominal MAC values. The median MAC was 7.8 ± 3.4 m2 g-1 from 12 aethalometers at 880 nm, and 10.6 ± 4.7 m2 g-1 from 10 MAAPs at 637 nm. The experimental MAC showed significant site and seasonal dependencies, with heterogeneous patterns between summer and winter in different regions. In addition, long-term trend analysis revealed statistically significant (s.s.) decreasing trends in EC. Interestingly, we showed that the corresponding corrected eBC trends are not independent of the way eBC is calculated due to the variability of MAC. NeBC and EC decreasing trends were consistent at sites with no significant trend in experimental MAC. Conversely, where MAC showed s.s. trend, the NeBC and EC trends were not consistent while ReBC concentration followed the same pattern as EC. These results underscore the importance of accounting for MAC variations when deriving eBC measurements from FAPs and emphasize the necessity of incorporating EC observations to constrain the uncertainty associated with eBC. [ABSTRACT FROM AUTHOR]

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). [ABSTRACT FROM AUTHOR]

• Generalized additive models were used to quantify particle number concentrations. • Meteorology, traffic and urban geometry were used as explanatory variables. • Adjusted R2 ranged from 0.44 to 0.51. • Ten-fold cross-validation was performed to validate the models. • The models represent emission, long-range transport, dilution and other processes. Quantification of the exposure of urban residents to ultrafine particle number concentrations (UFP) is challenging due to its high spatial and temporal variability. Hence, statistical models, e.g. generalized additive models (GAM), may be used to estimate time series or spatial characteristics of UFP. The GAM approach allows the representation of non-linear relations of a response variable with explanatory variables without the need to pre-define model functions. Up to now, GAMs were usually fitted to UFP data from a single site or from mobile measurement campaigns with limited temporal coverage. In this study, GAMs were used to determine UFP, accumulation mode particle (ACC) and total number concentration (TNC) at five urban sites in the cities of Leipzig and Dresden, Germany for the period 2011–2013. As explanatory variables, reanalysis data sets of meteorological quantities, urban geometry and traffic volume data were evaluated. Variables causing concurvity, which is the equivalent to collinearity in non-linear model approaches, were neglected to guarantee the interpretability of the final models. The models were then validated in a ten-fold cross-validation approach. The final models contained smooth functions for the building surface fraction, planetary boundary layer height, traffic volume, air temperature, wind direction, atmospheric pressure, relative humidity, global radiation and precipitation. Adjusted coefficients of determination (R2 adj.) for the final models were R2 adj. = 0.44 for UFP, R2 adj. = 0.51 for ACC and R2 adj. = 0.48 for TNC. Coefficients of determination of the cross-validation were in a similar range (0.44 for UFP, 0.51 for ACC, 0.49 for TNC). Finally, our study shows that GAMs are able to represent important processes that contribute to the particle number concentration from the smooth functions, i.e. emission, dilution, nucleation, deposition and long-range transport. [ABSTRACT FROM AUTHOR]

Interactions between water and nanoparticles are relevant for atmospheric multiphase processes, physical chemistry, and materials science. Current knowledge of the hygroscopic and related physicochemical properties of nanoparticles, however, is restricted by the limitations of the available measurement techniques. Here, we present the design and performance of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. Detailed methods of calibration and validation are provided. Besides maintaining accurate and stable sheath and aerosol flow rates (±1 %), high accuracy of the differential mobility analyzer (DMA) voltage (±0.1 %) in the range of ∼0 –50 V is crucial for achieving accurate sizing and small sizing offsets between the two DMAs (<1.4 %). To maintain a stable relative humidity (RH), the humidification system and the second DMA are placed in a well-insulated and air conditioner housing (±0.1 K). We also tested and discussed different ways of preventing predeliquescence in the second DMA. Our measurement results for ammonium sulfate nanoparticles are in good agreement with Biskos et al. (2006b), with no significant size effect on the deliquescence and efflorescence relative humidity (DRH and ERH, respectively) at diameters down to 6 nm. For sodium sulfate nanoparticles, however, we find a pronounced size dependence of DRH and ERH between 20 and 6 nm nanoparticles. [ABSTRACT FROM AUTHOR]

The aerosol chemical speciation monitor (ACSM) is nowadays widely used to identify and quantify the main components of fine particles in ambient air. As such, its deployment at observatory platforms is fully incorporated within the European Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS). Regular intercomparisons are organized at the Aerosol Chemical Monitoring Calibration Center (ACMCC; part of the European Center for Aerosol Calibration, Paris, France) to ensure the consistency of the dataset, as well as instrumental performance and variability. However, in situ quality assurance remains a fundamental aspect of the instrument's stability. Here, we present and discuss the main outputs of long-term quality assurance efforts achieved for ACSM measurements at the research station Melpitz (Germany) since 2012 onwards. In order to validate the ACSM measurements over the years and to characterize seasonal variations, nitrate, sulfate, ammonium, organic, and particle mass concentrations were systematically compared against the collocated measurements of daily offline high-volume PM 1 and PM 2.5 filter samples and particle number size distribution (PNSD) measurements. Mass closure analysis was made by comparing the total particle mass (PM) concentration obtained by adding the mass concentration of equivalent black carbon (eBC) from the multi-angle absorption photometer (MAAP) to the ACSM chemical composition, to that of PM 1 and PM 2.5 during filter weighing, as well as to the derived mass concentration of PNSD. A combination of PM 1 and PM 2.5 filter samples helped identifying the critical importance of the upper size cutoff of the ACSM during such exercises. The ACSM–MAAP-derived mass concentrations systematically deviated from the PM 1 mass when the mass concentration of the latter represented less than 60 % of PM 2.5 , which was linked to the transmission efficiency of the aerodynamic lenses of the ACSM. The best correlations are obtained for sulfate (slope =0.96 ; R2=0.77) and total PM (slope =1.02 ; R2=0.90). Although, sulfate did not exhibit a seasonal dependency, total PM mass concentration revealed a small seasonal variability linked to the increase in non-water-soluble fractions. The nitrate suffers from a loss of ammonium nitrate during filter collection, and the contribution of organo-nitrate compounds to the ACSM nitrate signal make it difficult to directly compare the two methods. The contribution of m/z 44 (f44) to the total organic mass concentration was used to convert the ACSM organic mass (OM) to organic carbon (OC) by using a similar approach as for the aerosol mass spectrometer (AMS). The resulting estimated OC ACSM was compared with the measured OC PM1 (slope =0.74 ; R2=0.77), indicating that the f44 signal was relatively free of interferences during this period. The PM 2.5 filter samples use for the ACSM data quality might suffer from a systematic bias due to a size truncation effect as well as to the presence of chemical species that cannot be detected by the ACSM in coarse mode (e.g., sodium nitrate and sodium sulfate). This may lead to a systematic underestimation of the ACSM particle mass concentration and/or a positive artifact that artificially decreases the discrepancies between the two methods. Consequently, ACSM data validation using PM 2.5 filters has to be interpreted with extreme care. The particle mass closure with the PNSD was satisfying (slope =0.77 ; R2=0.90 over the entire period), with a slight overestimation of the mobility particle size spectrometer (MPSS)-derived mass concentration in winter. This seasonal variability was related to a change on the PNSD and a larger contribution of the supermicrometer particles in winter. This long-term analysis between the ACSM and other collocated instruments confirms the robustness of the ACSM and its suitability for long-term measurements. Particle mass closure with the PNSD is strongly recommended to ensure the stability of the ACSM. A near-real-time mass closure procedure within the entire ACTRIS–ACSM network certainly represents an optimal quality control and assurance of both warranting the quality assurance of the ACSM measurements as well as identifying cross-instrumental biases. [ABSTRACT FROM AUTHOR]

Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system. [ABSTRACT FROM AUTHOR]

The effect of the baseline drift on the resulting extinction values of three cavity attenuated phase shift-based extinction monitors (CAPS PMex) with different wavelengths and the respective correlation with NO2 was analysed for an urban background station. A drift of more than 0.8 Mm-1min-1 was observed for ambient air, with high probability caused by traffic-emissions-driven changes in carrier gas composition. The baseline drift leads to characteristic measurement artefacts for particle extinction. Artificial particle extinction values of approximately 4 Mm-1 were observed using a baseline period of 5 min. These values can be even higher for longer baseline periods. Two methods are shown to minimize this effect. Modified continuous baseline values are calculated in a post-processing step using simple linear interpolation and cubic smoothing splines. Both methods are useful to reduce artefacts, although the use of cubic smoothing splines gives slightly better results. The extinction artefacts are diminished and the effective scattering of the resulting extinction values is reduced by about 50 %. [ABSTRACT FROM AUTHOR]

Interactions between water and nanoparticles are relevant for atmospheric multiphase processes, physical chemistry, and materials science. Current knowledge of the hygroscopic and related physico-chemical properties of nanoparticles, however, is restricted by limitations of the available measurement techniques. Here, we present the design and performance of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. Detailed methods of calibration and validation are provided. Beside maintaining accurate and stable sheath/aerosol flow rates (± 1 %), high accuracy of DMA voltage (± 0.1 %) in the range of ~0-50 V is crucial to achieve accurate sizing and small sizing offsets between the two DMAs (< 1.4 %). To maintain a stable relative humidity (RH), the humidification system and the second DMA are placed in a well-insulated and air conditioner housing (± 0.1 K). We also tested and discussed different ways of preventing pre-deliquescence in the second DMA. Our measurement results for ammonium sulfate nanoparticles are in good agreement with Biskos et al. (2006b), with no significant size-effect on the deliquescence and efflorescence relative humidity (DRH, ERH) at diameters down to 6 nm. For sodium sulfate nanoparticles, however, we find a pronounced size-dependence of DRH and ERH between 20 and 6 nm nanoparticles. [ABSTRACT FROM AUTHOR]

Aerosol particles are essential constituents of the Earth’s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence time resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in-situ near-surface segment of the atmospheric observations system. This paper will provide the widest effort so far to document variability of climate-relevant in-situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High quality data from more than 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single scattering albedo and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information including data provision procedures, quality control and analysis, data policy and usage of the ground-based aerosol measurements network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully-characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system. [ABSTRACT FROM AUTHOR]

The effect of the baseline drift on the resulting extinction values of three CAPS PMex monitors with different wavelengths and the respective correlation with NO2 was analysed for an urban background station. A drift of more than 0.8 Mm-1 min-1 was observed for ambient air, with high probability caused by traffic emissions driven changes in carrier gas composition. The baseline drift leads to characteristic measurement artefacts for particle extinction. Artificial particle extinction values of approximately 4 Mm-1 where observed using a baseline period of 5 min. These values can be even higher for longer baseline periods. A new method is shown to minimize this effect. Modified continuous baseline values are calculated in a post-processing step using cubic smoothing splines. With this approach the extinction artefacts are diminished and the effective scattering of the resulting extinction values is reduced by about 50%. [ABSTRACT FROM AUTHOR]

Measuring vertical profiles of the particle light-absorption coefficient by using absorption photometers may face the challenge of fast changes in relative humidity (RH). These absorption photometers determine the particle light-absorption coefficient due to a change in light attenuation through a particle-loaded filter. The filter material, however, takes up or releases water with changing relative humidity (RH in %), thus influencing the light attenuation. A sophisticated set of laboratory experiments was therefore conducted to investigate the effect of fast RH changes (dRH / d t) on the particle light-absorption coefficient (σabs in Mm -1) derived with two absorption photometers. The RH dependence was examined based on different filter types and filter loadings with respect to loading material and areal loading density. The Single Channel Tricolor Absorption Photometer (STAP) relies on quartz-fiber filter, and the microAeth® MA200 is based on a polytetrafluoroethylene (PTFE) filter band. Furthermore, three cases were investigated: clean filters, filters loaded with black carbon (BC), and filters loaded with ammonium sulfate. The filter areal loading densities (ρ*) ranged from 3.1 to 99.6 mg m -2 in the case of the STAP and ammonium sulfate and 1.2 to 37.6 mg m -2 in the case the MA200. Investigating BC-loaded cases, ρBC* was in the range of 2.9 to 43.0 and 1.1 to 16.3 mg m -2 for the STAP and MA200, respectively. Both instruments revealed opposing responses to relative humidity changes (Δ RH) with different magnitudes. The STAP shows a linear dependence on relative humidity changes. The MA200 is characterized by a distinct exponential recovery after its filter was exposed to relative humidity changes. At a wavelength of 624 nm and for the default 60 s running average output, the STAP reveals an absolute change in σabs per absolute change of RH (Δσabs/Δ RH) of 0.14 Mm -1 % -1 in the clean case, 0.29 Mm -1 % -1 in the case of BC-loaded filters, and 0.21 Mm -1 % -1 in the case filters loaded with ammonium sulfate. The 60 s running average of the particle light-absorption coefficient at 625 nm measured with the MA200 revealed a response of around -0.4 Mm -1 % -1 for all three cases. Whereas the response of the STAP varies over the different loading materials, in contrast, the MA200 was quite stable. The response was, for the STAP, in the range of 0.17 to 0.24 Mm -1 % -1 and, in the case of ammonium sulfate loading and in the BC-loaded case, 0.17 to 0.62 Mm -1 % -1. In the ammonium sulfate case, the minimum response shown by the MA200 was -0.42 with a maximum of -0.36 Mm -1 % -1 and a minimum of -0.42 and maximum -0.37 Mm -1 % -1 in the case of BC. A linear correction function for the STAP was developed here. It is provided by correlating 1 Hz resolved recalculated particle light-absorption coefficients and RH change rates. The linear response is estimated at 10.08 Mm -1 s -1 % -1. A correction approach for the MA200 is also provided; however, the behavior of the MA200 is more complex. Further research and multi-instrument measurements have to be conducted to fully understand the underlying processes, since the correction approach resulted in different correction parameters across various experiments. However, the exponential recovery after the filter of the MA200 experienced a RH change could be reproduced. However, the given correction approach has to be estimated with other RH sensors as well, since each sensor has a different response time. And, for the given correction approaches, the uncertainties could not be estimated, which was mainly due to the response time of the RH sensor. Therefore, we do not recommend using the given approaches. But they point in the right direction, and despite the imperfections, they are useful for at least estimating the measurement uncertainties due to relative humidity changes. Due to our findings, we recommend using an aerosol dryer upstream of absorption photometers to reduce the RH effect significantly. Furthermore, when absorption photometers are used in vertical measurements, the ascending or descending speed through layers of large relative humidity gradients has to be low to minimize the observed RH effect. But this is simply not possible in some scenarios, especially in unmixed layers or clouds. Additionally, recording the RH of the sample stream allows correcting for the bias during post-processing of the data. This data correction leads to reasonable results, according to the given example in this study. [ABSTRACT FROM AUTHOR]

The Aerosol Chemical Speciation Monitor (ACSM) is an instrument for identifying and quantifying the influence of air quality mitigations. For this purpose, a European ACSM network has been developed within the research infrastructure project ACTRIS (European Research Infrastructure for the observation of Aerosol, Clouds and Trace Gases). To ensure the uniformity of the dataset, as well as instrumental performance and variability, regular intercomparisons are organized at the Aerosol Chemical Monitoring Calibration Center (ACMCC, part of the European Center for Aerosol Calibration, Paris, France). However, in-situ quality assurance remains a fundamental tracking point of the instrument's stability. In order to check the robustness of the ACSM over the years and to characterize the seasonality effect, nitrate, sulfate, ammonium, organic, and particle mass concentrations were systematically compared with collocated measurements including daily off-line high-volume PM1 and PM2.5 filter samples. Mass closure analysis was made by comparing the total particle mass (PM) concentration obtained by adding the mass concentration of equivalent black carbon (eBC) from the Multi-Angle Absorption Photometer (MAAP) to the ACSM chemical composition, to that of PM1 and PM2.5 during filter weighting, as well as to the derived mass concentration of particle number size distribution measurements (PNSD). A combination of PM1 and PM2.5 filter samples helps identify the critical importance of the upper size cut-off of the ACSM during such exercises. The ACSM-MAAP-derived mass concentrations systematically deviate from the PM1 samples when the mass concentration of the latter represents less than 60% of PM2.5, which is linked to the transmission efficiency of the aerodynamic lenses of the ACSM. The best correlations are obtained for sulfate (slope 0.96, R2=0.77) and total PM (slope 1.02, R2=0.90). Although, sulfate does not exhibit a seasonal dependency, total PM mass concentration shows a small seasonal effect associated with an increase in non-water-soluble fractions. The nitrate suffers from a loss of ammonium nitrate during filter collection, and the contribution of organo-nitrate compounds to the ACSM nitrate signal make it difficult to directly compare the two methods. The contribution of m/z44 (f44) to the total organic mass concentration was used to convert the ACSM organic mass to OC by using a similar approach as for the AMS. The resulting estimated OC-ACSM was compared with the measured OC-PM1 (slope 0.74, R2=0.77), indicating that the f44 signal was relatively free of interferences during this period. The PM2.5 filter samples use for the ACSM data quality might suffer from a systematic bias due to a size cutting effect as well as to the presence of chemical species that cannot be detected by the ACSM in coarse mode (e.g. sodium nitrate and sodium sulfate). This may lead to a systematic underestimation of the ACSM particle mass concentration and/or a positive artefact that artificially decreases the discrepancies between the two methods. Consequently, ACSM data validation using PM2.5 filters has to be interpreted with extreme care. The particle mass closure with the PNSD was satisfying (slope 0.77, R2=0.90 over the entire period), with a slightly overestimation of the MPSS derived mass concentration in winter. This seasonal variability was related to a change on the PNSD and a larger contribution of the super-µm particles in winter. [ABSTRACT FROM AUTHOR]

Measurements of air pollutants such as black carbon (BC) and particle mass concentration in general, using mobile platforms equipped with high-time-resolution instruments, have gained popularity over the last decade due to their wide range of applicability. Assuring the quality of mobile measurement, data have become more essential, particularly when the personal exposure to pollutants is related to their spatial distribution. In the following, we suggest a methodology to achieve data from mobile measurements of equivalent black carbon (eBC) and PM 2.5 mass concentrations with high data quality. Besides frequent routine quality assurance measures of the instruments, the methodology includes the following steps: (a) measures to ensure the quality of mobile instruments through repeated collocated measurements using identical instrumentation, (b) inclusion of a fixed station along the route containing quality-assured reference instruments, and (c) sufficiently long and frequent intercomparisons between the mobile and reference instruments to correct the particle number and mass size distributions obtained from mobile measurements. The application of the methodology can provide the following results. First, collocated mobile measurements with sets of identical instruments allow identification of undetected malfunctions of the instruments. Second, frequent intercomparisons against the reference instruments will ensure the quality of the mobile measurement data of the eBC mass concentration. Third, the intercomparison data between the mobile optical particle size spectrometer (OPSS) and a reference mobility particle size spectrometer (MPSS) allow for the adjustment of the OPSS particle number size distribution using physically meaningful corrections. Matching the OPSS and MPSS volume particle size distributions is crucial for the determination of PM 2.5 mass concentration. Using size-resolved complex refractive indices and time-resolved fine-mode volume correction factors of the fine-particle range, the calculated PM 2.5 from the OPSS was within 5 % of the reference instruments (MPSS + APSS). However, due to the nonsphericity and an unknown imaginary part of the complex refractive index of supermicrometer particles, a conversion to a volume equivalent diameter yields high uncertainties of the particle mass concentration greater than PM 2.5. The proposed methodology addresses issues regarding the quality of mobile measurements, especially for health impact studies, validation of modeled spatial distribution, and development of air pollution mitigation strategies. [ABSTRACT FROM AUTHOR]

Abstract Recent studies demonstrate that Black Carbon (BC) pollution in economically developing megacities remain higher than the values, which the World Health Organization considers to be safe. Despite the scientific evidence of the degrees of BC exposure, there is still a lack of understanding on how the severe levels of BC pollution affect human health in these regions. We consider information on the respiratory tract deposition dose (DD) of BC to be essential in understanding the link between personal exposure to air pollutants and corresponding health effects. In this work, we combine data on fine and ultrafine refractory particle number concentrations (BC proxy), and activity patterns to derive the respiratory tract deposited amounts of BC particles for the population of the highly polluted metropolitan area of Manila, Philippines. We calculated the total DD of refractory particles based on three metrics: refractory particle number, surface area, and mass concentrations. The calculated DD of total refractory particle number in Metro Manila was found to be 1.6 to 17 times higher than average values reported from Europe and the U.S. In the case of Manila, ultrafine particles smaller than 100 nm accounted for more than 90% of the total deposited refractory particle dose in terms of particle number. This work is a first attempt to quantitatively evaluate the DD of refractory particles and raise awareness in assessing pollution-related health effects in developing megacities. We demonstrate that the majority of the population may be highly affected by BC pollution, which is known to have negative health outcomes if no actions are taken to mitigate its emission. For the governments of such metropolitan areas, we suggest to revise currently existing environmental legislation, raise public awareness, and to establish supplementary monitoring of black carbon in parallel to already existing PM 10 and PM 2.5 measures. Graphical abstract Unlabelled Image Highlights • Population from developing regions faces upraise in health related problems. • Refractory fine particle deposition dose was determined in a developing megacity. • The observed deposition dose of refractory fine particles was unprecedentedly high. • The ultrafine refractory particles dominated deposited particle dose. • Decisive actions have to be taken to reduce immense black carbon emissions. [ABSTRACT FROM AUTHOR]

Measuring vertical profiles of the particle light absorption coefficient by using absorption photometers may face the challenge of fast changes in relative humidity. These absorption photometers determine the particle light absorption coefficient due to a change in light attenuation through a particle-loaded filter. The filter material, however, takes up or releases water with changing relative humidity (rh in %), influencing thus the light attenuation. A sophisticated set of laboratory experiments was therefore conducted to investigate the effect of fast rh changes (drh/dt) on the particle light absorption coefficient (σabs in Mm-1) derived with two absorption photometers. The rh dependency was examined based on different filter types and filter loadings with respect to loading material and loading areal density. Different filter material was used in the two examined instruments. The Single Channel Tri-Color Absorption Photometer (STAP; Brechtel Manufacturing Inc, 1789 Addison Way, Hayward, CA 94544, USA) relies on quartz-fiber filter (PALL LifeScience, Pallflex Membrane Filters Type E70-2075W) and the microAeth® MA200 (AethLabs, 1640 Valencia St, Suite 2C, San Francisco, CA 94110, USA) is based on a Polytetrafluoroethylene (PTFE) filter band. Furthermore, three cases were investigated: clean filter, filter loaded with black carbon (BC) and filter loaded with ammonium sulfate. The filter loading areal densities (ρ*) ranged from 3.1 to 99.6 mg m-2 in the case of the STAP and ammonium sulfate, 1.2 to 37.6 mg m-2 considering the MA200. Investigating BC loaded cases, ρ*BC was in the range of 2.9 to 43.0 and 1.1 to 16.3 mg m-2 for the STAP and MA200, respectively. In addition, the effect of a silica-bead based diffusion on the rh effect was investigated. Both instruments revealed opposing responses to relative humidity changes (Δrh) with different amplitudes. Whereas the STAP shows a linear dependence to relative humidity changes, the MA200 is characterized by an exponential recovery after its filter was exposed to relative humidity changes. At a wavelength of 624 nm and for the default 60 second average output, the STAP reveals an absolute change in σabs per absolute change of rh (Δσabs/Δrh) of 0.14 Mm-1 %-1 in the clean case, 0.29 Mm-1 %-1 in the case of BC loaded filters, and 0.21 Mm-1 %-1 considering filters loaded with ammonium sulfate. The 60-second running average of the particle light absorption coefficient at 625 nm measured with the MA200 revealed response of around -0.4 Mm-1 %-1 for all three cases. Whereas the response of the STAP varies over the different loading materials in contrast the MA200 was quite stable. The minimum and maximum response was for the STAP 0.17 Mm-1 %-1 and 0.24 Mm-1 %-1 considering ammonium sulfate loading and in the BC loaded case 0.17 Mm-1 %-1 and 0.62 Mm-1 %-1, respectively. The minimum response shown by the MA200 was -0.42 Mm-1 %-1 and -0.36 Mm-1 %-1 at maximum for ammonium sulfate and -0.42 Mm-1 %-1 and -0.37 Mm-1 %-1 in case of BC loading, respectively. Using the aerosol dryer upstream, the STAP did not change the behavior, but the amplitude of the observed effect was reduced by a factor of up to three. A linear correction function for the STAP was developed here. It is provided by correlating recalculated particle light absorption coefficients at 1 Hz time resolution against the change rate of rh. The linear response is estimated with 10.08 Mm-1 s-1 %-1 and can be used to correct for bias induced to rh changes at this time resolution. A correction approach for the MA200 is also provided, however, the behavior of the MA200 is more complex. Further research and multi-instrument measurements have to be conducted to fully understand the underlying processes, since the correction approach resulted in different correction parameters across various experiments. However, the exponential recovery after the filter of the MA200 experienced a rh change could be reproduced. Due to our findings, we recommend to use an aerosol dryer upstream of absorption photometers to reduce the rh effect significantly. Furthermore, when absorption photometers are used in vertical measurements, the ascending or descending speed through layers of large rh gradients has to be low to minimize the observed rh effect. Additionally, recording the rh of the sample stream allows correcting for the bias during post processing of the data. This data correction leads to reasonable results, according the given example in this study. [ABSTRACT FROM AUTHOR]

Measurements of air pollutants such as black carbon (BC) and particle mass concentration in general, using mobile platforms equipped with high time-resolution instruments have gained popularity over the last decade due to its wide range of applicability. Assuring the quality of mobile measurement, data has become more essential particularly, when the personal exposure to pollutants is related to its spatial distribution. In the following, we suggest a methodology to achieve data from mobile measurements of equivalent black carbon (eBC) and PM2.5 mass concentrations with high data quality. Besides frequent routine quality assurance measures of the instruments, the methodology includes the following steps. a) Measures to ensure the quality of mobile instruments through repeated collocated measurements using identical instrumentation, b) inclusion of a fixed station along the route containing quality-assured reference instruments and c) sufficiently long and frequent intercomparisons between the mobile and reference instruments to correct the particle number and mass size distributions obtained from mobile measurements. The application of the methodology can provide following results. First, collocated mobile measurements with sets of identical instruments allow identification of undetected malfunctions of the instruments. Second, frequent intercomparisons against the reference instruments will ensure the quality of the mobile measurement data of the eBC mass concentration. Third, the intercomparison data between the mobile optical particle size spectrometer (OPSS) and a reference mobility particle size spectrometer (MPSS) allows for the adjustment of the OPSS particle number size distribution using physical meaningful corrections. Matching the OPSS and MPSS volume particle size distributions is crucial for the determination of PM2.5 mass concentration. Using size-resolved complex refractive indices and time-resolved fine mode volume correction factors of the fine particle range, the calculated PM2.5 was within 5% of the reference instruments (MPSS+APSS). However, due to the non-sphericity and an unknown imaginary part of the complex refractive index of supermicrometer particles, a conversion to a volume equivalent diameter yields high uncertainties of the particle mass concentration greater than PM2.5. The proposed methodology addresses issues regarding the quality of mobile measurements, especially for health impact studies, validation of modelled spatial distribution, and development of air pollution mitigation strategies. [ABSTRACT FROM AUTHOR]

Abstract The mass loading and composition of atmospheric particles are important in determining their climate and health effects, and are typically measured by filter sampling. However, particle sampling under ambient conditions can lead to a shift in the size cut-off threshold induced by hygroscopic growth, and the influence of this on measurement of particle loading and composition has not been adequately quantified. Here, we propose a method to assess this influence based on κ-Köhler theory. A global perspective is presented based on previously reported annual climatological values of hygroscopic properties, meteorological parameters and particle volume size distributions. Measurements at background sites in Europe may be more greatly influenced by the cut-off shift than those from other continents, with a median influence of 10–20% on the total mass of sampled particles. However, the influence is generally much smaller (<7%) at urban sites, and is negligible for dust and particles in the Arctic. Sea-salt particles experience the largest influence (median value ∼50%), resulting from their large size, high hygroscopicity and the high relative humidity (RH) in marine air-masses. We estimate a difference of ∼30% in this influence of sea-salt particle sampling between relatively dry (RH = 60%) and humid (RH = 90%) conditions. Given the variation in the cut-off shift in different locations and at different times, a consistent consideration of this influence using the approach we introduce here is critical for observational studies of the long-term and spatial distribution of particle loading and composition, and crucial for robust validation of aerosol modules in modelling studies. Graphical abstract Image 1 Highlights • Hygroscopic growth leads to a shift in the size of dry particles cut off by impactors during sampling. • We propose a method to assess this influence on aerosol measurements, quantifying its global importance for the first time. • Observational comparison and model validation must account for the large temporal and spatial variations in this influence. [ABSTRACT FROM AUTHOR]

Air pollution and particulate matter are recognised cause of increased disease incidence in exposed population. The toxicological processes underlying air pollution associated effects have been investigated by in vivo and/or in vitro experimentation. The latter is usually performed by exposing cells cultured under submerged condition to particulate matter concentration quite far from environmental exposure expected in humans. Here we report for the first time the feasibility of a direct exposure of air liquid interface cultured cells to environmental concentration of particulate matter. Inflammatory proteins release was analysed in cell medium while differential expression of selected genes was analysed in cells. Significant association of anti-oxidant genes was observed with secondary and aged aerosol, while cytochrome activation with primary and PAHs enriched ultrafine particles. The results obtained clearly show the opportunity to move from the lab bench to the field for properly understanding the toxicological effects also of ultrafine particles on selected in vitro models. [ABSTRACT FROM AUTHOR]

Cooking emission is one of sources for ambient volatile organic compounds (VOCs), which is deleterious to air quality, climate and human health. These emissions are especially of great interest in large cities of East and Southeast Asia. We conducted a case study in which VOC emissions from kitchen extraction stacks have been sampled in total 57 times in the Megacity Shanghai. To obtain representative data, we sampled VOC emissions from kitchens, including restaurants of seven common cuisine types, canteens, and family kitchens. VOC species profiles and their chemical reactivities have been determined. The results showed that 51.26% ± 23.87% of alkane and 24.33 ± 11.69% of oxygenated VOCs (O-VOCs) dominate the VOC cooking emissions. Yet, the VOCs with the largest ozone formation potential (OFP) and secondary organic aerosol potential (SOAP) were from the alkene and aromatic categories, accounting for 6.8–97.0% and 73.8–98.0%, respectively. Barbequing has the most potential of harming people's heath due to its significant higher emissions of acetaldehyde, hexanal, and acrolein. Methodologies for calculating VOC emission factors ( EF ) for restaurants that take into account VOCs emitted per person ( EF person ), per kitchen stove ( EF kitchen stove ) and per hour ( EF hour ) are developed and discussed. Methodologies for deriving VOC emission inventories (S) from restaurants are further defined and discussed based on two categories: cuisine types ( S type ) and restaurant scales ( S scale ). The range of S type and S scale are 4124.33–7818.04 t/year and 1355.11–2402.21 t/year, respectively. We also found that S type and S scale for 100,000 people are 17.07–32.36 t/year and 5.61–9.95 t/year, respectively. Based on Environmental Kuznets Curve, the annual total amount of VOCs emissions from catering industry in different provinces in China was estimated, which was 5680.53 t/year, 6122.43 t/year, and 66,244.59 t/year for Shangdong and Guangdong provinces and whole China, respectively. Large and medium-scaled restaurants should be paid more attention with respect to regulation of VOCs. [ABSTRACT FROM AUTHOR]

Surface concentration of black carbon (BC) is a key factor for the understanding of the impact of anthropogenic pollutants on human health. The majority of Italian cities lack long-term measurements of BC concentrations since such a metric is not regulated by EU legislation. This work attempts a long-term (2001-2017) inference of equivalent black carbon (eBC) concentrations in the city of Rome (Italy) based on sun-photometry data. To this end, aerosol light absorption coefficients at the surface are inferred from the "columnar" aerosol aerosol light absorption coefficient records from the Rome Tor Vergata AERONET sun-photometer. The main focus of this work is to rescale aerosol light absorption columnar data (AERONET) to ground-level BC data. This is done by using values of mixing layer height (MLH) derived from ceilometer measurements and then by converting the absorption into eBC mass concentration through a mass-to-absorption conversion factor, the Mass Absorption Efficiency (MAE). The final aim is to obtain relevant data representative of the BC aerosol at the surface (i.e., in-situ)-so within the MLH- and then to infer a long-term record of "surface" equivalent black carbon mass concentration in Rome. To evaluate the accuracy of this procedure, we compared the AERONET-based results to in-situ measurements of aerosol light absorption coefficients (αabs) collected during some intensive field campaigns performed in Rome between 2010 and 2017. This analysis shows that different measurement methods, local emissions, and atmospheric conditions (MLH, residual layers) are some of the most important factors influencing differences between inferred and measured αabs. As a general result, "inferred" and "measured" αabs resulted to reach quite a good correlation (up to r = 0.73) after a screening procedure that excludes one of the major cause of discrepancy between AERONET inferred and in-situ measured αabs: the presence of highly absorbing aerosol layers at high altitude (e.g., dust), which frequently affects the Mediterranean site of Rome. Long-term trends of "inferred" αabs, eBC, and of the major optical variables that control aerosol's direct radiative forcing (extinction aerosol optical depth, AODEXT, absorption aerosol optical depth, AODABS, and single scattering albedo, SSA) have been estimated. The Mann-Kendall statistical test associated with Sen's slope was used to test the data for long-term trends. These show a negative trend for both AODEXT (-0.047/decade) and AODABS (-0.007/decade). The latter converts into a negative trend for the αabs of -5.9 Mm-1/decade and for eBC mass concentration of -0.76 μg/m3/decade. A positive trend is found for SSA (+0.014/decade), indicating that contribution of absorption to extinction is decreasing faster than that of scattering. These long-term trends are consistent with those of other air pollutant concentrations (i.e., PM2.5 and CO) in the Rome area. Despite some limitations, findings of this study fill a current lack in BC observations and may bear useful implications with regard to the improvement of our understanding of the impact of BC on air quality and climate in this Mediterranean urban region. [ABSTRACT FROM AUTHOR]

The take-up of water of aerosol particles plays an important role in heavy haze formation over North China Plain, since it is related with particle mass concentration, visibility degradation, and particle chemistry. In the present study, we investigated the size-resolved hygroscopic growth factor ( HGF ) of sub-micrometer aerosol particles (smaller than 350 nm) on a basis of 9-month Hygroscopicity-Tandem Differential Mobility Analyzer measurement in the urban background atmosphere of Beijing. The mean hygroscopicity parameter (κ) values derived from averaging over the entire sampling period for particles of 50 nm, 75 nm, 100 nm, 150 nm, 250 nm, and 350 nm in diameters were 0.14 ± 0.07, 0.17 ± 0.05, 0.18 ± 0.06, 0.20 ± 0.07, 0.21 ± 0.09, and 0.23 ± 0.12, respectively, indicating the dominance of organics in the sub-micrometer urban aerosols. In the spring, summer, and autumn, the number fraction of hydrophilic particles increased with increasing particle size, resulting in an increasing trend of overall particle hygroscopicity with enhanced particle size. Differently, the overall mean κ values peaked in the range of 75–150 nm and decreased for particles larger than 150 nm in diameter during wintertime. Such size-dependency of κ in winter was related to the strong primary particle emissions from coal combustion during domestic heating period. The number fraction of hydrophobic particles such as freshly emitted soot decreased with increasing PM 2.5 mass concentration, indicating aged and internal mixed particles were dominant in the severe particulate matter pollution. Parameterization schemes of the HGF as a function of relative humidity (RH) and particle size between 50 and 350 nm were determined for different seasons and pollution levels. The HGF s calculated from the parameterizations agree well with the measured HGF s at 20–90% RH. The parameterizations can be applied to determine the hygroscopic growth of aerosol particles at ambient conditions for the area of Beijing (ultrafine and fine particles) and the North China plain (fine particles). [ABSTRACT FROM AUTHOR]

Particulate emissions from crop residue burning decrease the air quality as well as influence aerosol radiative properties on a regional scale. The North China Plain (NCP) is known for the large scale biomass burning (BB) of field residues, which often results in heavy haze pollution episodes across the region. We have been able to capture a unique BB episode during the international CAREBeijing-NCP intensive field campaign in Wangdu in the NCP (38.6°N, 115.2°E) from June to July 2014. It was found that aerosol particles originating from this BB event showed a significantly different mixing state compared with clean and non-BB pollution episodes. BB originated particles showed a narrower probability density function (PDF) of shrink factor (SF). And the maximum was found at shrink factor of 0.6, which is higher than in other episodes. The non-volatile particle number fraction during the BB episode decreased to 3% and was the lowest measured value compared to all other predefined episodes. To evaluate the influence of particle mixing state on aerosol single scattering albedo (SSA), SSA at different RHs was simulated using the measured aerosol physical-chemical properties. The differences between the calculated SSA for biomass burning, clean and pollution episodes are significant, meaning that the variation of SSA in different pollution conditions needs to be considered in the evaluation of aerosol direct radiative effects in the NCP. And the calculated SSA was found to be quite sensitive on the mixing state of BC, especially at low-RH condition. The simulated SSA was also compared with the measured values. For all the three predefined episodes, the measured SSA are very close to the calculated ones with assumed mixing states of homogeneously internal and core-shell internal mixing, indicating that both of the conception models are appropriate for the calculation of ambient SSA in the NCP. [ABSTRACT FROM AUTHOR]

The Arctic is a rapidly changing ecosystem, with complex aerosol-cloud-climate feedbacks contributing to more rapid warming of the region as compared to the mid-latitudes. Understanding changes to particle number concentration and size distributions is important to constraining estimates of the effect of anthropogenic activity on the region. During six years of semi-continuous measurements of particle number size distributions conducted near Utqiaġvik (Barrow), Alaska, 37 particle-growth events were observed. The majority of events occurred during spring and summer with a monthly maximum in June, similar to other Arctic sites. Based on backward air mass trajectory analysis, similar numbers of particle-growth events were influenced by marine (46%) and Prudhoe Bay air masses (33%), despite air primarily coming from the Arctic Ocean (75 ± 2% of days) compared to Prudhoe Bay (8 ± 2% of days). The corresponding normalized particle-growth event frequency suggests that emissions from Prudhoe Bay could induce an average of 92 particle-growth events, more than all other air mass sources combined, at Barrow annually. Prudhoe Bay is currently the third largest oil and gas field in the United States, and development in the Arctic region is expected to expand throughout the 21st century as the extent of summertime sea ice decreases. Elevated particle number concentrations due to human activity are likely to have profound impacts on climate change in the Arctic through direct, indirect, and surface albedo feedbacks, particularly through the addition of cloud condensation nuclei. [ABSTRACT FROM AUTHOR]

Lung Deposited Surface Area (LDSA) has been identified as a potential metric for the correlation of a physical aerosol particle properties with health outcomes. Currently, there is little urban LDSA data. As a case study, we investigated measurements of LDSA (alveolar) concentrations in a mid-size European city. LDSA and associated measurements were carried out over 1.5 years at an urban background site in Leicester, UK. Average LDSA concentrations in the cold (November–April) and warm (May–October) seasons of UK were 37 and 23 μm 2 cm −3 , respectively. LDSA correlates well (R 2 = 0.65–0.7, r = 0.77–0.8) with traffic related pollutants, such as equivalent black carbon (eBC) and NO X . We also report for the first time in the UK the correlation between an empirically derived LDSA and eBC. Furthermore, the effect of wind speed and direction on the LDSA was explored. Higher LDSA concentrations are observed at low wind speeds (1–2 m s −1 ), owing to local traffic emissions. In addition, the diurnal variation of LDSA showed a second peak in the afternoon under warm and relatively clean atmospheric conditions, which can be attributed to photochemical new particle formation (NPF) and growth into the Aitken mode range. These NPF events increased the average background LDSA concentrations from 15.5 to 35.5 μm 2 cm −3 , although they might not be health-relevant. Overall, the results support the notion that local traffic emissions are a major contributor to observed LDSA concentrations with a clear seasonal pattern with higher values during winter. [ABSTRACT FROM AUTHOR]

Methanesulfonic acid (MSA) has been widely used as a proxy for marine biogenic sources, but it is still a challenge to provide an accurate MSA mass concentration with high time resolution. This study offers an improved MSA quantification method using high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Particularly, the method was validated based on an excellent agreement with parallel offline measurements (slope = 0.88, R2 = 0.89). This comparison is much better than those using previously reported methods, resulting in underestimations of 31-54% of MSA concentration. With this new method, MSA mass concentrations were obtained during 4 North/South Atlantic cruises in spring and autumn of 2011 and 2012. The seasonal and spatial variation of the particulate MSA mass concentration as well as the MSA to non-sea-salt sulfate ratio (MSA:nssSO4) over the North/South Atlantic Ocean were determined for the first time. Seasonal variation of the MSA mass concentration was observed, with higher values in spring (0.03 ?g m-3) than in autumn (0.01 ?g m-3). The investigation of MSA:nssSO4 suggests a ubiquitous and significant influence of anthropogenic sources on aerosols in the marine boundary layer. [ABSTRACT FROM AUTHOR]

For atmospheric aerosol particles, the ubiquitous surfactants can significantly influence their hygroscopicity. However, the hygroscopicity of nanoscale particles containing surfactants are not well understood under subsaturated conditions, especially at high relative humidity (RH = 90–100%), due to the limitation of traditional instruments and the diversity of surfactants. Here, the hygroscopicity of nanoscale particles composed of a strong surfactant sodium dodecyl sulfate (SDS) and its mixture with ammonium sulfate (AS) was measured using the high humidity tandem differential mobility analyzer (HHTDMA) at RH up to about 99.9%. Three different models based on Köhler theory but different representations of surfactant characteristics were employed to reproduce the measurement outcomes. Results show that SDS particles start gradual hygroscopic growth after RH reaching 97.5%. For SDS-AS mixed particles with 25% w/w SDS, prompt deliquescence and gradual deliquescence are observed for smaller (20 and 40 nm) and larger particles (100 and 200 nm), respectively. For particles with ≥50% w/w SDS, the onset deliquescence is difficult to found. In general, the model that comprehensively accounts for the surfactant properties including bulk-to-surface partitioning, surface tension reduction, micellization and the effect of RH on hygroscopicity parameter, ĸ (for SDS-AS particles) provides the best predictions for the experimental hygroscopicity of SDS and SDS-AS particles at subsaturation conditions. Besides, factors affecting the accuracy of theoretical model are discussed in detail. The ĸ derived from subsaturated measurement is strongly dependent on RH and dry diameter. [Display omitted] • The hygroscopicity of SDS (SDS-AS) aerosols at RH up to 99.9% is measured by HHTDMA. • Models with different surfactant descriptions are adopted to predict hygroscopicity. • Accuracy of models and the mechanism of hygroscopicity are analyzed. • ĸ derived from subsaturated measurement is strongly dependent on RH and dry diameter. [ABSTRACT FROM AUTHOR]

The German Ultrafine Aerosol Network (GUAN) is a cooperative atmospheric observation network, which aims at improving the scientific understanding of aerosol-related effects in the troposphere. The network addresses research questions dedicated to both climate- and health-related effects. GUAN's core activity has been the continuous collection of tropospheric particle number size distributions and black carbon mass concentrations at 17 observation sites in Germany. These sites cover various environmental settings including urban traffic, urban background, rural background, and Alpine mountains. In association with partner projects, GUAN has implemented a high degree of harmonisation of instrumentation, operating procedures, and data evaluation procedures. The quality of the measurement data is assured by laboratory intercomparisons as well as on-site comparisons with reference instruments. [ABSTRACT FROM AUTHOR]

The particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOSCARIBIC observatory: In-service Aircraft for a Global Observing System - Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130-1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50%particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOSCARIBIC observatory. [ABSTRACT FROM AUTHOR]

The particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System -- Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130-1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50% particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98%. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory. [ABSTRACT FROM AUTHOR]