Off-Line Data Evaluation of Elemental Maps Obtained from Scanning Nuclear Microprobe Analyses

The results of scanning nuclear microprobe (SNM) analyses are normally presented as elemental maps showing the number of detector events, acquired within a certain energy region, for every pixel irradiated. Such elemental maps can be misleading if they are interpreted as directly reflecting the variations in the elemental concentrations across the analysed sample. The aim of this paper is to demonstrate how such elemental maps can be treated in order to facilitate the interpretation and extract the information contained in the data set, such as the covariation between elements. Examples of sample thickness correction, image processing and spectrum filtering as well as multivariate statistical data reduction are given

Aerosol exposure versus aerosol cooling of climate: what is the optimal emission reduction strategy for human health?

Particles, climate change, and health have thought-provoking interactions. Air pollution is one of the largest environmental problems concerning human health. On the other hand, aerosol particles can have a cooling effect on climate and a reduction of those emissions may result in an increased temperature globally, which in turn may have negative health effects. The objective of this work was to investigate the "total health effects" of aerosol emissions, which include both exposure to particles and consequences for climate change initiated by particles. As a case study the "total health effect" from ship emissions was derived by subtracting the number of deaths caused by exposure with the estimated number of lives saved from the cooling effect of the emissions. The analysis showed that, with current level of scientific understanding, it could not be determined whether ship emissions are negative or positive for human health on a short time scale. This first attempt to approximate the combined effect of particle emissions on health shows that reductions of particulate air pollution will in some cases (black carbon) have win-win effects on health and climate, but sometimes also cause a shift from particle exposure-related health effects towards an increasing risk of health consequences from climate change. Thus, measures to reduce aerosol emissions have to be coupled with climate change mitigation actions to achieve a full health benefit on a global level

Results and recommendations from an intercomparison of six Hygroscopicity-TDMA systems

The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyser (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonise H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty, and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulphate particles or an external mixture of ammonium sulphate and soot particles. The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. Measurements of ammonium sulphate aerosol found deviations equivalent to 4.5% RH from the set point of 90% RH compared to results from previous experiments in the literature. Evaluation of the number fraction of particles within the clearly separated growth factor modes of a laboratory generated externally mixed aerosol was done. The data from the H-TDMAs was analysed with a single fitting routine to investigate differences caused by the different data evaluation procedures used for each H-TDMA. The differences between the H-TDMAs were reduced from +12/-13% to +8/-6% when the same analysis routine was applied. We conclude that a common data evaluation procedure to determine number fractions of externally mixed aerosols will improve the comparability of H-TDMA measurements. It is recommended to ensure proper calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the aerosol humidification unit and the second DMA and to monitor these temperatures to an accuracy of 0.2 degrees C. For the correct determination of external mixtures, it is necessary to take into account size-dependent losses due to diffusion in the plumbing between the DMAs and in the aerosol humidification unit.Peer reviewe

Size distribution and hygroscopic properties of aerosol particles from dry-season biomass burning in Amazonia

International audienceAerosol particle number size distributions and hygroscopic properties were measured at a pasture site in the southwestern Amazon region (Rondonia). The measurements were performed 11 September-14 November 2002 as part of LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia - SMOke aerosols, Clouds, rainfall and Climate), and cover the later part of the dry season (with heavy biomass burning), a transition period, and the onset of the wet period. Particle number size distributions were measured with a DMPS (Differential Mobility Particle Sizer, 3-850nm) and an APS (Aerodynamic Particle Sizer), extending the distributions up to 3.3 µm in diameter. An H-TDMA (Hygroscopic Tandem Differential Mobility Analyzer) measured the hygroscopic diameter growth factors (Gf) at 90% relative humidity (RH), for particles with dry diameters (dp) between 20-440 nm, and at several occasions RH scans (30-90% RH) were performed for 165nm particles. These data provide the most extensive characterization of Amazonian biomass burning aerosol, with respect to particle number size distributions and hygroscopic properties, presented until now. The evolution of the convective boundary layer over the course of the day causes a distinct diel variation in the aerosol physical properties, which was used to get information about the properties of the aerosol at higher altitudes. The number size distributions averaged over the three defined time periods showed three modes; a nucleation mode with geometrical median diameters (GMD) of ~12 nm, an Aitken mode (GMD=61-92 nm) and an accumulation mode (GMD=128-190 nm). The two larger modes were shifted towards larger GMD with increasing influence from biomass burning. The hygroscopic growth at 90% RH revealed a somewhat external mixture with two groups of particles; here denoted nearly hydrophobic (Gf~1.09 for 100 nm particles) and moderately hygroscopic (Gf~1.26). While the hygroscopic growth factors were surprisingly similar over the periods, the number fraction of particles belonging to each hygroscopic group varied more, with the dry period aerosol being more dominated by nearly hydrophobic particles. As a result the total particle water uptake rose going into the cleaner period. The fraction of moderately hygroscopic particles was consistently larger for particles in the accumulation mode compared to the Aitken mode for all periods. Scanning the H-TDMA over RH (30-90% RH) showed no deliquescence behavior. A parameterization of both Gf(RH) and Gf(dp), is given

Physical properties of the sub-micrometer aerosol over the Amazon rain forest during the wet-to-dry season transition - comparison of modeled and measured CCN concentrations

Sub-micrometer atmospheric aerosol particles were studied in the Amazon region, 125 km northeast of Manaus, Brazil (-1°55.2'S, 59°28.1'W). The measurements were performed during the wet-to-dry transition period, 4-28 July 2001 as part of the LBA (Large-Scale Biosphere Atmosphere Experiment in Amazonia) CLAIRE-2001 (Cooperative LBA Airborne Regional Experiment) experiment. The number size distribution was measured with two parallel differential mobility analyzers, the hygroscopic growth at 90% RH with a Hygroscopic Tandem Mobility Analyzer (H-TDMA) and the concentrations of cloud condensation nuclei (CCN) with a cloud condensation nuclei counter. A model was developed that uses the H-TDMA data to predict the number of soluble molecules or ions in the individual particles and the corresponding minimum particle diameter for activation into a cloud droplet at a certain supersaturation. Integrating the number size distribution above this diameter, CCN concentrations were predicted with a time resolution of 10 min and compared to the measured concentrations. During the study period, three different air masses were identified and compared: clean background, air influenced by aged biomass burning, and moderately polluted air from recent local biomass burning. For the clean period 2001, similar number size distributions and hygroscopic behavior were observed as during the wet season at the same site in 1998, with mostly internally mixed particles of low diameter growth factor (~1.3 taken from dry to 90% RH). During the periods influenced by biomass burning the hygroscopic growth changed slightly, but the largest difference was seen in the number size distribution. The CCN model was found to be successful in predicting the measured CCN concentrations, typically within 25%. A sensitivity study showed relatively small dependence on the assumption of which model salt that was used to predict CCN concentrations from H-TDMA data. One strength of using H-TDMA data to predict CCN concentrations is that the model can also take into account soluble organic compounds, insofar as they go into solution at 90% RH. Another advantage is the higher time resolution compared to using size-resolved chemical composition data

Quantification of differences between occupancy and total monitoring periods for better assessment of exposure to particles in indoor environments

For the assessment of personal exposure, information about the concentration of pollutants when people are in given indoor environments (occupancy time) are of prime importance. However this kind of data frequently is not reported. The aim of this study was to assess differences in particle characteristics between occupancy time and the total monitoring period, with the latter being the most frequently used averaging time in the published data. Seven indoor environments were selected in Sweden and Finland: an apartment, two houses, two schools, a supermarket, and a restaurant. They were assessed for particle number and mass concentrations and number size distributions. The measurements using a Scanning Mobility Particle Sizer and two photometers were conducted for seven consecutive days during winter in each location. Particle concentrations in residences and schools were, as expected, the highest during occupancy time. In the apartment average and median PM2.5 mass concentrations during the occupancy time were 29% and 17% higher, respectively compared to total monitoring period. In both schools, the average and medium values of the PM2.5 mass concentrations were on average higher during teaching hours compared to the total monitoring period by 16% and 32%, respectively. When it comes to particle number concentrations (PNC), in the apartment during occupancy, the average and median values were 33% and 58% higher, respectively than during the total monitoring period. In both houses and schools the average and median PNC were similar for the occupancy and total monitoring periods. General conclusions on the basis of measurements in the limited number of indoor environments cannot be drawn. However the results confirm a strong dependence on type and frequency of indoor activities that generate particles and site specificity. The results also indicate that the exclusion of data series during non-occupancy periods can improve the estimates of particle concentrations and characteristics suitable for exposure assessment, which is crucial for estimating health effects in epidemiological and toxicological studies. (C) 2014 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/3.0/).Peer reviewe

Cloud condensation nuclei closure study on summer arctic aerosol

We present an aerosol – cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker <i>Oden</i>. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker <i>Oden</i> was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. <br><br> CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. <br><br> For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble (κ<sub>org</sub>=0.02), leading to a mean total κ, κ<sub>tot</sub>, of 0.33 ± 0.13. However, several settings led to closure and κ<sub>org</sub>=0.2 is found to be an upper limit at 0.1% supersaturation. κ<sub>org</sub>≤0.2 leads to a κ<sub>tot</sub> range of 0.33 ± 013 to 0.50 ± 0.11. Thus, the organic material ranges from being sparingly soluble to effectively insoluble. These results suggest that an increase in organic mass fraction in particles of a certain size would lead to a suppression of the Arctic CCN activity

Organic aerosol and global climate modelling: a review

The present paper reviews existing knowledge with regard to Organic Aerosol (OA) of importance for global climate modelling and defines critical gaps needed to reduce the involved uncertainties. All pieces required for the representation of OA in a global climate model are sketched out with special attention to Secondary Organic Aerosol (SOA): The emission estimates of primary carbonaceous particles and SOA precursor gases are summarized. The up-to-date understanding of the chemical formation and transformation of condensable organic material is outlined. Knowledge on the hygroscopicity of OA and measurements of optical properties of the organic aerosol constituents are summarized. The mechanisms of interactions of OA with clouds and dry and wet removal processes parameterisations in global models are outlined. This information is synthesized to provide a continuous analysis of the flow from the emitted material to the atmosphere up to the point of the climate impact of the produced organic aerosol. The sources of uncertainties at each step of this process are highlighted as areas that require further studies

Particulate PAH Emissions from Residential Biomass Combustion: Time-Resolved Analysis with Aerosol Mass Spectrometry

Time-resolved emissions of particulate polycyclic aromatic hydrocarbons (PAHs) and total organic particulate matter (OA) from a wood log stove and an adjusted pellet stove were investigated with high-resolution time-of-flight aerosol mass spectrometry (ANIS). The highest OA emissions were found during the addition of log wood on glowing embers, that is, slow burning pyrolysis conditions. These emissions contained about 1% PAHs (of OA). The highest PAH emissions were found during fast burning under hot air starved combustion conditions, in both stoves. In the latter case, PAHs contributed up to 40% of OA, likely due to thermal degradation of other condensable species. The distribution of PAHs was also shifted toward larger molecules in these emissions. ANIS signals attributed to PAHs were found at molecular weights up to 600 Da. The vacuum aerodynamic size distribution was found to be bimodal with a smaller mode (D-va similar to 200 nm) dominating under hot air starved combustion and a larger sized mode dominating under slow burning pyrolysis (D-va similar to 600 nm). Simultaneous reduction of PAHs, OA and total particulate matter from residential biomass combustion may prove to be a challenge for environmental legislation efforts as these classes of emissions are elevated at different combustion conditions