Individual aerosol particles from biomass burning in southern Africa: 1. Compositions and size distributions of carbonaceous particles

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy ( TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic ( K- salt) inclusions, " tar ball'' particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged ( similar to 1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/ sulfate and soot/ sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/ sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea- salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles

Aerosol light absorption in the North Atlantic: trends and seasonal characteristics during the period 1989 to 2003

Aerosol light attenuation on quartz fibre filters has been measured since February 1989 at the Mace Head Atmospheric Research station near Carna, Co. Galway, Ireland, using an Aethalometer. <P style='line-height: 20px;'> The frequency of occurrence of the hourly averaged aerosol absorption data is found to be bimodally distributed. The two modes result from clean marine air and anthropogenically polluted continental air both being advected to the station dependent on the prevailing wind direction. The hourly averages of the marine portion of the aerosol light absorption are found to follow closely a lognormal distribution with a geometric mean of 0.310&nbsp;Mm^-1. The&nbsp;hourly averages of continental sector aerosol absorption are neither normally nor lognormally distributed and have an arithmetic mean of 6.36&nbsp;Mm^-1, indicating the presence of anthropogenic sources for BC east of the Mace Head station. <P style='line-height: 20px;'> The time series of the monthly averaged attenuation coefficient &sigma;_att of both marine and continental sector aerosol shows an increase from 1989 to 1997 and a levelling off thereafter. <P style='line-height: 20px;'> The monthly maximum of marine sector &sigma;_att is found in May. Trend and seasonal characteristics of the clean marine aerosol attenuation coefficients observed at Mace Head appear to be driven by meteorological factors, as indicated by rainfall data and by trends in&nbsp;the North Atlantic Oscillation (NAO) indices. The observed increasing trends of the continental sector &sigma;_att from 1989 up to 1997 are possibly related to changes in BC emissions over Ireland, calculated from UNSTAT (2002) fuel consumption data

Regularization in Image Non-Rigid Registration: I. Trade-off between Smoothness and Intensity Similarity

In this report, we first propose a new classification of non-rigid registratio- n algorithms into three main categories: in one hand, the geometric algorithms- , and in the other hand, intensity based methods that we split here into standard intensity-based (SIB) and pair-and-smooth (P&S) algorithms. We then focus on the subset of SIB and P&S algorithms that are competitive, i.e. that use a regularization energy which is minimized together with the intensity similarity energy. In SIB algorithms, these two energies are combined in a weighted sum, and thus the trade-off between them is direct. P&S algorithms alternates their respective minimization, leading to the characteristic two steps: pairing of points, and smoothing. We theoretically compare the behavior of SIB and P&S algorithms, and more precisely, we explain why in practice the smoothness of the transforms estimated by SIB algorithms is non-uniform, thus difficult to control, while P&S algorithms estimate a motion that is more uniformly smooth. We give an example illustrating this behavior. Very few P&S algorithms minimize a global energy. We therefore propose a new image registration energy whose minimization leads to a \PAS algorithm. This energy is general, and can use any existing similarity or regularization energy. Its behavior is also compared to the previous SIB and \PAS algorithms. This new energy allows uniformly smooth solutions, as for our previous P&S algorithm, while preventing registration of non-informative, noisy areas, as for SIB algorithms

Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July–August 2001: a multi-analytical approach

International audienceDuring the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T>550ºC) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) mass concentrations were on average respectively 1.19±0.56 and 3.62±1.08 mgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 mgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope=1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between these two methods for determining BC brings here new insights on the origin of carbonaceous aerosols in a complex mixture of different sources. It brings also to our attention that important deviations in BC levels are observed using three widely used EGA's techniques and most probably none of the EGA tested here are well adapted to fully characterize this aerosol mixture. Spherical, smooth and silico-aluminated fly-ash observed by an Analytical Scanning Electron Microscope (ASEM) confirm the influence of coal combustion on the carbonaceous aerosol load throughout the campaign. A rough calculation based on a BC/nss-SO4 mass ratio suggests that biomass burning could be responsible for half of the BC concentration recorded during the MINOS campaign. From the plot of BC as a function of TC, two linear correlations were observed corresponding to 2 times series (before and after 12 August). Such good correlations suggest, from a first look, that both BC and OC have similar origin and atmospheric transport. On the other hand, the plot of BC as a function of TC obtained from the 2-step thermal method applied to DEKATI Low Pressure Cascade Impactor samples does not show a similar correlation and points out a non conservative distribution of this ratio with 2 super micron modes enriched in OC, correlated with sea salt aerosols and probably originating from gas-to-particle conversion

Long-term measurements of carbonaceous aerosols in the Eastern Mediterranean: evidence of long-range transport of biomass burning

Long-term (5-year) measurements of Elemental Carbon (EC) and Organic Carbon (OC) in bulk aerosols are presented here for the first time in the Mediterranean Basin (Crete Island). A multi-analytical approach (including thermal, optical, and thermo-optical techniques) was applied for these EC and OC measurements. Light absorbing dust aerosols were shown to poorly contribute (+12% on a yearly average) to light absorption coefficient (&lt;i&gt;b&lt;/i&gt;&lt;sub&gt;abs&lt;/sub&gt;) measurements performed by an optical method (aethalometer). Long-range transport of agricultural waste burning from European countries surrounding the Black Sea was shown for each year during two periods (March–April and July–September). The contribution of biomass burning to the concentrations of EC and OC was shown to be rather small (20 and 14%, respectively, on a yearly basis), although this contribution could be much higher on a monthly basis and showed important seasonal and interannual variability. By removing the biomass burning influence, our data revealed an important seasonal variation of OC, with an increase by almost a factor of two for the spring months of May and June, whereas BC was found to be quite stable throughout the year. Preliminary measurements of Water Soluble Organic Carbon (WSOC) have shown that the monthly mean WSOC/OC ratio remains stable throughout the year (0.45&amp;plusmn;0.12), suggesting that the partitioning between water soluble and water insoluble organic matter is not significantly affected by biomass burning and secondary organic aerosol (SOA) formation. A chemical mass closure performed in the fine mode (Aerodynamic Diameter, A.D.&amp;lt;1.5μm) showed that the mass contribution of organic matter (POM) was found to be essentially invariable during the year (monthly average of 26&amp;plusmn;5%)

Fast Non Rigid Matching by Gradient Descent: Study and Improvements of the "Demons" Algorithm

Most iconic methods for rigid matching consist in finding and minimizing a registration criterion specifically chosen to solve a given problem. For non-rigid matching, attention has rather focussed on the type of smoothing or physical model of deformation to be used. In this report, we propose to place the non-rigid matching problem into a minimization framework. We have developped our theoretical idea in the case of the least squares criterion, corresponding to the assumption that the intensities of points do not change over time, and we have implemented a first order gradient descent which, along with a multiresolution approach, minimizes this criterion- . We also prove that the «demons» algorithm, thought of until now as an as hoc matching technique, can be seen as an approximation of a second order gradient descent on this criterion. Analysis of the mechanisms of this gradient descent incites us to introduce two different weightings into the filters used to smooth the solution, which we called an a priori weighting improves the solution found for the minimization problem, which is shown by comparing results in a distance-roughness space, while the a posteriori weighting helps tackle the appearance or disappearance of matter and occlusions, both sensitive issues for non-rigid iconic methods

Size-partitioning of an urban aerosol to identify particle determinants involved in the proinflammatory response induced in airway epithelial cells

<p>Abstract</p> <p>Background</p> <p>The contribution of air particles in human cardio-respiratory diseases has been enlightened by several epidemiological studies. However the respective involvement of coarse, fine and ultrafine particles in health effects is still unclear. The aim of the present study is to determine which size fraction from a chemically characterized background aerosol has the most important short term biological effect and to decipher the determinants of such a behaviour.</p> <p>Results</p> <p>Ambient aerosols were collected at an urban background site in Paris using four 13-stage low pressure cascade impactors running in parallel (winter and summer 2005) in order to separate four size-classes (PM_0.03–0.17(defined here as ultrafine particles), PM_0.17–1(fine), PM_1–2.5(intermediate) and PM_2.5–10(coarse)). Accordingly, their chemical composition and their pro-inflammatory potential on human airway epithelial cells were investigated. Considering isomass exposures (same particle concentrations for each size fractions) the pro-inflammatory response characterized by Granulocyte Macrophage-Colony Stimulating Factor (GM-CSF) release was found to decrease with aerosol size with no seasonal dependency. When cells were exposed to isovolume of particle suspensions in order to respect the particle proportions observed in ambient air, the GM-CSF release was maximal with the fine fraction. In presence of a recombinant endotoxin neutralizing protein, the GM-CSF release induced by particles is reduced for all size-fractions, with exception of the ultra-fine fraction which response is not modified. The different aerosol size-fractions were found to display important chemical differences related to the various contributing primary and secondary sources and aerosol age. The GM-CSF release was correlated to the organic component of the aerosols and especially its water soluble fraction. Finally, Cytochrome P450 1A1 activity that reflects PAH bioavailability varied as a function of the season: it was maximal for the fine fraction in winter and for the ultrafine fraction in summer.</p> <p>Conclusion</p> <p>In the frame of future regulations, a particular attention should thus be paid to the ultrafine/fine (here referred to as PM1) fraction due to their overwhelming anthropogenic origin and predominance in the urban aerosol and their pro-inflammatory potential.</p

Measurements of carbonaceous aerosols at urban and remote marine sites

Concentrations of total carbon (TC) and black carbon (BC) in ambient air at Delhi (urban site) and over Indian Ocean (remote marine) were determined as a part of INDOEX programme. Over Indian Ocean, the TC and BC concentrations varied from 1.81 to 10.05 &#956;g/m3 and 0.13 to 1.36 &#956;g/m3 respectively during FFP-98. During the same season at Delhi, the TC and BC ranged from 7.50 to 40.27 &#956;g/m3 and 0.49 to 2.84 &#956;g/m3 respectively. In addition, at Delhi, the TC and BC concentrations were noticed very low during the monsoon season. However, the percentage BC during monsoon season was very high compared to winter season. High concentrations of TC were observed due to high organic carbon (OC) which might be due to biomass burning of various kinds. Similar to Delhi, near Indian coast, the concentration of OC was very high while towards ITCZ and across ITCZ, OC content was relatively lower

Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July–August 2001: a multi-analytical approach

During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T>550ºC) under the pure helium step of the analysis.<br> <br> During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) mass concentrations were on average respectively 1.19±0.56 and 3.62±1.08 <font face='Symbol'>m</font>gC/m³ for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 <font face='Symbol'>m</font>gC/m³ for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope=1.00, <i>r</i>²=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO₄), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between these two methods for determining BC brings here new insights on the origin of carbonaceous aerosols in a complex mixture of different sources. It brings also to our attention that important deviations in BC levels are observed using three widely used EGA's techniques and most probably none of the EGA tested here are well adapted to fully characterize this aerosol mixture.<br> <br> Spherical, smooth and silico-aluminated fly-ash observed by an Analytical Scanning Electron Microscope (ASEM) confirm the influence of coal combustion on the carbonaceous aerosol load throughout the campaign. A rough calculation based on a BC/nss-SO₄ mass ratio suggests that biomass burning could be responsible for half of the BC concentration recorded during the MINOS campaign.<br> <br> From the plot of BC as a function of TC, two linear correlations were observed corresponding to 2 times series (before and after 12 August). Such good correlations suggest, from a first look, that both BC and OC have similar origin and atmospheric transport. On the other hand, the plot of BC as a function of TC obtained from the 2-step thermal method applied to DEKATI Low Pressure Cascade Impactor samples does not show a similar correlation and points out a non conservative distribution of this ratio with 2 super micron modes enriched in OC, correlated with sea salt aerosols and probably originating from gas-to-particle conversion