scholarly journals Physico-chemical characterisation of atmospheric aerosols in Tanzania, with emphasis on the carbonaceous aerosol components and on chemical mass closure

Afrika Focus ◽  
2008 ◽  
Vol 21 (2) ◽  
Author(s):  
Stelyus Lazaro Mkoma ◽  
Willy Maenhaut
Keyword(s):  
Atmospheric Aerosols ◽  
Carbonaceous Aerosol ◽  
Mass Closure ◽  
Physico Chemical ◽  
Chemical Mass Closure

scholarly journals Retrieval of desert dust and carbonaceous aerosol emissions over Africa from POLDER/PARASOL products generated by the GRASP algorithm

2018 ◽  
Vol 18 (16) ◽  
pp. 12551-12580 ◽  
Author(s):  
Cheng Chen ◽  
Oleg Dubovik ◽  
Daven K. Henze ◽  
Tatyana Lapyonak ◽  
Mian Chin ◽  
...  
Keyword(s):  
Optical Depth ◽  
Atmospheric Aerosols ◽  
Carbonaceous Aerosol ◽  
Desert Dust ◽  
Modelling Framework ◽  
Aerosol Absorption ◽  
Modelling Studies ◽  
Distribution Composition ◽  
Gocart Model ◽  
Aerosol Emissions

Abstract. Understanding the role atmospheric aerosols play in the Earth–atmosphere system is limited by uncertainties in the knowledge of their distribution, composition and sources. In this paper, we use the GEOS-Chem based inverse modelling framework for retrieving desert dust (DD), black carbon (BC) and organic carbon (OC) aerosol emissions simultaneously. Aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) retrieved from the multi-angular and polarimetric POLDER/PARASOL measurements generated by the GRASP algorithm (hereafter PARASOL/GRASP) have been assimilated. First, the inversion framework is validated in a series of numerical tests conducted with synthetic PARASOL-like data. These tests show that the framework allows for retrieval of the distribution and strength of aerosol emissions. The uncertainty of retrieved daily emissions in error free conditions is below 25.8 % for DD, 5.9 % for BC and 26.9 % for OC. In addition, the BC emission retrieval is sensitive to BC refractive index, which could produce an additional factor of 1.8 differences for total BC emissions. The approach is then applied to 1 year (December 2007 to November 2008) of data over the African and Arabian Peninsula region using PARASOL/GRASP spectral AOD and AAOD at six wavelengths (443, 490, 565, 670, 865 and 1020 nm). Analysis of the resulting retrieved emissions indicates 1.8 times overestimation of the prior DD online mobilization and entrainment model. For total BC and OC, the retrieved emissions show a significant increase of 209.9 %–271.8 % in comparison to the prior carbonaceous aerosol emissions. The model posterior simulation with retrieved emissions shows good agreement with both the AOD and AAOD PARASOL/GRASP products used in the inversion. The fidelity of the results is evaluated by comparison of posterior simulations with measurements from AERONET that are completely independent measurements and more temporally frequent than PARASOL observations. To further test the robustness of our posterior emissions constrained using PARASOL/GRASP, the posterior emissions are implemented in the GEOS-5/GOCART model and the consistency of simulated AOD and AAOD with other independent measurements (MODIS and OMI) demonstrates promise in applying this database for modelling studies.

scholarly journals Two-wavelength thermal–optical determination of light-absorbing carbon in atmospheric aerosols

2019 ◽  
Vol 12 (6) ◽  
pp. 3173-3182 ◽  
Author(s):  
Dario Massabò ◽  
Alessandro Altomari ◽  
Virginia Vernocchi ◽  
Paolo Prati
Keyword(s):  
Laser Diode ◽  
Atmospheric Aerosols ◽  
Direct Determination ◽  
Optical Transmittance ◽  
Carbonaceous Aerosol ◽  
Electromagnetic Spectrum ◽  
Multi Wavelength ◽  
Physics Department ◽  
The University

Abstract. Thermal–optical analysis is widely adopted for the quantitative determination of total (TC), organic (OC), and elemental (EC) carbon in atmospheric aerosol sampled by suitable filters. Nevertheless, the methodology suffers from several uncertainties and artifacts such as the well-known issue of charring affecting the OC–EC separation. In the standard approach, the effect of the possible presence of brown carbon, BrC, in the sample is neglected. BrC is a fraction of OC, usually produced by biomass burning with a thermic behavior intermediate between OC and EC. BrC is optically active: it shows an increasing absorbance when the wavelength moves to the blue–UV region of the electromagnetic spectrum. Definitively, the thermal–optical characterization of carbonaceous aerosol should be reconsidered to address the possible BrC content in the sample under analysis. We introduce here a modified Sunset Lab Inc. EC–OC analyzer. Starting from a standard commercial instrument, the unit has been modified at the physics department of the University of Genoa (Italy), making possible the alternative use of the standard laser diode at λ=635 nm and of a new laser diode at λ=405 nm. In this way, the optical transmittance through the sample can be monitored at both wavelengths. Since at shorter wavelengths the BrC absorbance is higher, a better sensitivity to this species is gained. The modified instrument also gives the possibility to quantify the BrC concentration in the sample at both wavelengths. The new unit has been thoroughly tested, with both artificial and real-world aerosol samples: the first experiment, in conjunction with the multi-wavelength absorbance analyzer (MWAA; Massabò et al., 2013, 2015), resulted in the first direct determination of the BrC mass absorption coefficient (MAC) at λ=405 nm: MAC =23±1 m2 g−1.

scholarly journals Geochemical perspectives from a new aerosol chemical mass closure

2007 ◽  
Vol 7 (6) ◽  
pp. 1657-1670 ◽  
Author(s):  
B. Guinot ◽  
H. Cachier ◽  
K. Oikonomou
Keyword(s):  
Urban Areas ◽  
Conversion Factor ◽  
Major Ions ◽  
Fine Fraction ◽  
Coarse Fraction ◽  
Urban Environments ◽  
Data Set ◽  
K Value ◽  
Mass Closure ◽  
Chemical Mass Closure

Abstract. The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC) and the black carbon (BC). Atmospheric particles are separated into coarse (AD>2 μm) and fine (AD<2 μm) fractions and are treated separately. For the coarse fraction the carbonaceous component is minor and assumption is made for the conversion factor k of OC-to-POM (Particulate Organic Matter) which is fixed to the value of 1.8 accounting for secondary species. The coarse soluble calcium is shown to display a correlation (regression coefficient f, y axis intercept b) with the missing mass. Conversely, the fine fraction is dominated by organic species and assumption is made for dust which is assumed to have the same f factor as the coarse mode dust. The fine mode mass obtained from chemical analyses is then adjusted to the actual weighed mass by tuning the k conversion factor. The k coefficient is kept different in the two modes due to the expected different origins of the organic particles. Using the f and k coefficient obtained from the data set, the mass closure is reached for each individual sample with an undetermined fraction less than 10%. The procedure has been applied to different urban and peri-urban environments in Europe and in Beijing and its efficiency and uncertainties on f and k values are discussed. The f and k coefficients are shown to offer consistent geochemical indications on aerosol origin and transformations. f allows to retrieve dust mass and its value accounting for Ca abundance in dust at the site of investigation may serve as an indicator of dust origin and aerosol interactions with anthropogenic acids. f values were found to vary in the 0.08–0.12 range in European urban areas, and a broader range in Beijing (0.01–0.16). As expected, k appears to be a relevant proxy for particle origin and ageing and varies in the 1.4–1.8 range. For Beijing, k exhibits high values of about 1.7 in winter and summer. Winter values suggest that fresh coal aerosol might be responsible for such a high k value, which was not taken into account in previous works.

scholarly journals Fossil versus contemporary sources of fine elemental and organic carbonaceous particulate matter during the DAURE campaign in Northeast Spain

2011 ◽  
Vol 11 (8) ◽  
pp. 23573-23618 ◽  
Author(s):  
M. C. Minguillón ◽  
N. Perron ◽  
X. Querol ◽  
S. Szidat ◽  
S. M. Fahrni ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Organic Carbon ◽  
Source Apportionment ◽  
Biomass Burning ◽  
Atmospheric Aerosols ◽  
Fine Particulate Matter ◽  
Western Mediterranean ◽  
Carbonaceous Aerosol ◽  
Carbonaceous Aerosols ◽  
Background Site

Abstract. We present results from the international field campaign DAURE (Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean), with the objective of apportioning the sources of fine carbonaceous aerosols. Submicron fine particulate matter (PM1) samples were collected during February-March 2009 and July 2009 at an urban background site in Barcelona (BCN) and at a forested regional background site in Montseny (MSY). We present radiocarbon (14C) analysis for elemental and organic carbon (EC and OC) and source apportionment for these data. We combine the results with those from component analysis of aerosol mass spectrometer (AMS) measurements, and compare to levoglucosan-based estimates of biomass burning OC, source apportionment of filter data with inorganic+EC+OC speciation, submicron bulk potassium (K) concentrations, and gaseous acetonitrile concentrations. At BCN, 87 % and 91 % of the EC on average, in winter and summer, respectively, had a fossil origin, whereas at MSY these fractions were 66 % and 79 %. The contribution of fossil sources to organic carbon (OC) at BCN was 40 % and 48 %, in winter and summer, respectively, and 31 % and 25 % at MSY. The combination of results obtained using the 14C technique, AMS data, and the correlations between fossil OC and fossil EC imply that the fossil OC at Barcelona is ~65 % primary whereas at MSY the fossil OC is mainly secondary (~85 %). Day-to-day variation in total carbonaceous aerosol loading and the relative contributions of different sources predominantly depended on the meteorological transport conditions. The estimated biogenic secondary OC at MSY only increased by ~40 % compared to the order-of-magnitude increase observed for biogenic volatile organic compounds (VOCs) between winter and summer, which highlights the uncertainties in the estimation of that component. Biomass burning contributions estimated using the 14C technique ranged from similar to higher than when estimated using other techniques, and the different estimations were highly or moderately correlated. Differences can be explained by the contribution of secondary organic matter (not included in the primary biomass burning source estimates), and/or by an overestimation of the biomass burning OC contribution by the 14C technique if the estimated biomass burning EC/OC ratio used for the calculations is too high for this region. Acetonitrile concentrations correlate well with the biomass burning EC determined by 14C. K is a noisy tracer for biomass burning.

scholarly journals Cloud Condensation Nuclei properties of model and atmospheric HULIS

2006 ◽  
Vol 6 (9) ◽  
pp. 2465-2482 ◽  
Author(s):  
E. Dinar ◽  
I. Taraniuk ◽  
E. R. Graber ◽  
S. Katsman ◽  
T. Moise ◽  
...  
Keyword(s):  
Molecular Weight ◽  
Fulvic Acid ◽  
Atmospheric Aerosols ◽  
Cloud Condensation Nuclei ◽  
Average Molecular Weight ◽  
Water Soluble ◽  
Cloud Droplets ◽  
Secondary Sources ◽  
Multifunctional Compounds ◽  
Physico Chemical

Abstract. Humic like substances (HULIS) have been identified as a major fraction of the organic component of atmospheric aerosols. These large multifunctional compounds of both primary and secondary sources are surface active and water soluble. Hence, it is expected that they could affect activation of organic aerosols into cloud droplets. We have compared the activation of aerosols containing atmospheric HULIS extracted from fresh, aged and pollution particles to activation of size fractionated fulvic acid from an aquatic source (Suwannee River Fulvic Acid), and correlated it to the estimated molecular weight and measured surface tension. A correlation was found between CCN-activation diameter of SRFA fractions and number average molecular weight of the fraction. The lower molecular weight fractions activated at lower critical diameters, which is explained by the greater number of solute species in the droplet with decreasing molecular weight. The three aerosol-extracted HULIS samples activated at lower diameters than any of the size-fractionated or bulk SRFA. The Köhler model was found to account for activation diameters, provided that accurate physico-chemical parameters are known.

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