Using Raman-lidar-based regularized microphysical retrievals and Aerosol Mass Spectrometer measurements for the characterization of biomass burning aerosols

2015 ◽  
Vol 299 ◽  
pp. 156-174 ◽  
Author(s):  
Stefanos Samaras ◽  
Doina Nicolae ◽  
Christine Böckmann ◽  
Jeni Vasilescu ◽  
Ioannis Binietoglou ◽  
...  
2015 ◽  
Vol 15 (20) ◽  
pp. 11807-11833 ◽  
Author(s):  
W. W. Hu ◽  
P. Campuzano-Jost ◽  
B. B. Palm ◽  
D. A. Day ◽  
A. M. Ortega ◽  
...  

Abstract. Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3 ‰) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a triangle plot of fCO2 vs. fC5H6O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2, if the fC5H6O of the local IEPOX-SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.


2013 ◽  
Vol 6 (11) ◽  
pp. 3271-3280 ◽  
Author(s):  
L. R. Williams ◽  
L. A. Gonzalez ◽  
J. Peck ◽  
D. Trimborn ◽  
J. McInnis ◽  
...  

Abstract. We have designed and characterized a new inlet and aerodynamic lens for the Aerodyne aerosol mass spectrometer (AMS) that transmits particles between 80 nm and more than 3 μm in vacuum aerodynamic diameter. The design of the inlet and lens was optimized with computational fluid dynamics (CFD) modeling of particle trajectories. Major changes include a redesigned critical orifice holder and valve assembly, addition of a relaxation chamber behind the critical orifice, and a higher lens operating pressure. The transmission efficiency of the new inlet and lens was characterized experimentally with size-selected particles. Experimental measurements are in good agreement with the calculated transmission efficiency.


2004 ◽  
Vol 4 (1) ◽  
pp. 65-80 ◽  
Author(s):  
J. Schneider ◽  
S. Borrmann ◽  
A. G. Wollny ◽  
M. Bläsner ◽  
N. Mihalopoulos ◽  
...  

Abstract. Mass spectrometric analysis of volatile and semi-volatile (=non-refractory) aerosol particles have been performed during a field study in the summer Eastern Mediterranean. A size-resolved, quantitative mass spectrometric technique (the Aerodyne Aerosol Mass Spectrometer, AMS) has been used, and the results are compared to filter sampling methods and particle sizing techniques. The different techniques agree with the finding that the fine particle mode (D<1.2 mm) consisted mostly of ammonium sulfate and of organic material. The aerosol sulfate ranged between 2 and 12 mg/m3. On most days, ammonium was closely correlated with sulfate, suggesting ammonium sulfate as the major aerosol component, but on days with high sulfate mass concentrations, the sulfate was not fully neutralized by ammonium. Trajectories indicate that the aerosol and/or its precursors originate from South-Eastern Europe. The source of the ammonium sulfate aerosol is most likely fossil fuel burning, whereas the organic aerosol may also originate from biomass burning. Ion series analysis of the organics fraction in the mass spectrometer indicated that the major component of the organics were oxygenated organics which are a marker for aged, photochemically processed aerosol or biomass burning aerosol. The non-refractory aerosol compounds, measured with the Aerosol Mass Spectrometer, contributed between 37 and 50% to the total aerosol mass in the fine mode. A second mass spectrometer for single particle analysis by laser ablation has been used for the first time in the field during this study and yielded results, which agree with filter samples of the coarse particle mode. This mode consisted of sea salt particles and dust aerosol.


2005 ◽  
Vol 39 (8) ◽  
pp. 760-770 ◽  
Author(s):  
N. Takegawa ◽  
Y. Miyazaki ◽  
Y. Kondo ◽  
Y. Komazaki ◽  
T. Miyakawa ◽  
...  

2015 ◽  
Vol 32 (6) ◽  
pp. 877-888 ◽  
Author(s):  
Junke Zhang ◽  
Yuesi Wang ◽  
Xiaojuan Huang ◽  
Zirui Liu ◽  
Dongsheng Ji ◽  
...  

2009 ◽  
Vol 9 (11) ◽  
pp. 3709-3720 ◽  
Author(s):  
M. Dall'Osto ◽  
R. M. Harrison ◽  
H. Coe ◽  
P. I. Williams ◽  
J. D. Allan

Abstract. Nitrate aerosols make a very major contribution to PM2.5 and PM10 in western Europe, but their sources and pathways have not been fully elucidated. An Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) and a Compact Time of Flight Aerosol Mass Spectrometer (C-ToF-AMS) were deployed in an urban background location in London, UK, collecting data as part of the REPARTEE-I experiment. During REPARTEE-I, daily PM10 concentrations ranged up to 43.6 μg m−3, with hourly nitrate concentrations (measured by AMS) of up to 5.3 μg m−3. The application of the ART-2a neural network algorithm to the ATOFMS data characterised the nitrate particles as occurring in two distinct clusters (i.e. particle types). The first (33.6% of particles by number) appeared to be locally produced in urban locations during nighttime, whilst the second (22.8% of particles by number) was regionally transported from continental Europe. Nitrate in locally produced aerosol was present mainly in particles smaller than 300 nm, whilst the regional nitrate presented a coarser mode, peaking at 600 nm. In both aerosol types, nitrate was found to be internally mixed with sulphate, ammonium, elemental and organic carbon. Nitrate in regional aerosol appeared to be more volatile than that locally formed. During daytime, a core of the regionally transported nitrate aerosol particle type composed of organic carbon and sulphate was detected.


2011 ◽  
Vol 11 (10) ◽  
pp. 27383-27420 ◽  
Author(s):  
C. Mohr ◽  
P. F. DeCarlo ◽  
M. F. Heringa ◽  
R. Chirico ◽  
J. G. Slowik ◽  
...  

Abstract. PM1 (particulate matter with an aerodynamic diameter <1 μm) non-refractory components and black carbon were measured continuously together with additional parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O/C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O/C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at m/z 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C3H3O+ and C3H5O+, even though their contributions to m/z 55 and 57 are low compared to the reduced ions C4H7+ and C4H9+. A simple estimation method based on the organic mass fragments at m/z 55, 57, and 44 is developed here and allows for a first-order-estimation of COA in urban air. This study emphasizes the importance of cooking activities for ambient air quality and confirms the importance of chemical composition measurements with a high mass and time resolution.


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