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Characterization of ambient aerosols in Mexico City during the MCMA-2003 campaign with aerosol mass spectrometry
Dara Salcedo, T. B. Onasch, Katja Džepina, M. R. Canagaratna, Qi Zhang, J. A. Huffman, P. F. DeCarlo, J. Jayne, P. Mortimer, D. Worsnop, 2006, original scientific article

Abstract: An Aerodyne Aerosol Mass Spectrometer (AMS) was deployed at the CENICA Supersite, during the Mexico City Metropolitan Area field study (MCMA-2003) from 31 March-4 May 2003 to investigate particle concentrations, sources, and processes. The AMS provides real time information on mass concentration and composition of the non-refractory species in particulate matter less than 1 mu m (NR-PM1) with high time and size-resolution. In order to account for the refractory material in the aerosol, we also present estimates of Black Carbon (BC) using an aethalometer and an estimate of the aerosol soil component obtained from Proton-Induced X-ray Emission Spectrometry (PIXE) analysis of impactor substrates. Comparisons of AMS + BC + soil mass concentration with other collocated particle instruments (a LASAIR Optical Particle Counter, a PM2.5 Tapered Element Oscillating Microbalance (TEOM), and a PM2.5 DustTrak Aerosol Monitor) show that the AMS + BC + soil mass concentration is consistent with the total PM2.5 mass concentration during MCMA-2003 within the combined uncertainties. In Mexico City, the organic fraction of the estimated PM2.5 at CENICA represents, on average, 54.6% (standard deviation sigma=10%) of the mass, with the rest consisting of inorganic compounds ( mainly ammonium nitrate and sulfate/ammonium salts), BC, and soil. Inorganic compounds represent 27.5% of PM2.5 (sigma=10%); BC mass concentration is about 11% (sigma=4%); while soil represents about 6.9% (sigma=4%). Size distributions are presented for the AMS species; they show an accumulation mode that contains mainly oxygenated organic and secondary inorganic compounds. The organic size distributions also contain a small organic particle mode that is likely indicative of fresh traffic emissions; small particle modes exist for the inorganic species as well. Evidence suggests that the organic and inorganic species are not always internally mixed, especially in the small modes. The aerosol seems to be neutralized most of the time; however, there were some periods when there was not enough ammonium to completely neutralize the nitrate, chloride and sulfate present. The diurnal cycle and size distributions of nitrate suggest local photochemical production. On the other hand, sulfate appears to be produced on a regional scale. There are indications of new particle formation and growth events when concentrations of SO2 were high. Although the sources of chloride are not clear, this species seems to condense as ammonium chloride early in the morning and to evaporate as the temperature increases and RH decreases. The total and speciated mass concentrations and diurnal cycles measured during MCMA-2003 are similar to measurements during a previous field campaign at a nearby location.
Found in: osebi
Keywords: aerosol mass-spectrometer, atmospheric aerosol, atmospheric chemistry, atmospheric physics
Published: 12.04.2021; Views: 155; Downloads: 0
.pdf Fulltext (2,53 MB)

Implementation of a Markov Chain Monte Carlo method to inorganic aerosol modeling of observations from the MCMA-2003 campaign
F. M. San Martini, E. J. Dunlea, R. M. Volkamer, T. B. Onasch, J. Jayne, M. R. Canagaratna, D. Worsnop, C. E. Kolb, J. H. Shorter, Katja Džepina, 2006, original scientific article

Abstract: A Markov Chain Monte Carlo model for integrating the observations of inorganic species with a thermodynamic equilibrium model was presented in Part I of this series. Using observations taken at three ground sites, i. e. a residential, industrial and rural site, during the MCMA-2003 campaign in Mexico City, the model is used to analyze the inorganic particle and ammonia data and to predict gas phase concentrations of nitric and hydrochloric acid. In general, the model is able to accurately predict the observed inorganic particle concentrations at all three sites. The agreement between the predicted and observed gas phase ammonia concentration is excellent. The NOz concentration calculated from the NOy, NO and NO2 observations is of limited use in constraining the gas phase nitric acid concentration given the large uncertainties in this measure of nitric acid and additional reactive nitrogen species. Focusing on the acidic period of 9-11 April identified by Salcedo et al. ( 2006), the model accurately predicts the particle phase observations during this period with the exception of the nitrate predictions after 10: 00 a. m. ( Central Daylight Time, CDT) on 9 April, where the model underpredicts the observations by, on average, 20%. This period had a low planetary boundary layer, very high particle concentrations, and higher than expected nitrogen dioxide concentrations. For periods when the particle chloride observations are consistently above the detection limit, the model is able to both accurately predict the particle chloride mass concentrations and provide well-constrained HCl ( g) concentrations. The availability of gas-phase ammonia observations helps constrain the predicted HCl ( g) concentrations. When the particles are aqueous, the most likely concentrations of HCl ( g) are in the sub-ppbv range. The most likely predicted concentration of HCl ( g) was found to reach concentrations of order 10 ppbv if the particles are dry. Finally, the atmospheric relevance of HCl ( g) is discussed in terms of its indicator properties for the possible influence of chlorine-mediated photochemistry in Mexico City.
Found in: osebi
Keywords: secondary organic aerosols, Mexico City, MCMA-2003 field campaign, thermodynamic equilibrium
Published: 11.04.2021; Views: 129; Downloads: 0
.pdf Fulltext (1,37 MB)

Technical note
Dara Salcedo, T. B. Onasch, M. R. Canagaratna, Katja Džepina, J. A. Huffman, J. Jayne, D. Worsnop, C. E. Kolb, S. Weimer, F. Drewnick, 2007, original scientific article

Abstract: Two Aerodyne Aerosol Mass Spectrometers (Q-AMS) were deployed in Mexico City, during the Mexico City Metropolitan Area field study (MCMA-2003) from 29 March - 4 May 2003 to investigate particle concentrations, sources, and processes. We report the use of a particle beam width probe (BWP) in the field to quantify potential losses of particles due to beam broadening inside the AMS caused by particle shape (nonsphericity) and particle size. Data from this probe show that no significant mass of particles was lost due to excessive beam broadening; i.e. the shape- and size-related collection efficiency (E-s) of the AMS during this campaign was approximately one. Comparison of the BWP data from MCMA-2003 with other campaigns shows that the same conclusion holds for several other urban, rural and remotes sites. This means that the aerodynamic lens in the AMS is capable of efficiently focusing ambient particles into a well defined beam and onto the AMS vaporizer for particles sampled in a wide variety of environments. All the species measured by the AMS during MCMA-2003 have similar attenuation profiles which suggests that the particles that dominate the mass concentration were internally mixed most of the time. Only for the smaller particles ( especially below 300 nm), organic and inorganic species show different attenuation versus particle size which is likely due to partial external mixing of these components. Changes observed in the focusing of the particle beam in time can be attributed, in part, to changes in particle shape (i.e. due to relative humidity) and size of the particles sampled. However, the relationships between composition, atmospheric conditions, and particle shape and size appear to be very complex and are not yet completely understood.
Found in: osebi
Keywords: atmospheric aerosol, organic aerosols, aerodynamic lenses, Mexico City
Published: 11.04.2021; Views: 125; Downloads: 0
.pdf Fulltext (341,65 KB)

Evolution of organic aerosols in the atmosphere
J. H. Kroll, P. F. DeCarlo, J. David Allan, H. Coe, Katja Džepina, Jose L. Jimenez, M. R. Canagaratna, N. M. Donahue, A. S. H. Prevot, Q. Zhang, 2009, original scientific article

Abstract: Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high–time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.
Found in: osebi
Keywords: secondary organic aerosol, source apportionment, aerodyne aerosol mass spectrometer, global field measurements, laboratory experiments
Published: 11.04.2021; Views: 117; Downloads: 0
.pdf Fulltext (721,30 KB)

Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes
Q. Zhang, Jose L. Jimenez, M. R. Canagaratna, J. David Allan, H. Coe, I. M. Ulbrich, M. R. Alfarra, A. Takami, A. M. Middlebrook, Katja Džepina, 2007, original scientific article

Abstract: Organic aerosol (OA) data acquired by the Aerosol Mass Spectrometer (AMS) in 37 field campaigns were deconvolved into hydrocarbon-like OA (HOA) and several types of oxygenated OA (OOA) components. HOA has been linked to primary combustion emissions (mainly from fossil fuel) and other primary sources such as meat cooking. OOA is ubiquitous in various atmospheric environments, on average accounting for 64%, 83% and 95% of the total OA in urban, urban downwind, and rural/remote sites, respectively. A case study analysis of a rural site shows that the OOA concentration is much greater than the advected HOA, indicating that HOA oxidation is not an important source of OOA, and that OOA increases are mainly due to SOA. Most global models lack an explicit representation of SOA which may lead to significant biases in the magnitude, spatial and temporal distributions of OA, and in aerosol hygroscopic properties.
Found in: osebi
Keywords: atmospheric aerosol, secondary organic aerosols, primary organic aerosols, aerodyne aerosol mass spectrometer
Published: 11.04.2021; Views: 151; Downloads: 0
.pdf Fulltext (1,15 MB)

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