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Evaluation of recently-proposed secondary organic aerosol models for a case study in Mexico City
Katja Džepina, R. M. Volkamer, Sasha Madronich, P. Tulet, I. M. Ulbrich, Q. Zhang, C. D. Cappa, P. J. Ziemann, Jose L. Jimenez, 2009, izvirni znanstveni članek

Opis: Recent field studies have found large discrepancies in the measured vs. modeled SOA mass loadings in both urban and regional polluted atmospheres. The reasons for these large differences are unclear. Here we revisit a case study of SOA formation in Mexico City described by Volkamer et al. (2006), during a photochemically active period when the impact of regional biomass burning is minor or negligible, and show that the observed increase in OA/Delta CO is consistent with results from several groups during MILAGRO 2006. Then we use the case study to evaluate three new SOA models: 1) the update of aromatic SOA yields from recent chamber experiments (Ng et al., 2007); 2) the formation of SOA from glyoxal (Volkamer et al., 2007a); and 3) the formation of SOA from primary semivolatile and intermediate volatility species (P-S/IVOC) (Robinson et al., 2007). We also evaluate the effect of reduced partitioning of SOA into POA (Song et al., 2007). Traditional SOA precursors (mainly aromatics) by themselves still fail to produce enough SOA to match the observations by a factor of similar to similar to 7. The new low-NOx aromatic pathways with very high SOA yields make a very small contribution in this high-NOx urban environment as the RO2 center dot+NO reaction dominates the fate of the RO2 center dot radicals. Glyoxal contributes several mu g m(-3) to SOA formation, with similar timing as the measurements. P-S/IVOC are estimated from equilibrium with emitted POA, and introduce a large amount of gas-phase oxidizable carbon that was not in models before. With the formulation in Robinson et al. (2007) these species have a high SOA yield, and this mechanism can close the gap in SOA mass between measurements and models in our case study. However the volatility of SOA produced in the model is too high and the O/C ratio is somewhat lower than observations. Glyoxal SOA helps to bring the O/C ratio of predicted and observed SOA into better agreement. The sensitivities of the model to some key uncertain parameters are evaluated.
Najdeno v: osebi
Ključne besede: polycyclic aromatic-hydrocarbons, positive matrix factorization, mass-spectrometry, volatility measurements
Objavljeno: 11.04.2021; Ogledov: 69; Prenosov: 0
.pdf Polno besedilo (1,18 MB)

Sources and transformations of particle-bound polycyclic aromatic hydrocarbons in Mexico City
L. C. Marr, Katja Džepina, Jose L. Jimenez, F. Reisen, H. L. Bethel, Janet Arey, J. S. Gaffney, N. A. Marley, Luisa T. Molina, Mario J. Molina, 2006, izvirni znanstveni članek

Opis: Understanding sources, concentrations, and transformations of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere is important because of their potent mutagenicity and carcinogenicity. The measurement of particle-bound PAHs by three different methods during the Mexico City Metropolitan Area field campaign in April 2003 presents a unique opportunity for characterization of these compounds and intercomparison of the methods. The three methods are ( 1) collection and analysis of bulk samples for time-integrated gas- and particle-phase speciation by gas chromatography/ mass spectrometry; ( 2) aerosol photoionization for fast detection of PAHs on particles' surfaces; and ( 3) aerosol mass spectrometry for fast analysis of size and chemical composition. This research represents the first time aerosol mass spectrometry has been used to measure ambient PAH concentrations and the first time that fast, real-time methods have been used to quantify PAHs alongside traditional filter-based measurements in an extended field campaign. Speciated PAH measurements suggest that motor vehicles and garbage and wood burning are important sources in Mexico City. The diurnal concentration patterns captured by aerosol photoionization and aerosol mass spectrometry are generally consistent. Ambient concentrations of particle-phase PAHs typically peak at similar to 110 ng m(-3) during the morning rush hour and rapidly decay due to changes in source activity patterns and dilution as the boundary layer rises, although surface-bound PAH concentrations decay faster. The more rapid decrease in surface versus bulk PAH concentrations during the late morning suggests that freshly emitted combustion-related particles are quickly coated by secondary aerosol material in Mexico City's atmosphere and may also be transformed by heterogeneous reactions.
Najdeno v: osebi
Ključne besede: aerosol mass-spectrometer, aerodynamic diameter measurements, oxygenated organic aerosols, relative rate constants
Objavljeno: 12.04.2021; Ogledov: 90; Prenosov: 0
.pdf Polno besedilo (1,06 MB)

Secondary organic aerosol formation from semi- and intermediate-volatility organic compounds and glyoxal
Jose L. Jimenez, Sasha Madronich, Rainer Volkamer, Eleanor M. Waxman, Katja Džepina, Barbara Ervens, Julia Lee-Taylor, Bernard Aumont, 2013, izvirni znanstveni članek

Opis: The role of aqueous multiphase chemistry in the formation of secondary organic aerosol (SOA) remains difficult to quantify. We investigate it here by testing the rapid formation of moderate oxygen-to-carbon (O/C) SOA during a case study in Mexico City. A novel laboratory-based glyoxal-SOA mechanism is applied to the field data, and explains why less gas-phase glyoxal mass is observed than predicted. Furthermore, we compare an explicit gas-phase chemical mechanism for SOA formation from semi- and intermediate-volatility organic compounds (S/IVOCs) with empirical parameterizations of S/IVOC aging. The mechanism representing our current understanding of chemical kinetics of S/IVOC oxidation combined with traditional SOA sources and mixing of background SOA underestimates the observed O/C by a factor of two at noon. Inclusion of glyoxal-SOA with O/C of 1.5 brings O/C predictions within measurement uncertainty, suggesting that field observations can be reconciled on reasonable time scales using laboratory-based empirical relationships for aqueous chemistry.
Najdeno v: osebi
Ključne besede: secondary organic aerosol, glyoxal, aqueous multiphase chemistry, oxygen-to-carbon ratio, single scattering albedo
Objavljeno: 11.04.2021; Ogledov: 61; Prenosov: 0
.pdf Polno besedilo (724,40 KB)

Secondary organic aerosol formation from anthropogenic air pollution
Rainer Volkamer, Jose L. Jimenez, F. M. San Martini, Katja Džepina, Q. Zhang, Dara Salcedo, Luisa T. Molina, D. Worsnop, 2006, izvirni znanstveni članek

Opis: The atmospheric chemistry of volatile organic compounds (VOCs) in urban areas results in the formation of 'photochemical smog', including secondary organic aerosol (SOA). State-of-the-art SOA models parameterize the results of simulation chamber experiments that bracket the conditions found in the polluted urban atmosphere. Here we show that in the real urban atmosphere reactive anthropogenic VOCs (AVOCs) produce much larger amounts of SOA than these models predict, even shortly after sunrise. Contrary to current belief, a significant fraction of the excess SOA is formed from first-generation AVOC oxidation products. Global models deem AVOCs a very minor contributor to SOA compared to biogenic VOCs (BVOCs). If our results are extrapolated to other urban areas, AVOCs could be responsible for additional 3 - 25 Tg yr(-1) SOA production globally, and cause up to - 0.1 W m(-2) additional top-of-the-atmosphere radiative cooling.
Najdeno v: osebi
Ključne besede: atmospheric aerosol, atmospheric chemistry, volatile organic compounds, secondary organic aerosols
Objavljeno: 12.04.2021; Ogledov: 66; Prenosov: 0
.pdf Polno besedilo (638,71 KB)

Modeling the multiday evolution and aging of secondary organic aerosol during MILAGRO 2006
Jose L. Jimenez, Peter F. DeCarlo, Rahul A. Zaveri, Katja Džepina, Christopher D. Cappa, Rainer Volkamer, Sasha Madronich, 2011, izvirni znanstveni članek

Opis: In this study, we apply several recently proposed models to the evolution of secondary organic aerosols (SOA) and organic gases advected from downtown Mexico City at: an altitude of similar to 3.5 km during three days of aging, in a way that is directly comparable to simulations in regional and global models. We constrain the model with and compare its results to available observations. The model SOA formed from oxidation of volatile organic compounds (V-SOA) when using a non-aging SOA parameterization cannot explain the observed SOA concentrations in aged pollution, despite the increasing importance of the low-NO, channel. However, when using an aging SOA parameterization, V-SOA alone is similar to the regional aircraft observations, highlighting the wide diversity in current V-SOA formulations. When the SOA formed from oxidation of semivolatile and intermediate volatility organic vapors (SI-SOA) is computed following Robinson et al. (2007) the model matches the observed SOA mass, but its 0/C is similar to 2 x too low. With the parameterization of Grieshop et al. (2009), the total SOA mass is similar to 2 x too high, but 0/C and volatility are closer to the observations. Heating or dilution cause the evaporation of a substantial fraction of the model SOA; this fraction is reduced by aging although differently for heating vs dilution. Lifting of the airmass to the free-troposphere during dry convection substantially increases SOA by condensation of semivolatile vapors; this effect is reduced by aging.
Najdeno v: osebi
Ključne besede: Mexico-city, volatility, semivolatile, transport, campaign
Objavljeno: 11.04.2021; Ogledov: 61; Prenosov: 0
.pdf Polno besedilo (3,95 MB)

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, izvirni znanstveni članek

Opis: 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.
Najdeno v: osebi
Ključne besede: secondary organic aerosol, source apportionment, aerodyne aerosol mass spectrometer, global field measurements, laboratory experiments
Objavljeno: 11.04.2021; Ogledov: 56; Prenosov: 0
.pdf Polno besedilo (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, izvirni znanstveni članek

Opis: 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.
Najdeno v: osebi
Ključne besede: atmospheric aerosol, secondary organic aerosols, primary organic aerosols, aerodyne aerosol mass spectrometer
Objavljeno: 11.04.2021; Ogledov: 85; Prenosov: 0
.pdf Polno besedilo (1,15 MB)

Detection of particle-phase polycyclic aromatic hydrocarbons in Mexico City using an aerosol mass spectrometer
Katja Džepina, Janet Arey, Linsey C. Marr, D. Worsnop, Dara Salcedo, Q. Zhang, Timothy B. Onasch, Luisa T. Molina, Mario J. Molina, Jose L. Jimenez, 2007, izvirni znanstveni članek

Opis: We report the quantification of ambient particle-bound polycyclic aromatic hydrocarbons (PAHs) for the first time using a real-time aerosol mass spectrometer. These measurements were carried out during the Mexico City Metropolitan Area field study (MCMA-2003) that took place from March 29 to May 4, 2003. This was the first time that two different fast, real-time methods have been used to quantify PAHs alongside traditional filter-based measurements in an extended field campaign. This paper focuses on the technical aspects of PAH detection in ambient air with the Aerodyne AMS equipped with a quadrupole mass analyzer (Q-AMS), on the comparison of PAHs measured by the Q-AMS to those measured with the other two techniques, and on some features of the ambient results. PAHs are very resistant to fragmentation after ionization. Based on laboratory experiments with eight PAH standards, we show that their molecular ions, which for most particulate PAHs in ambient particles are larger than 200 amu, are often the largest peak in their Q-AMS spectra. Q-AMS spectra of PAH are similar to those in the NIST database, albeit with more fragmentation. We have developed a subtraction method that allows the removal of the contribution from non-PAH organics to the ion signals of the PAHs in ambient data. We report the mass concentrations of all individual groups of PAHs with molecular weights of 202, 216, 226 + 228, 240 + 242, 250 + 252, 264 + 266, 276 + 278, 288 + 290, 300 + 302, 316 and 326 + 328, as well as their sum as the total PAH mass concentration. The time series of the Photoelectric Aerosol Sensor (PAS) and Q-AMS PAH measurements during MCMA-2003 are well correlated, with the smallest difference between measured PAH concentrations observed in the mornings when ambient aerosols loadings are dominated by fresh traffic emissions. The Q-AMS PAH measurements are also compared to those from GC–MS analysis of filter samples. Several groups of PAHs show agreement within the uncertainties, while the Q-AMS measurements are larger than the GC–MS ones for several others. In the ambient Q-AMS measurements the presence of ions tentatively attributed to cyclopenta[cd]pyrene and dicyclopentapyrenes causes signals at m/z 226 and 250, which are significantly stronger than the signals in GC–MS analysis of filter samples. This suggests that very labile, but likely toxic, PAHs were present in the MCMA atmosphere that decayed rapidly due to reaction during filter sampling, and this may explain at least some of the differences between the Q-AMS and GC–MS measurements.
Najdeno v: osebi
Ključne besede: AMS, PAH, Mexico City
Objavljeno: 11.04.2021; Ogledov: 100; Prenosov: 0
.pdf Polno besedilo (4,12 MB)

Comparative Analysis of urban atmospheric aerosol by particle-induced X-ray emission (PIXE), proton elastic scattering analysis (PESA), and aerosol mass spectrometry (AMS)
Katja Džepina, Mario J. Molina, V. Shutthanandan, Luisa T. Molina, Dara Salcedo, K.S. Johnson, A. Laskin, Jose L. Jimenez, 2008, izvirni znanstveni članek

Opis: A multifaceted approach to atmospheric aerosol analysis is often desirable infield studies where an understanding of technical comparability among different measurement techniques is essential. Herein, we report quantitative intercomparisons of particle-induced X-ray emission (PIXE) and proton elastic scattering analysis (PESA), performed offline under a vacuum, with analysis by aerosol mass spectrometry (AMS) carried out in real-time during the MCMA-2003 Field Campaign in the Mexico City Metropolitan Area. Good agreement was observed for mass concentrations of PIXE-measured sulfur (assuming it was dominated by SO42-) and AMS-measured sulfate during most of the campaign. PESA-measured hydrogen mass was separated into sulfate H and organic H mass fractions, assuming the only major contributions were (NH4)(2)SO4 and organic compounds. Comparison of the organic H mass with AMS organic aerosol measurements indicates that about 75% of the mass of these species evaporated under a vacuum. However similar to 25% of the organics does remain under a vacuum, which is only possible with low-vapor-pressure compounds, and which supports the presence of high-molecular-weight or highly oxidized organics consistent with atmospheric aging. Approximately 10% of the chloride detected by AMS was measured by PIXE, possibly in the form of metal-chloride complexes, while the majority of Cl was likely present as more volatile species including NH4Cl. This is the first comparison of PIXE/PESA and AMS and, to our knowledge, also the first report of PESA hydrogen measurements for urban organic aerosols.
Najdeno v: osebi
Ključne besede: organic aerosols, secondary organic aerosols, Mexico City, MCMA-2003 field campaign
Objavljeno: 11.04.2021; Ogledov: 76; Prenosov: 0
.pdf Polno besedilo (1,74 MB)

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