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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: 178; 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: 175; 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: 166; Prenosov: 0
.pdf Polno besedilo (3,95 MB)

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