skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Multiday production of condensing organic aerosol mass in urban and forest outflow

Journal Article · · Atmospheric Chemistry and Physics (Online)

Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. Here, the results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.

Research Organization:
National Center for Atmospheric Research (NCAR), Boulder, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC0006780
OSTI ID:
1197838
Alternate ID(s):
OSTI ID: 1441388
Journal Information:
Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 15 Journal Issue: 2; ISSN 1680-7324
Publisher:
Copernicus Publications, EGUCopyright Statement
Country of Publication:
Germany
Language:
English
Citation Metrics:
Cited by: 20 works
Citation information provided by
Web of Science

References (111)

Heterogeneous oxidation of atmospheric aerosol particles by gas-phase radicals journal August 2010
Two hundred fifty years of aerosols and climate: the end of the age of aerosols journal January 2014
Atmospheric lifetimes and fates of a series of sesquiterpenes journal January 1995
Relationship between Oxidation Level and Optical Properties of Secondary Organic Aerosol journal May 2013
Atmospheric organic particulate matter: From smoke to secondary organic aerosol journal January 2009
Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part B): tropospheric degradation of aromatic volatile organic compounds journal January 2003
Gas/Particle Partitioning and Secondary Organic Aerosol Yields journal July 1996
Branching Ratios for the Reaction of Selected Carbonyl-Containing Peroxy Radicals with Hydroperoxy Radicals journal February 2012
Missing peroxy radical sources within a summertime ponderosa pine forest journal January 2014
Investigative modeling of new pathways for secondary organic aerosol formation journal January 2007
Functionalization vs. fragmentation: n-aldehyde oxidation mechanisms and secondary organic aerosol formation journal January 2010
Detailed chemical characterization of unresolved complex mixtures in atmospheric organics: Insights into emission sources, atmospheric processing, and secondary organic aerosol formation: UCM COMPOSITION IN ATMOSPHERIC ORGANICS journal June 2013
Chemical evolution of secondary organic aerosol from OH-initiated heterogeneous oxidation journal January 2010
Estimation of the mass absorption cross section of the organic carbon component of aerosols in the Mexico City Metropolitan Area journal January 2008
Undisturbed and disturbed above canopy ponderosa pine emissions: PTR-TOF-MS measurements and MEGAN 2.1 model results journal January 2013
Yields of oxidized volatile organic compounds during the OH radical initiated oxidation of isoprene, methyl vinyl ketone, and methacrolein under high-NO x conditions journal January 2011
Modeling the influence of alkane molecular structure on secondary organic aerosol formation journal January 2013
Atmospheric evolution of organic aerosol: ATMOSPHERIC EVOLUTION OF ORGANIC AEROSOL journal November 2004
Estimation of pure component properties journal July 2008
Aerosol mass spectrometer constraint on the global secondary organic aerosol budget journal January 2011
A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution journal January 2012
A simplified description of the evolution of organic aerosol composition in the atmosphere: VAN KREVELEN DIAGRAM OF ORGANIC AEROSOL journal April 2010
An absorption model of gas/particle partitioning of organic compounds in the atmosphere journal January 1994
Effect of chemical structure on secondary organic aerosol formation from C 12 alkanes journal January 2013
An overview of the MILAGRO 2006 Campaign: Mexico City emissions and their transport and transformation journal January 2010
Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes: UBIQUITY AND DOMINANCE OF OXYGENATED OA journal July 2007
Explicit modelling of SOA formation from α-pinene photooxidation: sensitivity to vapour pressure estimation journal January 2011
Development of a detailed chemical mechanism (MCMv3.1) for the atmospheric oxidation of aromatic hydrocarbons journal January 2005
The formation, properties and impact of secondary organic aerosol: current and emerging issues journal January 2009
Formation of brown carbon via reactions of ammonia with secondary organic aerosols from biogenic and anthropogenic precursors journal December 2012
Can 3-D models explain the observed fractions of fossil and non-fossil carbon in and near Mexico City? journal January 2010
Does the POA–SOA split matter for global CCN formation? journal January 2014
Estimation of Pure-Component Properties from Group-Contributions journal July 1987
Estimation of pure component properties journal December 2004
Secondary organic aerosol formation from anthropogenic air pollution: Rapid and higher than expected journal January 2006
Explicit modeling of organic chemistry and secondary organic aerosol partitioning for Mexico City and its outflow plume journal January 2011
Assessment of the reduction methods used to develop chemical schemes: building of a new chemical scheme for VOC oxidation suited to three-dimensional multiscale HO<sub>x</sub>-NO<sub>x</sub>-VOC chemistry simulations journal January 2005
Secondary organic aerosol yields of 12-carbon alkanes journal January 2014
Effects of anthropogenic emissions on the molecular composition of urban organic aerosols: An ultrahigh resolution mass spectrometry study journal June 2014
Volatility dependence of Henry's law constants of condensable organics: Application to estimate depositional loss of secondary organic aerosols: Solubility and removal of organic vapors journal July 2014
Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions—Part 1: aldehydes and ketones journal August 2004
Effects of Molecular Structure on Aerosol Yields from OH Radical-Initiated Reactions of Linear, Branched, and Cyclic Alkanes in the Presence of NO x journal April 2009
Contribution of First- versus Second-Generation Products to Secondary Organic Aerosols Formed in the Oxidation of Biogenic Hydrocarbons journal April 2006
Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach journal January 2005
Analysis of secondary organic aerosol formation and aging using positive matrix factorization of high-resolution aerosol mass spectra: application to the dodecane low-NO x system journal January 2012
Limited influence of dry deposition of semivolatile organic vapors on secondary organic aerosol formation in the urban plume: IMPACT OF DRY DEPOSITION OF VOCs ON SOA journal June 2013
A secondary organic aerosol formation model considering successive oxidation aging and kinetic condensation of organic compounds: global scale implications journal January 2011
Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 1: measurement and simulation of organic aerosol evolution journal January 2009
Evaluation of the Montsouris series of ozone measurements made in the nineteenth century journal March 1988
Modeling the Role of Alkanes, Polycyclic Aromatic Hydrocarbons, and Their Oligomers in Secondary Organic Aerosol Formation journal May 2012
Sources of particulate matter in the northeastern United States in summer: 1. Direct emissions and secondary formation of organic matter in urban plumes journal January 2008
Coupled Partitioning, Dilution, and Chemical Aging of Semivolatile Organics journal April 2006
Modeling SOA formation from the oxidation of intermediate volatility n -alkanes journal January 2012
Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications journal January 2014
Modeling ultrafine particle growth at a pine forest site influenced by anthropogenic pollution during BEACHON-RoMBAS 2011 journal January 2014
Laboratory studies of organic peroxy radical chemistry: an overview with emphasis on recent issues of atmospheric significance journal January 2012
Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging journal March 2007
Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area journal January 2010
Modeling the Multiday Evolution and Aging of Secondary Organic Aerosol During MILAGRO 2006 journal April 2011
The effect of physical and chemical aerosol properties on warm cloud droplet activation journal January 2006
A new mechanism for regional atmospheric chemistry modeling journal November 1997
Analyzing experimental data and model parameters: implications for predictions of SOA using chemical transport models journal January 2013
Known and Unexplored Organic Constituents in the Earth's Atmosphere journal March 2007
Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the volatility-basis-set approach within the CHIMERE model journal January 2013
Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations journal January 2013
Global modeling of SOA formation from dicarbonyls, epoxides, organic nitrates and peroxides journal January 2012
Rate constants for the gas-phase reactions of O 3 with a series of monoterpenes and related compounds at 296 ± 2 K : GAS-PHASE REACTIONS OF O journal August 1990
The AeroCom evaluation and intercomparison of organic aerosol in global models journal January 2014
Species Contributions to PM2.5 Mass Concentrations: Revisiting Common Assumptions for Estimating Organic Mass journal July 2001
Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: implications for oxidation of intermediate volatility organic compounds (IVOCs) journal January 2009
Overview of the Manitou Experimental Forest Observatory: site description and selected science results from 2008 to 2013 journal January 2014
Investigation of the sources and processing of organic aerosol over the Central Mexican Plateau from aircraft measurements during MILAGRO journal January 2010
Comparison of different real time VOC measurement techniques in a ponderosa pine forest journal January 2013
O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry journal June 2008
Investigation of the correlation between odd oxygen and secondary organic aerosol in Mexico City and Houston journal January 2010
Maximum efficiency in the hydroxyl-radical-based self-cleansing of the troposphere journal July 2014
Organic aerosol and global climate modelling: a review journal January 2005
Modeling organic aerosols during MILAGRO: importance of biogenic secondary organic aerosols journal January 2009
Decomposition of substituted alkoxy radicals—part I: a generalized structure–activity relationship for reaction barrier heights journal January 2009
Chemical evolution of volatile organic compounds in the outflow of the Mexico City Metropolitan area journal January 2010
Air Quality Model Evaluation Data for Organics. 4. C 2 −C 36 Non-Aromatic Hydrocarbons journal August 1997
Evolution of Organic Aerosols in the Atmosphere journal December 2009
Heterogeneous OH Oxidation of Motor Oil Particles Causes Selective Depletion of Branched and Less Cyclic Hydrocarbons journal September 2012
Secondary Organic Aerosol Formation from Low-NO x Photooxidation of Dodecane: Evolution of Multigeneration Gas-Phase Chemistry and Aerosol Composition journal February 2012
Simulation of Mexico City plumes during the MIRAGE-Mex field campaign using the WRF-Chem model journal January 2009
Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles journal January 2010
The heterogeneous reaction of hydroxyl radicals with sub-micron squalane particles: a model system for understanding the oxidative aging of ambient aerosols journal January 2009
Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City journal January 2010
Recent tropospheric ozone changes – A pattern dominated by slow or no growth journal March 2013
Isoprene photooxidation: new insights into the production of acids and organic nitrates journal January 2009
Effect of aerosols and NO 2 concentration on ultraviolet actinic flux near Mexico City during MILAGRO: measurements and model calculations journal January 2013
Rate Constants for the Gas-Phase Reactions of OH Radicals with a Series of Hydroxyaldehydes at 296 ± 2 K journal August 2004
Photo-Oxidation of Low-Volatility Organics Found in Motor Vehicle Emissions: Production and Chemical Evolution of Organic Aerosol Mass journal March 2010
The critical assessment of vapour pressure estimation methods for use in modelling the formation of atmospheric organic aerosol journal January 2010
Exploring the vertical profile of atmospheric organic aerosol: comparing 17 aircraft field campaigns with a global model journal January 2011
The time evolution of aerosol composition over the Mexico City plateau journal January 2008
Secondary organic aerosol formation from <i>m</i>-xylene, toluene, and benzene journal January 2007
SMILES, a chemical language and information system. 1. Introduction to methodology and encoding rules journal February 1988
Functionalization and fragmentation during ambient organic aerosol aging: application of the 2-D volatility basis set to field studies journal January 2012
Atmospheric removal times of the aerosol-bound radionuclides 137 Cs and 131 I measured after the Fukushima Dai-ichi nuclear accident – a constraint for air quality and climate models journal January 2012
The magnitude and sources of uncertainty in global aerosol journal January 2013
Effects of chemical aging on global secondary organic aerosol using the volatility basis set approach journal December 2013
Simulating secondary organic aerosol formation using the volatility basis-set approach in a chemical transport model journal October 2008
Improving the representation of secondary organic aerosol (SOA) in the MOZART-4 global chemical transport model journal January 2013
The SOA/VOC/NO<sub>x</sub> system: an explicit model of secondary organic aerosol formation journal January 2007
Molecular chemistry of organic aerosols through the application of high resolution mass spectrometry journal January 2011
Alkyl Nitrate, Hydroxyalkyl Nitrate, and Hydroxycarbonyl Formation from the NO x −Air Photooxidations of C 5 −C 8 n -Alkanes journal February 2001
Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere journal May 2008
Estimating Pure Component Vapor Pressures of Complex Organic Molecules journal June 1997
The Atmospheric Chemistry of Alkoxy Radicals journal December 2003
Evaluation of detailed aromatic mechanisms (MCMv3 and MCMv3.1) against environmental chamber data journal January 2005