scholarly journals Model evaluation of NO<sub>3</sub> secondary organic aerosol (SOA) source and heterogeneous organic aerosol (OA) sink in the Western United States

2012 ◽  
Vol 12 (2) ◽  
pp. 5189-5223 ◽  
Author(s):  
J. L. Fry ◽  
K. Sackinger
Keyword(s):  
United States ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Chemical Mechanism ◽  
Western United States ◽  
Urban Centers ◽  
Aerosol Composition ◽  
Organic Gases ◽  
Source And Sink ◽  
Loss Rates

Abstract. The relative importance of NO3-initiated source and heterogeneous sink of organic aerosol in the Western United States is investigated using the WRF/Chem regional weather and chemistry model. The model is run for the four individual months, representing the four seasons, of January, May, August, and October, to produce hourly spatial maps of surface concentrations of NO3, organic aerosol (OA), and reactive organic gases (ROG, a sum of alkene species tracked in the lumped chemical mechanism employed). These "baseline" simulations are used in conjunction with literature data on secondary organic aerosol (SOA) mass yields, average organic aerosol composition, and reactive uptake coefficients for NO3 on organic surfaces to predict SOA source and OA heterogeneous loss rates due to reactions initiated by NO3. We find both source and sink rates maximized downwind of urban centers, therefore with a varying location that depends on wind direction. Both source and sink terms are maximum in summer, and SOA source dominates over OA loss by approximately three orders of magnitude, with large day-to-day variability. The NO3 source of SOA is found to be atmospherically significant (peak production rates of 0.4–3.0 μg kg−1 h−1), while the heterogeneous sink of OA via NO3 surface reactions (peak loss rates of 0.11–2.3 × 10−3 μg kg−1 h−1) is likely too small to significantly impact the atmospheric lifetime of either organic aerosol or oxidized nitrogen (NOy).

scholarly journals Model investigation of NO<sub>3</sub> secondary organic aerosol (SOA) source and heterogeneous organic aerosol (OA) sink in the western United States

2012 ◽  
Vol 12 (18) ◽  
pp. 8797-8811 ◽  
Author(s):  
J. L. Fry ◽  
K. Sackinger
Keyword(s):  
United States ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Chemical Mechanism ◽  
Western United States ◽  
Urban Centers ◽  
Aerosol Composition ◽  
Organic Gases ◽  
Source And Sink ◽  
Loss Rates

Abstract. The relative importance of NO3-initiated source and heterogeneous sink of organic aerosol in the western United States is investigated using the WRF/Chem regional weather and chemistry model. The model is run for the four individual months, representing the four seasons, of January, May, August, and October, to produce hourly spatial maps of surface concentrations of NO3, organic aerosol (OA), and reactive organic gases (ROG, a sum of alkene species tracked in the lumped chemical mechanism employed). These "baseline" simulations are used in conjunction with literature data on secondary organic aerosol (SOA) mass yields, average organic aerosol composition, and reactive uptake coefficients for NO3 on organic surfaces to predict SOA source and OA heterogeneous loss rates due to reactions initiated by NO3. We find both source and sink rates maximized downwind of urban centers, therefore with a varying location that depends on wind direction. Both source and sink terms are maximum in summer, and SOA source dominates over OA loss by approximately three orders of magnitude, with large day-to-day variability. The NO3 source of SOA (peak production rates of 0.4–3.0 μg kg−1 h−1) is found to be significantly larger than the heterogeneous sink of OA via NO3 surface reactions (peak loss rates of 0.5–8 × 10−4 μg kg−1 h−1).

scholarly journals The impact of bark beetle infestation on monoterpene emissions and secondary organic aerosol formation in Western North America

2012 ◽  
Vol 12 (11) ◽  
pp. 29763-29800 ◽  
Author(s):  
A. R. Berg ◽  
C. L. Heald ◽  
K. E. Huff Hartz ◽  
A. G. Hallar ◽  
A. J. H. Meddens ◽  
...  
Keyword(s):  
United States ◽  
British Columbia ◽  
North America ◽  
Bark Beetle ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Western United States ◽  
Mortality Data ◽  
Western North America ◽  
The Impact

Abstract. Over the last decade, extensive beetle outbreaks in Western North America have destroyed over 100 000 km2 of forest throughout British Columbia and the Western United States. Beetle infestations impact monoterpene emissions through both decreased emissions as trees are killed (mortality effect) and increased emissions in trees under attack (attack effect). We use 14 yr of beetle mortality data together with beetle-induced monoterpene concentration data in the National Center for Atmospheric Research (NCAR) Community Earth System Model (CESM) to investigate the impact of beetle mortality and attack on monoterpene emissions and secondary organic aerosol (SOA) formation in Western North America. Regionally, beetle infestations may have a significant impact on monoterpene emissions and SOA concentrations, with up to a 4-fold increase in monoterpene emissions and up to a 40% increase in SOA concentrations in some years (following a scenario where the attack effect is based on observed lodgepole pine response). Responses to beetle attack depend on the extent of previous mortality and the number of trees under attack in a given year, which can vary greatly over space and time. Simulated enhancements peak in 2004 (British Columbia) and 2008 (US). Responses to beetle attack are shown to be substantially larger (up to a 3-fold localized increase in SOA concentrations) when following a scenario based on bark-beetle attack in spruce trees. Placed in the context of observations from the IMPROVE network, the changes in SOA concentrations due to beetle attack are in most cases small compared to the large annual and interannual variability in total organic aerosol which is driven by wildfire activity in Western North America. This indicates that most beetle-induced SOA changes are not likely detectable in current observation networks; however these changes may impede efforts to achieve natural visibility conditions in the national parks and wilderness areas of the Western United States.

scholarly journals Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

2010 ◽  
Vol 10 (6) ◽  
pp. 2825-2845 ◽  
Author(s):  
J. G. Slowik ◽  
C. Stroud ◽  
J. W. Bottenheim ◽  
P. C. Brickell ◽  
R. Y.-W. Chang ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Coniferous Forest ◽  
Organic Aerosol ◽  
Chemical Mechanism ◽  
Rural Site ◽  
Chemical Transport Model ◽  
Aerosol Composition ◽  
Aerosol Mass

Abstract. Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.

scholarly journals The impact of bark beetle infestations on monoterpene emissions and secondary organic aerosol formation in western North America

2013 ◽  
Vol 13 (6) ◽  
pp. 3149-3161 ◽  
Author(s):  
A. R. Berg ◽  
C. L. Heald ◽  
K. E. Huff Hartz ◽  
A. G. Hallar ◽  
A. J. H. Meddens ◽  
...  
Keyword(s):  
United States ◽  
British Columbia ◽  
North America ◽  
Bark Beetle ◽  
Tree Mortality ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Western United States ◽  
Western North America ◽  
The Impact

Abstract. Over the last decade, extensive beetle outbreaks in western North America have destroyed over 100 000 km2 of forest throughout British Columbia and the western United States. Beetle infestations impact monoterpene emissions through both decreased emissions as trees are killed (mortality effect) and increased emissions in trees under attack (attack effect). We use 14 yr of beetle-induced tree mortality data together with beetle-induced monoterpene emission data in the National Center for Atmospheric Research (NCAR) Community Earth System Model (CESM) to investigate the impact of beetle-induced tree mortality and attack on monoterpene emissions and secondary organic aerosol (SOA) formation in western North America. Regionally, beetle infestations may have a significant impact on monoterpene emissions and SOA concentrations, with up to a 4-fold increase in monoterpene emissions and up to a 40% increase in SOA concentrations in some years (in a scenario where the attack effect is based on observed lodgepole pine response). Responses to beetle attack depend on the extent of previous mortality and the number of trees under attack in a given year, which can vary greatly over space and time. Simulated enhancements peak in 2004 (British Columbia) and 2008 (US). Responses to beetle attack are shown to be substantially larger (up to a 3-fold localized increase in summertime SOA concentrations) in a scenario based on bark-beetle attack in spruce trees. Placed in the context of observations from the IMPROVE network, the changes in SOA concentrations due to beetle attack are in most cases small compared to the large annual and interannual variability in total organic aerosol which is driven by wildfire activity in western North America. This indicates that most beetle-induced SOA changes are not likely detectable in current observation networks; however, these changes may impede efforts to achieve natural visibility conditions in the national parks and wilderness areas of the western United States.

scholarly journals The effect of temperature and water on secondary organic aerosol formation from ozonolysis of limonene, Δ³-carene and α-pinene

2008 ◽  
Vol 8 (3) ◽  
pp. 9323-9346 ◽  
Author(s):  
Å. M. Jonsson ◽  
M. Hallquist ◽  
E. Ljungström
Keyword(s):  
Temperature Dependence ◽  
Low Temperatures ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Reaction Rates ◽  
Chemical Mechanism ◽  
Positive Temperature ◽  
Aerosol Formation ◽  
Aerosol Composition ◽  
Secondary Chemistry

Abstract. The effect of reaction temperature and how water vapour influences the formation of secondary organic aerosol (SOA) in ozonolysis of limonene, Δ3-carene and α-pinene, both regarding number and mass of particles, has been investigated by using a laminar flow reactor G-FROST. Experiments with cyclohexane and 2-butanol (~3.5×1014 molecules cm−3) as OH scavengers were compared to experiments without any scavenger. The reactions were conducted in the temperature range between 298 and 243 K, and at relative humidities between <10 and 80%. Results showed that there is still a scavenger effect on number and mass concentrations at low temperatures between experiments with and without OH scavenger. This shows that the OH chemistry is influencing the SOA formation also at these temperatures. The overall temperature dependence on SOA formation is not as strong as expected from the partitioning theory. In some cases there is even a positive temperature dependence that must be related to changes in the chemical mechanism and/or reduced rates of secondary chemistry at low temperatures. The water effect at low temperature could be explained by physical uptake and cluster stabilisation. At higher temperatures, only a physical explanation is not sufficient and the observations are in line with water changing the chemical mechanism or reaction rates. The data presented adds to the understanding of SOA contribution to atmospheric aerosol composition, new particle formation and atmospheric degradation mechanisms.

scholarly journals Secondary organic aerosol formation from biomass burning emissions

2019 ◽  
Author(s):  
Christopher Y. Lim ◽  
David H. Hagan ◽  
Matthew M. Coggon ◽  
Abigail R. Koss ◽  
Kanako Sekimoto ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Secondary Organic Aerosol ◽  
Total Concentration ◽  
Organic Aerosol ◽  
Oh Radicals ◽  
Aerosol Formation ◽  
Atmospheric Aging ◽  
Aerosol Mass ◽  
Photochemical Aging ◽  
Organic Gases

Abstract. Biomass burning is an important source of aerosol and trace gases to the atmosphere, but how these emissions change chemically during their lifetimes is not fully understood. As part of the Fire Influence on Regional and Global Environments Experiment (FIREX 2016), we investigated the effect of photochemical aging on biomass burning organic aerosol (BBOA), with a focus on fuels from the western United States. Emissions were sampled into a small (150 L) environmental chamber and photochemically aged via the addition of ozone and irradiation by 254 nm light. While some fraction of species undergoes photolysis, the vast majority of aging occurs via reaction with OH radicals, with total OH exposures corresponding to the equivalent of up to 10 days of atmospheric oxidation. For all fuels burned, large and rapid changes are seen in the ensemble chemical composition of BBOA, as measured by an aerosol mass spectrometer (AMS). Secondary organic aerosol (SOA) formation is seen for all aging experiments and continues to grow with increasing OH exposure, but the magnitude of the SOA formation is highly variable between experiments. This variability can be explained well by a combination of experiment-to-experiment differences in OH exposure and the total concentration of non-methane organic gases (NMOGs) in the chamber before oxidation, measured by PTR-ToF-MS (r2 values from 0.64 to 0.83). From this relationship, we calculate the fraction of carbon from biomass burning NMOGs that is converted to SOA as a function of equivalent atmospheric aging time, with carbon yields ranging from 24 ± 4 % after 6 hours to 56 ± 9 % after 4 days.

scholarly journals Chemical and physical characteristics of aerosol particles at a remote coastal location, Mace Head, Ireland, during NAMBLEX

2006 ◽  
Vol 6 (11) ◽  
pp. 3289-3301 ◽  
Author(s):  
H. Coe ◽  
J. D. Allan ◽  
M. R. Alfarra ◽  
K. N. Bower ◽  
M. J. Flynn ◽  
...  
Keyword(s):  
Surf Zone ◽  
Organic Aerosol ◽  
Sea Salt ◽  
Research Station ◽  
Aerosol Composition ◽  
Gaseous Species ◽  
Accumulation Mode ◽  
Coarse Mode ◽  
Wide Range ◽  
Loss Rates

Abstract. A suite of aerosol physical and chemical measurements were made at the Mace Head Atmospheric Research Station, Co. Galway, Ireland, a coastal site on the eastern seaboard of the north Atlantic Ocean during NAMBLEX. The data have been used in this paper to show that over a wide range of aerosol sizes there is no impact of the inter-tidal zone or the surf zone on measurements made at 7 m above ground level or higher. During the measurement period a range of air mass types were observed. During anticyclonic periods and conditions of continental outflow Aitken and accumulation mode were enhanced by a factor of 5 compared to the marine sector, whilst coarse mode particles were enhanced during westerly conditions. Baseline marine conditions were rarely met at Mace Head during NAMBLEX and high wind speeds were observed for brief periods only. The NAMBLEX experiment focussed on a detailed assessment of photochemistry in the marine environment, investigating the linkage between the HOx and the halogen radical cycles. Heterogeneous losses are important in both these cycles. In this paper loss rates of gaseous species to aerosol surfaces were calculated for a range of uptake coefficients. Even when the accommodation coefficient is unity, lifetimes due to heterogeneous loss of less than 10 s were never observed and rarely were they less than 500 s. Diffusional limitation to mass transfer is important in most conditions as the coarse mode is always significant. We calculate a minimum overestimate of 50% in the loss rate if this is neglected and so it should always be considered when calculating loss rates of gaseous species to particle surfaces. HO2 and HOI have accommodation coefficients of around 0.03 and hence we calculate lifetimes due to loss to particle surfaces of 2000 s or greater under the conditions experienced during NAMBLEX. Aerosol composition data collected during this experiment provide representative information on the input aerosol characteristics to western Europe. During NAMBLEX the submicron aerosol was predominately acidified sulphate and organic material, which was most likely internally mixed. The remaining accumulation mode aerosol was sea salt. The organic and sulphate fractions were approximately equally important, though the mass ratio varies considerably between air masses. Mass spectral fingerprints of the organic fraction in polluted conditions are similar to those observed at other locations that are characterised by aged continental aerosol. In marine conditions, the background input of both sulphate and organic aerosol into Europe was observed to be between 0.5 and 1 µg m−3. Key differences in the mass spectra were observed during the few clean periods but were insufficient to ascertain whether these changes reflect differences in the source fingerprint of the organic aerosol. The coarse mode was composed of sea salt and showed significant displacement of chloride by nitrate and to a lesser extent sulphate in polluted conditions.

Gas-phase kinetics modifies the CCN activity of a biogenic SOA

2018 ◽  
Vol 20 (9) ◽  
pp. 6591-6597
Author(s):  
A. E. Vizenor ◽  
A. A. Asa-Awuku
Keyword(s):  
Particle Size ◽  
Thermodynamic Properties ◽  
Gas Phase ◽  
Secondary Organic Aerosol ◽  
Cloud Condensation Nuclei ◽  
Organic Aerosol ◽  
Aerosol Composition ◽  
Phase Partitioning ◽  
Gas Phase Kinetics ◽  
Ccn Activity

Cloud condensation nuclei (CCN) activity and the hygroscopicity of secondary organic aerosol (SOA) depends on the particle size and composition, explicitly, the thermodynamic properties of the aerosol solute and subsequent interactions with water. The gas-to-aerosol phase partitioning is critical for aerosol composition and thus gas-phase vapors and kinetics can play an important role in the CCN activity of SOA.

scholarly journals Light Absorption of Secondary Organic Aerosol: Composition and Contribution of Nitroaromatic Compounds

2017 ◽  
Vol 51 (20) ◽  
pp. 11607-11616 ◽  
Author(s):  
Mingjie Xie ◽  
Xi Chen ◽  
Michael D. Hays ◽  
Michael Lewandowski ◽  
John Offenberg ◽  
...  
Keyword(s):  
Light Absorption ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Nitroaromatic Compounds ◽  
Aerosol Composition

scholarly journals Simulating regional scale secondary organic aerosol formation during the TORCH 2003 campaign in the southern UK

2006 ◽  
Vol 6 (2) ◽  
pp. 403-418 ◽  
Author(s):  
D. Johnson ◽  
S. R. Utembe ◽  
M. E. Jenkin ◽  
R. G. Derwent ◽  
G. D. Hayman ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Regional Scale ◽  
Organic Aerosol ◽  
Chemical Mechanism ◽  
Background Concentration ◽  
Aerosol Formation ◽  
Organic Species ◽  
Voc Oxidation ◽  
Partitioning Coefficients

Abstract. A photochemical trajectory model has been used to simulate the chemical evolution of air masses arriving at the TORCH field campaign site in the southern UK during late July and August 2003, a period which included a widespread and prolonged photochemical pollution episode. The model incorporates speciated emissions of 124 non-methane anthropogenic VOC and three representative biogenic VOC, coupled with a comprehensive description of the chemistry of their degradation. A representation of the gas/aerosol absorptive partitioning of ca. 2000 oxygenated organic species generated in the Master Chemical Mechanism (MCM v3.1) has been implemented, allowing simulation of the contribution to organic aerosol (OA) made by semi- and non-volatile products of VOC oxidation; emissions of primary organic aerosol (POA) and elemental carbon (EC) are also represented. Simulations of total OA mass concentrations in nine case study events (optimised by comparison with observed hourly-mean mass loadings derived from aerosol mass spectrometry measurements) imply that the OA can be ascribed to three general sources: (i) POA emissions; (ii) a "ubiquitous" background concentration of 0.7 µg m-3; and (iii) gas-to-aerosol transfer of lower volatility products of VOC oxidation generated by the regional scale processing of emitted VOC, but with all partitioning coefficients increased by a species-independent factor of 500. The requirement to scale the partitioning coefficients, and the implied background concentration, are both indicative of the occurrence of chemical processes within the aerosol which allow the oxidised organic species to react by association and/or accretion reactions which generate even lower volatility products, leading to a persistent, non-volatile secondary organic aerosol (SOA). The contribution of secondary organic material to the simulated OA results in significant elevations in the simulated ratio of organic carbon (OC) to EC, compared with the ratio of 1.1 assigned to the emitted components. For the selected case study events, [OC]/[EC] is calculated to lie in the range 2.7-9.8, values which are comparable with the high end of the range reported in the literature.

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