scholarly journals Observations and analysis of organic aerosol evolution in some prescribed fire smoke plumes

2015 ◽  
Vol 15 (11) ◽  
pp. 6323-6335 ◽  
Author(s):  
A. A. May ◽  
T. Lee ◽  
G. R. McMeeking ◽  
S. Akagi ◽  
A. P. Sullivan ◽  
...  
Keyword(s):  
South Carolina ◽  
Biomass Burning ◽  
Atmospheric Transport ◽  
Organic Aerosol ◽  
Chemical Transformations ◽  
Chemical Production ◽  
Mixing Ratios ◽  
Fractional Contribution ◽  
Smoke Plumes ◽  
Aerosol Aging

Abstract. Open biomass burning is a significant source of primary air pollutants such as particulate matter (PM) and non-methane organic gases (NMOG). However, the physical and chemical atmospheric processing of these emissions during transport is poorly understood. Atmospheric transformations of biomass burning emissions have been investigated in environmental chambers, but there have been limited opportunities to investigate these transformations in the atmosphere. In this study, we deployed a suite of real-time instrumentation on a Twin Otter aircraft to sample smoke from prescribed fires in South Carolina, conducting measurements at both the source and downwind to characterize smoke evolution with atmospheric aging. Organic aerosol (OA) within the smoke plumes was quantified using an aerosol mass spectrometer (AMS); refractory black carbon (rBC) was quantified using a single-particle soot photometer, and carbon monoxide (CO) and carbon dioxide (CO2) were measured using a cavity ring-down spectrometer. During the two fires for which we were able to obtain aerosol aging data, normalized excess mixing ratios and "export factors" of conserved species (rBC, CO, CO2) suggested that changes in emissions at the source did not account for most of the differences observed in samples of increasing age. An investigation of AMS mass fragments indicated that the in-plume fractional contribution (fm/z) to OA of the primary fragment (m/z 60) decreased downwind, while the fractional contribution of the secondary fragment (m/z 44) increased. Increases in f44 are typically interpreted as indicating chemical aging of OA. Likewise, we observed an increase in the O : C elemental ratio downwind, which is usually associated with aerosol aging. However, the rapid mixing of these plumes into the background air suggests that these chemical transformations may be attributable to the different volatilities of the compounds that fragment to these m/z in the AMS. The gas–particle partitioning behavior of the bulk OA observed during the study was consistent with the predictions from a parameterization developed for open biomass burning emissions in the laboratory. Furthermore, we observed no statistically significant increase in total organic mass with atmospheric transport. Hence, our results suggest that dilution-driven evaporation likely dominated over the chemical production of secondary organic aerosol (SOA) within our smoke plumes, presumably due to the fast dilution and limited aging times (< ~ 5 h) that we could sample.

scholarly journals Observations and analysis of organic aerosol evolution in some prescribed fire smoke plumes

2015 ◽  
Vol 15 (2) ◽  
pp. 1953-1988 ◽  
Author(s):  
A. A. May ◽  
T. Lee ◽  
G. R. McMeeking ◽  
S. Akagi ◽  
A. P. Sullivan ◽  
...  
Keyword(s):  
South Carolina ◽  
Biomass Burning ◽  
Atmospheric Transport ◽  
Organic Aerosol ◽  
Chemical Transformations ◽  
Chemical Production ◽  
Mixing Ratios ◽  
Fractional Contribution ◽  
Smoke Plumes ◽  
Aerosol Aging

Abstract. Open biomass burning is a significant source of primary air pollutants such as particulate matter and non-methane organic gases. However, the physical and chemical atmospheric processing of these emissions during transport is poorly understood. Atmospheric transformations of biomass burning emissions have been investigated in environmental chambers, but there have been limited opportunities to investigate these transformations in the atmosphere. In this study, we deployed a suite of real-time instrumentation on a Twin Otter aircraft to sample smoke from prescribed fires in South Carolina, conducting measurements at both the source and downwind to characterize smoke evolution with atmospheric aging. Organic aerosol (OA) within the smoke plumes was quantified using an Aerosol Mass Spectrometer (AMS), along with refractory black carbon (rBC) using a Single Particle Soot Photometer and carbon monoxide (CO) and carbon dioxide (CO2) using a Cavity Ring-Down Spectrometer. During the two fires for which we were able to obtain aerosol aging data, normalized excess mixing ratios and "export factors" of conserved species (rBC, CO, CO2) were unchanged with increasing sample age. Investigation of AMS mass fragments indicated that the in-plume fractional contribution (fm/z) to OA of the primary fragment (m/z 60) decreased downwind, while the fractional contribution of the secondary fragment (m/z 44) increased. Increases in f44 are typically interpreted as indicating chemical production of secondary OA (SOA). Likewise, we observed an increase in the O : C elemental ratio downwind, which is usually associated with aerosol aging. However, the rapid mixing of these plumes into the background air suggests that these chemical transformations may be attributable to the different volatilities of the compounds that fragment to these m/z in the AMS. The gas-particle partitioning behavior of the bulk OA observed during the study was consistent with the predictions from a parameterization developed for open biomass burning emissions in the laboratory. Furthermore, we observed no statistically-significant increase in total organic mass with atmospheric transport. Hence, our results suggest that dilution-driven evaporation likely dominated over chemical production of SOA within our smoke plumes, likely due to the fast dilution and limited aging times (

scholarly journals Insights into the aging of biomass burning aerosol from satellite observations and 3D atmospheric modeling: evolution of the aerosol optical properties in Siberian wildfire plumes

2021 ◽  
Vol 21 (1) ◽  
pp. 357-392
Author(s):  
Igor B. Konovalov ◽  
Nikolai A. Golovushkin ◽  
Matthias Beekmann ◽  
Meinrat O. Andreae
Keyword(s):  
Optical Properties ◽  
Long Range ◽  
Biomass Burning ◽  
Organic Aerosol ◽  
Satellite Observations ◽  
Long Range Transport ◽  
Aerosol Optical Properties ◽  
Smoke Plumes ◽  
Range Transport ◽  
Aerosol Aging

Abstract. Long-range transport of biomass burning (BB) aerosol from regions affected by wildfires is known to have a significant impact on the radiative balance and air quality in receptor regions. However, the changes that occur in the optical properties of BB aerosol during long-range transport events are insufficiently understood, limiting the adequacy of representations of the aerosol processes in chemistry transport and climate models. Here we introduce a framework to infer and interpret changes in the optical properties of BB aerosol from satellite observations of multiple BB plumes. Our framework includes (1) a procedure for analysis of available satellite retrievals of the absorption and extinction aerosol optical depths (AAOD and AOD) and single-scattering albedo (SSA) as a function of the BB aerosol photochemical age and (2) a representation of the AAOD and AOD evolution with a chemistry transport model (CTM) involving a simplified volatility basis set (VBS) scheme with a few adjustable parameters. We apply this framework to analyze a large-scale outflow of BB smoke plumes from Siberia toward Europe that occurred in July 2016. We use AAOD and SSA data derived from OMI (Ozone Monitoring Instrument) satellite measurements in the near-UV range along with 550 nm AOD and carbon monoxide (CO) columns retrieved from MODIS (Moderate Resolution Imaging Spectroradiometer) and IASI (Infrared Atmospheric Sounding Interferometer) satellite observations, respectively, to infer changes in the optical properties of Siberian BB aerosol due to its atmospheric aging and to get insights into the processes underlying these changes. Using the satellite data in combination with simulated data from the CHIMERE CTM, we evaluate the enhancement ratios (EnRs) that allow isolating AAOD and AOD changes due to oxidation and gas–particle partitioning processes from those due to other processes, including transport, deposition, and wet scavenging. The behavior of EnRs for AAOD and AOD is then characterized using nonlinear trend analysis. It is found that the EnR for AOD strongly increases (by about a factor of 2) during the first 20–30 h of the analyzed evolution period, whereas the EnR for AAOD does not exhibit a statistically significant increase during this period. The increase in AOD is accompanied by a statistically significant enhancement of SSA. Further BB aerosol aging (up to several days) is associated with a strong decrease in EnRs for both AAOD and AOD. Our VBS simulations constrained by the observations are found to be more consistent with satellite observations of strongly aged BB plumes than “tracer” simulations in which atmospheric transformations of BB organic aerosol were disregarded. The simulation results indicate that the upward trends in EnR for AOD and in SSA are mainly due to atmospheric processing of secondary organic aerosol (SOA), leading to an increase in the mass scattering efficiency of BB aerosol. Evaporation and chemical fragmentation of the SOA species, part of which is assumed to be absorptive (to contain brown carbon), are identified as likely reasons for the subsequent decrease in the EnR for both AAOD and AOD. Hence, our analysis reveals that the long-range transport of smoke plumes from Siberian fires is associated with major changes in BB aerosol optical properties and chemical composition. Overall, this study demonstrates the feasibility of using available satellite observations for evaluating and improving representations in atmospheric models of the BB aerosol aging processes in different regions of the world at much larger temporal scales than those typically addressed in aerosol chamber experiments.

Trace gases and organic aerosol at a rural site in Vietnam during large scale biomass burning

2021 ◽  
Author(s):  
Simone M. Pieber ◽  
Dac-Loc Nguyen ◽  
Hendryk Czech ◽  
Stephan Henne ◽  
Nicolas Bukowiecki ◽  
...  
Keyword(s):  
Air Quality ◽  
Chemical Composition ◽  
Biomass Burning ◽  
Large Scale ◽  
Trace Gases ◽  
Organic Aerosol ◽  
Trace Gas ◽  
Rural Site ◽  
Air Masses ◽  
Mixing Ratios

&lt;p&gt;Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt;, CO, and O&lt;sub&gt;3&lt;/sub&gt; conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM&lt;sub&gt;2.5 &lt;/sub&gt;chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt; and O&lt;sub&gt;3&lt;/sub&gt; mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O&lt;sub&gt;3&lt;/sub&gt; levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM&lt;sub&gt;2.5 &lt;/sub&gt;composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&lt;strong&gt;REFERENCES&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172&amp;#8211;1187 (2019).&lt;/p&gt;&lt;p&gt;[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.&lt;/p&gt;

scholarly journals Brominated VSLS and their influence on ozone under a changing climate

2017 ◽  
Vol 17 (18) ◽  
pp. 11313-11329 ◽  
Author(s):  
Stefanie Falk ◽  
Björn-Martin Sinnhuber ◽  
Gisèle Krysztofiak ◽  
Patrick Jöckel ◽  
Phoebe Graf ◽  
...  
Keyword(s):  
21St Century ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Atmospheric Transport ◽  
Stratospheric Ozone ◽  
Chemical Transformations ◽  
Mixing Ratios ◽  
Ocean Atmosphere ◽  
The Impact

Abstract. Very short-lived substances (VSLS) contribute as source gases significantly to the tropospheric and stratospheric bromine loading. At present, an estimated 25 % of stratospheric bromine is of oceanic origin. In this study, we investigate how climate change may impact the ocean–atmosphere flux of brominated VSLS, their atmospheric transport, and chemical transformations and evaluate how these changes will affect stratospheric ozone over the 21st century. Under the assumption of fixed ocean water concentrations and RCP6.0 scenario, we find an increase of the ocean–atmosphere flux of brominated VSLS of about 8–10 % by the end of the 21st century compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Our model simulations reveal that this increase is counteracted by a corresponding reduction of inorganic bromine. Therefore the total amount of bromine from VSLS in the stratosphere will not be changed by an increase in upwelling. Part of the increase of VSLS in the tropical lower stratosphere results from an increase in the corresponding tropopause height. As the depletion of stratospheric ozone due to bromine depends also on the availability of chlorine, we find the impact of bromine on stratospheric ozone at the end of the 21st century reduced compared to present day. Thus, these studies highlight the different factors influencing the role of brominated VSLS in a future climate.

scholarly journals Secondary organic aerosol formation and primary organic aerosol oxidation from biomass-burning smoke in a flow reactor during FLAME-3

2013 ◽  
Vol 13 (22) ◽  
pp. 11551-11571 ◽  
Author(s):  
A. M. Ortega ◽  
D. A. Day ◽  
M. J. Cubison ◽  
W. H. Brune ◽  
D. Bon ◽  
...  
Keyword(s):  
Mass Spectrometer ◽  
Biomass Burning ◽  
Flow Reactor ◽  
Organic Aerosol ◽  
Proton Transfer Reaction ◽  
Oxidation Products ◽  
Chemical Transformations ◽  
Aerosol Formation ◽  
Aerosol Mass ◽  
Smog Chambers

Abstract. We report the physical and chemical effects of photochemically aging dilute biomass-burning smoke. A "potential aerosol mass" (PAM) flow reactor was used with analysis by a high-resolution aerosol mass spectrometer and a proton-transfer-reaction ion-trap mass spectrometer during the FLAME-3 campaign. Hydroxyl (OH) radical concentrations in the reactor reached up to ~1000 times average tropospheric levels, producing effective OH exposures equivalent to up to 5 days of aging in the atmosphere, and allowing for us to extend the investigation of smoke aging beyond the oxidation levels achieved in traditional smog chambers. Volatile organic compound (VOC) observations show aromatics and terpenes decrease with aging, while formic acid and other unidentified oxidation products increase. Unidentified gas-phase oxidation products, previously observed in atmospheric and laboratory measurements, were observed here, including evidence of multiple generations of photochemistry. Substantial new organic aerosol (OA) mass ("net SOA"; secondary OA) was observed from aging biomass-burning smoke, resulting in total OA average of 1.42 ± 0.36 times the initial primary OA (POA) after oxidation. This study confirms that the net-SOA-to-POA ratio of biomass-burning smoke is far lower on average than that observed for urban emissions. Although most fuels were very reproducible, significant differences were observed among the biomasses, with some fuels resulting in a doubling of the OA mass, while for others a very small increase or even a decrease was observed. Net SOA formation in the photochemical reactor increased with OH exposure (OHexp), typically peaking around three days of equivalent atmospheric photochemical age (OHexp~3.9 × 1011 molecules cm−3 s), then leveling off at higher exposures. The amount of additional OA mass added from aging is positively correlated with initial POA concentration, but not with the total VOC concentration or the concentration of known SOA precursors. The mass of SOA formed often exceeded the mass of the known VOC precursors, indicating the likely importance of primary semivolatile/intermediate volatility species, and possibly of unidentified VOCs as SOA precursors in biomass burning smoke. Chemical transformations continued even after mass concentration stabilized. Changes in the biomass-burning tracer f60 ranged from substantially decreasing to remaining constant with increased aging. With increased OHexp, oxidation was always detected (as indicated by f44 and O/C). POA O/C ranged from 0.15 to 0.5, while aged OA O/C reached up to 0.87. The rate of oxidation and maximum O/C achieved differs for each biomass, and appears to increase with the initial O/C of the POA.

Characterizing the Aging of Biomass Burning Organic Aerosol by Use of Mixing Ratios: A Meta-analysis of Four Regions

2012 ◽  
Vol 46 (24) ◽  
pp. 13093-13102 ◽  
Author(s):  
Matthew D. Jolleys ◽  
Hugh Coe ◽  
Gordon McFiggans ◽  
Gerard Capes ◽  
James D. Allan ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Meta Analysis ◽  
Organic Aerosol ◽  
Mixing Ratios

scholarly journals Summertime contributions of isoprene, monoterpenes, and sesquiterpene oxidation to the formation of secondary organic aerosol in the troposphere over Mt. Tai, Central East China during MTX2006

2009 ◽  
Vol 9 (4) ◽  
pp. 16941-16972 ◽  
Author(s):  
P. Q. Fu ◽  
K. Kawamura ◽  
P. Pochanart ◽  
H. Tanimoto ◽  
Y. Kanaya ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Secondary Organic Aerosol ◽  
Atmospheric Transport ◽  
Organic Aerosol ◽  
Early Summer ◽  
Oxidation Products ◽  
East China ◽  
Gas Chromatography Mass Spectrometry ◽  
High Mountain ◽  
Night Time

Abstract. To better understand the contribution of biogenic volatile organic compounds to the formation of secondary organic aerosol (SOA) in high mountain regions, ambient aerosols were collected at the summit of Mt. Tai (1534 m, a.s.l.), Central East China (CEC) during the Mount Tai eXperiment 2006 campaign (MTX2006) in early summer. Biogenic SOA tracers of isoprene, monoterpenes, and β-caryophyllene oxidation products were measured using gas chromatography/mass spectrometry. All the biogenic SOA tracers showed no clear diurnal variations, suggesting that they are formed during long-range atmospheric transport. Although isoprene- and monoterpene-derived SOA tracers did not correlate with levoglucosan (a biomass burning tracer), β-caryophyllinic acid showed a good correlation with levoglucosan, indicating that biomass burning may be a source for this compound. Total concentrations of isoprene oxidation products are much higher than those of monoterpene and β-caryophyllene oxidation products. The ratio of isoprene to monoterpene oxidation products (Riso/mono) was found to co-vary with ozone and NOx during the summer campaign. The average Riso/mono value was 6.94 at daytime and 10.0 at nighttime. These values are among the highest in the aerosols studied in different regions, which may be due to the large isoprene fluxes, high O3 and NOx levels and relatively high OH concentrations in CEC. Using a tracer-based method, we estimated the average concentrations of secondary organic carbon (SOC) derived from isoprene, monoterpenes, and β-caryophyllene to be 1.76 μgC m−3 at daytime and 1.85 μgC m−3 at nighttime. These values correspond to 11.2% and 11.0% of the total OC concentrations, in which isoprene-derived SOC are 7.4% and 8.0% at day- and night-time, respectively. This study suggests that isoprene is a more significant precursor for biogenic SOA than monoterpenes and β-caryophyllene in high altitude in CEC.

scholarly journals Dilution impacts on smoke aging: Evidence in BBOP data

2020 ◽  
Author(s):  
Anna L. Hodshire ◽  
Emily Ramnarine ◽  
Ali Akherati ◽  
Matthew L. Alvarado ◽  
Delphine K. Farmer ◽  
...  
Keyword(s):  
Observational Data ◽  
Biomass Burning ◽  
Field Measurements ◽  
Measurable Quantity ◽  
Initial Field ◽  
Field Campaign ◽  
Smoke Aerosol ◽  
Smoke Plumes ◽  
Climate And Health ◽  
Aerosol Aging

Abstract. Biomass burning emits vapors and aerosols into the atmosphere that can rapidly evolve as smoke plumes travel downwind and dilute, affecting climate- and health-relevant properties of the smoke. To date, theory has been unable to explain variability in smoke evolution. Here, we use observational data from the BBOP field campaign and show that initial smoke concentrations can help predict changes in smoke aerosol aging markers, number, and diameter. Because initial field measurements of plumes are generally > 10 minutes downwind, smaller plumes will have already undergone substantial dilution relative to larger plumes. However, the extent to which dilution has occurred prior to the first observation is not a measurable quantity. Hence, initial observed concentrations can serve as an indicator of dilution, which impacts photochemistry and aerosol evaporation. Cores of plumes have higher concentrations than edges. By segregating the observed plumes into cores and edges, we infer that particle aging, evaporation, and coagulation occurred before the first measurement, and we find that edges generally undergo higher increases in oxidation tracers, more decreases in semivolatile compounds, and less coagulation than the cores.

scholarly journals Insights into the aging of biomass burning aerosol from satellite observations and 3D atmospheric modeling: Evolution of the aerosol optical properties in Siberian wildfire plumes

2020 ◽  
Author(s):  
Igor B. Konovalov ◽  
Nikolai A. Golovushkin ◽  
Matthias Beekmann ◽  
Meinrat O. Andreae
Keyword(s):  
Optical Properties ◽  
Long Range ◽  
Biomass Burning ◽  
Satellite Observations ◽  
The Arctic ◽  
Long Range Transport ◽  
Aerosol Optical Properties ◽  
Smoke Plumes ◽  
Range Transport ◽  
Aerosol Aging

Abstract. Long-range transport of biomass burning (BB) aerosol from regions affected by wildfires is known to have a significant impact on the radiative balance and air quality in receptor regions, including the Arctic. However, the atmospheric evolution of the optical properties of BB aerosol during the long-range transport events is insufficiently understood, limiting the adequacy of representations of the aerosol processes in chemistry transport and climate models. Here we introduce a framework to infer and interpret changes of the optical properties of BB aerosol from satellite observations of multiple BB plumes. Our framework includes (1) a procedure for analysis of available satellite retrievals of the absorption and extinction aerosol optical depths (AAOD and AOD) and single scattering albedo (SSA) as a function of the BB aerosol photochemical age, and (2) a representation of the AAOD and AOD evolution with a chemistry transport model (CTM) involving a simplified volatility basis set (VBS) scheme with a few adjustable parameters. We apply this framework to analyze a large-scale outflow of BB smoke plumes from Siberia toward Europe that occurred in July 2016. We use AAOD and SSA data derived from OMI (Ozone Monitoring Instrument) satellite measurements in the near-UV range along with 550 nm AOD and carbon monoxide (CO) columns retrieved from MODIS (Moderate Resolution Imaging Spectroradiometer) and IASI (Infrared Atmospheric Sounding Interferometer) satellite observations, respectively, to infer changes in the optical properties of Siberian BB aerosol due to its atmospheric aging and to get insights into the processes underlying these changes. Using the satellite data in combination with simulated data from the CHIMERE CTM, we evaluate the enhancement ratios (EnR) that allow isolating AAOD and AOD changes due to oxidation and gas-particle partitioning processes from those due to other processes, including transport, deposition, and wet scavenging. The behavior of EnRs for AAOD and AOD is then characterized using nonlinear trend analysis. It is found that the EnR for AOD strongly increases (by about a factor of 2) during the first 20–30 hours of the analyzed evolution period, whereas the EnR for AAOD does not exhibit a statistically significant increase during this period. The increase in AOD is accompanied by a statistically significant enhancement of SSA. Further BB aerosol aging (up to several days) is associated with a strong decrease of EnRs for both AAOD and AOD. Our simulations constrained by the observations indicate that the upward trends in EnR for AOD and in SSA are mainly due to atmospheric processing of secondary organic aerosol (SOA), leading to an increase in the mass scattering efficiency of BB aerosol. Evaporation and chemical fragmentation of the SOA species, part of which is assumed to be absorptive (to contain brown carbon), are identified as a likely reason for the subsequent decrease of the EnR for both AAOD and AOD. Hence, our analysis reveals that the long-range transport of smoke plumes from Siberian fires is associated with major changes in BB aerosol optical properties and chemical composition. Overall, this study demonstrates the feasibility of using available satellite observations for evaluating and improving representations in atmospheric models of the BB aerosol aging processes in different regions of the world at much larger temporal scales than those typically addressed in aerosol chamber experiments.

scholarly journals Nonlinear behavior of organic aerosol in biomass burning plumes: a microphysical model analysis

2019 ◽  
Author(s):  
Igor B. Konovalov ◽  
Matthias Beekmann ◽  
Nikolai A. Golovushkin ◽  
Meinrat O. Andreae
Keyword(s):  
Biomass Burning ◽  
Linear Part ◽  
Nonlinear Behavior ◽  
Organic Aerosol ◽  
Basis Set ◽  
Aging Effects ◽  
Transport Models ◽  
Smoke Plume ◽  
Smoke Plumes ◽  
The Impact

Abstract. Organic aerosol (OA) is a major component of smoke plumes from open biomass burning (BB). Therefore, adequate representation of the atmospheric transformations of BB OA in chemistry-transport and climate models is an important prerequisite for accurate estimates of the impact of BB emissions on air quality and climate. However, field and laboratory studies of atmospheric transformations (aging) of BB OA have yielded a wide diversity of observed effects. This diversity is still not sufficiently understood and thus not addressed in models. As OA evolution is governed by complex nonlinear processes, it is likely that at least a part of the observed variability of the BB OA aging effects is due to the factors associated with the intrinsic nonlinearity of the OA system. In this study, we performed a numerical analysis in order to gain a deeper understanding of such factors. We employ a microphysical dynamic model that represents gas-particle partitioning and OA oxidation chemistry within the volatility basis set (VBS) framework and includes a schematic parameterization of BB OA dilution due to dispersion of an isolated smoke plume. Several VBS schemes of different complexity, which have been suggested in the literature to represent BB OA aging in regional and global chemistry-transport models, are applied to simulate BB OA evolution over a five-day period representative of a BB aerosol lifetime in the dry atmosphere. We consider the BB OA mass enhancement ratio (EnR), which is defined as the ratio of the mass concentration of BB OA to that of an inert tracer and allows us to eliminate the linear part of the dilution effects. We also analyze the behavior of the hygroscopicity parameter, κ, that was simulated in a part of our numerical experiments. As a result, five qualitatively different regimes of OA evolution are identified, which comprise (1) a monotonic saturating increase of EnR, (2) an increase of EnR followed by a decrease, (3) an initial rapid decrease of EnR followed by a gradual increase, (4) an EnR increase between two intermittent stages of its decrease, or (5) a gradual decrease of EnR. We find that the EnR for BB aerosol aged from a few hours to a few tens of hours typically increases for larger initial sizes of the smoke plume (and therefore, smaller dilution rates) or for lower initial OA concentrations (and thus more organic gases available to form secondary OA). However, these dependencies can be weakened or even reversed, depending on the BB OA age and on the ratio between the fragmentation and functionalization oxidation pathways. Nonlinear behavior of BB OA is also exhibited in the dependencies of κ on the parameters of the plume. Application of the different VBS schemes results in large quantitative and qualitative differences between the simulations, although our analysis suggests also that the main qualitative features of OA evolution simulated with a complex two-dimensional VBS scheme can also be reproduced with a much simpler scheme. Overall, this study indicates that the BB aerosol evolution may strongly depend on parameters of the individual BB smoke plumes (such as the initial organic aerosol concentration and plume size) that are typically not resolved in chemistry transport models.

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