scholarly journals The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

2016 ◽  
Vol 16 (12) ◽  
pp. 7709-7724 ◽  
Author(s):  
Kimiko M. Sakamoto ◽  
James R. Laing ◽  
Robin G. Stevens ◽  
Daniel A. Jaffe ◽  
Jeffrey R. Pierce
Keyword(s):  
Wind Speed ◽  
Size Distribution ◽  
Biomass Burning ◽  
Independent Set ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
Atmospheric Conditions ◽  
Mixing Depth ◽  
Fire Area ◽  
Biomass Burning Aerosol

Abstract. Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The size distribution is particularly sensitive to the mass emissions flux, fire area, wind speed, and time, and we provide simplified fits of the aged size distribution to just these input variables. The simplified fits were tested against 11 aged biomass-burning size distributions observed at the Mt. Bachelor Observatory in August 2015. The simple fits captured over half of the variability in observed Dpm and modal width even though the freshly emitted Dpm and modal widths were unknown. These fits may be used in global and regional aerosol models. Finally, we show that coagulation generally leads to greater changes in the particle size distribution than OA evaporation/formation does, using estimates of OA production/loss from the literature.

scholarly journals The evolution of biomass-burning aerosol size distributions due to coagulation: dependence on fire and meteorological details and parameterization

2016 ◽  
Author(s):  
K. M. Sakamoto ◽  
R. G. Stevens ◽  
J. R. Pierce
Keyword(s):  
Wind Speed ◽  
Size Distribution ◽  
Biomass Burning ◽  
Independent Set ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
Atmospheric Conditions ◽  
Mixing Depth ◽  
Fire Area ◽  
Biomass Burning Aerosol

Abstract. Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, to account for biomass-burning aerosol size in global models accurately requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emissions-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations, and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The aged size distribution is particularly sensitive to the mass emissions flux, fire area, wind speed, and time, and we provide simplified fits of the aged size distribution to just these input variables. These fits may be used in global and regional aerosol models. Finally, we show that variability in coagulation may lead to greater variability in the particle size distribution than does OA evaporation/formation using estimates of OA production/loss from the literature.

scholarly journals Effects of near-source coagulation of biomass burning aerosols on global predictions of aerosol size distributions and implications for aerosol radiative effects

2019 ◽  
Vol 19 (9) ◽  
pp. 6561-6577 ◽  
Author(s):  
Emily Ramnarine ◽  
John K. Kodros ◽  
Anna L. Hodshire ◽  
Chantelle R. Lonsdale ◽  
Matthew J. Alvarado ◽  
...  
Keyword(s):  
Size Distribution ◽  
Biomass Burning ◽  
Indirect Effect ◽  
Size Distributions ◽  
Aerosol Indirect Effect ◽  
Fresh Biomass ◽  
Biomass Burning Aerosol ◽  
Aerosol Radiative Effects ◽  
The Impact ◽  
Aerosol Radiative

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models have ignored sub-grid coagulation and instantly mixed fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem–TOMAS (TwO-Moment Aerosol Sectional) global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This cloud condensation nuclei (CCN) reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2, with assumed external mixing of black carbon and from −188 to −197 mW m−2 and with assumed internal mixing of black carbon with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories to various assumptions about the fresh biomass burning aerosol size distribution and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.

scholarly journals Effects of Near-Source Coagulation of Biomass Burning Aerosols on Global Predictions of Aerosol Size Distributions and Implications for Aerosol Radiative Effects

2018 ◽  
Author(s):  
Emily Ramnarine ◽  
John K. Kodros ◽  
Anna L. Hodshire ◽  
Chantelle R. Lonsdale ◽  
Matthew J. Alvarado ◽  
...  
Keyword(s):  
Size Distribution ◽  
Biomass Burning ◽  
Indirect Effect ◽  
Size Distributions ◽  
Aerosol Indirect Effect ◽  
Fresh Biomass ◽  
Biomass Burning Aerosol ◽  
Aerosol Radiative Effects ◽  
The Impact ◽  
Aerosol Radiative

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models ignore sub-grid coagulation and instantly mix fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem-TOMAS global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This CCN reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2 with assumed external mixing and from −188 to −197 mW m−2 with assumed internal mixing with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories, to various assumptions about the fresh biomass burning aerosol size distribution, and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.

scholarly journals Biomass burning aerosol size distribution and modeled optical properties

1998 ◽  
Vol 103 (D24) ◽  
pp. 31879-31891 ◽  
Author(s):  
L. A. Remer ◽  
Y. J. Kaufman ◽  
B. N. Holben ◽  
A. M. Thompson ◽  
D. McNamara
Keyword(s):  
Optical Properties ◽  
Size Distribution ◽  
Biomass Burning ◽  
Aerosol Size Distribution ◽  
Biomass Burning Aerosol

Determination of atmospheric aerosol particle size distribution and visibility using a mobile laboratory

1982 ◽  
Vol 60 (8) ◽  
pp. 1101-1107
Author(s):  
C. V. Mathai ◽  
A. W. Harrison
Keyword(s):  
Particle Size ◽  
Particle Size Distribution ◽  
Size Distribution ◽  
Atmospheric Aerosols ◽  
Suspended Particle ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
Mobile Laboratory ◽  
Mean Values ◽  
The City

As part of an ongoing general research program on the effects of atmospheric aerosols on visibility and its dependence on aerosol size distributions in Calgary, this paper presents the results of a comparative study of particle size distribution and visibility in residential (NW) and industrial (SE) sections of the city using a mobile laboratory. The study was conducted in the period October–December, 1979. An active scattering aerosol spectrometer measured the size distributions and the corresponding visibilities were deduced from scattering coefficients measured with an integrating nephelometer.The results of this transit study show significantly higher suspended particle concentrations and reduced visibilities in the SE than in the NW. The mean values of the visibilities are 44 and 97 km for the SE and the NW respectively. The exponent of R (particle radius) in the power law aerosol size distribution has a mean value of −3.36 ± 0.24 in the SE compared with the corresponding value of −3.89 ± 0.39 for the NW. These results arc in good agreement with the observations of Alberta Environment; however, they are in contradiction with a recent report published by the City of Calgary.

scholarly journals An investigation of processes controlling the evolution of the boundary layer aerosol size distribution properties at the Swedish background station Aspvreten

2004 ◽  
Vol 4 (4) ◽  
pp. 4507-4543 ◽  
Author(s):  
P. Tunved ◽  
J. Ström ◽  
H.-C. Hansson
Keyword(s):  
Size Distribution ◽  
Wet Deposition ◽  
Source Area ◽  
Aerosol Size Distribution ◽  
Back Trajectory ◽  
Main Process ◽  
Size Distributions ◽  
Back Trajectory Analysis ◽  
The One ◽  
Precipitating Clouds

Abstract. Aerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E). Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing the different stages of the aerosol lifecycle. The aerosol was interpreted as belonging to fresh, intermediate and aged type of size distribution and different magnitudes thereof. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features likely related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability. Processing by non-precipitating clouds most obviously affect aerosols in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions bearing signs of recent new particle formation (~30% of the observed size distributions) represent the first stage in the lifecycle. Aging may proceed in two directions: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area) in environments similar to the one studied.

scholarly journals Aged boreal biomass burning aerosol size distributions from BORTAS 2011

2014 ◽  
Vol 14 (17) ◽  
pp. 24349-24385 ◽  
Author(s):  
K. M. Sakamoto ◽  
J. D. Allan ◽  
H. Coe ◽  
J. W. Taylor ◽  
T. J. Duck ◽  
...  
Keyword(s):  
Size Distribution ◽  
Biomass Burning ◽  
Radiative Forcing ◽  
Climate Model ◽  
Sampling Period ◽  
Characteristic Size ◽  
Entrainment Rate ◽  
Size Distributions ◽  
Eastern Canada ◽  
Median Diameter

Abstract. Biomass-burning aerosols contribute to aerosol radiative forcing on the climate system. The magnitude of this effect is partially determined by aerosol size distributions, which are functions of source fire characteristics (e.g. fuel type, MCE) and in-plume microphysical processing. The uncertainties in biomass-burning emission number size-distributions in climate model inventories lead to uncertainties in the CCN concentrations and forcing estimates derived from these models. The BORTAS-B measurement campaign was designed to sample boreal biomass-burning outflow over Eastern Canada in the summer of 2011. Using these BORTAS-B data, we implement plume criteria to isolate the characteristic size-distribution of aged biomass-burning emissions (aged ∼1–2 days) from boreal wildfires in Northwestern Ontario. The composite median size-distribution yields a single dominant accumulation mode with Dpm = 230 nm (number-median diameter), σ = 1.7, which are comparable to literature values of other aged plumes of a similar type. The organic aerosol enhancement ratios (ΔOA / ΔCO) along the path of Flight b622 show values of 0.05–0.18 μg m−3 ppbv−1 with no significant trend with distance from the source. This lack of enhancement ratio increase/decrease with distance suggests no detectable net OA production/evaporation within the aged plume over the sampling period. A Lagrangian microphysical model was used to determine an estimate of the freshly emitted size distribution corresponding to the BORTAS-B aged size-distributions. The model was restricted to coagulation and dilution processes based on the insignificant net OA production/evaporation derived from the ΔOA / ΔCO enhancement ratios. We estimate that the fresh-plume median diameter was in the range of 59–94 nm with modal widths in the range of 1.7–2.8 (the ranges are due to uncertainty in the entrainment rate). Thus, the size of the freshly emitted particles is relatively unconstrained due to the uncertainties in the plume dilution rates.

scholarly journals Quantifying aerosol size distributions and their temporal variability in the Southern Great Plains, USA

2019 ◽  
Vol 19 (18) ◽  
pp. 11985-12006 ◽  
Author(s):  
Peter J. Marinescu ◽  
Ezra J. T. Levin ◽  
Don Collins ◽  
Sonia M. Kreidenweis ◽  
Susan C. van den Heever
Keyword(s):  
Size Distribution ◽  
Great Plains ◽  
Diurnal Cycle ◽  
Particle Formation ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
New Particle Formation ◽  
Scanning Mobility Particle Sizer ◽  
Southern Great Plains ◽  
Particle Sizer

Abstract. A quality-controlled, 5-year dataset of aerosol number size distributions (particles with diameters (Dp) from 7 nm through 14 µm) was developed using observations from a scanning mobility particle sizer, aerodynamic particle sizer, and a condensation particle counter at the Department of Energy's Southern Great Plains (SGP) site. This dataset was used for two purposes. First, typical characteristics of the aerosol size distribution (number, surface area, and volume) were calculated for the SGP site, both for the entire dataset and on a seasonal basis, and size distribution lognormal fit parameters are provided. While the median size distributions generally had similar shapes (four lognormal modes) in all the seasons, there were some significant differences between seasons. These differences were most significant in the smallest particles (Dp<30 nm) and largest particles (Dp>800 nm). Second, power spectral analysis was conducted on this long-term dataset to determine key temporal cycles of total aerosol concentrations, as well as aerosol concentrations in specified size ranges. The strongest cyclic signal was associated with a diurnal cycle in total aerosol number concentrations that was driven by the number concentrations of the smallest particles (Dp<30 nm). This diurnal cycle in the smallest particles occurred in all seasons in ∼50 % of the observations, suggesting a persistent influence of new particle formation events on the number concentrations observed at the SGP site. This finding is in contrast with earlier studies that suggest new particle formation is observed primarily in the springtime at this site. The timing of peak concentrations associated with this diurnal cycle was shifted by several hours depending on the season, which was consistent with seasonal differences in insolation and boundary layer processes. Significant diurnal cycles in number concentrations were also found for particles with Dp between 140 and 800 nm, with peak concentrations occurring in the overnight hours, which were primarily associated with both nitrate and organic aerosol cycles. Weaker cyclic signals were observed for longer timescales (days to weeks) and are hypothesized to be related to the timescales of synoptic weather variability. The strongest periodic signals (3.5–5 and 7 d cycles) for these longer timescales varied depending on the season, with no cyclic signals and the lowest variability in the summer.

scholarly journals Biomass Burning Aerosol as a Modulator of Droplet Number in the Southeast Atlantic Region

2019 ◽  
Author(s):  
Mary Kacarab ◽  
K. Lee Thornhill ◽  
Amie Dobracki ◽  
Steven G. Howell ◽  
Joseph R. O'Brien ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Marine Boundary Layer ◽  
Cloud Condensation Nuclei ◽  
Central Africa ◽  
Aerosol Size Distribution ◽  
Atlantic Region ◽  
Radiative Impact ◽  
Biomass Burning Aerosol ◽  
Aerosol Cloud Interactions ◽  
Southeastern Atlantic

Abstract. The southeastern Atlantic (SEA) and its associated cloud deck, off the west coast of central Africa, is an area where aerosol-cloud interactions can have a strong radiative impact. Seasonally, extensive biomass burning (BB) aerosol plumes from southern Africa reach this area. The NASA ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) study focused on quantitatively understanding these interactions and their importance. Here we present measurements of cloud condensation nuclei (CCN) concentration, aerosol size distribution, and vertical updraft velocity in and around the marine boundary layer (MBL) collected by the NASA P-3B aircraft during the August 2017 ORACLES deployment. BB aerosol levels vary considerably but systematically with time; high aerosol concentrations were observed in the MBL (800–1000 cm−3) early on, decreasing mid-campaign to concentrations between 500–800 cm−3. By late August and early September, relatively clean MBL conditions were sampled (

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