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 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 Modelling the optical properties of fresh biomass burning aerosol produced in a smoke chamber: results from the EFEU campaign

2007 ◽  
Vol 7 (4) ◽  
pp. 12657-12686 ◽  
Author(s):  
K. Hungershöfer ◽  
K. Zeromskiene ◽  
Y. Iinuma ◽  
G. Helas ◽  
J. Trentmann ◽  
...  
Keyword(s):  
Optical Properties ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
Absorption Efficiency ◽  
Max Planck ◽  
Fresh Biomass ◽  
Biomass Burning Aerosol ◽  
Smoke Chamber ◽  
The Impact ◽  
Mass Absorption Efficiency

Abstract. A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the 'Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere' (EFEU) project. Using the measured size distributions as well as mass scattering and absorption efficiencies, Mie calculations provided mean effective refractive indices of 1.60−0.010i and 1.56−0.010i (λ=0.55 μm) for smoke particles emitted from the combustion of savanna grass and an African hardwood (musasa), respectively. The relatively low imaginary parts suggest that the light-absorbing carbon of the investigated fresh biomass burning aerosol is only partly graphitized, resulting in strongly scattering and less absorbing particles. While the observed variability in mass scattering efficiencies was consistent with changes in particle size, the changes in the mass absorption efficiency can only be explained, if the chemical composition of the particles varies with combustion conditions.

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 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 Aged boreal biomass-burning aerosol size distributions from BORTAS 2011

2015 ◽  
Vol 15 (4) ◽  
pp. 1633-1646 ◽  
Author(s):  
K. M. Sakamoto ◽  
J. D. Allan ◽  
H. Coe ◽  
J. W. Taylor ◽  
T. J. Duck ◽  
...  
Keyword(s):  
Size Distribution ◽  
Biomass Burning ◽  
Forest Fires ◽  
Radiative Forcing ◽  
Organic Aerosol ◽  
Satellite Measurement ◽  
Entrainment Rate ◽  
Size Distributions ◽  
Median Diameter ◽  
The Impact

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 (cloud condensation nuclei) concentrations and forcing estimates derived from these models. The BORTAS-B (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellite) 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) and σ = 1.5, 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 0.09–0.17 μg m−3 ppbv−1 (parts per billion by volume) with no significant trend with distance from the source. This lack of enhancement ratio increase/decrease with distance suggests no detectable net OA (organic aerosol) production/evaporation within the aged plume over the sampling period (plume age: 1–2 days), though it does not preclude OA production/loss at earlier stages. 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 young-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.

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