Biomass burning emits particles (black carbon and primary organic aerosol) and precursor vapors to the atmosphere that chemically and physically age in the atmosphere. This theoretical study explores the relationships between fire size (determining the initial plume width and concentration), dilution rate, and entrainment of background aerosol on particle coagulation, organic aerosol (OA) evaporation, and secondary organic aerosol (SOA) condensation in smoke plumes. We examine the impacts of these processes on aged smoke OA mass, geometric mean diameter (Dg), peak lognormal modal width (σg), particle extinction (E), and cloud condensation nuclei (CCN) concentrations. In our simulations, aging OA mass is controlled by competition between OA evaporation and SOA condensation. Large, slowly diluting plumes evaporate little in our base set of simulations, which may allow for net increases in mass, E, CCN , and Dg from SOA condensation. Smaller, quickly diluting fire plumes lead to faster evaporation, which favors decreases in mass, E, CCN, and Dg. However, the SOA fraction of the smoke OA increases more rapidly in smaller fires due to faster primary organic aerosol evaporation leading to more SOA precursors. Net mass changes for smaller fires depend on background OA concentrations; increasing background aerosol concentrations decrease evaporation rates. Although coagulation does not change mass, it can decrease the number of particles in large/slowly diluting plumes, increasing Dg and E, and decreasing σg. While our conclusions are limited by being a theoretical study, we hope they help motivate future smoke‐plume analyses to consider the effects of fire size, meteorology, and background OA concentrations.

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 observed variability in smoke evolution. Here, we use observational data from the Biomass Burning Observation Project (BBOP) field campaign and show that initial smoke organic aerosol mass concentrations can help predict changes in smoke aerosol aging markers, number concentration, and number mean diameter between 40–262 nm. Because initial field measurements of plumes are generally >10 min downwind, smaller plumes will have already undergone substantial dilution relative to larger plumes and have lower concentrations of smoke species at these observations closest to the fire. The extent to which dilution has occurred prior to the first observation is not a directly measurable quantity. We show that initial observed plume concentrations can serve as a rough indicator of the extent of dilution prior to the first measurement, which impacts photochemistry, aerosol evaporation, and coagulation. Cores of plumes have higher concentrations than edges. By segregating the observed plumes into cores and edges, we find evidence that particle aging, evaporation, and coagulation occurred before the first measurement. We further find that on the plume edges, the organic aerosol is more oxygenated, while a marker for primary biomass burning aerosol emissions has decreased in relative abundance compared to the plume cores. Finally, we attempt to decouple the roles of the initial concentrations and physical age since emission by performing multivariate linear regression of various aerosol properties (composition, size) on these two factors.

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.

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.

Particle-phase air pollution is a leading risk factor for premature death globally and impacts climate by scattering or absorbing radiation and changing cloud properties. Within the Beijing-Tianjin-Hebei region of China, where there are severe air quality problems, several municipalities have begun implementing a coal-to-electricity program that bans residential coal and provides subsidies for electricity and electric-powered heat pumps. We used GEOS-Chem to evaluate two complete residential coal-to-electricity transitions-a Beijing-off scenario and Beijing-Tianjin-Hebei-off scenario-each relative to a base case. We estimate that within China, the ambient fine particulate matter (PM2.5) reductions in the Beijing-off scenario could lead to 1,900 (95% CI: 1,200-2,700) premature deaths avoided annually, while the Beijing-Tianjin-Hebei-off scenario could lead to 13,700 (95% CI: 8,900-19,600) premature deaths avoided annually. Additionally, we estimate that the residential-coal-ban scenarios will result in a positive top-of-the-atmosphere aerosol direct radiative effect (DRE) (model domain average: Beijing-off: 0.023 W m -2 ; Beijing-Tianjin-Hebei-off: 0.30 W m -2 ) and a negligible cloud-albedo aerosol indirect effect (AIE) (Beijing-off: 0.0001 W m -2 ; Beijing-Tianjin-Hebei-off: 0.0027 W m -2 ). To evaluate the uncertainty of the radiative effects, we calculated the DRE under four black-carbon mixing-state assumptions and both the DRE and AIE assuming three different black-carbon-to-organic-aerosol (BC:OA) ratios for residential-coal emissions. Although the magnitude of our radiative forcing estimates varied across sensitivity cases, the domain average remained positive. When only considering the aerosol-related effects of the aforementioned coal-ban scenarios, we predict substantial health benefits, but do not anticipate a climate "co-benefit", because removing aerosol emissions leads to a warming tendency. However, if the coal-to-electricity program results in less net greenhouse gas emissions due to the replacement heaters, the policy may be able to achieve health and climate "co-benefits".

Abstract. Biomass burning is a major source of trace gases and aerosols that can ultimately impact health, air quality, and climate. Global and regional-scale three-dimensional Eulerian chemical transport models (CTMs) use estimates of the primary emissions from fires and can unphysically mix them across large-scale grid boxes, leading to incorrect estimates of the impact of biomass burning events. On the other hand, plume-scale process models allow for explicit simulation and examination of the chemical and physical transformations of trace gases and aerosols within biomass burning smoke plumes, and they may be used to develop parameterizations of this aging process for coarser grid-scale models. Here we describe the coupled SAM-ASP plume-scale process model, which consists of coupling the large-eddy simulation model, the System for Atmospheric Modelling (SAM), with the detailed gas and aerosol chemistry model, the Aerosol Simulation Program (ASP). We find that the SAM-ASP version 1.0 model is able to correctly simulate the dilution of CO in a California chaparral smoke plume, as well as the chemical loss of NOx, HONO, and NH3 within the plume, the formation of PAN and O3, the loss of OA, and the change in the size distribution of aerosols as compared to measurements and previous single-box model results. The newly coupled model is able to capture the cross-plume vertical and horizontal concentration gradients as the fire plume evolves downwind of the emission source. The integration and evaluation of SAM-ASP version 1.0 presented here will support the development of parameterizations of near-source biomass burning chemistry that can be used to more accurately simulate biomass burning chemical and physical transformations of trace gases and aerosols within coarser grid-scale CTMs.

<p><strong>Abstract.</strong> 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.</p> <p>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<sup>−2</sup>. 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<sup>−2</sup> with assumed external mixing and from −188 to −197 mW m<sup>−2</sup> 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.</p>

Biomass burning is a major source of trace gases and aerosols that can ultimately impact health, air quality, and climate. Global and regional-scale three-dimensional Eulerian chemical transport models (CTMs) use estimates of the primary emissions from fires and can unphysically mix them across large-scale grid boxes, leading to incorrect estimates of the impact of biomass 10 burning events. On the other hand, plume-scale process models allow for explicit simulation and examination of the chemical and physical transformations of trace gases and aerosols within biomass burning smoke plumes, and they may be used to develop parameterizations of this aging process for coarser grid-scale models. Here we describe the coupled SAM-ASP plume-scale process model, which consists of coupling the large-eddy simulation model, the System for Atmospheric Modelling (SAM), with the detailed gas and aerosol chemistry model, the Aerosol Simulation Program (ASP). We find that the SAM-ASP version 1.0 model 15 is able to correctly simulate the dilution of CO in a California chaparral smoke plume, as well as the chemical loss of NOx, HONO, and NH3 within the plume, the formation of PAN and O3, the loss of OA, and the change in the size distribution of aerosols as compared to measurements and previous single-box model results. The newly coupled model is able to capture the cross-plume vertical and horizontal concentration gradients as the fire plume evolves downwind of the emission source. The integration and evaluation of SAM-ASP version 1.0 presented here will support the development of parameterizations of near-source biomass 20 burning chemistry that can be used to more accurately simulate biomass burning chemical and physical transformations of trace gases and aerosols within coarser grid-scale CTMs.