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Abstract Injections of wildfire smoke plumes into the free troposphere impact air quality, yet model forecasts of injections are poor. Here, we use aircraft observations obtained during the 2019 western US wildfires (FIREX-AQ) to evaluate a commonly used smoke plume rise parameterization in two atmospheric chemistry-transport models (WRF-Chem and HRRR-Smoke). Observations show that smoke injections into the free troposphere occur in 35% of plumes, whereas the models forecast 59–95% indicating false injections in the simulations. False injections were associated with both models overestimating fire heat flux and terrain height, and with WRF-Chem underestimating planetary boundary layer height. We estimate that the radiant fraction of heat flux is 0.5 to 25 times larger in models than in observations, depending on fuel type. Model performance was substantially improved by using observed heat flux and boundary layer heights, confirming that models need accurate heat fluxes and boundary layer heights to correctly forecast plume injections. 

Abstract. Accurate representation of aerosol optical properties is essential for the modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, the use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. Inthis study, airborne measurements over the United States (DISCOVER-AQ) andSouth Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organicmatter (OM) and sulfate–nitrate–ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r=0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation(GEOS-Chem-TOMAS) indicates that MSNAOM and theratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of the dry effective radius (Reff) for SNA and OM aerosol is designed to represent the airborne measurements (R2=0.74; slope = 1.00) and the GEOS-Chem-TOMAS simulation (R2=0.72; slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R2 from 0.68 to 0.73 and slope from 0.75 to 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. 

Abstract. Extensive airborne measurements of non-methane organic gases (NMOGs), methane, nitrogen oxides, reduced nitrogen species, and aerosol emissions from US wild and prescribed fires were conducted during the 2019 NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality campaign (FIREX-AQ). Here, we report the atmospheric enhancement ratios (ERs) and inferred emission factors (EFs) for compounds measured on board the NASA DC-8 research aircraft for nine wildfires and one prescribed fire, which encompass a range of vegetation types. We use photochemical proxies to identify young smoke and reduce the effects of chemical degradation on our emissions calculations. ERs and EFs calculated from FIREX-AQ observations agree within a factor of 2, with values reported from previous laboratory and field studies for more than 80 % of the carbon- and nitrogen-containing species. Wildfire emissions are parameterized based on correlations of the sum of NMOGs with reactive nitrogen oxides (NOy) to modified combustion efficiency (MCE) as well as other chemical signatures indicative of flaming/smoldering combustion, including carbon monoxide (CO), nitrogen dioxide (NO2), and black carbon aerosol. The sum of primary NMOG EFs correlates to MCE with an R2 of 0.68 and a slope of −296 ± 51 g kg−1, consistent with previous studies. The sum of the NMOG mixing ratios correlates well with CO with an R2 of 0.98 and a slope of 137 ± 4 ppbv of NMOGs per parts per million by volume (ppmv) of CO, demonstrating that primary NMOG emissions can be estimated from CO. Individual nitrogen-containing species correlate better with NO2, NOy, and black carbon than with CO. More than half of the NOy in fresh plumes is NO2 with an R2 of 0.95 and a ratio of NO2 to NOy of 0.55 ± 0.05 ppbv ppbv−1, highlighting that fast photochemistry had already occurred in the sampled fire plumes. The ratio of NOy to the sum of NMOGs follows trends observed in laboratory experiments and increases exponentially with MCE, due to increased emission of key nitrogen species and reduced emission of NMOGs at higher MCE during flaming combustion. These parameterizations will provide more accurate boundary conditions for modeling and satellite studies of fire plume chemistry and evolution to predict the downwind formation of secondary pollutants, including ozone and secondary organic aerosol. 

Abstract. Wildfire smoke is one of the most significant concerns ofhuman and environmental health, associated with its substantial impacts onair quality, weather, and climate. However, biomass burning emissions andsmoke remain among the largest sources of uncertainties in air qualityforecasts. In this study, we evaluate the smoke emissions and plumeforecasts from 12 state-of-the-art air quality forecasting systemsduring the Williams Flats fire in Washington State, US, August 2019, whichwas intensively observed during the Fire Influence on Regional to GlobalEnvironments and Air Quality (FIREX-AQ) field campaign. Model forecasts withlead times within 1 d are intercompared under the same framework basedon observations from multiple platforms to reveal their performanceregarding fire emissions, aerosol optical depth (AOD), surface PM2.5,plume injection, and surface PM2.5 to AOD ratio. The comparison ofsmoke organic carbon (OC) emissions suggests a large range of daily totalsamong the models, with a factor of 20 to 50. Limited representations of thediurnal patterns and day-to-day variations of emissions highlight the needto incorporate new methodologies to predict the temporal evolution andreduce uncertainty of smoke emission estimates. The evaluation of smoke AOD(sAOD) forecasts suggests overall underpredictions in both the magnitude andsmoke plume area for nearly all models, although the high-resolution modelshave a better representation of the fine-scale structures of smoke plumes.The models driven by fire radiativepower (FRP)-based fire emissions or assimilating satellite AODdata generally outperform the others. Additionally, limitations of thepersistence assumption used when predicting smoke emissions are revealed bysubstantial underpredictions of sAOD on 8 August 2019, mainly over thetransported smoke plumes, owing to the underestimated emissions on7 August. In contrast, the surface smoke PM2.5 (sPM2.5) forecastsshow both positive and negative overall biases for these models, with mostmembers presenting more considerable diurnal variations of sPM2.5.Overpredictions of sPM2.5 are found for the models driven by FRP-basedemissions during nighttime, suggesting the necessity to improve verticalemission allocation within and above the planetary boundary layer (PBL).Smoke injection heights are further evaluated using the NASA LangleyResearch Center's Differential Absorption High Spectral Resolution Lidar(DIAL-HSRL) data collected during the flight observations. As the firebecame stronger over 3–8 August, the plume height became deeper, with aday-to-day range of about 2–9 km a.g.l. However, narrower ranges arefound for all models, with a tendency of overpredicting the plume heights forthe shallower injection transects and underpredicting for the days showingdeeper injections. The misrepresented plume injection heights lead toinaccurate vertical plume allocations along the transects corresponding totransported smoke that is 1 d old. Discrepancies in model performance forsurface PM2.5 and AOD are further suggested by the evaluation of theirratio, which cannot be compensated for by solely adjusting the smoke emissionsbut are more attributable to model representations of plume injections,besides other possible factors including the evolution of PBL depths andaerosol optical property assumptions. By consolidating multiple forecastsystems, these results provide strategic insight on pathways to improvesmoke forecasts.