The vertical distribution of wildfire smoke aerosols is important in determining its environmental impacts but existing observations of smoke heights generally do not possess the temporal resolution required to fully resolve the diurnal behavior of wildfire smoke injection. We use Weather Surveillance Radar-1988 Doppler (WSR-88D) dual polarization data to estimate injection heights of Biomass Burning Debris (BBD) generated by fires. We detect BBD as a surrogate for smoke aerosols, which are often collocated with BBD near the fire but are not within the size range detectable by these radars. Injection heights of BBD are derived for 2-10 August 2019, using radar reflectivity (Z≥10 dBZ) and dual polarization correlation coefficients (0.2<C.C.<0.9) to study the Williams Flats Fire event. Results show the expected diurnal cycles with maximum injection heights present during the late afternoon period when the fire’s intensity and convective mixing are maximized. Radar and airborne lidar injection height comparisons reveal that this method is sensitive to outliers and generally overpredicts maximum heights by 40%, though mean and median heights are better captured (<20% mean error). Radar heights between the 75th and 90thpercentile seem to accurately represent the maximum, with the exception of heights estimated during the occurrence of pyro-cumulonimbus. Location specific mapping of radar and lidar injection heights reveal that they diverge further away from the fire due to BBD settling. Most importantly, radar-derived injection height estimates provide near continuous smoke height information, allowing for the study of diurnal variability of smoke injections.  

Process modeling of aerosol-cloud interaction is essential to bridging gaps between observational analysis and climate modeling of aerosol effects in the Earth system and eventually reducing climate projection uncertainties. In this study, we examine aerosol-cloud interaction in summertime precipitating shallow cumuli observed during the Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). Aerosols and precipitating shallow cumuli were extensively observed with in-situ and remote-sensing instruments during two research flight cases on 02 June and 07 June, respectively, during the ACTIVATE summer 2021 deployment phase. We perform observational analysis and large-eddy simulation (LES) of aerosol effect on precipitating cumulus in these two cases. Given the measured aerosol size distributions and meteorological conditions, LES is able to reproduce the observed cloud properties by aircraft such as liquid water content (LWC), cloud droplet number concentration (Nc) and effective radius reff. However, it produces smaller liquid water path (LWP) and larger Nc compared to the satellite retrievals. Both 02 and 07 June cases are over warm waters of the Gulf Stream and have a cloud top height over 3 km, but the 07 June case is more polluted and has larger LWC. We find that the aerosol-induced LWP adjustment is dominated by precipitation and is anticorrelated with cloud-top entrainment for both cases. A negative cloud fraction adjustment due to an increase of aerosol number concentration is also shown in the simulations.

Accurate fire emissions inventories are crucial to predict the impacts of wildland fires on air quality and atmospheric composition. Two traditional approaches are widely used to calculate fire emissions: a satellite-based top-down approach and a fuels-based bottom-up approach. However, these methods often considerably disagree on the amount of particulate mass emitted from fires. Previously available observational datasets tended to be sparse, and lacked the statistics needed to resolve these methodological discrepancies. Here, we leverage the extensive and comprehensive airborne in situ and remote sensing measurements of smoke plumes from the recent Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign to statistically assess the skill of the two traditional approaches. We use detailed campaign observations to calculate and compare emission rates at an exceptionally high resolution using three separate approaches: top-down, bottom-up, and a novel approach based entirely on integrated airborne in situ measurements. We then compute the daily average of these high-resolution estimates and compare with estimates from lower resolution, global top-down and bottom-up inventories. We uncover strong, linear relationships between all of the high-resolution emission rate estimates in aggregate, however no single approach is capable of capturing the emission characteristics of every fire. Global inventory emission rate estimates exhibited weaker correlations with the high-resolution approaches and displayed evidence of systematic bias. The disparity between the low resolution global inventories and the high resolution approaches is likely caused by high levels of uncertainty in essential variables used in bottom-up inventories and imperfect assumptions in top-down inventories.

Wildland fires involve complicated processes that are challenging to represent in chemical transport models. Recent airborne measurements reveal remarkable chemical tomography in fresh wildland fire plumes, which remain yet to be fully explored using models. Here we present a high-resolution large eddy simulation (LES) model coupled to chemistry to study the chemical evolution in fresh wildland fire plume. The model is configured for a large fire heavily sampled during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign, and a variety of airborne measurements are used to evaluate the chemical heterogeneity revealed by the model. We show that the model captures the observed cross-transect variations of a number of compounds quite well, including ozone (O3), nitrous acid (HONO), and peroxyacetyl nitrate (PAN), etc. The combined observational and modeling results suggest that the top and edges of fresh plume drive the photochemistry, while dark chemistry is also present but in the lower part of the plume. The model spatial resolution is shown to be very important as it may shift the chemical regime, leading to biases in O3 and NOx chemistry. Based on findings in this work, we speculate that the impact of small fires on air quality may be largely underestimated in models with coarse spatial resolutions.

The southeast Atlantic Ocean provides an excellent natural laboratory to study smoke-cloud interactions, a large driver of uncertainty in climate projections. The value of studying this in particular region is largely attributable to two factors---the expansive, bright, semi-permanent stratocumulus cloud deck and the fact that southern Africa is the largest source of biomass-burning aerosols in the world. We study this region using the WRF-Chem model with CAM5 aerosols and in situ observations from the ORACLES, LASIC, and CLARIFY field campaigns, all of which overlapped in August 2017. Across these campaigns, we compare aerosol, cloud, and thermodynamic variables to quantify model performance and expand upon observational findings of aerosol-cloud effects. Specifically, our approach is to analyze aerosol and cloud properties along flight tracks, picking out uniform legs within tropospheric smoke plumes and in the boundary layer. This unique approach allows us to sample the high spatiotemporal variability that can get lost to large-scale averaging. It also allows process-level comparison of local cloud responses to aerosol conditions, and measure model performance in those same processes. Along with better quantifying model predictive power, we find and justify updates to model parameters and processes to better emulate observations, notably aerosol size parameters. Preliminary results suggest that WRF-CAM5 is activating a smaller percentage of aerosols into cloud droplets than shown in observations, which could lead to biased modeling of aerosol indirect radiative effects on a larger scale. We explore this effect further with CCN activation tendency, updraft, particle sizing, and composition analysis, as well as broader dynamics like entrainment and removal rates. Comparing the model with similar instrument suites across multiple colocated campaigns also allows us to quantify instrument uncertainty in ways that a focus on a single campaign cannot and gives further context to the model performance.

Aerosol-cloud interactions are both uncertain and important in global and regional climate models, and especially in the southeast Atlantic Ocean. This uncertainty in the region is largely due to two correlated factors---the expansive, bright, semi-permanent stratocumulus cloud deck and the fact that southern Africa is the largest source of biomass-burning aerosols in the world. We study this region using the WRF-Chem model with CAM5 aerosols and in situ observations from the ORACLES and LASIC field campaigns in August-October of 2016 through 2018. We compare aerosol and cloud properties to measure and improve model performance and expand upon observational findings of aerosol-cloud effects. Relevant comparison variables include aerosol number concentration, mean particle diameter and spread, CCN activation tendency, hygroscopicity, and cloud droplet number concentrations. Specifically, our approach is to analyze colocated model data along flight tracks to resolve aerosol-cloud interactions. Within and between single-day flights, there is high spatiotemporal variability that can get lost to large-scale averaging analyses. We have found that CCN is substantially under-represented in the model compared to observations. For a given aerosol number concentration, size, supersaturation and hygroscopicity, the model will consider fewer particles as CCN than observations indicate. We plan to explore this result further, diagnosing the model-observation differences more consistently and updating the model with more physically accurate values of aerosol size, concentration, or hygroscopicity based on observations. We will also intercompare multiple instrument platforms involved with the ORACLES and LASIC campaigns. With improved small-scale aerosol-cloud interactions, this work also shows promise to substantially improve that representation in climate models.