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.

Heterogeneous chemical cycles of pyrogenic nitrogen and halides influence tropospheric ozone and affect the stratosphere during extreme pyrocumulonimbus (PyroCB) events. We report field-derived N2O5 uptake coefficients, γ(N2O5), and ClNO2 yields, φ(ClNO2), from two aircraft campaigns observing fresh smoke in the lower and mid troposphere and processed/aged smoke in the upper troposphere and lower stratosphere (UTLS). Derived φ(ClNO2) varied across the full 0–1 range but was typically < 0.5 and smallest in a PyroCB (< 0.05). Derived γ(N2O5) was low in agricultural smoke (0.2–3.6 ×10-3), extremely low in mid-tropospheric wildfire smoke (0.1 × 10-3), but larger in PyroCB processed smoke (0.7–5.0 × 10–3). Aged BB aerosol in the UTLS had a higher median γ(N2O5) of 17 × 10–3 that increased with sulfate and liquid water, but that was nevertheless 1–2 orders of magnitude lower than values for aqueous sulfuric aerosol used in stratospheric models.

Southeast Asian biomass burning is a major pollutant source that contributes to poor air quality throughout the region. Thus, understanding these emissions is critical for predicting and mitigating their health impacts. While many studies have reported ground-based and satellite measurements, airborne measurements at a regional scale capable of tying the two together have not been common. The 2019 Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) field project examined Southeast Asian regional sources and their effects on aerosol/cloud interactions using a combination of airborne, shipboard, and ground-based measurements. These flights sampled a variety of airmass sources over the Philippine, South China, and Sulu seas during both the southwest monsoon and monsoon transition periods. Measurements during CAMP2Ex provide a unique opportunity to investigate how these transported and local emissions affected air quality trends and airmass chemical composition. We present correlated airborne in situ enhancement ratios of CH4 to CO, using them to identify source regimes of either high urban or biomass burning influence as well as urban regimes with different emission factors. Combined with backtrajectory analysis using HYSPLIT, source regimes were examined for differences in ozone, reactive nitrogen, and aerosol chemical composition. While observed O3/CO enhancement ratios remain constant for differing urban source regimes, NOy/CO ratios varied across these regimes. For biomass burning sources, O3/CO enhancement ratios are observed to be lower than previously reported by measurements in the region.

High resolution in-situ measurements of carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and water vapor (H2O) were made onboard the NASA HU-25 aircraft during the ACTIVATE (Aerosol Cloud meteorology Interactions oVer the western Atlantic Experiment) campaign during 2020 and 2021 in different seasons (winter through summer) over the mid-latitude western Atlantic Ocean. As most of the flights focused on the marine boundary layer (MBL) during the campaign, these trace gas observations are an excellent data set to examine seasonal variability of trace gas background values in the MBL without the influence of localized point sources. We will describe the variability of these trace gases in the MBL background by filtering out concentrated point sources using back trajectory analysis along with trace gas ratios. Additionally, the ocean is a significant sink of anthropogenic CO2 capturing about one quarter of total anthropogenic carbon. By looking at the MBL CO2 variation as a function of season, we discuss observed changes in CO2 uptake over the ocean. These high accuracy observations of trace gas backgrounds in the MBL along with characterizing seasonal effects on oceanic sequestering of anthropogenic CO2 will improve the understanding of seasonal variations and change in climate and inverse modelling over the ocean.

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.

Particles containing meteoric material were observed in the lower stratosphere during five aircraft research missions in recent years. Single particle laser ablation technique in a bipolar configuration was used to measure the chemical composition of particles in a size range of approximately 150 nm to 3 µm. The five aircraft missions, conducted between 2014 and 2018, cover a latitude range from 15 to 68°N. In total, more than 330 000 single particles were analyzed. A prominent fraction (more than 50 000) of the analyzed particles was characterized by strong abundances of magnesium, iron, and rare iron oxide compounds, together with sulfuric acid. This particle type was found almost exclusively in the stratosphere and is interpreted as meteoric material immersed or dissolved in stratospheric sulfuric acid particles. Below the tropopause the fraction of this particle type decreases sharply. However, small abundances were observed below 3000 m a.s.l. in the Canadian Arctic and also at the Jungfraujoch high altitude station (3600 m a.s.l.). Thus, the removal pathway by sedimentation and/or mixing into the troposphere is confirmed. Our data show that particles containing meteoric material are present in the lower stratosphere in very similar relative abundances, regardless of latitude or season. This finding suggests that the meteoric material is transported from the mesosphere into the stratosphere in the downward branch of the Brewer-Dobson-Circulation and efficiently distributed towards low latitudes by isentropic mixing. As a result, meteoric material is found in particles of the stratospheric Junge layer at all latitudes.

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.

We present observations of local enhancements in carbon dioxide (CO2) from local emissions sources over three eastern US regions during four deployments of the Atmospheric Carbon Transport-America (ACT-America) campaign between summer 2016 and spring 2018. Local CO2 emissions were characterized by carbon monoxide (CO) to CO2 enhancement ratios (i.e. ΔCO/ΔCO2) in airmass mixing observed during aircraft transects within the atmospheric boundary layer. By analyzing regional-scale variability of CO2 enhancements as a function of ΔCO/ΔCO2 enhancement ratios, observed relative contributions to CO2 emissions were contrasted between different combustion regimes across regions and seasons. Ninety percent of observed summer combustion in all regions was attributed to high efficiency fossil fuel (FF) combustion (ΔCO/ΔCO2 < 0.5%). In other seasons, regional contributions increased from less efficient forms of FF combustion (ΔCO/ΔCO2 0.5-2%) to as much as 60% of observed combustion. CO2 emission contributions attributed to biomass burning (BB) (ΔCO/ΔCO2 > 4%) were negligible during summer and fall in all regions, but climbed to 10-12% of observed combustion in the South during winter and spring. Vulcan v3 CO2 2015 emission analysis showed increases in residential and commercial sectors seasonally matching increases in less efficient FF combustion, but could not explain regional trends. WRF-Chem modeling, driven by CarbonTracker CO2 fire emissions, matched observed winter and spring BB contributions, but conflictingly predicted similar levels of BB during fall. Satellite fire data from MODIS and VIIRS suggested higher spatial resolution fire data might improve modeled BB emissions.

Wildfire smoke influences on air quality and atmospheric chemistry have been underscored by the increasing fire prevalence in recent years, and yet, the connection between fire, smoke emissions, and the subsequent transformation of this smoke in the atmosphere remains poorly constrained. Toward improving these linkages, we present a new method for coupling high-time-resolution satellite observations of fire radiative power (FRP) with in situ observations of smoke aerosols and trace gases. We apply this technique to thirteen fire plumes comprehensively characterized during the recent FIREX-AQ mission and show that changes in FRP directly translate into changes in conserved smoke tracers (CO2, CO, and black carbon aerosol) observed in the downwind smoke plume. The correlation is particularly strong for CO2 (mean r>0.9). This method is important for untangling the competing effects of changing fire behavior versus the influence of dilution and atmospheric processing on the down-wind evolution of measured smoke properties.