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Abstract The BlueFlux field campaign, supported by NASA’s Carbon Monitoring System, will develop prototype blue carbon products to inform coastal carbon management. While blue carbon has been suggested as a nature-based climate solution (NBS) to remove carbon dioxide (CO 2 ) from the atmosphere, these ecosystems also release additional greenhouse gases (GHGs) such as methane (CH 4 ) and are sensitive to disturbances including hurricanes and sea-level rise. To understand blue carbon as an NBS, BlueFlux is conducting multi-scale measurements of CO 2 and CH 4 fluxes across coastal landscapes, combined with long-term carbon burial, in Southern Florida using chambers, flux towers, and aircraft combined with remote-sensing observations for regional upscaling. During the first deployment in April 2022, CO 2 uptake and CH 4 emissions across the Everglades National Park averaged −4.9 ± 4.7 μ mol CO 2 m −2 s −1 and 19.8 ± 41.1 nmol CH 4 m −2 s −1 , respectively. When scaled to the region, mangrove CH 4 emissions offset the mangrove CO 2 uptake by about 5% (assuming a 100 year CH 4 global warming potential of 28), leading to total net uptake of 31.8 Tg CO 2 -eq y −1 . Subsequent field campaigns will measure diurnal and seasonal changes in emissions and integrate measurements of long-term carbon burial to develop comprehensive annual and long-term GHG budgets to inform blue carbon as a climate solution. 

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.

 

The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) experiment was a multi‐agency, inter‐disciplinary research effort to: (a) obtain detailed measurements of trace gas and aerosol emissions from wildfires and prescribed fires using aircraft, satellites and ground‐based instruments, (b) make extensive suborbital remote sensing measurements of fire dynamics, (c) assess local, regional, and global modeling of fires, and (d) strengthen connections to observables on the ground such as fuels and fuel consumption and satellite products such as burned area and fire radiative power. From Boise, ID western wildfires were studied with the NASA DC‐8 and two NOAA Twin Otter aircraft. The high‐altitude NASA ER‐2 was deployed from Palmdale, CA to observe some of these fires in conjunction with satellite overpasses and the other aircraft. Further research was conducted on three mobile laboratories and ground sites, and 17 different modeling forecast and analyses products for fire, fuels and air quality and climate implications. From Salina, KS the DC‐8 investigated 87 smaller fires in the Southeast with remote and in‐situ data collection. Sampling by all platforms was designed to measure emissions of trace gases and aerosols with multiple transects to capture the chemical transformation of these emissions and perform remote sensing observations of fire and smoke plumes under day and night conditions. The emissions were linked to fuels consumed and fire radiative power using orbital and suborbital remote sensing observations collected during overflights of the fires and smoke plumes and ground sampling of fuels.

 

Abstract. Fires emit sufficient sulfur to affect local and regional airquality and climate. This study analyzes SO2 emission factors andvariability in smoke plumes from US wildfires and agricultural fires, as well as theirrelationship to sulfate and hydroxymethanesulfonate (HMS) formation.Observed SO2 emission factors for various fuel types show goodagreement with the latest reviews of biomass burning emission factors,producing an emission factor range of 0.47–1.2 g SO2 kg−1 C.These emission factors vary with geographic location in a way that suggeststhat deposition of coal burning emissions and application ofsulfur-containing fertilizers likely play a role in the larger observedvalues, which are primarily associated with agricultural burning. A 0-D boxmodel generally reproduces the observed trends of SO2 and total sulfate(inorganic + organic) in aging wildfire plumes. In many cases, modeled HMSis consistent with the observed organosulfur concentrations. However, acomparison of observed organosulfur and modeled HMS suggests that multipleorganosulfur compounds are likely responsible for the observations but thatthe chemistry of these compounds yields similar production and loss rates asthat of HMS, resulting in good agreement with the modeled results. Weprovide suggestions for constraining the organosulfur compounds observedduring these flights, and we show that the chemistry of HMS can alloworganosulfur to act as an S(IV) reservoir under conditions of pH > 6 and liquid water content>10−7 g sm−3. This canfacilitate long-range transport of sulfur emissions, resulting in increasedSO2 and eventually sulfate in transported smoke. 

Oceans emit large quantities of dimethyl sulfide (DMS) to the marine atmosphere. The oxidation of DMS leads to the formation and growth of cloud condensation nuclei (CCN) with consequent effects on Earth’s radiation balance and climate. The quantitative assessment of the impact of DMS emissions on CCN concentrations necessitates a detailed description of the oxidation of DMS in the presence of existing aerosol particles and clouds. In the unpolluted marine atmosphere, DMS is efficiently oxidized to hydroperoxymethyl thioformate (HPMTF), a stable intermediate in the chemical trajectory toward sulfur dioxide (SO 2 ) and ultimately sulfate aerosol. Using direct airborne flux measurements, we demonstrate that the irreversible loss of HPMTF to clouds in the marine boundary layer determines the HPMTF lifetime ( τ HPMTF < 2 h) and terminates DMS oxidation to SO 2 . When accounting for HPMTF cloud loss in a global chemical transport model, we show that SO 2 production from DMS is reduced by 35% globally and near-surface (0 to 3 km) SO 2 concentrations over the ocean are lowered by 24%. This large, previously unconsidered loss process for volatile sulfur accelerates the timescale for the conversion of DMS to sulfate while limiting new particle formation in the marine atmosphere and changing the dynamics of aerosol growth. This loss process potentially reduces the spatial scale over which DMS emissions contribute to aerosol production and growth and weakens the link between DMS emission and marine CCN production with subsequent implications for cloud formation, radiative forcing, and climate. 

Abstract. Formaldehyde (HCHO) has been measured from space for morethan 2 decades. Owing to its short atmospheric lifetime, satellite HCHOdata are used widely as a proxy of volatile organic compounds (VOCs; pleaserefer to Appendix A for abbreviations and acronyms), providing constraintson underlying emissions and chemistry. However, satellite HCHO products fromdifferent satellite sensors using different algorithms have received littlevalidation so far. The accuracy and consistency of HCHO retrievals remainlargely unclear. Here we develop a validation platform for satellite HCHOretrievals using in situ observations from 12 aircraft campaigns with a chemicaltransport model (GEOS-Chem) as the intercomparison method. Application tothe NASA operational OMI HCHO product indicates negative biases (−44.5 %to −21.7 %) under high-HCHO conditions, while it indicates high biases (+66.1 % to+112.1 %) under low-HCHO conditions. Under both conditions, HCHO a priorivertical profiles are likely not the main driver of the biases. By providingquick assessment of systematic biases in satellite products over largedomains, the platform facilitates, in an iterative process, optimization ofretrieval settings and the minimization of retrieval biases. It is alsocomplementary to localized validation efforts based on ground observationsand aircraft spirals. 

Abstract. Anthropogenic secondary organic aerosol (ASOA), formed from anthropogenicemissions of organic compounds, constitutes a substantial fraction of themass of submicron aerosol in populated areas around the world andcontributes to poor air quality and premature mortality. However, theprecursor sources of ASOA are poorly understood, and there are largeuncertainties in the health benefits that might accrue from reducinganthropogenic organic emissions. We show that the production of ASOA in 11urban areas on three continents is strongly correlated with the reactivityof specific anthropogenic volatile organic compounds. The differences inASOA production across different cities can be explained by differences inthe emissions of aromatics and intermediate- and semi-volatile organiccompounds, indicating the importance of controlling these ASOA precursors.With an improved model representation of ASOA driven by the observations,we attribute 340 000 PM2.5-related premature deaths per year to ASOA, which isover an order of magnitude higher than prior studies. A sensitivity casewith a more recently proposed model for attributing mortality to PM2.5(the Global Exposure Mortality Model) results in up to 900 000 deaths. Alimitation of this study is the extrapolation from cities with detailedstudies and regions where detailed emission inventories are available toother regions where uncertainties in emissions are larger. In addition tofurther development of institutional air quality management infrastructure,comprehensive air quality campaigns in the countries in South and CentralAmerica, Africa, South Asia, and the Middle East are needed for furtherprogress in this area. 

Dimethyl sulfide (DMS), emitted from the oceans, is the most abundant biological source of sulfur to the marine atmosphere. Atmospheric DMS is oxidized to condensable products that form secondary aerosols that affect Earth’s radiative balance by scattering solar radiation and serving as cloud condensation nuclei. We report the atmospheric discovery of a previously unquantified DMS oxidation product, hydroperoxymethyl thioformate (HPMTF, HOOCH 2 SCHO), identified through global-scale airborne observations that demonstrate it to be a major reservoir of marine sulfur. Observationally constrained model results show that more than 30% of oceanic DMS emitted to the atmosphere forms HPMTF. Coincident particle measurements suggest a strong link between HPMTF concentration and new particle formation and growth. Analyses of these observations show that HPMTF chemistry must be included in atmospheric models to improve representation of key linkages between the biogeochemistry of the ocean, marine aerosol formation and growth, and their combined effects on climate. 

Agricultural and prescribed burning activities emit large amounts of trace gases and aerosols on regional to global scales. We present a compilation of emission factors (EFs) and emission ratios from the eastern portion of the Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) campaign in 2019 in the United States, which sampled burning of crop residues and other prescribed fire fuels. FIREX‐AQ provided comprehensive chemical characterization of 53 crop residue and 22 prescribed fires. Crop residues burned at different modified combustion efficiencies (MCE), with corn residue burning at higher MCE than other fuel types. Prescribed fires burned at lower MCE (<0.90) which is typical, while grasslands burned at lower MCE (0.90) than normally observed due to moist, green, growing season fuels. Most non‐methane volatile organic compounds (NMVOCs) were significantly anticorrelated with MCE except for ethanol and NMVOCs that were measured with less certainty. We identified 23 species where crop residue fires differed by more than 50% from prescribed fires at the same MCE. Crop residue EFs were greater for species related to agricultural chemical use and fuel composition as well as oxygenated NMVOCs possibly due to the presence of metals such as potassium. Prescribed EFs were greater for monoterpenes (5×). FIREX‐AQ crop residue average EFs generally agreed with the previous agricultural fire study in the US but had large disagreements with global compilations. FIREX‐AQ observations show the importance of regionally‐specific and fuel‐specific EFs as first steps to reduce uncertainty in modeling the air quality impacts of fire emissions.