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Abstract Iodine is a reactive trace element in atmospheric chemistry that destroys ozone and nucleates particles. Iodine emissions have tripled since 1950 and are projected to keep increasing with rising O 3 surface concentrations. Although iodic acid (HIO 3 ) is widespread and forms particles more efficiently than sulfuric acid, its gas-phase formation mechanism remains unresolved. Here, in CLOUD atmospheric simulation chamber experiments that generate iodine radicals at atmospherically relevant rates, we show that iodooxy hypoiodite, IOIO, is efficiently converted into HIO 3 via reactions (R1) IOIO + O 3 → IOIO 4 and (R2) IOIO 4 + H 2 O → HIO 3 + HOI + (1) O 2 . The laboratory-derived reaction rate coefficients are corroborated by theory and shown to explain field observations of daytime HIO 3 in the remote lower free troposphere. The mechanism provides a missing link between iodine sources and particle formation. Because particulate iodate is readily reduced, recycling iodine back into the gas phase, our results suggest a catalytic role of iodine in aerosol formation.Free, publicly-accessible full text available November 14, 2023
Biomass burning nitrogen dioxide emissions derived from space with TROPOMI: methodology and validationAbstract. Smoke from wildfires is a significant source of air pollution, which can adversely impact air quality and ecosystems downwind. With the recently increasing intensity and severity of wildfires, the threat to air quality is expected to increase. Satellite-derived biomass burning emissions can fill in gaps in the absence of aircraft or ground-based measurement campaigns and can help improve the online calculation of biomass burning emissions as well as the biomass burning emissions inventories that feed air quality models. This study focuses on satellite-derived NOx emissions using the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI) NO2 dataset. Advancements and improvements to the satellite-based determination of forest fire NOx emissions are discussed, including information on plume height and effects of aerosol scattering and absorption on the satellite-retrieved vertical column densities. Two common top-down emission estimation methods, (1) an exponentially modified Gaussian (EMG) and (2) a flux method, are applied to synthetic data to determine the accuracy and the sensitivity to different parameters, including wind fields, satellite sampling, noise, lifetime, and plume spread. These tests show that emissions can be accurately estimated from single TROPOMI overpasses.The effect of smoke aerosols on TROPOMI NO2 columns (via air mass factors, AMFs) is estimated, and these satellitemore »
Wildfire Smoke Observations in the Western United States from the Airborne Wyoming Cloud Lidar during the BB-FLUX Project. Part I: Data Description and Methodology
During the summer of 2018, the upward-pointing Wyoming Cloud Lidar (WCL) was deployed on board the University of Wyoming King Air (UWKA) research aircraft for the Biomass Burning Flux Measurements of Trace Gases and Aerosols (BB-FLUX) field campaign. This paper describes the generation of calibrated attenuated backscatter coefficients and aerosol extinction coefficients from the WCL measurements. The retrieved aerosol extinction coefficients at the flight level strongly correlate (correlation coefficient, rr > 0.8) with in situ aerosol concentration and carbon monoxide (CO) concentration, providing a first-order estimate for converting WCL extinction coefficients into vertically resolved CO and aerosol concentration within wildfire smoke plumes. The integrated CO column concentrations from the WCL data in nonextinguished profiles also correlate (rr = 0.7) with column measurements by the University of Colorado Airborne Solar Occultation Flux instrument, indicating the validity of WCL-derived extinction coefficients. During BB-FLUX, the UWKA sampled smoke plumes from more than 20 wildfires during 35 flights over the western United States. Seventy percent of flight time was spent below 3 km above ground level (AGL) altitude, although the UWKA ascended up to 6 km AGL to sample the top of some deep smoke plumes. The upward-pointing WCL observed a nearly equalmore »