East Asian summer monsoon delivers large abundances of very-short-lived organic chlorine substances to the lower stratosphere.

Deep convection in the Asian summer monsoon is a significant transport process for lifting pollutants from the planetary boundary layer to the tropopause level. This process enables efficient injection into the stratosphere of reactive species such as chlorinated very-short-lived substances (Cl-VSLSs) that deplete ozone. Past studies of convective transport associated with the Asian summer monsoon have focused mostly on the south Asian summer monsoon. Airborne observations reported in this work identify the East Asian summer monsoon convection as an effective transport pathway that carried record-breaking levels of ozone-depleting Cl-VSLSs (mean organic chlorine from these VSLSs ~500 ppt) to the base of the stratosphere. These unique observations show total organic chlorine from VSLSs in the lower stratosphere over the Asian monsoon tropopause to be more than twice that previously reported over the tropical tropopause. Considering the recently observed increase in Cl-VSLS emissions and the ongoing strengthening of the East Asian summer monsoon under global warming, our results highlight that a reevaluation of the contribution of Cl-VSLS injection via the Asian monsoon to the total stratospheric chlorine budget is warranted.

Evaluating the Impact of Chemical Complexity and Horizontal Resolution on Tropospheric Ozone Over the Conterminous US With a Global Variable Resolution Chemistry Model.

A new configuration of the Community Earth System Model (CESM)/Community Atmosphere Model with full chemistry (CAM-chem) supporting the capability of horizontal mesh refinement through the use of the spectral element (SE) dynamical core is developed and called CESM/CAM-chem-SE. Horizontal mesh refinement in CESM/CAM-chem-SE is unique and novel in that pollutants such as ozone are accurately represented at human exposure relevant scales while also directly including global feedbacks. CESM/CAM-chem-SE with mesh refinement down to ∼14 km over the conterminous US (CONUS) is the beginning of the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICAv0). Here, MUSICAv0 is evaluated and used to better understand how horizontal resolution and chemical complexity impact ozone and ozone precursors over CONUS as compared to measurements from five aircraft campaigns, which occurred in 2013. This field campaign analysis demonstrates the importance of using finer horizontal resolution to accurately simulate ozone precursors such as nitrogen oxides and carbon monoxide. In general, the impact of using more complex chemistry on ozone and other oxidation products is more pronounced when using finer horizontal resolution where a larger number of chemical regimes are resolved. Large model biases for ozone near the surface remain in the Southeast US as compared to the aircraft observations even with updated chemistry and finer horizontal resolution. This suggests a need for adding the capability of replacing sections of global emission inventories with regional inventories, increasing the vertical resolution in the planetary boundary layer, and reducing model biases in meteorological variables such as temperature and clouds.

Exposure to Particulate Matter and Estimation of Volatile Organic Compounds across Wildland Firefighter Job Tasks.

Wildland firefighters are exposed to smoke-containing particulate matter (PM) and volatile organic compounds (VOCs) while suppressing wildfires. From 2015 to 2017, the U.S. Forest Service conducted a field study collecting breathing zone measurements of PM4 (particulate matter with aerodynamic diameter ≤4 µm) on wildland firefighters from different crew types and while performing various fire suppression tasks on wildfires. Emission ratios of VOC (parts per billion; ppb): PM1 (particulate matter with aerodynamic diameter ≤1 µm; mg/m3) were calculated using data from a separate field study conducted in summer 2018, the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) Campaign. These emission ratios were used to estimate wildland firefighter exposure to acrolein, benzene, and formaldehyde. Results of this field sampling campaign reported that exposure to PM4 and VOC varied across wildland firefighter crew type and job task. Type 1 crews had greater exposures to both PM4 and VOCs than type 2 or type 2 initial attack crews, and wildland firefighters performing direct suppression had statistically higher exposures than those performing staging and other tasks (mean differences = 0.82 and 0.75 mg/m3; 95% confidence intervals = 0.38-1.26 and 0.41-1.08 mg/m3, respectively). Of the 81 personal exposure samples collected, 19% of measured PM4 exposures exceeded the recommended National Wildland Fire Coordinating Group occupational exposure limit (0.7 mg/m3). Wildland fire management should continue to find strategies to reduce smoke exposures for wildland firefighters.

Unpiloted Aircraft System Instrument for the Rapid Collection of Whole Air Samples and Measurements for Environmental Monitoring and Air Quality Studies.

A new airborne system, the Whole Air Sampling Pilotless Platform (WASPP), is described for the collection of whole air samples and in situ meteorological measurements onboard a commercial hexacopter. Rapid sample collection enables the collection ≤15 air samples per flight in positively pressurized miniature canisters, subsequently analyzed on a mated analytical system for up to 80 nonmethane volatile organic compounds (VOCs). The WASPP is well suited to investigate VOC gradients in urban environments impacted by traffic, industry, and oil and natural gas (O&NG) development, but has the sensitivity to characterize continental background conditions, as shown here using a subset of >40 species. We document empirical tests to minimize the influence of rotor wash and other sampling artifacts and report favorable results of laboratory-based calibrations of the WASPP's meteorological sensors and field-based comparisons of WASPP's VOC measurements and horizontal wind velocity measurements. Airborne WASPP measurements can complement and enhance ground-based VOC monitoring efforts by providing substantial meteorological and VOC measurement capability across vertical and horizontal spatial scales. These measurements reveal strong vertical gradients in VOC mixing ratios, depending on local meteorology and sources. WASPP has wide applicability for pollution source identification and quantification of hazardous air pollutants and precursors of criteria pollutants, including monitoring O&NG emissions or industry fenceline monitoring.

HONO Emissions from Western U.S. Wildfires Provide Dominant Radical Source in Fresh Wildfire Smoke.

Wildfires are an important source of nitrous acid (HONO), a photolabile radical precursor, yet in situ measurements and quantification of primary HONO emissions from open wildfires have been scarce. We present airborne observations of HONO within wildfire plumes sampled during the Western Wildfire Experiment for Cloud chemistry, Aerosol absorption and Nitrogen (WE-CAN) campaign. ΔHONO/ΔCO close to the fire locations ranged from 0.7 to 17 pptv ppbv-1 using a maximum enhancement method, with the median similar to previous observations of temperate forest fire plumes. Measured HONO to NOx enhancement ratios were generally factors of 2, or higher, at early plume ages than previous studies. Enhancement ratios scale with modified combustion efficiency and certain nitrogenous trace gases, which may be useful to estimate HONO release when HONO observations are lacking or plumes have photochemical exposures exceeding an hour as emitted HONO is rapidly photolyzed. We find that HONO photolysis is the dominant contributor to hydrogen oxide radicals (HOx = OH + HO2) in early stage (<3 h) wildfire plume evolution. These results highlight the role of HONO as a major component of reactive nitrogen emissions from wildfires and the main driver of initial photochemical oxidation.

Carbon monoxide total column retrievals by use of the measurements of pollution in the troposphere airborne test radiometer.

The Measurements of Pollution in the Troposphere (MOPITT) Airborne Test Radiometer (MATR) uses gas correlation filter radiometry from high-altitude aircraft to measure tropospheric carbon monoxide. This radiometer is used in support of the ongoing validation campaign for the MOPITT instrument aboard the Earth Observation System Terra satellite. A recent study of MATR CO retrievals that used data from the autumn of 2001 in the western United States is presented. Retrievals of the CO total column were performed and compared to in situ sampling with less than 10% retrieval error. Effects that influence retrieval, such as instrument sensitivity, retrieval sensitivity, and the bias between observations and the radiative transfer model, are discussed. Comparisons of MATR and MOPITT retrievals show promising consistency. A preliminary interpretation of MATR results is also presented.