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East Asia is the strongest global source region for anthropogenic black carbon (BC), the most important light-absorbing aerosol contributing to direct radiative climate forcing. To provide extended observational constraints on regional BC distributions and impacts, in situ measurements of BC were obtained with a single particle soot photometer during the May/June 2016 Korean-United States Air Quality aircraft campaign (KORUS-AQ) in South Korea. Unique chemical tracer relationships were associated with BC sourced from different regions. The extent and variability in vertical BC mass burden for 48 profiles over a single site near Seoul were investigated using back trajectory and chemical tracer analysis. Meteorologically driven changes in transport influenced the relative importance of different source regions, impacting observed BC loadings at all altitudes. Internal mixing and size distributions of BC further demonstrated dependence on source region: BC attributed to China had a larger mass median diameter (180 ± 13 nm) than BC attributed to South Korea (152 ± 25 nm), and BC associated with long-range transport was less thickly coated (60 ± 4 nm) than that sourced from South Korea (75 ± 16 nm). The column BC direct radiative effect at the top of the atmosphere was estimated to be 1.0+0.90.5 W/m2, with average values for different meteorological periods varying by a factor of 2 due to changes in the BC vertical profile. During the campaign, BC sourced from South Korea (≤ 31%), China (22%), and Russia (14%) were the most significant single-region contributors to the column direct radiative effect.

Using measurements from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) experiment, we show that methyl peroxy nitrate (CH3O2NO2) is present in concentrations of ~5–15 pptv in the springtime arctic upper troposphere. We investigate the regional and global effects of CH3O2NO2 by including its chemistry in the GEOS-Chem 3-D global chemical transport model. We find that at temperatures below 240 K inclusion of CH3O2NO2 chemistry results in decreases of up to ~20 % in NOx, ~20 % in N2O5, ~5 % in HNO3, ~2 % in ozone, and increases in methyl hydrogen peroxide of up to ~14 %. Larger changes are observed in biomass burning plumes lofted to high altitude. Additionally, by sequestering NOx at low temperatures, CH3O2NO2 decreases the cycling of HO2 to OH, resulting in a larger upper tropospheric HO2 to OH ratio. These results may impact some estimates of lightning NOx sources as well as help explain differences between models and measurements of upper tropospheric composition.

Alkyl and multifunctional nitrates (RONO2, Sigma ANs) have been observed to be a significant fraction of NOy in a number of different chemical regimes. Their formation is an important free radical chain termination step ending production of ozone and possibly affecting formation of secondary organic aerosol. Sigma ANs also represent a potentially large, unmeasured contribution to OH reactivity and are a major pathway for the removal of nitrogen oxides from the atmosphere. Numerous studies have investigated the role of nitrate formation from biogenic compounds and in the remote atmosphere. Less attention has been paid to the role Sigma ANs may play in the complex mixtures of hydrocarbons typical of urban settings. Measurements of total alkyl and multifunctional nitrates, NO2, total peroxy nitrates (Sigma PNs), HNO3 and a representative suite of hydrocarbons were obtained from the NASA DC-8 aircraft during spring of 2006 in and around Mexico City and the Gulf of Mexico. Sigma ANs were observed to be 10-20% of NOy in the Mexico City plume and to increase in importance with increased photochemical age. We describe three conclusions: (1) Correlations of Sigma ANs with odd-oxygen (O-x) indicate a stronger role for Sigma ANs in the photochemistry of Mexico City than is expected based on currently accepted photochemical mechanisms, (2) Sigma AN formation suppresses peak ozone production rates by as much as 40% in the near-field of Mexico City and (3) Sigma ANs play a significant role in the export of NOy from Mexico City to the Gulf Region.

Formation of isoprene nitrates (INs) is an important free radical chain termination step ending production of ozone and possibly affecting formation of secondary organic aerosol. Isoprene nitrates also represent a potentially large, unmeasured contribution to OH reactivity and are a major pathway for the removal of nitrogen oxides from the atmosphere. Current assessments indicate that formation rates of isoprene nitrates are uncertain to a factor of 2-3 and the subsequent fate of isoprene nitrates remains largely unconstrained by laboratory, field or modeling studies. Measurements of total alkyl and multifunctional nitrates (Sigma ANs), NO2, total peroxy nitrates (Sigma PNs), HNO3, CH2O, isoprene and other VOC were obtained from the NASA DC-8 aircraft during summer 2004 over the continental US during the INTEX-NA campaign. These observations represent the first characterization of Sigma ANs over a wide range of land surface types and in the lower free troposphere. Sigma ANs were a significant, 12-20%, fraction of NOy throughout the experimental domain and Sigma ANs were more abundant when isoprene was high. We use the observed hydrocarbon species to calculate the relative contributions of Sigma AN precursors to their production. These calculations indicate that isoprene represents at least three quarters of the Sigma AN source in the summertime continental boundary layer of the US. An observed correlation between Sigma ANs and CH2O is used to place constraints on nitrate yields from isoprene oxidation, atmospheric lifetimes of the resulting nitrates and recycling efficiencies of nitrates during subsequent oxidation. We find reasonable fits to the data using sets of production rates, lifetimes and recycling efficiencies of INs as follows (4.4%, 16 h, 97%), (8%, 2.5h, 79%) and (12%, 95 min, 67%). The analysis indicates that the lifetime of Sigma ANs as a pool of compounds is considerably longer than the lifetime of the individual isoprene nitrates to reaction with OH, implying that the organic nitrate functionality is at least partially maintained through a second oxidation cycle.

We present a statistical representation of the aggregate effects of deep convection on the chemistry and dynamics of the upper troposphere (UT) based on direct aircraft observations of the chemical composition of the UT over the eastern United States and Canada during summer. These measurements provide unique observational constraints on the chemistry occurring downwind of convection and the rate at which air in the UT is recycled. These results provide quantitative measures that can be used to evaluate global climate and chemistry models.

We use the Weather Research and Forecasting with Chemistry (WRF-Chem) model with new implementations of GOES-16 fire radiative power (FRP) based wildfire emissions and plume-rise to interpret aerosol observations during the 2019 NASA-NOAA FIREX-AQ field campaign and perform model evaluations. We compare simulated aerosol concentrations and optical properties against observations of black carbon aerosol from the NOAA Single Particle Soot Photometer (NOAA-SP2), organic aerosol from the CU High Resolution Aerosol Mass Spectrometer (HR36 AMS) and aerosol backscatter coefficients from the High Spectral Resolution Lidar (HSRL) system. This study focuses on the Williams Flats fire in Washington, which was repeatedly sampled during four science flights by the NASA DC-8 (August 3 – August 8, 2019). The emissions and plume-rise methodologies are implemented following NOAA’s operational High Resolution Rapid Refresh coupled with Smoke (HRRR-Smoke) forecasting model. In addition, new GOES-16 FRP based diurnal cycle functions are developed and incorporated in WRF-Chem. The FIREX-AQ observations represented a diverse set of sampled environments ranging from fresh/aged smoke from the Williams Flats fire to remnants of plumes transported over long distances. The Williams Flats fire resulted in significant aerosol enhancements during August 3- 8, 2019, which were substantially underestimated by the standard version of WRF-Chem. The simulated BC and OC concentrations increased between 92 – 125 times (BC) and 28-78 times (OC) with the new implementation compared to the standard WRF-Chem version. These increases resulted in better agreement with the FIREX-AQ airborne observations for BC and OC concentrations (particularly for fresh smoke sampling phases) and aerosol backscatter coefficients. The model still showed a low bias in simulating the aerosol loadings observed in aged plumes from Williams Flats. WRF-Chem with the FRP-based plumerise simulated similar plume heights to the standard plumerise model in WRF-52 Chem. The simulated plume heights (for both versions) compared well with estimated plume heights using the HSRL measurements. Therefore, the improvements in the model simulation were mainly driven by the higher emissions in the FRP55 based version. The model evaluations also highlighted the importance of accurately accounting for the wildfire diurnal cycle and including adequate representation of the underlying chemical mechanisms, both of which could significantly impact model forecasting performance. [ABSTRACT FROM AUTHOR]

Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between Jul. and Aug. 2019 onboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated; highly spectrally-resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in-situ bulk aerosol particle light absorption measured at three wavelengths (405, 532, 664nm) with a photo acoustic spectrometer (PAS). A light absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher, but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm-1 ppbv-1, emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion, or constant levels with age were all observed in the first 8 hours after emission in different plumes. Within 8 hours following emissions, 4-nitrocatechol, a well characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped possibly due to temperaturedriven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 hours) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer time and spatial scales, where its environmental impacts are likely to be greater. [ABSTRACT FROM AUTHOR]

Bioaerosols are produced by biological processes and directly emitted into the atmosphere, where they contribute to ice nucleation and the formation of precipitation. Previous studies have suggested that fungal spores constitute a substantial portion of the atmospheric bioaerosol budget. However, our understanding of what controls the emission and burden of fungal spores on the global scale is limited. Here, we use a previously unexplored source of fungal spore count data from the American Academy of Allergy, Asthma, and Immunology (AAAAI) to gain insight into the drivers of their emissions. First, we derive emissions from observed concentrations at 66 stations by applying the boundary layer equilibrium assumption. We estimate an annual mean emission of 62±31 m-2 s-1 across the USA. Based on these pseudo-observed emissions, we derive two models for fungal spore emissions at seasonal scales: a statistical model, which links fungal spore emissions to meteorological variables that show similar seasonal cycles (2 m specific humidity, leaf area index and friction velocity), and a population model, which describes the growth of fungi and the emission of their spores as a biological process that is driven by temperature and biomass density. Both models show better skill at reproducing the seasonal cycle in fungal spore emissions at the AAAI stations than the model previously developed by Heald and Spracklen (2009) (referred to as HS09). We implement all three emissions models in the chemical transport model GEOS-Chem to evaluate global emissions and burden of fungal spore bioaerosol. We estimate annual global emissions of 3.7 and 3.4 Tg yr-1 for the statistical model and the population model, respectively, which is about an order of magnitude lower than the HS09 model. The global burden of the statistical and the population model is similarly an order of magnitude lower than that of the HS09 model. A comparison with independent datasets shows that the new models reproduce the seasonal cycle of fluorescent biological aerosol particles (FBAP) concentrations at two locations in Europe somewhat better than the HS09 model, although a quantitative comparison is hindered by the ambiguity in interpreting measurements of fluorescent particles. Observed vertical profiles of FBAP show that the convective transport of spores over source regions is captured well by GEOS-Chem, irrespective of which emission scheme is used. However, over the North Atlantic, far from significant spore sources, the model does not reproduce the vertical profiles. This points to the need for further exploration of the transport, cloud processing, and wet removal of spores. In addition, more long-term observational datasets are needed to assess whether drivers of seasonal fungal spore emissions are similar across continents and biomes. [ABSTRACT FROM AUTHOR]

Detection of bioaerosols, or primary biological aerosol particles (PBAPs), has become increasingly important for a wide variety of research communities and scientific questions. In particular, real-time (RT) techniques for autonomous, online detection and characterization of PBAP properties in both outdoor and indoor environments are becoming more commonplace and have opened avenues of research. With advances in technology, however, come challenges to standardize practices so that results are both reliable and comparable across technologies and users. Here, we present a critical review of major RT instrument classes that have been applied to PBAP research, especially with respect to environmental science, allergy monitoring, agriculture, public health, and national security. Eight major classes of RT techniques are covered, including the following: (i) fluorescence spectroscopy, (ii) elastic scattering, microscopy, and holography, (iii) Raman spectroscopy, (iv) mass spectrometry, (v) breakdown spectroscopy, (vi) remote sensing, (vii) microfluidic techniques, and (viii) paired aqueous techniques. For each class of technology we present technical limitations, misconceptions, and pitfalls, and also summarize best practices for operation, analysis, and reporting. The final section of the article presents pressing scientific questions and grand challenges for RT sensing of PBAP as well as recommendations for future work to encourage high-quality results and increased cross-community collaboration. [ABSTRACT FROM AUTHOR]