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  • 1
    In: Elem Sci Anth, University of California Press, Vol. 8 ( 2020-01-01)
    Abstract: The Korea – United States Air Quality Study (May – June 2016) deployed instrumented aircraft and ground-based measurements to elucidate causes of poor air quality related to high ozone and aerosol concentrations in South Korea. This work synthesizes data pertaining to aerosols (specifically, particulate matter with aerodynamic diameters & lt;2.5 micrometers, PM2.5) and conditions leading to violations of South Korean air quality standards (24-hr mean PM2.5 & lt; 35 µg m–3). PM2.5 variability from AirKorea monitors across South Korea is evaluated. Detailed data from the Seoul vicinity are used to interpret factors that contribute to elevated PM2.5. The interplay between meteorology and surface aerosols, contrasting synoptic-scale behavior vs. local influences, is presented. Transboundary transport from upwind sources, vertical mixing and containment of aerosols, and local production of secondary aerosols are discussed. Two meteorological periods are probed for drivers of elevated PM2.5. Clear, dry conditions, with limited transport (Stagnant period), promoted photochemical production of secondary organic aerosol from locally emitted precursors. Cloudy humid conditions fostered rapid heterogeneous secondary inorganic aerosol production from local and transported emissions (Transport/Haze period), likely driven by a positive feedback mechanism where water uptake by aerosols increased gas-to-particle partitioning that increased water uptake. Further, clouds reduced solar insolation, suppressing mixing, exacerbating PM2.5 accumulation in a shallow boundary layer. The combination of factors contributing to enhanced PM2.5 is challenging to model, complicating quantification of contributions to PM2.5 from local versus upwind precursors and production. We recommend co-locating additional continuous measurements at a few AirKorea sites across South Korea to help resolve this and other outstanding questions: carbon monoxide/carbon dioxide (transboundary transport tracer), boundary layer height (surface PM2.5 mixing depth), and aerosol composition with aerosol liquid water (meteorologically-dependent secondary production). These data would aid future research to refine emissions targets to further improve South Korean PM2.5 air quality.
    Type of Medium: Online Resource
    ISSN: 2325-1026
    Language: English
    Publisher: University of California Press
    Publication Date: 2020
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  • 2
    In: Bulletin of the American Meteorological Society, American Meteorological Society, Vol. 103, No. 3 ( 2022-03), p. E761-E790
    Abstract: This article provides an overview of the NASA Atmospheric Tomography (ATom) mission and a summary of selected scientific findings to date. ATom was an airborne measurements and modeling campaign aimed at characterizing the composition and chemistry of the troposphere over the most remote regions of the Pacific, Southern, Atlantic, and Arctic Oceans, and examining the impact of anthropogenic and natural emissions on a global scale. These remote regions dominate global chemical reactivity and are exceptionally important for global air quality and climate. ATom data provide the in situ measurements needed to understand the range of chemical species and their reactions, and to test satellite remote sensing observations and global models over large regions of the remote atmosphere. Lack of data in these regions, particularly over the oceans, has limited our understanding of how atmospheric composition is changing in response to shifting anthropogenic emissions and physical climate change. ATom was designed as a global-scale tomographic sampling mission with extensive geographic and seasonal coverage, tropospheric vertical profiling, and detailed speciation of reactive compounds and pollution tracers. ATom flew the NASA DC-8 research aircraft over four seasons to collect a comprehensive suite of measurements of gases, aerosols, and radical species from the remote troposphere and lower stratosphere on four global circuits from 2016 to 2018. Flights maintained near-continuous vertical profiling of 0.15–13-km altitudes on long meridional transects of the Pacific and Atlantic Ocean basins. Analysis and modeling of ATom data have led to the significant early findings highlighted here.
    Type of Medium: Online Resource
    ISSN: 0003-0007 , 1520-0477
    Language: Unknown
    Publisher: American Meteorological Society
    Publication Date: 2022
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  • 3
    In: Geophysical Research Letters, American Geophysical Union (AGU), Vol. 47, No. 23 ( 2020-12-16)
    Abstract: Geostationary satellite observations of fire radiative power are highly correlated with in situ airborne measurements of primary‐emission smoke tracers High‐resolution satellite observations are needed to disentangle how fire activity and plume dilution impact the downwind evolution of smoke Diurnal fire activity for wildfires observed during FIREX‐AQ is best parameterized using a bimodal Gaussian distribution to inform models
    Type of Medium: Online Resource
    ISSN: 0094-8276 , 1944-8007
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2020
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    detail.hit.zdb_id: 7403-2
    SSG: 16,13
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 12 ( 2022-06-21), p. 8009-8036
    Abstract: Abstract. Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard 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 and 664 nm) with a photoacoustic 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 h after emission in different plumes. Within 8 h 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 temperature-driven 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 h) 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 timescales and spatial scales, where its environmental impacts are likely to be greater.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 19 ( 2021-10-08), p. 15023-15063
    Abstract: Abstract. In situ measurements of aerosol microphysical, chemical, and optical properties were made during global-scale flights from 2016–2018 as part of the Atmospheric Tomography Mission (ATom). The NASA DC-8 aircraft flew from ∼ 84∘ N to ∼ 86∘ S latitude over the Pacific, Atlantic, Arctic, and Southern oceans while profiling nearly continuously between altitudes of ∼ 160 m and ∼ 12 km. These global circuits were made once each season. Particle size distributions measured in the aircraft cabin at dry conditions and with an underwing probe at ambient conditions were combined with bulk and single-particle composition observations and measurements of water vapor, pressure, and temperature to estimate aerosol hygroscopicity and hygroscopic growth factors and calculate size distributions at ambient relative humidity. These reconstructed, composition-resolved ambient size distributions were used to estimate intensive and extensive aerosol properties, including single-scatter albedo, the asymmetry parameter, extinction, absorption, Ångström exponents, and aerosol optical depth (AOD) at several wavelengths, as well as cloud condensation nuclei (CCN) concentrations at fixed supersaturations and lognormal fits to four modes. Dry extinction and absorption were compared with direct in situ measurements, and AOD derived from the extinction profiles was compared with remotely sensed AOD measurements from the ground-based Aerosol Robotic Network (AERONET); this comparison showed no substantial bias. The purpose of this work is to describe the methodology by which ambient aerosol properties are estimated from the in situ measurements, provide statistical descriptions of the aerosol characteristics of different remote air mass types, examine the contributions to AOD from different aerosol types in different air masses, and provide an entry point to the ATom aerosol database. The contributions of different aerosol types (dust, sea salt, biomass burning, etc.) to AOD generally align with expectations based on location of the profiles relative to continental sources of aerosols, with sea salt and aerosol water dominating the column extinction in most remote environments and dust and biomass burning (BB) particles contributing substantially to AOD, especially downwind of the African continent. Contributions of dust and BB aerosols to AOD were also significant in the free troposphere over the North Pacific. Comparisons of lognormally fitted size distribution parameters to values in the Optical Properties of Aerosols and Clouds (OPAC) database commonly used in global models show significant differences in the mean diameters and standard deviations for accumulation-mode particles and coarse-mode dust. In contrast, comparisons of lognormal parameters derived from the ATom data with previously published shipborne measurements in the remote marine boundary layer show general agreement. The dataset resulting from this work can be used to improve global-scale representation of climate-relevant aerosol properties in remote air masses through comparison with output from global models and assumptions used in retrievals of aerosol properties from both ground-based and satellite remote sensing.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 24, No. 2 ( 2024-01-23), p. 929-956
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2024
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  • 7
    Online Resource
    Online Resource
    American Meteorological Society ; 2016
    In:  Journal of the Atmospheric Sciences Vol. 73, No. 6 ( 2016-06-01), p. 2445-2464
    In: Journal of the Atmospheric Sciences, American Meteorological Society, Vol. 73, No. 6 ( 2016-06-01), p. 2445-2464
    Abstract: Numerical simulations of cirrus formation in the tropical tropopause layer (TTL) during boreal wintertime are used to evaluate the impact of heterogeneous ice nuclei (IN) abundance on cold cloud microphysical properties and occurrence frequencies. The cirrus model includes homogeneous and heterogeneous ice nucleation, deposition growth/sublimation, and sedimentation. Reanalysis temperature and wind fields with high-frequency waves superimposed are used to force the simulations. The model results are constrained by comparison with in situ and satellite observations of TTL cirrus and relative humidity. Temperature variability driven by high-frequency waves has a dominant influence on TTL cirrus microphysical properties and occurrence frequencies, and inclusion of these waves is required to produce agreement between the simulated and observed abundance of TTL cirrus. With homogeneous freezing only and small-scale gravity waves included in the temperature curtains, the model produces excessive ice concentrations compared with in situ observations. Inclusion of relatively numerous heterogeneous ice nuclei (NIN ≥ 100 L−1) in the simulations improves the agreement with observed ice concentrations. However, when IN contribute significantly to TTL cirrus ice nucleation, the occurrence frequency of large supersaturations with respect to ice is less than indicated by in situ measurements. The model results suggest that the sensitivity of TTL cirrus extinction and ice water content statistics to heterogeneous ice nuclei abundance is relatively weak. The simulated occurrence frequencies of TTL cirrus are quite insensitive to ice nuclei abundance, both in terms of cloud frequency height distribution and regional distribution throughout the tropics.
    Type of Medium: Online Resource
    ISSN: 0022-4928 , 1520-0469
    RVK:
    Language: English
    Publisher: American Meteorological Society
    Publication Date: 2016
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  • 8
    Online Resource
    Online Resource
    American Chemical Society (ACS) ; 2009
    In:  Environmental Science & Technology Vol. 43, No. 3 ( 2009-02-01), p. 790-795
    In: Environmental Science & Technology, American Chemical Society (ACS), Vol. 43, No. 3 ( 2009-02-01), p. 790-795
    Type of Medium: Online Resource
    ISSN: 0013-936X , 1520-5851
    RVK:
    Language: English
    Publisher: American Chemical Society (ACS)
    Publication Date: 2009
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    detail.hit.zdb_id: 1465132-4
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  • 9
    In: Atmospheric Environment, Elsevier BV, Vol. 49 ( 2012-3), p. 403-410
    Type of Medium: Online Resource
    ISSN: 1352-2310
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2012
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    detail.hit.zdb_id: 1499889-0
    SSG: 14
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  • 10
    In: Elementa: Science of the Anthropocene, University of California Press, Vol. 10, No. 1 ( 2022-12-23)
    Abstract: Emissions and secondary photochemical products from the Daesan petrochemical complex (DPCC), on the west coast of South Korea, were measured from the NASA DC-8 research aircraft during the Korea-United States Air Quality campaign in 2016. The chemical evolution of petrochemical emissions was examined utilizing near-source and downwind plume transects. Small alkenes, such as ethene (C2H4), propene (C3H6), and 1,3-butadiene (C4H6), dominated the hydroxyl (OH) radical reactivity near the source region. The oxidation of these alkenes in the petrochemical plumes led to efficient conversion of nitrogen oxides (NOx) to nitric acid (HNO3), peroxycarboxylic nitric anhydrides (PANs), and alkyl nitrates (ANs), where the sum of the speciated reactive nitrogen contributes more than 80% of NOy within a few hours. Large enhancements of short-lived NOx oxidation products, such as hydroxy nitrates (HNs) and peroxyacrylic nitric anhydride, were observed, in conjunction with high ozone levels of up to 250 ppb, which are attributed to oxidation of alkenes such as 1,3-butadiene. Instantaneous ozone production rates, P(O3), near and downwind of the DPCC ranged from 9 to 24 ppb h−1, which were higher than those over Seoul. Ozone production efficiencies ranged from 6 to 10 downwind of the DPCC and were lower than 10 over Seoul. The contributions of alkenes to the instantaneous secondary organic aerosol (SOA) production rate, P(SOA), were estimated to be comparable to those of more common SOA precursors such as aromatics at intermediate distances from the DPCC. A model case study constrained to an extensive set of observations provided a diagnostic of petrochemical plume chemistry. The simulated plume chemistry reproduced the observed evolution of ozone and short-lived reactive nitrogen compounds, such as PANs and HNs as well as the rate and efficiency of ozone production. The simulated peroxy nitrates (PNs) budget included large contributions (approximately 30%) from unmeasured PNs including peroxyhydroxyacetic nitric anhydride and peroxybenzoic nitric anhydride. The large, predicted levels of these PAN compounds suggest their potential importance in chemical evolution of petrochemical plumes. One unique feature of the DPCC plumes is the substantial contribution of 1,3-butadiene to ozone and potentially SOA production. This work suggests that reductions in small alkene, especially 1,3-butadiene, emissions from the DPCC should be a priority for reducing downwind ozone.
    Type of Medium: Online Resource
    ISSN: 2325-1026
    Language: English
    Publisher: University of California Press
    Publication Date: 2022
    detail.hit.zdb_id: 2745461-7
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