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Glenn Diskin

Publications and source records attributed to Glenn Diskin.

At least 19 records

Stratospheric Air Intrusions Promote Global-Scale New Particle Formation

New particle formation in the free troposphere is a major source of cloud condensation nuclei globally. The prevailing view is that in the free troposphere, new particles are formed predominantly in convective cloud outflows. We present another mechanism using global observations. We find that during stratospheric air intrusion events, the mixing of descending ozone-rich stratospheric air with more moist free tropospheric background results in elevated hydroxyl radical (OH) concentrations. Such mixing is most prevalent near the tropopause where the sulfur dioxide (SO 2 ) mixing ratios are high. The combination of elevated SO 2 and OH levels leads to enhanced sulfuric acid concentrations, promoting particle formation. Such new particle formation occurs frequently and over large geographic regions, representing an important particle source in the midlatitude free troposphere.

Jiaoshi Zhang

Measurement Report :Emission Factors of NH3 and NHx for Wildfires and Agricultural Fires in the United States

During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study, the NASA DC-8 carried out in situ chemical measurements in smoke plumes emitted from wildfires and agricultural fires in the contiguous United States. The DC-8 payload included a modified proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) for the fast measurement of gaseous ammonia (NH 3 ) and a high-resolution time-of-flight aerosol mass spectrometer (AMS) for the fast measurement of submicron particulate ammonium (NH 4 + ). We herein report data collected in smoke plumes emitted from 6 wildfires in the Western United States, 2 prescribed grassland fires in the Central United States, 1 prescribed forest fire in the Southern United States, and 66 small agricultural fires in the Southeastern United States. Smoke plumes contained double to triple digit ppb levels of NH 3 . In the wildfire plumes, a significant fraction of NH 3 had already been converted to NH 4 + at the time of sampling (≥2 h after emission). Substantial amounts of NH 4 + were also detected in freshly emitted smoke from corn and rice field fires. We herein present a comprehensive set of emission factors of NH 3 and NH x , with NH x = NH 3 + NH 4 + . Average NH 3 and NH x emission factors for wildfires in the Western United States were 1.86±0.75 g kg −1 and 2.47±0.80 g kg −1 of fuel burned, respectively. Average NH 3 and NH x emission factors for agricultural fires in the Southeastern United States were 0.89±0.58 and 1.74±0.92 g kg −1 , respectively. Our data show no clear inverse correlation between modified combustion efficiency (MCE) and NH 3 emissions. The observed NH 3 emissions were significantly higher than measured in previous laboratory experiments in the FIREX FireLab 2016 study.

Laura Tomsche

Heterogeneity and Chemical Reactivity of the Remote Troposphere Defined By Aircraft Measurements - Corrected

The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O3 and CH4 (O3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O3 and CH4. Models distinctly underestimate O3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation.

Tropospheric Chemistry

Polarimeter + Lidar–Derived Aerosol Particle Number Concentration

In this study, we propose a simple method to derive vertically resolved aerosol particle number concentration (Na) using combined polarimetric and lidar remote sensing observations. This method relies on accurate polarimeter retrievals of the fine-mode column-averaged aerosol particle extinction cross section and accurate lidar measurements of vertically resolved aerosol particle extinction coefficient such as those provided by multiwavelength high spectral resolution lidar. We compare the resulting lidar + polarimeter vertically resolved N(a) product to in situ N(a) data collected by airborne instruments during the NASA aerosol cloud meteorology interactions over the western Atlantic experiment (ACTIVATE). Based on all 35 joint ACTIVATE flights in 2020, we find a total of 32 collocated in situ and remote sensing profiles that occur on 11separate days, which contain a total of 322 cloud-free vertically resolved altitude bins of 150 m resolution. We demonstrate that the lidar + polarimeter N(a) agrees to within 106% for 90% of the 322 vertically resolved points. We also demonstrate similar agreement to within 121% for the polarimeter-derived column-averaged N(a). We find that the range-normalized mean absolute deviation (NMAD) for the polarimeter-derived column-averaged Na is 21%, and the NMAD for the lidar + polarimeter-derived vertically resolved Na is 16%. Taken together, these findings suggest that the error in the polarimeter-only column-averaged N(a) and the lidar + polarimeter vertically resolved N(a) are of similar magnitude and represent a significant improvement upon current remote sensing estimates of N(a).

RSP

Photochemical Evolution of the 2013 California Rim Fire: Synergistic Impacts of Reactive Hydrocarbons and Enhanced Oxidants

Large wildfires markedly alter regional atmospheric composition, but chemical complexity challenges model predictions of downwind impacts. Here, we elucidate key facets of gas-phase photochemistry and assess novel chemical processes via a case study of the 2013 California Rim Fire plume. Airborne in situ observations, acquired during the NASA Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) mission, illustrate the evolution of volatile organic compounds (VOC), oxidants, and reactive nitrogen over 12 hours of atmospheric aging. Measurements show rapid formation of ozone and peroxyacyl nitrates (PNs), sustained peroxide production, and prolonged enhancements in oxygenated VOC and nitrogen oxides (NOX). Measurements and Lagrangian trajectories constrain a 0-D puff model that approximates plume photochemical history and provides a framework for evaluating key processes. Simulations examine the effects of 1) previously-unmeasured reactive VOC identified in recent laboratory studies, and 2) emissions and secondary production of nitrous acid (HONO). Inclusion of estimated unmeasured VOC leads to a 250% increase in OH reactivity and a 70% increase in radical production via oxygenated VOC photolysis. HONO amplifies radical cycling and serves as a downwind NOX source, although two different HONO production mechanisms (particulate nitrate photolysis and heterogeneous NO2 conversion) exhibit markedly different effects on ozone, NOX, and PNs. Analysis of radical initiation rates suggests that oxygenated VOC photolysis is a major radical source, exceeding HONO photolysis when averaged over the first 2 hours of aging. Ozone production chemistry transitions from VOC-sensitive to NOX-sensitive within the first hour of plume aging, with both peroxide and organic nitrate formation contributing significantly to radical termination. To simulate smoke plume chemistry accurately, models should simultaneously account for the full reactive VOC pool and all relevant oxidant sources.

SEAC4RS

Influence of Cloud, Fog, and High Relative Humidity during Pollution Transport Events in South Korea: Aerosol Properties and PM2.5 Variability

This investigation examines aerosol dynamics during major fine mode aerosol transboundary pollution events in South Korea primarily during the KORUS-AQ campaign from May 1 – June 10, 2016, particularly when cloud fraction was high and/or fog was present to quantify the change in aerosol characteristics due to near-cloud or fog interaction. We analyze the new AERONET Version 3 data that have significant changes to cloud screening algorithms, allowing many more fine-mode observations in the near vicinity of clouds or fog. Case studies for detailed investigation include May 25–26, 2016 when cloud fraction was high over much of the peninsula, associated with a weak frontal passage and advection of pollution from China. These cloud-influenced Chinese transport dates also had the highest aerosol optical depth (AOD), surface PM2.5 concentrations and fine mode particle sizes of the entire campaign. Another likewise cloud/high relative humidity (RH) case is June 9 and 10, 2016 when fog was present over the Yellow Sea that appears to have affected aerosol properties well downwind over the Korean peninsula. In comparison we also investigated aerosol properties on air stagnation days with very low cloud cover and relatively low RH (May 17 & 18, 2016), when local Korean emissions dominated. Aerosol volume size distributions show marked differences between the transport days (with high RH and cloud influences) and the local pollution stagnation days, with total column-integrated particle fine mode volume being an order of magnitude greater on the pollution transport dates. The PM2.5 over central Seoul were significantly greater than for coastal sites on the transboundary transport days yet not on stagnation days, suggesting addi-tional particle formation from gaseous urban emissions in cloud/fog droplets and/or in the high RH humidified aerosol environment. Many days had KORUS-AQ research aircraft flights that provided observations of aerosol absorption, particle chemistry and vertical profiles of extinction. AERONET retrievals and aircraft in situ mea-surements both showed high single scattering albedo (weak absorption) on the cloudy or cloud influenced days, plus aircraft profile in situ measurements showed large AOD enhancements (versus dried aerosol) at ambient relative humidity (RH) on the pollution transport days, consistent with the significantly larger fine mode particle radii and weak absorption.

Aerosol

Comparing the Regional Variability of Emission Factors of Greenhouse Gases Over Different Landscape During FIREX-AQ Campaign

Biomass burning (wildfires, prescribed and agricultural burning) is one of the major sources of trace gases and particulate emissions and annual variability in growth rates. Biomass burning can impact local, regional, and global air quality, as well as climate. Measurements of emissions from biomass burning are crucial to a better understanding of how it influences and interacts with biogeochemical cycles. High resolution in-situ measurements were recorded onboard the NASA DC-8 aircraft during the FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality) airborne field campaign July-September, 2019, which was conducted over the continental U.S. Fire emission factors (EF) are essential input for emissions models used to develop biomass burning emission inventories. Here we present the Emission Ratio (ER), MCE (Modified Combustion Efficiency), and EF (Emission Factor) of CO2, CO, and CH4, which constitute the majority of carbon emitted from the wildland, prescribed, and agricultural fires. EFCO2, EFCO, and EFCH4 from the Wildland fires at Williams Flats, WA (primarily Douglas Fir, Ponderosa pine, wheatgrass: 50-75%), ranged from 1527 – 1820 g/kg (Avg. 1641±42), 6.5 – 174.1 g/kg (110.5±24.1), and 0.7 – 11.3 g/kg (6.2±1.9), respectively. EFs from the Arizona CASTLE fire, with somewhat different fuel sources (primarily Ponderosa pine, Douglas fir: 40-70%) ranged from 1266 – 1667 g/kg (1596±59), 99.5 – 344.5 g/kg (136.7±36.8), and 0.4 – 9.2 g/kg (7.2±1.7), respectively. Another primary driver of EFs is likely fire weather. Detailed variability of greenhouse gas EFs will be examined and presented in accordance with different fuels and fire conditions at burned areas, specifically within unique wildland and croplands, using the FCCS (Fuel Characteristic Classification System) 30m land cover identification and the Cropland Data Layer (CDL).

Biomass burning

Airborne High Spectral Resolution Lidar-2 Measurements of Enhanced Depolarization in Marine Aerosols

Airborne NASA Langley Research Center (LaRC) High Spectral Resolution Lidar-2 (HSRL-2) measurements acquired during the recent NASA EVS-3 Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE) revealed enhanced particulate linear depolarization associated with aerosols within the marine boundary layer. These HSRL-2 observations were acquired off the east coast of the United States in February and March 2020 when this lidar was deployed on the NASA LaRC UC-12 aircraft. HSRL-2 measured profiles of aerosol backscattering, extinction,and depolarization at 355 and 532nm and aerosol backscattering and depolarization at 1064nm. Typically HSRL-2 measures low (<5%) linear particulate depolarization associated with marine sea salt aerosols. However, during several ACTIVATE flights, particularly those that occurred with outbreaks of cold, dry air, linear particulate depolarization exceeded 15-20% (532nm) for aerosols within a few hundred meters above the surface. These high values indicated that these particles were nonspherical. Elevated depolarization values were also observed at 355 and 1064 nm. HSRL-2 measured aerosol extinction/backscatter ratio (“lidar ratio”) values around 20-25 sr (355 and 532 nm) that are typically associated with sea salt particles. Coincident measurements of relative humidity from dropsondes released from the UC-12and in situ Diode Laser Hygrometer (DLH) measurements flown on the NASA HU-25 aircraft showed that highest depolarization values of these nonspherical particles were found when the relative humidity (RH)was below 50-60%.These lidar observations of elevated depolarization associated with sea salt aerosol are consistent with previous lidar measurements of sea salt aerosols in dry conditions. We discuss these HSRL-2 measurements also in the context of coincident airborne in situ measurements of particle size and composition acquired on the HU-25 aircraft. We also found that CALIOP satellite measurements observed elevated depolarization during some similar cold air outbreaks. In such cases, the operational CALIOP algorithms attributed the elevated depolarization to nonspherical dust particles rather than the more likely scenario of nonspherical sea salt particles associated with low RH.

aerosols

Comparing the regional variability of emission factors of greenhouse gases over different landscape during FIREX-AQ campaign

Biomass burning (wildfires, prescribed and agricultural burning) is one of the major sources of trace gases and particulate emissions and annual variability in growth rates. Biomass burning can impact local, regional, and global air quality, as well as climate. Measurements of emissions from biomass burning are crucial to a better understanding of how it influences and interacts with biogeochemical cycles. High resolution in-situ measurements were recorded onboard the NASA DC-8 aircraft during the FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality) airborne field campaign July-September, 2019, which was conducted over the continental U.S. Fire emission factors (EF) are essential input for emissions models used to develop biomass burning emission inventories. Here we present the Emission Ratio (ER), MCE (Modified Combustion Efficiency), and EF (Emission Factor) of CO2, CO, and CH4, which constitute the majority of carbon emitted from the wildland, prescribed, and agricultural fires. EFCO2, EFCO, and EFCH4 from the Wildland fires at Williams Flats, WA (primarily Douglas Fir, Ponderosa pine, wheatgrass: 50-75%), ranged from 1527 – 1820 g/kg (Avg. 1641±42), 6.5 – 174.1 g/kg (110.5±24.1), and 0.7 – 11.3 g/kg (6.2±1.9), respectively. EFs from the Arizona CASTLE fire, with somewhat different fuel sources (primarily Ponderosa pine, Douglas fir: 40-70%) ranged from 1266 – 1667 g/kg (1596±59), 99.5 – 344.5 g/kg (136.7±36.8), and 0.4 – 9.2 g/kg (7.2±1.7), respectively. Another primary driver of EFs is likely fire weather. Detailed variability of greenhouse gas EFs will be examined and presented in accordance with different fuels and fire conditions at burned areas, specifically within unique wildland and croplands, using the FCCS (Fuel Characteristic Classification System) 30m land cover identification and the Cropland Data Layer (CDL).

Biomass burning

Observation of Trace Gases Seasonal Variability in the Marine Boundary Layer over the Atlantic Ocean during the ACTIVATE Field Campaign

High resolution in-situ measurements of carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and water vapor (H2O) were made onboard the NASA HU-25 aircraft during the ACTIVATE (Aerosol Cloud meteorology Interactions oVer the western Atlantic Experiment) campaign during 2020 and 2021 in different seasons (winter through summer) over the mid-latitude western Atlantic Ocean. As most of the flights focused on the marine boundary layer (MBL) during the campaign, these trace gas observations are an excellent data set to examine seasonal variability of trace gas background values in the MBL without the influence of localized point sources. We will describe the variability of these trace gases in the MBL background by filtering out concentrated point sources using back trajectory analysis along with trace gas ratios. Additionally, the ocean is a significant sink of anthropogenic CO2 capturing about one quarter of total anthropogenic carbon. By looking at the MBL CO2 variation as a function of season, we discuss observed changes in CO2 uptake over the ocean. These high accuracy observations of trace gas backgrounds in the MBL along with characterizing seasonal effects on oceanic sequestering of anthropogenic CO2 will improve the understanding of seasonal variations and change in climate and inverse modelling over the ocean.

Yonghoon Choi

Exploring the Continuum of Stratiform and Cumulus Cloudiness: Observational Insights Related to Marine Boundary Layer Clouds

Low-level marine clouds take on a wide range of morphological states owing to external forcing and internal feedbacks. Rarely are shallow marine clouds adequately described by a single simplified framework but instead exhibit features that partially conform to several states that could be considered “limiting”. Perhaps the most apparent dichotomy is whether to consider shallow clouds as existing within a surface-driven mixed layer or as convective “plume” elements positioned on top. Do the rules that govern the limiting cases transition smoothly through the hybrid scenarios found in nature, or are there particular regions of attraction or repulsion?We have identified 3 ”axes” along which to investigate how the energetics, thermodynamics and cloud macro structure relate to the intermediate spaces between idealizations.

Ewan Crosbie