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All sourcesNASA NTRSDOE OSTI
NASA NTRS2018

Decadal Changes in Summertime Reactive Oxidized Nitrogen and Surface Ozone over the Southeast United States

Widespread efforts to abate ozone (O3) smog have significantly reduced emissions of nitrogen oxides (NOx) over the past 2 decades in the Southeast US, a place heavily influenced by both anthropogenic and biogenic emissions. How reactive nitrogen speciation responds to the reduction in NOx emissions in this region remains to be elucidated. Here we exploit aircraft measurements from ICARTT (International Consortium for Atmospheric Research on Transport and Transformation - July-August 2004), SENEX (Southeast Nexus - June-July 2013), and SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys - August-September 2013) and long-term ground measurement networks alongside a global chemistry-climate model to examine decadal changes in summertime reactive oxidized nitrogen (RON) and ozone over the Southeast US. We show that our model can reproduce the mean vertical profiles of major RON species and the total (NO (sub y)) in both 2004 and 2013. Among the major RON species, nitric acid (HNO3) is dominant (approximately 42-45 percent), followed by NOx (31 percent), total peroxy nitrates (Sigma PNs; 14 percent), and total alkyl nitrates (Sigma ANs; 9-12 percent) on a regional scale. We find that most RON species, including NOx, Sigma PNs, and HNO3, decline proportionally with decreasing NOx emissions in this region, leading to a similar decline in NO (sub y). This linear response might be in part due to the nearly constant summertime supply of biogenic VOC (Volatile Organic Compounds) emissions in this region. Our model captures the observed relative change in RON and surface ozone from 2004 to 2013. Model sensitivity tests indicate that further reductions of NOx emissions will lead to a continued decline in surface ozone and less frequent high-ozone events.

Li, Jingyi↗
NASA NTRS2016

Using Airborne In-Situ Profiles to Evaluate TCCON Data from Armstrong Flight Research Center

A Fourier Transform Spectrometer (FTS) was deployed to the Armstrong Flight Research Center (AFRC) in Edwards, CA as a member of the Total Carbon Column Observing Network (TCCON) and has now been in operation for over 3 years. The data record from AFRC will be presented as well as airborne validation profiles obtained during the NASA SEAC4RS, SARP, KORUS-AQ, and ATom missions utilizing various NASA aircraft. One of the reasons that the AFRC location was selected is due to its proximity to a highly reflective lakebed, which has proven to be difficult for accurate satellite retrievals. As such, the data from AFRC has been used for OCO-2 calibration. In order for accurate calibration of OCO-2, the validity of the TCCON measurements must be established. To this end, integrated airborne in-situ vertical profiles will be presented and compared with the TCCON FTS measurements, where good agreement has been found.

Iraci, Laura T.↗
NASA NTRS2016

Spaceborne Remote Sensing of Aerosol Type: Global Distribution, Model Evaluation and Translation into Chemical Speciation

It is essential to evaluate and refine aerosol classification methods applied to passive satellite remote sensing. We have developed an aerosol classification algorithm (called Specified Clustering and Mahalanobis Classification, SCMC) that assigns an aerosol type to multi-parameter retrievals by spaceborne, airborne or ground-based passive remote sensing instruments [1]. The aerosol types identified by our scheme are pure dust, polluted dust, urban-industrialdeveloped economy, urban-industrialdeveloping economy, dark biomass smoke, light biomass smoke and pure marine. We apply the SCMC method to inversions from the ground-based AErosol RObotic NETwork (AERONET [2]) and retrievals from the space-borne Polarization and Directionality of Earths Reflectances instrument (POLDER, [3]). The POLDER retrievals that we use differ from the standard POLDER retrievals [4] as they make full use of multi-angle, multispectral polarimetric data [5]. We analyze agreement in the aerosol types inferred from both AERONET and POLDER and evaluate GEOS-Chem [6] simulations over the globe. Finally, we use in-situ observations from the SEAC4RS airborne field experiment to bridge the gap between remote sensing-inferred qualitative SCMC aerosol types and their corresponding quantitative chemical speciation. We apply the SCMC method to airborne in-situ observations from the NASA Langley Aerosol Research Group Experiment (LARGE, [7]) and the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP, [8]) instruments; we then relate each coarsely defined SCMC type to a sum of percentage of individual aerosol species, using in-situ observations from the Particle Analysis by Laser Mass Spectrometry (PALMS, [9]), the Soluble Acidic Gases and Aerosol (SAGA, [10]), and the High - Resolution Time - of - Flight Aerosol Mass Spectrometer (HR ToF AMS, [11]).

airborne↗
NASA NTRS2016

Emissions Relationships Among Western Forest Fire Plumes: II. Plume Typing for Sources of Ozone and Aerosol Absorption

Previous studies of emission factors from biomass burning are prone to largeerrors since they ignore the interplay of mixing and varying pre-fire backgroundCO2 levels. Such complications severely affected our studies of 446 forest fireplume samples measured in the Western US by the science teams of NASAs SEAC4RS and ARCTAS airborne missions. Consequently we propose a MixedEffects Regression Emission Technique (MERET) to check techniques like theNormalized Emission Ratio Method (NERM), where use of sequentialobservations cannot disentangle emissions and mixing. We also evaluate asimpler consensus technique. All techniques relate emissions to fuel burnedusing Cburn Ctot added to the fire plume, where Ctot (CO2 + CO). Mixed-effectsregression can estimate pre-fire background values of Ctot (indexed byobservation j) simultaneously with emissions factors indexed by individualspecies i, xi (Cburn )i,j., MERET and consensus require more than twoemissions indicators. Our studies excluded samples where exogenous CO orCH4 might have been fed into a fire plume, mimicking emission.We sought to let the data on 13 gases and particulate properties suggest clustersof variables and plume types, using non-negative matrix factorization (NMF).While samples were mixtures, the NMF unmixing suggested purer burn types.Particulate properties (bscat, babs, SSA, AE) and gas-phase emissions were interrelated.Finally, we sought a simple categorization useful for modeling ozone productionin plumes. Two kinds of fires produced high ozone: those with large fuel nitrogenas evidenced by remnant CH3CN in the plumes, and also those from veryintense large burns. Fire types with optimal ratios of delta-NOydelta-HCHO associate with the highest additional ozone per unit Cburn, Perhaps theseplumes exhibit limited NOx binding to reactive organics. Perhaps these plumesexhibit limited NOx binding to reactive organics.

ozone↗
NASA NTRS2017

Retrievals of Aerosol Optical and Microphysical Properties from Imaging Polar Nephelometer Scattering Measurements

A method for the retrieval of aerosol optical and microphysical properties from in situ light-scattering measurements is presented and the results are compared with existing measurement techniques. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to airborne and laboratory measurements made by a novel polar nephelometer. This instrument, the Polarized Imaging Nephelometer (PI-Neph), is capable of making high-accuracy field measurements of phase function and degree of linear polarization, at three visible wavelengths, over a wide angular range of 3 to 177°. The resulting retrieval produces particle size distributions (PSDs) that agree, within experimental error, with measurements made by commercial optical particle counters (OPCs). Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salt particles, with a refractive index that is well established. The airborne measurements used in this work were made aboard the NASA DC-8 aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign, and the inversion of this data represents the first aerosol retrievals of airborne polar nephelometer data. The results provide confidence in the real refractive index product, as well as in the retrieval's ability to accurately determine PSD, without assumptions about refractive index that are required by the majority of OPCs.

Espinosa, W. Reed↗
NASA NTRS2016

Significant Tropospheric O3 Production from Extratropical Forest Fires:When? When Not?

There is significant controversy on whether extratropical fires contribute importantly to widespread ozone productionabsent the addition of urban pollutant nitrogen oxides (Jaffe and Widger, 2012, Singh et al., 2012,2013). Wereport a significant range of O3 production early in the fire plume history and report controls on which notable O3production occurs. The current data set is the airborne observations made on board NASAs highly instrumentedDC-8 aircraft during the ARCTAS (2008) and SEAC4RS (2013) campaigns within the Western United States. Aclear analysis of fire emissions was aided considerably by MERET (a Mixed Effects Regressions Emissions Technique).This technique allows consistent emission factors and enhancement ratios for O3 for individual aircraftsamples largely free from uncertainties resulting from mixing and entrainment which plague many published estimates.(Yokelson et al, 2013, Chatfield and Andreae, 2016). We find support for the reasonable idea that the ratioof nitrogen oxides (NOx) to volatile organic carbon (VOC) emissions controls new O3 production. The evidence isfor significant O3 production from high-fuel-nitrogen fuels (as evidenced by acetonitrile) and extremely hot largefires (like the Yosemite Rim Fire of 2013 which we analyze), while others do not. VOC emissions factors varysignificantly from fire to fire (and from different samples in the Rim Fire). Relative CO production (aka modifiedcombustion efficiency) is only one factor describing VOC emissions factors.

Chatfield, R.↗
NASA NTRS2019

Emissions Relationships in Western Forest Fire Plumes: I. Reducing the Effect of Mixing Errors on Emission Factors

Studies of emission factors from biomass burning using aircraft data complement the results of lab studies and extend them to conditions of immense hot conflagrations. We illustrate and discuss emission relationships for 422 individual samples from many forest-fire plumes in the Western US. The samples are from two NASA investigations: ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) and SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys). This work provides sample-by-sample enhancement ratios (EnRs) for 23 gases and particulate properties. Many EnRs provide candidates for emission ratios (ERs, corresponding to the EnR at the source) when the origin and degree of transformation is understood and appropriate. From these, emission factors (EFs) can be estimated when the fuel dry mass consumed is known or can be estimated using the carbon mass budget approach. This analysis requires understanding the interplay of mixing of the plume with surrounding air. Some initial examples emphasize that measured C(tot) = CO2 + CO in a fire plume does not necessarily describe the emissions of the total carbon liberated in the flames, C(burn). Rather, it represents C(tot) = C(burn) + C(bkgd), which includes possibly varying background concentrations for entrained air. Consequently, we present a simple theoretical description for plume entrainment for multiple tracers from flame to hundreds of kilometers downwind and illustrate some intrinsic linear behaviors. The analysis suggests a Mixed Effects Regression Emission Technique (MERET), which can eliminate occasional strong biases associated with the commonly used normalized excess mixing ratio (NEMR) method. MERET splits C(tot) to reveal C(burn) by exploiting the fact that C(burn) and all tracers respond linearly to dilution, while each tracer has consistent EnR behavior (slope of tracer concentration with respect to C(burn)). The two effects are separable. Two or three or preferably more emission indicators are required as a minimum; here we used ten. Limited variations in the EnRs for each tracer can be incorporated and the variations and co-variations analyzed. The percentage CO yield (or the modified combustion efficiency) plays some role. Other co-relationships involving nitrogen and organic classes are more prominent; these have strong relationships to the C(burn) to O3 emission relationship. In summary, MERET allows fine spatial resolution (EnRs for individual observations) and comparison of similar plumes distant in time and space. Alkene ratios provide us with an approximate photochemical timescale. This allows discrimination and definition, by fire situation, of ERs, allowing us to estimate emission factors.

Chatfield, Robert B.↗
NASA NTRSDate not supplied

TPSAS-NF1676L-21193-DND

Researchers at NASA Langley Research Center have been developing an automated pattern recognition algorithm to identify overshooting convective cloud tops (OTs) in support of the GOES-R satellite program. This algorithm identify regions of overshooting at the individual 1-4 km geostationary satellite pixel scale using visible (during daytime only) and infrared channel imagery and numerical weather analysis data. The algorithm has been developed based upon analysis of 0.25-1 km spatial resolution Aqua MODIS imagery, using a database of over 2000 manually identified OT features throughout the world in storms with varying intensity and morphology. The OT database includes storms ranging from small, warm topped cells in Alaska and Mongolia, tornadic supercells over the U.S. Central Plains and Europe, large tropical mesoscale convective systems, and overshooting in the eyewalls and spiral bands of category 5 tropical cyclones. This database is available for use by the research community. The algorithm is designed to operate on data from any current and historical satellite imager, allowing for development of a highly accurate global OT detection climatology that extends back into the 1990's at up to a 15-30 min temporal resolution throughout the diurnal cycle. As members of the McIDAS Users Group, NASA LaRC has immediate access to the full global archive of geostationary imager data which would allows rapid development of OT climatologies and short-term databases. This type of capability has never been available within the weather and climate research community. Regional geostationary OT databases have been already developed over CONUS during SEAC4RS, for 18-years over the Eastern U.S., and for 5-10 years over Australia, Europe, Southeast Asia, and East Africa among many other regions. Some of these datasets are being used by climate researchers and private industry to examine UTLS-penetrating storm spatial distributions and their temporal variability, in addition to weather hazards associated with these storms at unprecedented spatial detail. This presentation will describe the OT pattern recognition algorithm and highlight recent product applications.

Kristopher Bedka↗
NASA NTRSDate not supplied

Identifying Chemical and Optical Smoke Signatures in Suborbital Observations to Improve Model Projections

Biomass Burning (BB) fires are expected to occur more frequently in the future due to climate change, the build‐up of fuels due to fire suppression, and the expansion of the wildland‐urban interface [Schoennagel et al., 2017; Shivdenko & Schepaschenko, 2013; Stevens et al., 2014; Turner et al., 2019; Yue et al., 2015; Tilman et al., 2001]. Accurate knowledge of the abundance, distribution, and optical properties of absorbing aerosols such as BB smoke is essential to understanding regional and global aerosol radiative effects [Boucher et al., 2013]. It is recognized that differing fuel types (e.g., rice straw, ponderosa pine), combustion modes (i.e., flaming, smoldering or both) and temperature/ moisture content produce smoke with differing optical characteristics (e.g., aerosol light scattering and absorption) and component mixing ratios [e.g., BC, OC and inorganic species such as sulfate, potassium, chloride; Streets et al. 2003; Reid et al., 2005a, b; Janhäll et al., 2010; Sayer et al., 2014]. However, climate models often ascribe a fixed set of emission factors [i.e., amount of particulate for a given species released in the atmosphere per unit dry fuel burned; Darmenov and Dasilva, 2013] and optical properties [Hess et al., 1998] to all BB aerosol plumes, inherently limiting accurate representation of the global and regional heterogeneity of BB. The overarching goal of the proposed work is to improve the microphysical and optical representation of different types of Biomass Burning in Chemistry Transport Models. Our strategy is to capitalize on multiple airborne campaigns (e.g., ARCTAS, SEAC4RS, ORACLES, FIREX-AQ), which sampled different types of BB plumes at different aging stages. Models, when improved and combined with satellite, airborne, and ground observations will help address many aerosol science objectives from the NASA Decadal survey [National Academies of Sciences, Engineering, and Medicine. 2018].

Meloe Shenandoah F Kacenelenbogen↗
NASA NTRS2020

Evaluation of Stratospheric Intrusions and Biomass Burning Plumes on the Vertical Distribution of Tropospheric Ozone Over the Midwestern U.S.

Naturally occurring ozone rich Stratosphere-to-Troposphere Transport (STT) intrusions and biomass burning plumes reaching the surface can contribute to exceedances of the U.S. National Ambient Air Quality Standards (NAAQS) for ground-level ozone (70 ppbv implemented in 2015). In addition, fires can inject significant pollution into the free troposphere where it can be transported long distances. The combined air quality impacts from these sources on ozone has only been analyzed in a few case studies for the Midwest U.S. Here we study ozone impacts in a major Midwestern city, for the first time in St. Louis, Missouri, using a series of ozonesonde profiles taken during the SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys) field campaign in August-September 2013. All ozonesondes showed some enhancements above the background profile levels (~55 ppbv) throughout each tropospheric column. Two models were used to estimate and quantify ozone origins within the columns. A chemical transport model identified enhancements from STT equivalent to 10to15 ppbv over the background with a 10 to15% contribution overall to the column. Two FLEXPART-WRF simulations, one with smoke in the boundary layer and the other with smoke above, identified enhancements from biomass burning equivalent to 10to 80 ppbv. Overall, the total biomass burning contribution is 15to 30% of the total column. Five ozonesondes showed signatures of mixed biomass burning plumes and STT intrusions. During this study period, biomass burning in the western U.S. contributed 70% to ozone enhancements in the total column compared to 3% from the central U.S and 27% from other areas.

National Ambient Air Quality Standards for ground‐↗
NASA NTRS2017

Ozone Production by Corona Discharges During a Convective Event in DISCOVER-AQ Houston

An ozonesonde launched near electrically active convection in Houston, TX on 5 September 2013 during the NASA DISCOVER-AQ project measured a large enhancement of ozone throughout the troposphere. A separate ozonesonde was launched from Smith Point, TX (approx. 58 km southeast of the Houston site) at approximately the same time as the launch from Houston and did not measure that enhancement. Furthermore, ozone profiles for the descent of both sondes agreed well with the ascending Smith Point profile, suggesting a highly localized event in both space and time in which an anomalously large enhancement of 70 - 100 ppbv appeared in the ascending Houston ozonesonde data. Compared to literature values, such an enhancement appears to be the largest observed to date. Potential sources of the localized ozone enhancement such as entrainment of urban or biomass burning emissions, downward transport from the stratosphere, photochemical production from lightning NO(sub x), and direct ozone production from corona discharges were investigated using model simulations. We conclude that the most likely explanation for the large ozone enhancement is direct ozone production by corona discharges. Integrating the enhancement seen in the Houston ozone profile and using the number of electrical discharges detected by the NLDN (or HLMA), we estimate a production of 2.48 x 10(exp. 28) molecules of ozone per flash which falls within the range of previously recorded values (9.89 x 10(exp. 26) - 9.82 x 10)exp. 28) molecules of ozone per flash). Since there is currently no parameterization for the direct production of ozone from corona discharges we propose the implementation of an equation into a chemical transport model. Ultimately, additional work is needed to further understand the occurrence and impact of corona discharges on tropospheric chemistry on short and long timescales.

ozone↗
NASA NTRS2022

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.

MUSICA↗