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At least 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
NASA NTRS2010

Composition Changes After the "Halloween" Solar Proton Event: The High-Energy Particle Precipitation in the Atmosphere (HEPPA) Model Versus MIPAS Data Intercomparison Study

We have compared composition changes of NO, NO2, H2O2,O3, N2O, HNO3 , N2O5, HNO4, ClO, HOCl, and ClONO2 as observed by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat in the aftermath of the "Halloween" solar proton event (SPE) in October/November 2003 at 25-0.01 hPa in the Northern hemisphere (40-90 N) and simulations performed by the following atmospheric models: the Bremen 2D model (B2dM) and Bremen 3D Chemical Transport Model (B3dCTM), the Central Aerological Observatory (CAO) model, FinROSE, the Hamburg Model of the Neutral and Ionized Atmosphere (HAMMONIA), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA), the ECHAM5/MESSY Atmospheric Chemistry (EMAC) model, the modeling tool for SO1ar Climate Ozone Links studies (SOCOL and SOCOLi), and the Whole Atmosphere Community Climate Model (WACCM4). The large number of participating models allowed for an evaluation of the overall ability of atmospheric models to reproduce observed atmospheric perturbations generated by SPEs, particularly with respect to NOS, and ozone changes. We have further assessed the meteorological conditions and their implications on the chemical response to the SPE in both the models and observations by comparing temperature and tracer (CH4 and CO) fields. Simulated SPE-induced ozone losses agree on average within 5% with the observations. Simulated NO(y) enhancements around 1 hPa, however, are typically 30% higher than indicated by the observations which can be partly attributed to an overestimation of simulated electron-induced ionization. The analysis of the observed and modeled NO(y) partitioning in the aftermath of the SPE has demonstrated the need to implement additional ion chemistry (HNO3 formation via ion-ion recombination and water cluster ions) into the chemical schemes. An overestimation of observed H2O2 enhancements by all models hints at an underestimation of the OH/HO2 ratio in the upper polar stratosphere during the SPE. The analysis of chlorine species perturbations has shown that the encountered differences between models and observations, particularly the underestimation of observed ClONO2 enhancements, are related to a smaller availability of ClO in the polar night region already before the SPE. In general, the intercomparison has demonstrated that differences in the meteorology and/or initial state of the atmosphere in the simulations causes a relevant variability of the model results, even on a short timescale of only a few days.

Funke, B.↗
NASA NTRS2017

Multi-Decadal Records of Stratospheric Composition and Their Relationship to Stratospheric Circulation Change

Constituent evolution for 1990-2015 simulated using the Global Modeling Initiative chemistry and transport model driven by meteorological fields from the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2) is compared with three sources of observations: ground-based column measurements of HNO3 and HCl from two stations in the Network for the Detection of Atmospheric Composition Change (NDACC, 1990- ongoing), profiles of CH4 from the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite (UARS, 1992-2005), and profiles of N2O from the Microwave Limb Sounder on the Earth Observing System satellite Aura (2005- ongoing). The differences between observed and simulated values are shown to be time dependent, with better agreement after 2000 compared with the prior decade. Furthermore, the differences between observed and simulated HNO3 and HCl columns are shown to be correlated with each other, suggesting that issues with the simulated transport and mixing cause the differences during the 1990s and that these issues are less important during the later years. Because the simulated fields are related to mean age in the lower stratosphere, we use these comparisons to evaluate the time dependence of mean age. The ongoing NDACC column observations provide critical information necessary to substantiate trends in mean age obtained using fields from MERRA-2 or any other reanalysis products.

Profiles of N2O from the Microwave Limb Sounde↗
NASA NTRS2018

Wintertime Overnight NOx Removal in a Southeastern United States Coal-Fired Power Plant Plume: A Model for Understanding Winter NOx Processing and Its Implications

Nitric oxide (NO) is emitted in large quantities from coal-burning power plants. During the day, the plumes from these sources are efficiently mixed into the boundary layer, while at night, they may remain concentrated due to limited vertical mixing during which they undergo horizontal fanning. At night, the degree to which NO is converted to HNO3 and therefore unable to participate in next-day ozone (O3) formation depends on the mixing rate of the plume, the composition of power plant emissions, and the composition of the background atmosphere. In this study, we use observed plume intercepts from the Wintertime INvestigation of Transport, Emissions and Reactivity (WINTER) campaign to test sensitivity of overnight NOx removal to the N2O5 loss rate constant, plume mixing rate, background O3, and background levels of volatile organic compounds using a 2-D box model of power plant plume transport and chemistry. The factor that exerted the greatest control over NOx removal was the loss rate constant of N2O5. At the lowest observed N2O5 loss rate constant, no other combination of conditions converts more than 10 percent of the initial NOx to HNO3. The other factors did not influence NOx removal to the same degree.

air quality↗
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 NTRSDate not supplied

Isotopically Tracking Nitrogen Oxides, Nitrous Acid, And Nitric Acid, Particulate Nitrate from Wildfire During FIREX-AQ

Wildfires are an important source of reactive nitrogen species including nitrogen oxides (NOx = NO + NO2) and nitrous acid (HONO), as well as products such as nitric acid (HNO3) and particulate nitrate (p-NO3-). These species have strongly influence air quality and climate. In summer of 2019 (July 25 —August 21), as part of the FIREX-AQ ground mission, we drove ~3000 miles and sampled smoke of different ages in both daytime and nighttime from 5 different wildfires in the western US. Using recently developed methods that have been validated in both laboratory and field settings, we conducted high time resolution collection of NOx, NO2, HONO, HNO3, and p-NO3- for off-line characterization of isotopic composition δ15N, δ18O and Δ17O (=δ17O−0.52 δ18O). δ15N serves as a potential tracer for tracking sources and reactive nitrogen cycling pathways, δ18O and Δ17O provide key information about oxidation pathways (i.e. O3 versus RO2). Our measured δ15N for HONO ranges from -4.9‰ to +5.2‰ and -8‰ to +5.2‰ respectively, in the majority overlapping with our prior lab controlled burning results, which suggests the capability of δ15N for tracing the biomass burning emissions against other sources including vehicular emissions and soil emissions. In addition, our measurements show δ18O and Δ17O for NO2 and HONO vary significantly day vs night, as well as in young smoke vs aged smoke, likely reflecting different oxidizing mechanisms under different smoke conditions. Preliminary results of isotopic signatures of all the above reactive nitrogen species will be presented, and their relationships will be explored to identify wildfire derived reactive nitrogen source signatures and to constrain atmospheric processing pathways (e.g. secondary formation of HONO) for different fires under various smoke conditions depending on fuel types, fire conditions and meteorological conditions.

Jiajue Chai↗
NASA NTRSDate not supplied

Improved Characterization of PSC Processes Derived from a Third-Generation CALIOP and MLS Detection and Composition Classification Algorithm

The new 3-year CloudSat and CALIPSO Science Team project described in this poster will use a unique combination of data from the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) instrument on CALIPSO and the Microwave Limb Sounder (MLS) on Aura, in conjunction with supporting meteorological information and detailed modeling studies, to advance our understanding of polar stratospheric cloud (PSC) processes and their role in ozone depletion. We will develop a third-generation (Gen3) PSC detection and composition algorithm that incorporates a new, more robust two-dimensional, multi-channel CALIOP feature detection scheme (2D-McDA). We will also devise and implement an improved two-dimensional PSC composition classification scheme that utilizes multiple parameters (e.g., CALIOP 532-nm parallel and perpendicular scattering ratios, CALIOP 1064-nm total scattering ratio, MLS HNO3 and H2O, ambient temperature, and temperature histories) in a Bayesian approach to determine the most likely PSC composition and help constrain solid PSC particle number density and size/shape. The combined CALIOP/MLS analyses will allow us to study in detail the full life cycle of PSCs and their resulting impact on gas-phase HNO3 and H2O, which should lead to improved parameterizations of PSC microphysics in global CCMs where detailed particle information is not available. The Gen3 CALIOP PSC algorithm will be a natural stepping-stone toward the analysis of data collected during future spaceborne lidar missions, such as NASA’s Atmosphere Observation System (AtmOS) mission currently scheduled for launch late in this decade. We will also investigate possible trends in PSC occurrence and composition over the entire CALIOP data record and through further comparisons with the Stratospheric Aerosol Measurement (SAM) II solar occultation PSC record from 1979-1989. Finally, we will validate the mountain-wave parameterization and PSC schemes used in the UM-UKCA (Unified Model coupled to the United Kingdom Chemistry and Aerosol module) chemistry-climate model through detailed comparisons with earlier CALIOP PSC data products and those developed under this proposal.

CALIPSO↗
NASA NTRSDate not supplied

Improved Characterization of PSC Processes Derived from a Third-Generation CALIOP and MLS Detection and Composition Classification Algorithm

The new 3-year CloudSat and CALIPSO Science Team project described in this poster will use a unique combination of data from the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) instrument on CALIPSO and the Microwave Limb Sounder (MLS) on Aura, in conjunction with supporting meteorological information and detailed modeling studies, to advance our understanding of polar stratospheric cloud (PSC) processes and their role in ozone depletion. We will develop a third-generation (Gen3) PSC detection and composition algorithm that incorporates a new, more robust two-dimensional, multi-channel CALIOP feature detection scheme (2D-McDA). We will also devise and implement an improved two-dimensional PSC composition classification scheme that utilizes multiple parameters (e.g., CALIOP 532-nm parallel and perpendicular scattering ratios, CALIOP 1064-nm total scattering ratio, MLS HNO3 and H2O, ambient temperature, and temperature histories) in a Bayesian approach to determine the most likely PSC composition and help constrain solid PSC particle number density and size/shape. The combined CALIOP/MLS analyses will allow us to study in detail the full life cycle of PSCs and their resulting impact on gas-phase HNO3 and H2O, which should lead to improved parameterizations of PSC microphysics in global chemistry-climate models (CCMs) where detailed particle information is not available. The Gen3 CALIOP PSC algorithm will be a natural stepping-stone toward the analysis of data collected during future spaceborne lidar missions, such as NASA’s Atmosphere Observation System (AOS) mission currently scheduled for launch late in this decade. We will also investigate possible trends in PSC occurrence and composition over the entire CALIOP data record and through further comparisons with the Stratospheric Aerosol Measurement (SAM) II solar occultation PSC record from 1979-1989. Finally, we will validate the mountain-wave parameterization and PSC schemes used in the UM-UKCA (Unified Model coupled to the United Kingdom Chemistry and Aerosol module) CCM through detailed comparisons with earlier CALIOP PSC data products and those developed under this proposal.

CALIPSO↗
NASA NTRSDate not supplied

Faster Tropical Upper Stratospheric Upwelling is Driving Changes in Ozone Chemistry

Trends in N2O and the chlorofluorocarbons (CFCs) cause trends in O3 through changes in their reactive product gases, NOx and ClOx, but transport plays an important role because it controls the distribution of the long‐lived source gases that produce ozone‐destroying radicals. In this study we show that increased tropical upwelling 10‐5 hPa from 2013‐2021 has changed upper stratospheric (UpS) composition and shifted the balance of O3 loss processes. We use N2O, HNO3, NOx, temperature and O3 data from the Aura Microwave Limb Sounder (MLS) and the SCI‐Sat Atmospheric Chemistry Experiment Fourier Transport Spectrometer (ACE‐FTS) over a 16‐year period to show how changes in reactive nitrogen species affected gas phase ozone chemistry above 30 hPa between June 2013‐May 2021 compared to the previous 8 years, June 2005‐May 2013. We use 2 simulations of the Global Modeling Initiative (GMI) chemistry transport model (CTM), with and without time varying MERRA2 meteorology, to understand how dynamical changes during this 16‐yr period affected O3 through changes in loss via the NOx and ClOx cycles. We also identify the role that the quasi‐biennial oscillation (QBO) in tropical zonal winds plays in the UpS composition changes. We find large increases in tropical upwelling and poleward transport in the northern branch of the UpS transport circulation since 2013 that dramatically increased the abundance of the N2O and its odd nitrogen product gases, NOx and HNO3. O3 loss by NOx in the Arctic UpS increased due to dynamically driven composition change, explaining the observed weak O3 recovery in that region since 2005. The increased upwelling also drove decreases in tropical NOx, leading to increased tropical O3 from 12‐6 hPa.

middle atmosphere chemistry and composition↗
NASA NTRSDate not supplied

A Golden Era of PSC Observations From the A-Train By CALIOP and MLS

The fundamental role of polar stratospheric clouds (PSCs) in the depletion of stratospheric ozone is well established. Heterogeneous reactions on PSCs convert the stable chlorine reservoirs HCl and ClONO2 to chlorine radicals that destroy ozone catalytically. PSCs also prolong ozone depletion by delaying chlorine deactivation through the removal of gas-phase HNO3 and H2O by sedimentation of large PSC particles. There has been substantial recent progress in our understanding of PSC processes due to the long-term, vortex-wide observations from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar on the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite and the MLS (Microwave Limb Sounder) on the Aura satellite. The CALIOP observations provide unprecedented high spatial resolution information on particulate aerosol/PSC morphology and composition, while MLS provides complementary collocated measurements of gas-phase HNO3 and H2O, the major constituents of all PSC particles. The combined analyses of these datasets have enabled better PSC composition discrimination and provided valuable new insight into PSC formation processes and particle growth kinetics. The more than 17 years of CALIOP and MLS data have uniquely captured the primary aspects of the seasonal and multi-year variability of PSCs in the Arctic and Antarctic, enabling the development of a state-of-the-art reference PSC data record and climatology. In this presentation, we highlight the significant advances in our understanding achieved during this golden era of spaceborne PSC observations and identify remaining gaps in our knowledge that future spaceborne lidar missions may help resolve.

polar stratospheric clouds↗
NASA NTRS1973

The distribution of odd nitrogen in the lower stratosphere and possible perturbations caused by stratospheric air transport

In the lower stratosphere a significant production of odd nitrogen results from the reaction N2O + O(D-1) yields 2NO. Since the transport is relatively slow, odd nitrogen builds up with a maximum mixing ratio of 2 x 10 to the minus 8th power at 30 Km. Profiles of odd nitrogen, for different latitudes, winter and summer, are computed from one-dimensional transport models. Variations with latitude are small. Horizontal transport is therefore not believed to alter our results significantly. In order to evaluate the effect of odd nitrogen upon the ozone layer, NO(x) profiles are calculated. OH is here a key component, since it converts NO2 to HNO3. In the region where ozone is determined by chemistry rather than by transport (above 25 km), NO2 is found to be relatively abundant. The effect of stratospheric transport on the NO(x) distribution is shown to depend critically upon the height of emission. The effect increases by a factor of 5 or more for a change of flight level from 18 km to 23 km. This strong dependence should be duely considered when future stratospheric transport is discussed.

Isaksen, I. S. A.↗
NASA NTRS1973

Air pollution measurements from satellites

A study is presented on the remote sensing of gaseous and particulate air pollutants which is an extension of a previous report. Pollutants can be observed by either active or passive remote sensing systems. Calculations discussed herein indicate that tropospheric CO, CO2, SO2, NO2, NH3, HCHO, and CH4 can be measured by means of nadir looking passive systems. Additional species such as NO, HNO3, O3, and H2O may be measured in the stratosphere through a horizon experiment. A brief theoretical overview of resonance Raman scattering and resonance fluorescence is given. It is found that radiance measurements are most promising for general global applications, and that stratospheric aerosols may be measured using a sun occultation technique. The instrumentation requirements for both active and passive systems are examined and various instruments now under development are described.

Ludwig, C. B.↗
NASA NTRS1974

Diurnal variations of HOx and NOx in the stratosphere

The diurnal variations of odd hydrogen (OH, HO2, H2O2) and odd nitrogen compounds (NO, NO2, HNO3) are investigated by using a one-dimensional time-dependent model containing both chemistry and eddy transport. These variations are discussed in terms of relevant processes.-

Whitten, R. C.↗
NASA NTRS1974

Effect of aerosol emission on the inference of trace gas concentrations from limb radiance data

This note reports on an analysis of atmospheric emission spectra in the 10-12 micron region measured with a limb-oriented balloon-borne spectrometer. Data clearly show the existence of an additional feature at 10.8 microns which is probably due to measurement contamination from aerosols. The 10.8 micron emitter has a strong reducing effect on the HNO3 mixing ratio profile as determined by application of a symmetrical band shape model to the 10.8 spectral feature.

Remsberg, E. E.↗
NASA NTRS1975

Some aspects of the ozone-depletion problem in the stratosphere

A preliminary investigation of O3 depletion by NOx in the exhaust of an SST wake is presented. Initial calculations were made using a model employing a two-step chemistry mechanism consisting of an NOx catalytic cycle and assuming total NOx and the ratio NO/NO2 to be conserved. The results indicate O3 depletion in the wake much less severe than reported in earlier investigations which used a much larger reaction rate constant. Subsequent investigation revealed, however, that even the current O3 depletion rates appear too large. Because of the apparent deficiencies in the two-step chemical model, a model is presented with a more realistic chemical mechanism without the requirement for NO conservation. Results indicate that total NOx and initial NO/NO2 ratio play an important role in determining O3 depletion. Furthermore, only in the case of rather extreme concentrations of water vapor or unrealistically large photolysis rates is there any significant conversion of NOx to HNO3.

Gupta, R. N.↗
NASA NTRS1974

Measurements of trace constituents from atmospheric infrared emission and absorption spectra, a feasibility study

The feasibility of detecting eight trace constituents (CH4, HCl, HF, HNO3, NH3, NO, NO2 and SO2) against the rest of the atmospheric background at various altitudes from infrared emission and absorption atmospheric spectra was studied. Line-by-line calculations and observational data were used to establish features that can be observed in the atmospheric spectrum due to each trace constituent. Model calculations were made for experimental conditions which approximately represent state of the art emission and absorption spectrometers.

Goldman, A.↗
NASA NTRS1975

Stratospheric distributions of odd nitrogen and odd hydrogen in a two-dimensional model

A two-dimensional pole-to-pole chemical model of the stratosphere is developed which extends from 8 to 38 km in altitude. Atmospheric motions are simulated by mean vertical and meridional winds and eddy diffusion coefficients. Seasonally averaged distributions of important odd nitrogen (NO, NO2, and HNO3) and odd hydrogen (H, OH, HO2, H2O2) compounds are computed. Photodissociation of N2O leads to production of odd nitrogen in the stratosphere, and the odd nitrogen is ultimately removed by downward transport into the troposphere and by rain-out (modeled by a rain-out lifetime of 30 days below 8-km altitude). Results are presented for a quasi-steady state in which seasonal cycles repeat themselves. These results show significant latitudinal as well as vertical variations in the predicted species which emphasize the need for at least two dimensions in accurate stratospheric modeling. Computed concentrations are compared with observations when they exist.

Prinn, R. G.↗
NASA NTRS1975

Seasonal variations of NO and O3 at altitudes of 18.3 and 21.3 km

Nitric oxide and ozone concentrations have been measured in situ from a high-altitude research aircraft. Data which show the variations of NO and O3 with the time of year are presented for altitudes of 18.3 and 21.3 km. The extreme values of the observed NO concentrations at 21.3 km are 1.2 billion per cu cm in summer and 0.2 billion per cu cm in winter. At 18.3 km the extreme values are 1.6 billion per cu cm in summer and 0.1 billion per cu cm in winter. The smoothed NO seasonal data show a variation of about a factor of 2.5 at 21.3 km and a factor of 4 at 18.3 km. The ozone data show the generally expected magnitude and seasonal variation. We have used a photochemical model employing the measured ozone concentrations, the mean solar zenith angle, and seasonal HNO3 data reported by others to predict the seasonal NO variation at 20 km. The result is a summer-to-winter NO ratio of 2.5 which is in fair agreement with the observed ratios.

Loewenstein, M.↗