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At least 127 records · Page 7

Source gases: Concentrations, emissions, and trends

Source gases are defined as those gases that influence levels of stratospheric ozone (O3) by transporting species containing halogen, hydrogen, and nitrogen to the stratosphere. Examples are the CFC's, methane (CH4), and nitrous oxide (N2O). Other source gases that also come under consideration in an atmospheric O3 context are those that are involved in the O3 or hydroxyl (OH) radical chemistry of the troposphere. Examples are CH4, carbon monoxide (CO), and nonmethane hydrocarbons (NMHC's). Most of the source gases, along with carbon dioxide (CO2) and water vapor (H2O), are climatically significant and thus affect stratospheric O3 levels by their influence on stratospheric temperatures. Carbonyl sulphide (COS) could affect stratospheric O3 through maintenance of the stratospheric sulphate aerosol layer, which may be involved in heterogeneous chlorine-catalyzed O3 destruction. The previous reviews of trends and emissions of source gases, either from the context of their influence on atmospheric O3 or global climate change, are updated. The current global abundances and concentration trends of the trace gases are given in tabular format.

Fraser, Paul J.↗

Open-path tunable diode laser absorption for eddy correlation flux measurements of atmospheric trace gases

Biogenic emissions from and dry deposition to terrestrial surfaces are important processes determining the trace gas composition of the atmosphere. An instrument has been developed for flux measurements of gases such as CH4, N2O, and O3 based on the eddy correlation technique which combines trace gas fluctuation measurements with simultaneous windfield measurements. The instrument combines a tunable diode laser infrared light source with an open-path multipass absorption cell in order to provide the fast time response and short base pathlength required for the eddy correlation method. Initial field tests using the instrument to measure methane emissions from a local wetland demonstrate the capability for high precision eddy correlation flux measurements.

Anderson, Stuart M.↗

The potential impact on atmospheric ozone and temperature of increasing trace gas concentrations

The response of the atmosphere to emissions of chlorofluorocarbons (CFCs) and other chlorocarbons, and to increasing concentrations of other radiatively active trace gases such as CO2, CH4, and N2O is calculated by a coupled chemical-radiative transport one-dimensional model. It is shown that significant reductions in the ozone concentration and in the temperature are expected in the upper stratosphere as a result of increasing concentrations of active chlorine produced by photodecomposition of the CFCs. The ozone content is expected to increase in the troposphere, as a consequence of increasing concentrations of methane and nitrogen oxides. Due to enhanced greenhouse effects, the Earth's surface should warm up by several degrees. The amplitude and even the sign of future changes in the ozone column are difficult to predict as they are strongly scenario-dependent. An early detection system to prevent noticeable ozone changes as a result of increasing concentrations of source gases should thus be based on a continuous monitoring of the ozone amount in the upper stratosphere rather than on measurements of the ozone column only. Measurements of NOx, Clx, and HOx are also required for unambiguous trend detection and interpretation.

Brasseur, G.↗

PyroCbs from Australia Fires and its Impact Using Satellite Observations from CrIS and TROPOMI and Reanalysis Data

Pyrocumulonimbus (pyroCb) clouds are thunder clouds created by intense heat from the Earth’s surface. They are formed similarly to cumulonimbus clouds, but the intense heat that results in the vigorous updraft comes from fire, either large wildfires or volcanic eruptions. Australia’s unprecedented fire disasters at the end of 2019 to early 2020 emitted huge amounts of carbon monoxide (CO) and fire aerosol particles to the atmosphere, particularly during the pyroCb outbreak that occurred in southeast Australia between 29 December 2019 and 4 January 2020. It was estimated that at least 18 pyroCbs were generated during this episode, and some of them injected ice, smoke, and biomass burning gases above the local tropopause. An unprecedented abundance of H2O and CO in the stratosphere, and the displacement of background ozone (O3) and N2O from rapid ascent of air from the troposphere and lower stratosphere were found from satellite observations. Some other studies also found that the fire emissions and their long-range transport resulted in stratospheric aerosol, temperature, and O3 anomalies after the 2020 Australian bushfires and altered the Antarctic ozone and vortex, posing great impact to local air quality and climate change. Further study on the atmospheric thermodynamic status of atmosphere associated with these pyroCbs, and the change of the cloud properties and trace gases during this unprecedented Australia fires will be made using a new single Field of View (SFOV) Sounder Atmospheric Products (SiFSAP). SiFSAP was developed by NASA using the Cross-track Infrared Sounder (CrIS) and Advanced Technology Microwave Sounder (ATMS) onboard SNPP and JPSS-1, and will soon be available to the public at NASA DAAC. Since this product has a spatial resolution of 15 km at nadir, which is better than most global weather and climate models and other current operational sounding products, a process-oriented analysis of the dynamic transport of CO and fire plumes during this unprecedented fire disasters will be made in this study. Based on a Principal Component Radiative Transfer Model (PCRTM) and an optimized estimation retrieval algorithm, a simultaneously retrieval is made using the whole spectral information measured by CrIS, and the derived SiFSAP include temperature, water vapor, trace gases (such as O3, CO2, CO, CH4 and N2O), cloud properties and surface properties. Use of ATMS together with CrIS allows SiFSAP to get accurate retrieval products under thick pyroCb conditions, and an algorithm to detect pyroCb based on the hyperspectral infrared sounder spectrum from CrIS will be developed and verified. In addition to SiFSAP sounding products, other products like CO, O3, NO2 from TROPOMI, O3 from OMPS will be used for retrospective analysis. The wind fields from the NASA’s Modern-Era Retrospective Analysis for Research and Applications Version-2 (MERRA-2) and ERA5 will be used to characterize the transport, and the SiFSAP temperature and water vapor profiles within and around pyroCbs will be compared with MERRA-2 and ERA5 products.

Xiaozhen (Shawn) Xiong↗

An analysis of aircraft exhaust plumes form accidental encounters

An analysis of data obtained during the second Airborne Arctic Stratospheric Expedition (AASE-II) was made with emphasis on aircraft exhaust plumes accidentally encountered during the mission. Twenty spikes were found with peak NO(y) increments greater than or equal to 1 ppbv. The examination of CO and CO2 indicated that there was only one NO(y) spike having clearly corresponding spikes of both CO and CO2 and another four with unambigious CO2 spikes. No significant increases were found for CH4 and N2O for these 5 spikes. The ratio of the excess CO2 and NO(y) compares well with the ratio of published subsonic aircraft emission indices. The study of the selected spikes from the DC-8 and another two spikes observed during other missions shows that the odd nitrogen other than NO(x) accounts for a very small percentage of the NO(y) increase associated with the observed spikes.

Zheng, J.↗

CRN Modeling of Ammonia RQL Combustion using a Partially-Stirred Reactor Approach

Ammonia is a promising alternative to hydrogen with high energy density and favorable storage and transport characteristics. However low flammability and a propensity for high nitrogen oxide (NOx) emissions make direct utilization challenging. Recently, two-stage rich-quench-lean (RQL) combustion strategies have shown promise in achieving low NOx emissions with ammonia. In this approach, the rich stage serves to oxidize a portion of the fuel, while thermally decomposing as much of the remaining ammonia as possible, generating hydrogen. In the second (lean) stage, air is rapidly introduced, burning out the hydrogen and residual ammonia. Two-stage RQL combustion of ammonia has been investigated in the open literature both experimentally and numerically. In general, idealized chemical reactor network (CRN) models predict NOx concentrations below that of 2D/3D computational fluid dynamics models and experiments. The primary drivers of these discrepancies may be largely attributed to finite rate mixing non-adiabatic operation. The typical CRN model is comprised of a perfectly-stirred-reactor (PSR), followed by a plug-flow-reactor (PFR), meant to represent the flame, and post-flame zones, respectively. In the two-stage RQL approach two PSR-PFR networks are arranged sequentially, corresponding to the rich and lean stages, with secondary air injection in between. In the authors’ past work, this arrangement has demonstrated the significant sensitivity of exit NOx to the rich stage equivalence ratio, while the amount of secondary air injection was shown to be less critical. In this paper, the CRN model is extended to (1) include the impacts of heat loss and (2) utilize a partially-stirred-reactor (PaSR) approach to study the impacts of mixing on emissions performance. Varying amounts of heat loss are applied to the rich relaxation zone to understand emissions performance and changes to optimization of equivalence ratio and residence time. Premixed and non-premixed configurations are considered in the rich stage PaSR, with varying degrees of mixing intensity to study the interaction between mixing, transport, and kinetic timescales. Critically, the impact of mixing between hot products and secondary air injection is studied to understand practical injector needs. Results show unburnt ammonia leaving the rich stage as a primary contributor to NOx emissions – driven both by increased heat loss and reduced mixing rates. Furthermore, heat losses have shown to create conditions which are conducive to increased N2O formation in the lean stage. The results of this study will be considered in the context of developing optimized two-stage RQL combustors for ammonia..

advanced gas turbines↗

Decomposition of NO studied by infrared emission and CO laser absorption

A diagnostic technique for monitoring the concentration of NO using absorption of CO laser radiation was developed and applied in a study of the decomposition kinetics of NO. Simultaneous measurements of infrared emission by NO at 5.3 microns were also made to validate the laser absorption technique. The data were obtained behind incident shocks in NO-N2O-Ar (or Kr) mixtures, with temperatures in the range 2400-4100 K. Rate constants for dominant reactions were inferred from comparisons with computer simulations of the reactive flow.

Hanson, R. K.↗

Decomposition of NO studied by infrared emission and CO laser absorption

A diagnostic technique for monitoring the concentration of NO using absorption of CO laser radiation has been developed and applied in a study of the decomposition kinetics of NO. Simultaneous measurements of infrared emission by NO at 5.3 microns were also made to validate the laser absorption technique. The data were obtained behind incident shocks in NO-N2O-Ar (or Kr) mixtures, with temperatures in the range 2400-4100 K. The rate constant for the dominant reaction of O and NO to yield N and O2 was inferred from comparisons with computer simulations of the reactive flow.

Hanson, R. K.↗

Sensitivity analysis of upwelling thermal radiance in presence of clouds

Total upwelling radiance at the top of the atmosphere is evaluated theoretically in the presence of clouds. The influence of cloud heights, thicknesses and different cloud covers on the upwelling radiance is also investigated. The characteristics of the two cloud types considered in this study closely correspond to altocumulus and cirrus with the cloud emissivity as a function of its liquid water (or ice) content. For calculation of the integrated transmittance of atmospheric gases such as, H2O, CO2, O3, and N2O, the Quasi Random Band (QRB) model approach is adopted. Results are obtained in three different spectral ranges and are compared with the clearsky radiance results. It is found that the difference between the clearsky and cloudy radiance increases with increasing cloud height and liquid water content. This difference also decreases as the surface temperature approaches the value of the cloud top temperature.

Subramanian, S. V.↗

The cryogenic limb array etalon spectrometer (CLAES) on UARS - Experiment description and performance

The design and the performance of the cryogenic limb array spectrometer (CLAES) aboard the NASA Upper Atmosphere Research Satellite are discussed. CLAES measures altitude profiles of temperature, pressure, O3, H2O, CH4, N2O, NO, NO2, N2O5, HNO3, ClONO2, HCl, CFC 11, CFC 12, and aerosol absorption coefficients for atmospheric layer between 10 and 60 km. Examples of atmospheric spectral emission profiles for a number of constituents are presented as well as responsivity and noise parameters.

Roche, A. E.↗

The atmospheric lifetime experiment. I - Introduction, instrumentation, and overview

The Atmospheric Lifetime Experiment is designed to determine accurately the atmospheric concentrations of the four halocarbons CFCl3, CF2Cl2, CCl4, and CH3CCl3, and also of N2O with emphasis on measurement of their long-term trends in the atmosphere. Comparison of these concentrations and trends for the four halocarbons with estimates of their industrial emission rates then enables calculations of their global circulation rates and globally averaged atmospheric lifetimes. The experiment utilizes automated dual-column electron-capture gas chromatographs which sample the background air about 4 times daily at the following globally distributed sites: Adrigole, Ireland, Cape Meares, Oregon; Ragged Point, Barbados; Point Matatula, American Samoa, and Cape Grim, Tasmania. The climatology of these 'clean air' sites and their ability to describe the global air mass are reviewed. The instrumentation and methods for data acquisition and processing are then described. An overview of the data obtained and the trends derived during the 3-year period from July 1978 through June 1981 for each of the five species being measured is presented.

Prinn, R. G.↗

Remote Sensing of Spatial Distributions of Greenhouse Gases in the Los Angeles Basin

The Los Angeles air basin is a significant anthropogenic source of greenhouse gasses and pollutants including CO2, CH4, N2O, and CO, contributing significantly to regional and global climate change. Recent legislation in California, the California Global Warning Solutions Act (AB32), established a statewide cap for greenhouse gas emissions for 2020 based on 1990 emissions. Verifying the effectiveness of regional greenhouse gas emissions controls requires high-precision, regional-scale measurement methods combined with models that capture the principal anthropogenic and biogenic sources and sinks. We present a novel approach for monitoring the spatial distribution of greenhouse gases in the Los Angeles basin using high resolution remote sensing spectroscopy. We participated in the CalNex 2010 campaign to provide greenhouse gas distributions for comparison between top-down and bottom-up emission estimates.

atmospheric remote sensing↗

Remote Sensing of Spatial Distributions of Greenhouse Gases in the Los Angles Basin

The Los Angeles air basin is a significant anthropogenic source of greenhouse gases and pollutants including CO2, CH4, N2O, and CO, contributing significantly to regional and global climate change. Recent legislation in California, the California Global Warming Solutions Act (AB32), established a statewide cap for greenhouse gas emissions for 2020 based on 1990 emissions. Verifying the effectiveness of regional greenhouse gas emissions controls requires high-precision, regional-scale measurement methods combined with models that capture the principal anthropogenic and biogenic sources and sinks. We present a novel approach for monitoring the spatial distributions of greenhouse gases in the Los Angeles basin using high resolution remote sensing spectroscopy. We participated in the CalNex 2010 campaign to provide greenhouse gas distributions for comparison between top-down and bottom-up emission estimates.

Los Angeles air basin↗

The MIPAS balloon borne trace constitutent experiment

A novel cryogenic Fourier transform spectrometer (FTS) has been developed for limb emission measurements in the mid IR-region from balloon-borne platforms. The FTS is a rapid scanning interferometer using a modified Michelson arrangement which allows a spectral resolution of 0.04 cm(exp -1) to be achieved. Solid carbon-dioxide cooling of the spectrometer and liquid-helium cooling of the detectors provide adequate sensitivity. The line of sight can be stabilized in terms of azimuth and elevation. A three-mirror off-axis telescope provides good vertical resolution and straylight rejection. Calibration is performed by high elevation and internal blackbody measurements. Four balloon flights were performed, two of them during spring turn-around 1989 and 1990 over mid-latitudes (Aire sur L'Adour, France, 44 deg N) and two near the northern polar circle in winter 1992 (Esrange, Sweden, 68 deg N). Limb emission spectra were collected from 32 km to 39 km floating altitudes covering tangent heights between the lower troposphere and the floating altitude. The trace gases CO2, H2O, O3, CH4, N2O, HNO3, N2O5, ClONO2, CF2Cl2, CFCl3, CHF2Cl, CCl4, and C2H6 have been identified in the measured spectra. The 1989 data have been analyzed to retrieve profiles of O3, HNO3, CFCl3 and CF2Cl2. The flights over Kiruna have provided the first ever reported profile measurements of the key reservoir species ClONO2 and N2O5 inside the polar vortex.

Oelhaf, H.↗

Atmospheric Beacons of Life from Exoplanets Around G and K Stars

The current explosion in detection and characterization of thousands of extrasolar planets from the Kepler mission, the Hubble Space Telescope, and large ground-based telescopes opens a new era in searches for Earth-analog exoplanets with conditions suitable for sustaining life. As more Earth-sized exoplanets are detected in the near future, we will soon have an opportunity to identify habitale worlds. Which atmospheric biosignature gases from habitable planets can be detected with our current capabilities? The detection of the common biosignatures from nitrogen-oxygen rich terrestrial-type exoplanets including molecular oxygen (O2), ozone (O3), water vapor (H2O), carbon dioxide (CO2), nitrous oxide (N2O), and methane (CH4) requires days of integration time with largest space telescopes, and thus are very challenging for current instruments. In this paper we propose to use the powerful emission from rotational-vibrational bands of nitric oxide, hydroxyl and molecular oxygen as signatures of nitrogen, oxygen, and water rich atmospheres of terrestrial type exoplanets "highlighted" by the magnetic activity from young G and K main-sequence stars. The signals from these fundamental chemical prerequisites of life we call atmospheric "beacons of life" create a unique opportunity to perform direct imaging observations of Earth-sized exoplanets with high signal-to-noise and low spectral resolution with the upcoming NASA missions.

exoplanets↗

Data from: Coupled machine learning-ecosystem ensemble models substantially improve predictions of nitrous oxide (N 2 O) fluxes from US croplands

Nitrous oxide (N₂O) is a potent and persistent greenhouse gas, with rising atmospheric concentrations driven in part by inefficient use of synthetic nitrogen (N) fertilizers in agriculture. Predicting soil N₂O emissions is challenging due to high spatial and temporal variability arising from complex soil biogeochemical processes. Process-based ecosystem models and standalone machine learning (ML) approaches without extensive site-specific calibration often miss high emission episodes. Here, we show how an Ensemble Modeling System (EMS) based on outputs from an ensemble of ecosystem models coupled to an ensemble of ML models can improve predictions and understanding of N2O fluxes from US cropland. Trained and validated on approximately 12,000 N2O chamber measurements at 17 U.S. Midwest sites (six crops, 35 management practices), the EMS accurately predicted daily fluxes of N2O at both training (R² = 0.84, RMSE = 16.4 g N ha⁻¹ d⁻¹) and held-out testing sites (R² = 0.84, RMSE = 6.2 g N ha⁻¹ d⁻¹). Analyses identified six dominant N₂O drivers: soil organic carbon (SOC), NH₄⁺, NO₃⁻, water-filled pore space (WFPS), soil temperature, and biomass production. Wet, warm soils produced large N₂O peaks only with sufficient SOC and mineral N; in low-SOC soils, fluxes remained low. Incorporating these drivers into process-based models might significantly improve their predictive capacity. The EMS demonstrates a strong potential to predict N₂O fluxes at unseen sites, enabling more reliable regional inventories, improved gap-filling where measurements are sparse, and enhanced understanding of mechanisms to advance targeted mitigation strategies in food, feed, and bioenergy crops.

agricultural sciences↗

Global climate changes as forecast by Goddard Institute for Space Studies three-dimensional model

The global climate effects of time-dependent atmospheric trace gas and aerosol variations are simulated by NASA-Goddard's three-dimensional climate model II, which possesses 8 x 10-deg horizontal resolution, for the cases of a 100-year control run and three different atmospheric composition scenarios in which trace gas growth is respectively a continuation of current exponential trends, a reduced linear growth, and a rapid curtailment of emissions due to which net climate forcing no longer increases after the year 2000. The experiments begin in 1958, run to the present, and encompass measured or estimated changes in CO2, CH4, N2O, chlorofluorocarbons, and stratospheric aerosols. It is shown that the greenhouse warming effect may be clearly identifiable in the 1990s.

Hansen, J.↗

Life-Cycle Emissions and Human Health Implications of Multi-Input, Multi-Output Biorefineries

To meaningfully broaden the supply of fuels for the transportation sector, biofuel production must be scaled up and this requires a wider array of biomass feedstocks, including agricultural residues and organic waste. Rather than pursuing conversion of lignocellulosic biomass to fuels and anaerobic digestion of wastes as separate pathways, there are economic and environmental advantages associated with integrating these processes in a single facility. However, existing research rarely goes beyond carbon footprints in quantifying the effects of such a shift in bioenergy production. In addition to CO2, CH4, and N2O, this study explores the life-cycle air pollution (NH3, volatile organic compounds, NOx, SO2, and PM2.5), marine eutrophication, acidification, and local external cost implications of biorefineries capable of taking in crop residues, food waste, and manure to produce liquid fuel, electricity, and/or other options such as renewable natural gas (RNG), hydrogen, bioplastics, and protein-rich livestock feed. Relative to a single-input, single-output baseline, biorefineries integrated with organic waste codigestion to coproduce electricity or RNG can reduce life-cycle CO2-equivalent emissions by 84-149%, and the monetized external impacts across all scenarios range from $1.07/gallon to -$0.75/gallon ethanol.

Air pollution↗