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At least 109 records · Page 6

Nitrous oxide in the tropical middle atmosphere, observed by ground-based mm-wave spectrometry

Measurements of stratospheric N2O were made from Mauna Kea in Hawaii in June 1983, and in May and June 1986, by observing thermal emission of the molecule in a rotational transition at about 1 mm wavelength. Analyses of the data yield altitude profiles in the middle and upper stratosphere. Useful measurements of N2O may be made in one to two hours. The N2O profiles agree reasonably well with model predictions and with published satellite data, though significantly more N2O is reported near the stratopause than shown by the satellite measurement, and significantly more N2O in the middle stratosphere than in one of the models. The discrepancy between these data and the satellite measurement may be due in part to variations induced by the solar cycle.

Connor, Brian J.↗

Mechanistic insights into N 2 O formation as a side product in NH 3 -SCR over small pore Cu-zeolites

Here, the present contribution provides clarity to N 2 O formation mechanisms and key influencing factors during low temperature NH 3 -SCR, with the goal of enabling the rational design of advanced SCR catalysts with low greenhouse gas impact. By studying more than 50 small pore Cu-exchanged zeolite SCR catalyst samples, including model catalysts synthesized in our laboratories and state-of-the-art industrial catalysts, we explored a wide range of factors affecting N 2 O formation. These factors included Cu loading, support Si/Al ratio, support topology, catalyst aging, reaction temperature and reactant feed composition effects. We probed N 2 O formation under both steady-state SCR, and during NH 4 NO 3 decomposition via temperature programmed desorption (TPD). Finally, we used DFT to probe energetics of possible N 2 O formation pathways. Based on these studies, we confirm that low temperature N 2 O formation occurs via multiple reaction pathways that all involve NH 4 NO 3 and are supported by Cu moieties that facilitate in-situ NO oxidation to NO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Infrared spectroscopy of the lower stratosphere with a balloon-borne cryogenic Fourier spectrometer

The IR limb emission of the lower stratosphere has been measured using a balloon-borne liquid nitrogen-cooled Michelson interferometer with liquid helium-cooled Si:Ga detectors. Portions of the thermal emission spectrum have been recorded between 650 and 2000/cm with an unapodized spectral resolution of 0.03/cm. This is the highest spectral resolution limb emission thus far obtained. A preliminary description is given of these data along with a discussion of the significant features. Species identified to date include CO2, O3, CFCl3, CF2Cl2, H2O, CH4, HNO3, N2O, NO2, and ClONO2. A tentative identification is made for NO, representing the first direct spectroscopic detection of NO in emission.

Kunde, Virgil G.↗

Increasing anthropogenic methane emissions arise equally from agricultural and fossil fuel sources

Climate stabilization remains elusive, with increased greenhouse gas concentrations already increasing global average surface temperatures 1.1°C above pre-industrial levels (World Meteorological Organization 2019). Carbon dioxide (CO2) emissions from fossil fuel use, deforestation, and other anthropogenic sources reached ~ 43 billion metric tonnes in 2019 (Friedlingstein et al 2019, Jackson et al 2019). Storms, floods, and other extreme weather events displaced a record 7 million people in the first half of 2019 (IDMC 2019). When global mean surface temperature four million years ago was 2°C–3°C warmer than today (a likely temperature increase before the end of the century), ice sheets in Greenland and West Antarctica melted and parts of East Antarctica’s ice retreated, causing sea levels to rise 10–20 m (World Meteorological Organization 2019). Methane (CH4) emissions have contributed almost one quarter of the cumulative radiative forcings for CO2, CH4, and N2O (nitrous oxide) combined since 1750 (Etminan et al 2016). Although methane is far less abundant in the atmosphere than CO2, it absorbs thermal infrared radiation much more efficiently and, in consequence, has a global warming potential (GWP) ~86 times stronger per unit mass than CO2 on a 20-year timescale and 28- times more powerful on a 100-year time scale (IPCC 2014). Global average methane concentrations in the atmosphere reached ~1875 parts per billion (ppb) at the end of 2019, more than two-and-a-half times preindustrial levels (Dlugokencky 2020). The largest methane sources include anthropogenic emissions from agriculture, waste, and the extraction and use of fossil fuels as well as natural emissions from wetlands, freshwater systems, and geological sources (Kirschke et al 2013, Saunois et al 2016a, Ganesan et al 2019). Here, we summarize new estimates of the global methane budget based on the analysis of Saunois et al (2020) for the year 2017, the last year of the new Global Methane Budget and the most recent year data are fully available. We compare these estimates to mean values for the reference ‘stabilization’ period of 2000–2006 when atmospheric CH4 concentrations were relatively stable. We present data for sources and sinks and provide insights for the geographical regions and economic sectors where emissions have changed the most over recent decades.

fossil fuel sources↗

Relative rates of nitric oxide and nitrous oxide production by nitrifiers, denitrifiers, and nitrate respirers

An account is given of the atmospheric chemical and photochemical effects of biogenic nitric and nitrous oxide emissions. The magnitude of the biogenic emission of NO is noted to remain uncertain. Possible soil sources of NO and N2O encompass nitrification by autotropic and heterotropic nitrifiers, denitrification by nitrifiers and denitrifiers, nitrate respiration by fermenters, and chemodenitrification. Oxygen availability is the primary determinant of these organisms' relative rates of activity. The characteristics of this major influence are presently investigated in light of the effect of oxygen partial pressure on NO and N2O production by a wide variety of common soil-nitrifying, denitrifying, and nitrate-respiring bacteria under laboratory conditions. The results obtained indicate that aerobic soils are primary sources only when there is sufficient moisture to furnish anaerobic microsites for denitrification.

Anderson, I. C.↗

Investigation of nitric oxide decomposition in the temperature range 2500-4100 K

The decomposition of nitric oxide has been studied in the temperature range 2500-4100 K using a shock-tube technique. The principle result of the study was the determination of the rate constant (k) for the reaction O + NO yields N + O2. Mixtures of NO and N2O diluted in argon or krypton were heated by incident shock waves and the infrared emission from the fundamental vibration-rotation band of NO at 5.3 microns was used to monitor the time-varying NO concentration. The experimental values of k are fit closely by the expression k = (2.36 times 10 to the 9th power) x T x exp(-38,640/RT) cm cu/mole-sec, which also provides a good fit to previous data at higher and lower temperatures.

Flower, W. L.↗

Options to Accelerate Ozone Recovery: Ozone and Climate Benefits

The humankind or anthropogenic influence on ozone primarily originated from the chlorofluorocarbons and halons (chlorine and bromine). Representatives from governments have met periodically over the years to establish international regulations starting with the Montreal Protocol in 1987, which greatly limited the release of these ozone-depleting substances (DDSs). Two global models have been used to investigate the impact of hypothetical reductions in future emissions of ODSs on total column ozone. The investigations primarily focused on chlorine- and bromine-containing gases, but some computations also included nitrous oxide (N2O). The Montreal Protocol with ODS controls have been so successful that further regulations of chlorine- and bromine-containing gases could have only a fraction of the impact that regulations already in force have had. if all anthropogenic ODS emissions were halted beginning in 2011, ozone is calculated to be higher by about 1-2% during the period 2030-2100 compared to a case of no additional ODS restrictions. Chlorine- and bromine-containing gases and nitrous oxide are also greenhouse gases and lead to warming of the troposphere. Elimination of N 20 emissions would result in a reduction of radiative forcing of 0.23 W/sq m in 2100 than presently computed and destruction of the CFC bank would produce a reduction in radiative forcing of 0.005 W/sq m in 2100. This paper provides a quantitative way to consider future regulations of the CFC bank and N 20 emissions

Fleming, E. L.↗

A comprehensive and synthetic dataset for global, regional, and national greenhouse gas emissions by sector 1970–2018 with an extension to 2019

To track progress towards keeping global warming well below 2 °C or even 1.5 °C, as agreed in the Paris Agreement, comprehensive up-to-date and reliable information on anthropogenic emissions and removals of greenhouse gas (GHG) emissions is required. Here we compile a new synthetic dataset on anthropogenic GHG emissions for 1970–2018 with a fast-track extension to 2019. Our dataset is global in coverage and includes CO 2 emissions, CH 4 emissions, N 2 O emissions, as well as those from fluorinated gases (F-gases: HFCs, PFCs, SF 6 , NF 3 ) and provides country and sector details. We build this dataset from the version 6 release of the Emissions Database for Global Atmospheric Research (EDGAR v6) and three bookkeeping models for CO 2 emissions from land use, land-use change, and forestry (LULUCF). We assess the uncertainties of global greenhouse gases at the 90 % confidence interval (5th–95th percentile range) by combining statistical analysis and comparisons of global emissions inventories and top-down atmospheric measurements with an expert judgement informed by the relevant scientific literature. We identify important data gaps for F-gas emissions. The agreement between our bottom-up inventory estimates and top-down atmospheric-based emissions estimates is relatively close for some F-gas species (~ 10 % or less), but estimates can differ by an order of magnitude or more for others. Our aggregated F-gas estimate is about 10 % lower than top-down estimates in recent years. However, emissions from excluded F-gas species such as chlorofluorocarbons (CFCs) or hydrochlorofluorocarbons (HCFCs) are cumulatively larger than the sum of the reported species. Using global warming potential values with a 100-year time horizon from the Sixth Assessment Report by the Intergovernmental Panel on Climate Change (IPCC), global GHG emissions in 2018 amounted to 58 ± 6.1 GtCO 2 eq. consisting of CO 2 from fossil fuel combustion and industry (FFI) 38 ± 3.0 GtCO 2 , CO 2 -LULUCF 5.7 ± 4.0 GtCO 2 , CH 4 10 ± 3.1 GtCO 2 eq., N2O 2.6 ± 1.6 GtCO 2 eq., and F-gases 1.3 ± 0.40 GtCO 2 eq. Initial estimates suggest further growth of 1.3 GtCO 2 eq. in GHG emissions to reach 59 ± 6.6 GtCO 2 eq. by 2019. Our analysis of global trends in anthropogenic GHG emissions over the past 5 decades (1970–2018) highlights a pattern of varied but sustained emissions growth. There is high confidence that global anthropogenic GHG emissions have increased every decade, and emissions growth has been persistent across the different (groups of) gases. There is also high confidence that global anthropogenic GHG emissions levels were higher in 2009–2018 than in any previous decade and that GHG emissions levels grew throughout the most recent decade. While the average annual GHG emissions growth rate slowed between 2009 and 2018 (1.2 % yr –1 ) compared to 2000–2009 (2.4 % yr –1 ), the absolute increase in average annual GHG emissions by decade was never larger than between 2000–2009 and 2009–2018. Our analysis further reveals that there are no global sectors that show sustained reductions in GHG emissions. There are a number of countries that have reduced GHG emissions over the past decade, but these reductions are comparatively modest and outgrown by much larger emissions growth in some developing countries such as China, India, and Indonesia. There is a need to further develop independent, robust, and timely emissions estimates across all gases. As such, tracking progress in climate policy requires substantial investments in independent GHG emissions accounting and monitoring as well as in national and international statistical infrastructures. The data associated with this article (Minx et al., 2021) can be found at https://doi.org/10.5281/zenodo.5566761.

54 ENVIRONMENTAL SCIENCES↗

Hyperspectral Radiatve Transfer Modeling and its Applications

We will describe a fast radiative transfer model that is specifically designed for hyperspectral remote sensing applications. The fast radiative transfer model is capable of performing efficient and accurate calculations under cloudy condition and in the presence of solar radiations. The model uses a Principal Component Analysis to speed up computational speed. The PCRTM model is capable of simulating top of atmospheric radiance or reflectance spectral from 50 wavenumber to 30000 wavenumber. The PCRTM has a very good accuracy relative to reference line-by-line radiative transfer models and it saves orders of magnitude computational time. We will show comparisons of the PCRTM model to AIRS, CrIS, IASI, NAST-I, and SCIAMACHY data. We will further show results of applying the PCRTM retrieval algorithm to these remote sensing data to retrieve atmospheric temperature and moisture profiles, CO2, CO, CH4, N2O, and O3 profiles, cloud optical depth, size, phase, and height. Surface properties such as surface emissivity spectra and surface skin temperatures are also retrieved simultaneously.

X Liu↗

Forward and Inverse Models for Satellite Remote Sensors using Principal Component Analysis

Satellite remote sensors such as AIRS on Aqua, CrIS on S-NPP, NOAA20 and JPSS-2, IASI on Metop A, B, and C make millions of observations each day with thousands of spectral channels for each observation; this poses challenges for efficiently inversion of the inherently large dataset as needed to retrieve atmospheric and surface properties. This presentation will illustrate the use of Principal Component Analysis (PCA) to speed up radiative transfer forward model calculations and to stabilize the inversion algorithms. A Principal Component-based radiative transfer model (PCRTM) developed at NASA Langley Research Center can simulate top of atmosphere (TOA) radiance or reflectance spectra from 50 cm-1 to 50000 cm-1 (200 m to 0.20 m quickly and accurately. PCRTM demonstrated very high accuracy relative to reference line-by-line radiative transfer models and it saves orders of magnitude computational time. Examples of the PCRTM model developed for hyperspectral sensors such as AIRS, CrIS, IASI, NAST-I, SHIS, CPF, TEMPO, SBG, OMI, and SCIAMACHY will be presented. In addition to using the PCRTM as forward model, the NASA Langley developed inversion algorithm also uses PCA to compress the state vector into a compressed dimension to speed up and stabilize the inversion process. Examples of retrieved atmospheric temperature, water vapor, CO2, CO, CH4, N2O, and O3 profiles, cloud properties (optical depth, size, phase, and height), and surface properties (surface emissivity spectra and skin temperatures) will be presented. This algorithm is being transitioned to the NASA Sounder SIPS and NASA's Goddard Earth Sciences Data and Information Services Center (GES DISC).

forward model↗

Infrared measurements of column abundances of several trace gases in the Antarctic atmosphere

Atmospheric emission measurements were made in 1978 from an LC 130 aircraft from Point Mugu, CA, to McMurdo Station, Antarctica, and from McMurdo over the Antarctic continent on several different flights. These included a number of flights over the South Pole. In December 1980, infrared solar spectra were obtained from the ground at South Pole Station. Infrared solar spectra were also obtained from South Pole during late November and early December of 1986. These latter measurements were extended to cover additional spectral regions to obtain column densities of a number of additional constituents. The results obtained from these measurement series are reviewed and, where measurements were made during both periods, compared. Spectral absorption or emission features due to HNO3, NO, NO2, HCl, (H-16)2O, (H-18)2O, HDO, CH4, and N2O were used to obtain data on the total column abundances for these compounds.

Murcray, F. J.↗

Remote sensing of the troposphere by infrared emission spectroscopy

This paper describes the concept of a cryogenic IR imaging Fourier transform spectrometer, called the Tropospheric Emission Spectrometer (TES), designed for observations of the troposphere and lower stratosphere from a near-earth orbit, using natural thermal emission and reflected sunlight. The principal molecular species to be measured by TES are O3, CO, CO2, N2O, H2O, H2O2, NO, NO2, HNO3, NH3, CH4, C2H6, C2H2, SO2, COS, CFCl3, and CF2Cl2. The TES is scheduled for a launch on the second polar platform of the Earth Observing System in 1998.

Beer, Reinhard↗

Validation of the Radiometric Stability of the Atmospheric Infrared Sounder

It has been widely accepted that an infrared sounder in low polar orbit is capable of producing climate quality data, if the spectral brightness temperatures have instrumental trends of less than 10 mK/yr. Achieving measurement stability at this level is not only very demanding of the design of the instrument, it is also pushes the state of art of measuring on orbit what stability is actually achieved. We discuss this using Atmospheric Infrared Sounder (AIRS) L1B data collected between 2002 and 2011. We compare the L1B brightness temperature observed in cloud filtered night tropical ocean spectra (obs) to the brightness temperature calculated based on the known surface emissivity, temperature and water vapor profiles from the ECMWF ReAnalysis (ERA) and the growth rates of CO2, N2O and Ozone. The trend in (obs-calc) is a powerful tool for the evaluation of the stability of the 2378 AIRS channels. We divided the channels into seven classes: All channels which sound in the stratosphere (at pressure levels below 150 hPa), 14 micron CO2 sounding, 4 micron CO2 P-branch sounding, 4 micron CO2 R-branch sounding, water vapor sounding, shortwave surface sounding and longwave surface sounding. The peak in the weighting function at 1050 hPa separates sounding and surface channels. The boundary between shortwave and longwave is 5 microns. Except for the stratosphere sounding channels, the remaining six groups have (obs-calc) trends of less than 20 mK/yr. The longwave surface channels have trends of 2 mK/yr, significantly less than the 8 mK/yr trend seem in the shortwave window channels. Based on the design of the instrument, trends within a group of channels should be the same. While the longwave and shortwave trends are less than the canonical 10 mK/yr, the larger trend in the shortwave channels could be an artifact of using the pre-launch determined calibration coefficients. This is currently under evaluation. The trend in (obs-calc) for the non-surface sounding channels, in particular for stratosphere sounding and upper tropospheric water channels, is dominated by artifacts created in calc, most likely due to changes in the ERA Ozone and water vapor. Based on this argument the best estimate of the trend for the channels within a channel group is given by the surface sensitive channels within the group. Based on this consideration we estimated the trend of all AIRS longwave channels as 2 mK/yr, while the shortwave channels have a trend of 8 mK/yr.

CO2↗

Thermal emission spectroscopy of the middle atmosphere

The general objective of this research is to obtain, via remote sensing, simultaneous measurements of the vertical distributions of stratospheric temperature, ozone, and trace constituents that participate in the catalytic destruction of ozone (NO(sub y): NO, NO2, NO3, HNO3, ClONO2, N2O5, HNO4; Cl(sub x): HOCl), and the source gases for the catalytic cycles (H2O, CH4, N2O, CF2Cl2, CFCl3, CCl4, CH3Cl, CHF2Cl, etc.). Data are collected during a complete diurnal cycle in order to test our present understanding of ozone chemistry and its associate catalytic cycles. The instrumentation employed is an emission-mode, balloon-borne, liquid-nitrogen-cooled Michelson interferometer-spectrometer (SIRIS), covering the mid-infrared range with a spectral resolution of 0.020 cm(exp -1). Cryogenic cooling combined with the use of extrinsic silicon photoconductor detectors allows the detection of weak emission features of stratospheric gaseous species. Vertical distributions of these species are inferred from scans of the thermal emission of the limb in a sequence of elevation angles. The fourth SIRIS balloon flight was carried out from Palestine, Texas on September 15-16, 1986 with 9 hours of nighttime data (40 km). High quality data with spectral resolution 0.022 cm(exp -1), were obtained for numerous limb sequences. Fifteen stratospheric species have been identified to date from this flight: five species from the NO(sub y) family (HNO3, NO2, NO, ClONO2, N2O5), plus CO2, O3, H2O, N2O, CH4, CCl3F, CCl2F2, CHF2Cl, CF4, and CCl4. The nighttime values of N2O5, ClONO2, and total odd nitrogen have been measured for the first time, and compared to model results. Analysis of the diurnal variation of N2O5 within the 1984 and 1986 data sets, and of the 1984 ClONO2 measurements, were presented in the literature. The demonstrated ability of SIRIS to measure all the major NO(sub y) species, and therefore to determine the partitioning of the nitrogen family over a continuous diurnal cycle, is a powerful tool in the verification and improvement of photochemical modeling.

Kunde, V. G.↗

Electric discharges in air - Near infrared emission spectrum.

The emission from glow discharges in flowing air has been investigated in the 1- to 5-micron wavelength region with a vacuum spectrometer. Most of the spectral features observed in the pressure range of .5 to 10 torr are identified, including atomic lines of OI, NI, and HI and molecular bands of N2, NO, N2O, CO2, and CO. The spectra are presented as a function of pressure and a table compiled of the atomic lines. Of particular interest are the contrasts between the emission of the air discharge and that of the pure gases, nitrogen and oxygen. In addition, the results of studies of several discharge modes, employing steady voltages and pulsed, provide data on details of the energy flow within the plasma.

Benesch, W. M.↗

A search for chemical laser action in low pressure metal vapor flames

Optical emissions were studied from low pressure (approximately 1 torr) dilute diffusion flames of Ca and Mg vapor with O2, N2O and mixtures of CCl4 and O2. The Ca flames with O2 and N2O revealed high vibrational excitation of the product CaO molecule (up to v=30). The flames with CCl4 revealed extreme nonequilibrium metal atom electronic excitation, up to the metal atom ionization limit (6.1 eV for Ca, 7.6 eV for Mg). The metal atom excited electronic state populations did not follow a Boltzmann distribution, but the excitation rates ('pumping rate') were found to obey an Arrhenius-type expression, with the electronic excitation energy playing the role of activation energy and a temperature of about 5000 K for triplet excited states and 2500 K for singlets (vs. approximately 500 K translational temperature).

Zwillenberg, M. L.↗

Reducing nitrous oxide emissions and optimizing nitrogen-use efficiency in dryland crop rotations with different nitrogen rates

Recent interests in improving agricultural production while minimizing environmental footprints emphasized the need for research on management strategies that reduce nitrous oxide (N 2 O) emissions and increase nitrogen-use efficiency (NUE) of cropping systems. This study aimed to evaluate N 2 O emissions, annualized crop grain yield, emission factor, and yield-scaled- and NUE-scaled N 2 O emissions under continuous spring wheat (Triticum aestivum L.) (CW) and spring wheat-pea (Pisum sativum L.) (WP) rotations with four N fertilization rates (0, 50, 100, and 150 kg N ha(-1)). The N 2 O fluxes peaked immediately after N fertilization, intense precipitation, and snowmelt, which accounted for 75-85% of the total annual flux. Cumulative N 2 O flux usually increased with increased N fertilization rate in all crop rotations and years. Annualized crop yield and NUE were greater in WP than CW for 0 kg N ha(-1) in all years, but the trend reversed with 100 kg N ha(-1) in 2013 and 2015. Crop yield maximized at 100 kg N ha(-1), but NUE declined linearly with increased N fertilization rate in all crop rotations and years. As N fertilization rate increased, N fertilizer-scaled N2O flux decreased, but NUE-scaled N 2 O flux increased non-linearly in all years, regardless of crop rotations. The yield-scaled N 2 O flux decreased from 0 to 50 kg N ha -1 and then increased with increased N fertilization rate. Because of non-significant difference of N 2 O fluxes between 50 and 100 kg N ha(-1), but increased crop yield, N 2 O emissions can be minimized while dryland crop yields and NUE can be optimized with 100 kg N ha -1 , regardless of crop rotations.

54 ENVIRONMENTAL SCIENCES↗

Integrated Modeling of U.S. Agricultural Soil Emissions of Reactive Nitrogen and Associated Impacts on Air Pollution, Health, and Climate

Agricultural soils are leading sources of reactive nitrogen (Nr) species including nitrogen oxides (NO x ), ammonia (NH 3 ), and nitrous oxide (N 2 O). Here, the propensity of NO x and NH 3 to generate ozone and fine particulate matter (PM) and associated impacts on health are highly variable, whereas the climate impacts of long-lived N 2 O are independent of emission timing and location. However, these impacts have rarely been compared on a spatially-resolved, monetized basis. In this study, we update the nitrogen scheme in an agroecosystem model to simulate the agricultural emissions of Nr from across the United States. We then apply a reduced-form air pollution health effects model to assess air quality impacts from NO x and NH 3 and a social cost of N 2 O to assess the climate impacts. Assuming an $\$$8.2 million Value of a Statistical Life (VSL) and a $\$$13,100/ton social cost of N 2 O, the air quality impacts are a factor of ~7 to 15 times as large as the climate impacts in heavily populated coastal regions, whereas the ratios are closer to 2.5 in sparsely populated regions. Our results show that air pollution, health, and climate should be considered jointly in future assessments of how farming practices affect Nr emissions.

54 ENVIRONMENTAL SCIENCES↗