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At least 343 records · Page 19

Quantitative Measurements of CH* Concentration in Normal Gravity and Microgravity Coflow Laminar Diffusion Flames

With the conclusion of the SLICE campaign aboard the ISS in 2012, a large amount of data was made available for the analysis of the effect of microgravity on laminar coflow diffusion flames. Previous work focused on the study of sooty flames in microgravity as well as the ability of numerical models to predict its formation in a simplified buoyancy-free environment. The current work shifts the investigation to soot-free flames, putting an emphasis on the chemiluminescence emission from electronically excited CH (CH*). This radical species is of significant interest in combustion studies: it has been shown that the CH* spatial distribution is indicative of the flame front position and, given the relatively simple diagnostic involved with its measurement, several works have been done trying to understand the ability of CH* chemiluminescence to predict the total and local flame heat release rate. In this work, a subset of the SLICE nitrogen-diluted methane flames has been considered, and the effect of fuel and coflow velocity on CH* concentration is discussed and compared with both normal gravity results and numerical simulations. Experimentally, the spectral characterization of the DSLR color camera used to acquire the flame images allowed the signal collected by the blue channel to be considered representative of the CH* emission centered around 431 nm. Due to the axisymmetric flame structure, an Abel deconvolution of the line-of-sight chemiluminescence was used to obtain the radial intensity profile and, thanks to an absolute light intensity calibration, a quantification of the CH* concentration was possible. Results show that, in microgravity, the maximum flame CH* concentration increases with the coflow velocity, but it is weakly dependent on the fuel velocity; normal gravity flames, if not lifted, tend to follow the same trend, albeit with different peak concentrations. Comparisons with numerical simulations display reasonably good agreement between measured and computed flame lengths and radii, and it is shown that the integrated CH* emission scales proportionally to the computed total heat release rate; the two-dimensional CH* spatial distribution, however, does not appear to be a good marker for the local heat release rate.

microgravity↗

Comparison of alternate fuels for aircraft

Liquid hydrogen, liquid methane, and synthetic aviation kerosene were assessed as alternate fuels for aircraft in terms of cost, capital requirements, and energy resource utilization. Fuel transmission and airport storage and distribution facilities are considered. Environmental emissions and safety aspects of fuel selection are discussed and detailed descriptions of various fuel production and liquefaction processes are given. Technological deficiencies are identified.

Witcofski, R. D.↗

Emissions of biogenic sulfur gases from northern bogs and fens

Sulfur gases are important components of the global cycle of S. They contribute to the acidity of precipitation and they influence global radiation balance and climate. The role of terrestrial sources of biogenic S and their effect on atmospheric chemistry remain as major unanswered questions in our understanding of the natural S cycle. The role of northern wetlands as sources and sinks of gaseous S by measuring rates of S gas exchange as a function of season, hydrologic conditions, and gradients in tropic status was investigated. Experiments were conducted in wetlands in New Hampshire, particularly a poor fen, and in Mire 239, a poor fen at the Experimental Lakes Area (ELA) in Ontario. Emissions were determined using Teflon enclosures, gas cryotrapping methods and gas chromatography (GC) with flame photometric detection. Dynamic (sweep flow) and static enclosures were employed which yielded similar results. Dissolved S gases and methane were determined by gas stripping followed by GC.

Demello, William Zamboni↗

Chemical Modeling of the Reactivity of Short-Lived Greenhouse Gases: A Model Inter-Comparison Prescribing a Well-Measured, Remote Troposphere

We develop a new protocol for merging in situ measurements with 3-D model simulations of atmospheric chemistry with the goal of integrating over the data to identify the most reactive air parcels in terms of tropospheric production and loss of the greenhouse gases ozone and methane. Presupposing that we can accurately measure atmospheric composition, we examine whether models constrained by such measurements agree on the chemical budgets for ozone and methane. In applying our technique to a synthetic data stream of 14,880 parcels along 180W, we are able to isolate the performance of the photochemical modules operating within their global chemistry-climate and chemistry-transport models, removing the effects of modules controlling tracer transport, emissions, and scavenging. Differences in reactivity across models are driven only by the chemical mechanism and the diurnal cycle of photolysis rates, which are driven in turn by temperature, water vapor, solar zenith angle, clouds, and possibly aerosols and overhead ozone, which are calculated in each model. We evaluate six global models and identify their differences and similarities in simulating the chemistry through a range of innovative diagnostics. All models agree that the more highly reactive parcels dominate the chemistry (e.g., the hottest 10% of parcels control 25-30% of the total reactivities), but do not fully agree on which parcels comprise the top 10%. Distinct differences in specific features occur, including the regions of maximum ozone production and methane loss, as well as in the relationship between photolysis and these reactivities. Unique, possibly aberrant, features are identified for each model, providing a benchmark for photochemical module development. Among the 6 models tested here, 3 are almost indistinguishable based on the inherent variability caused by clouds, and thus we identify 4, effectively distinct, chemical models. Based on this work, we suggest that water vapor differences in model simulations of past and future atmospheres may be a cause of the different evolution of tropospheric O3 and CH4, and lead to different chemistry-climate feedbacks across the models.

greenhouse gases↗

Uncertainties in Isoprene Photochemistry and Emissions: Implications for the Oxidative Capacity of Past and Present Atmospheres and for Climate Forcing Agents

Current understanding of the factors controlling biogenic isoprene emissions and of the fate of isoprene oxidation products in the atmosphere has been evolving rapidly. We use a climate-biosphere-chemistry modeling framework to evaluate the sensitivity of estimates of the tropospheric oxidative capacity to uncertainties in isoprene emissions and photochemistry. Our work focuses on trends across two time horizons: from the Last Glacial Maximum (LGM, 21 000 years BP) to the preindustrial (1770s); and from the preindustrial to the present day (1990s). We find that different oxidants have different sensitivities to the uncertainties tested in this study, with OH being the most sensitive: changes in the global mean OH levels for the LGM-to-preindustrial transition range between -29 and +7, and those for the preindustrial-to-present day transition range between -8 and +17, across our simulations. Our results suggest that the observed glacial-interglacial variability in atmospheric methane concentrations is predominantly driven by changes in methane sources as opposed to changes in OH, the primary methane sink. However, the magnitudes of change are subject to uncertainties in the past isoprene global burdens, as are estimates of the change in the global burden of secondary organic aerosol (SOA) relative to the preindustrial. We show that the linear relationship between tropospheric mean OH and tropospheric mean ozone photolysis rates, water vapor, and total emissions of NOx and reactive carbon first reported in Murray et al. (2014) does not hold across all periods with the new isoprene photochemistry mechanism. Our results demonstrate that inadequacies in our understanding of present-day OH and its controlling factors must be addressed in order to improve model estimates of the oxidative capacity of past and present atmospheres.

methane↗

Lidar Measurements of Methane and Applications for Aircraft and Spacecraft

Atmospheric methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but observations since 2007 show that levels may be increasing. This trend may be caused by increased fossil fuel production, rice farming, livestock and landfills, but the underlying causes are quite uncertain. One hypothesis is that reservoirs of carbon trapped in the permafrost regions of northern Canada, Europe, and Siberia thaw as global temperatures rise and are releasing increasing amounts of methane. Another hypothesis points to increased production of methane by microbes as the permafrost warms. Currently most observations of greenhouse gases are limited to in-situ (surface and tower sites) and limited airborne in-situ measurements. Space column density measurements are starting to become available from the GOSAT mission. Although methane survives for a shorter time in the atmosphere than CO2, its impact on climate change per molecule is about 23 times than that of CO2. Accurate global observations of several greenhouse gases, including methane, are urgently needed in order to better understand climate change processes and to reduce the uncertainty in the carbon budget. Differential absorption lidar is a well-established technique to measure atmospheric gases, and methane has optical absorption bands near 1.65,2.2,3.4 and 7.8 micron. The near infrared overtones lines of CH4 near 1650 nm are relatively free of interference from other species. There are absorption lines near 1651 nm which are both temperature insensitive and have line strengths well suited for lidar measurements. We have developed a laser and demonstrated lidar measurements of CH4 using lines in this band. Our laser uses a narrow linewidth 1064 nm laser pulse passing through a nonlinear crystal. We generate the tunable laser signals near 1651 nm by using the optical parametric amplification (OPA) process. Inside the crystal the 1064 nm beam overlaps with an injection seed laser near 1651 nm from a wavelength tunable diode laser. Incident photons from the pump laser pulse are converted into two photons, with one at the wavelength of the injection seeder. The wavelength of the OPA output is tuned via the wavelength of diode laser. Our laser is tunable, operates near 1651 nm and generates approximately 4 uJ/pulse at 6 KHz. We vary the emission wavelengths within this band by tuning the diode laser's wavelength. We have used this OPA transmitter to make measurements of CH4 at various pressures in a gas cell and over open outdoor horizontal paths. We have measured the lineshape of methane in a 6 cm long cell at various energy levels with this transmitter, with excellent agreement with the lineshape calculated by HITRAN. We have also measured the absorption lineshape of atmospheric methane in an open 3 km outdoor path. The agreement between the measurements and HITRAN, for 1746 ppb and 760 Torr was quite good. We have also made pulsed two wavelength lidar measurements of methane line absorption in the column to a tower at 1.5 km range. These used on- and off-line wavelengths of 1650.957 nm, and 1651.072 nm, and a 20 cm diameter receiver telescope with an infrared PMT detector. The absorption of the on-line photons was 30%. The methane column absorption was estimated via HITRAN, and was in good agreement with the expected methane absorption for a concentration of 1750 ppm. Finally we have calculated the measurement performance of an airborne methane lidar using this transmitter, as well as the energy and telescope scaling needed for a lidar for space. These results, and more details of our experiments will be described in the presentation.

Riris, Haris↗

Future instrumentation and missions for measurements of tropospheric trace species from space: Workshop recommendations

It was recommended that gas filter correlation radiometry and high-resolution interferometry be exploited and expanded for measurements of the distribution of tropospheric trace gases. Instruments and missions were identified and discussed. Several instrument/measurement/mission feasibility studies were recommended, including: a three-layer measurement of carbon monoxide, using a nadir-viewing gas filter correlation radiometer; a lower or middle tropospheric measurement of methane, using a nadir-viewing gas filter correlation radiometer; and a survey of lower, middle, and upper tropospheric trace gases using a nadir-viewing high-resolution interferometer operating in the thermal emission mode. It was also concluded that lidar systems appear to have the potential of obtaining measurments of tropospheric trace gases and aerosols from space. In addition to the specific instrument/mission recommendations, the panels made several general recommendations that may lead to future spaceborne instruments, techniques, and missions for tropospheric research.

Source record↗

Organic synthesis in the outer Solar System: Recent laboratory simulations for Titan, the Jovian planets, Triton and comets

We tabulate the most abundant gases and their radiation yields, for two experimental pressures: 0.24 mb, more relevant to upper atmosphere excitation, and 17 mb, more relevant to tropospheric, cosmic ray excitation. The yields computed in the 0.24 mb experiment combined with measured electronic fluxes and a simple, eddy diffusion model of Titan's atmosphere predict abundances of detected molecules in agreement with those found by Voyager and for heavier products, in somewhat better agreement with observation than photochemical absolute reaction rate kinetics models. All Voyager organics are accounted for and no detectable products are found that Voyager did not detect. A striking increase of products with multiple bonds is found with decreasing pressure. Hydrocarbon abundances decline slowly with increasing carbon number. Additionally, we list preliminary estimates for the yield of the heteropolymer, which seems to be produced in a quantity comparable (in moles of C+N consumed) to the total amount of gaseous product. The production rate required to sustain Titan's haze against sedimentation also indicates yields of this order. As can be seen from the table, over 10(exp 9) years substantial amounts of these products can accumulate on the surface -- ranging from cm thickness for the (C+N equals 4) species to a meter or more for HCN and C2H2; we also expect a meter or more of tholins. Similar analyses have been or are being done for the Jovian planets and Triton. Charged particle irradiation of hydrocarbon clathrates or mixed hydrocarbon/water ices produces a range of organic products, reddening and darkening of the ices and characteristic infrared spectra. From such spectra, the predicted emission by fine particles in cometary comae well-matches the observed 3.4 micron emission spectra of Comet Halley and other recent comets. Heliocentric evolution of organic emission features in comets is predicted. Organic products of such ice irradiation may account for colors and albedos on some of the satellites in the outer solar system, especially Triton and Pluto, where solid methane is known to exist.

Sagan, C.↗

Quantitative Measurements of Electronically Excited CH Concentration in Normal Gravity and Microgravity Coflow Laminar Diffusion Flames

With the conclusion of the SLICE campaign aboard the ISS in 2012, a large amount of data was made available for the analysis of the effect of microgravity on laminar coflow diffusion flames. Previous work focused on the study of sooty flames in microgravity as well as the ability of numerical models to predict its formation in a simplified buoyancy-free environment. The current work shifts the investigation to soot-free flames, putting an emphasis on the chemiluminescence emission from electronically excited CH (CH*). This radical species is of significant interest in combustion studies: it has been shown that the electronically excited CH spatial distribution is indicative of the flame front position and, given the relatively simple diagnostic involved with its measurement, several works have been done trying to understand the ability of electronically excited CH chemiluminescence to predict the total and local flame heat release rate. In this work, a subset of the SLICE nitrogen-diluted methane flames has been considered, and the effect of fuel and coflow velocity on electronically excited CH concentration is discussed and compared with both normal gravity results and numerical simulations. Experimentally, the spectral characterization of the DSLR color camera used to acquire the flame images allowed the signal collected by the blue channel to be considered representative of the electronically excited CH emission centered around 431 nm. Due to the axisymmetric flame structure, an Abel deconvolution of the line-of-sight chemiluminescence was used to obtain the radial intensity profile and, thanks to an absolute light intensity calibration, a quantification of the electronically excited CH concentration was possible. Results show that, in microgravity, the maximum flame electronically excited CH concentration increases with the coflow velocity, but it is weakly dependent on the fuel velocity; normal gravity flames, if not lifted, tend to follow the same trend, albeit with different peak concentrations. Comparisons with numerical simulations display reasonably good agreement between measured and computed flame lengths and radii, and it is shown that the integrated electronically excited CH emission scales proportionally to the computed total heat release rate; the two-dimensional electronically excited CH spatial distribution, however, does not appear to be a good marker for the local heat release rate.

chemiluminescence↗

The Geostationary Fourier Transform Spectrometer

The Geostationary Fourier Transform Spectrometer (GeoFTS) is an imaging spectrometer designed for a geostationary orbit (GEO) earth science mission to measure key atmospheric trace gases and process tracers related to climate change and human activity. GEO allows GeoFTS to continuously stare at a region of the earth for frequent sampling to capture the variability of biogenic fluxes and anthropogenic emissions from city to continental spatial scales and temporal scales from diurnal, synoptic, seasonal to interannual. The measurement strategy provides a process based understanding of the carbon cycle from contiguous maps of carbon dioxide (CO2), methane (CH4), carbon monoxide (CO), and chlorophyll fluorescence (CF) collected many times per day at high spatial resolution (~2.7kmx2.7km at nadir). The CO2/CH4/CO/CF measurement suite in the near infrared spectral region provides the information needed to disentangle natural and anthropogenic contributions to atmospheric carbon concentrations and to minimize uncertainties in the flow of carbon between the atmosphere and surface. The half meter cube size GeoFTS instrument is based on a Michelson interferometer design that uses all high TRL components in a modular configuration to reduce complexity and cost. It is self-contained and as independent of the spacecraft as possible with simple spacecraft interfaces, making it ideal to be a "hosted" payload on a commercial communications satellite mission. The hosted payload approach for measuring the major carbon-containing gases in the atmosphere from the geostationary vantage point will affordably advance the scientific understating of carbon cycle processes and climate change.

atmospheric trace gases↗

Inland Water Greenhouse Gas Budgets for RECCAP2: 2. Regionalization and Homogenization of Estimates

Inland waters are important emitters of the greenhouse gasses (GHGs) carbon dioxide (CO 2 ), methane (CH 4 ), and nitrous oxide (N 2 O) to the atmosphere. In the framework of the 2 nd phase of the REgional Carbon Cycle Assessment and Processes (RECCAP-2) initiative, we synthesize existing estimates of GHG emissions from streams, rivers, lakes and reservoirs, and homogenize them with regard to underlying global maps of water surface area distribution and the effects of seasonal ice cover. We then produce regionalized estimates of GHG emissions over 10 extensive land regions. According to our synthesis, inland water GHG emissions have a global warming potential of an equivalent emission of 13.5 (9.9-20.1) and 8.3 (5.7-12.7) Pg CO 2 -eq. yr -1 at a 20 and 100 year horizon (GWP 20 and GWP 100 ), respectively. Contributions of CO 2 dominate GWP100, with rivers being the largest emitter. For GWP 20 , lakes and rivers are equally important emitters, and the warming potential of CH4 is more important than that of CO2. Contributions from N 2 O are about two orders of magnitude lower. Normalized to the area of RECCAP-2 regions, S-America and SE-Asia show the highest emission rates, dominated by riverine CO 2 emissions.

Ronny Lauerwald↗

The Behavior of Methane-Air Partially Premixed Flames Under Normal- and Zero-G Conditions

Partially premixed flames (PPFs) represent a class of hybrid flames containing multiple reaction zones. These flames are established when less than stoichiometric quantity of oxidizer is molecularly mixed with the fuel stream before entering the reaction zone where additional oxidizer is available for complete combustion. This mode of combustion can be used to exploit the advantages of both nonpremixed and premixed flames regarding operational safety, lower pollutant emissions and flame stabilization. A double flame containing a fuel-rich premixed reaction zone, which is anchored by a nonpremixed reaction zone, is one example of a partially premixed flame. A triple flame is also a PPF that contains three reaction zones, namely, a fuel-rich premixed zone, a fuel-lean premixed zone, and a nonpremixed reaction zone. Herein we focus on two aspects of our investigation, one involving the development of optical diagnostics that can be used on a microgravity rig, which has been recently fabricated, and the other on the numerically predicted differences between normal- and zero-gravity PPFs. Both the measurements and simulations examine the detailed structure of methane-air PPFs stabilized on a Wolfhard-Parker slot burner.

Puri, Ishwar K.↗

Dependence of Surface Contrast on Emission Angle in Cassini ISS 938-nm Images of Titan

Titan, the largest of Saturn s moons, is one of the most difficult solid surfaces in the Solar System to study. It is shrouded in a thick atmosphere with fine haze particles extending up to 500 km. [1] The atmosphere itself is rich in methane, which allows clear viewing of the surface only through narrow "windows" in the methane spectrum. Even in these methane windows, the haze absorbs and scatters light, blurring surface features and reducing the contrast of images. The haze optical depth is high at visible wavelengths, and decreases at longer (infrared) wavelengths. [2]

Fussner, S.↗

CH(A, B-X) fluorescence from vacuum ultraviolet excitation of CH3

The fluorescence due to single-photon and two-photon excitation of CH3 produced by the reaction of CH4 with F or Cl in a flow tube is investigated experimentally. The excitation source is an excimer laser operating with pulse duration 6 nsec and repetition rate 20 Hz, and the fluorescence is observed using a 0.25-m spectrometer and a 1024-channel diode array; the results are presented graphically. Emission is detected at 157 nm (with approximate cross section 8 x 10 to the -19th sq cm) and 193 nm, but not at 248 nm. The applicability of these data to studies of hydrocarbon combustion, the methane oxidation cycle in the atmosphere, interstellar molecule formation, and diamond film fabrication is indicated.

Ye, Chao↗

AIRS Observations of Deep Convective Clouds

Large thunderstorms can be identified in the AIRS data as areas where the brightness temperature of the 1231 cm-1 atmospheric window channel in non-polar areas is less than 210 K. Each day about 6000 large thunderstorms are identified, almost exclusively within 30 degrees of the equator. Since the size of the AIRS footprint at nadir is 13.5 km, a brightness temperature of less than 210 K indicates that the top of the anvil of the thunderstorm protrudes well into the tropopause. Such objects are commonly referred to as Deep Convective Clouds (DCC). Our interest in DCC was motivated by the question 'Are severe weather events increasing due to global warming'. Each DCC is a severe weather event, although not on the scale of the much less frequent hurricanes, which can be identified in the AIRS data as clusters of several hundred DCC. The number of DCC per day has been fairly stable over the past four years for the mean of the tropical oceans, but a significant increase can be seen day and night in the Atlantic Ocean. The number of DCC per day shows a strong seasonal and latitudinal dependence, with the peak count lagging the solstice of the latitude zone by about 2 months. The most prominent features in brightness temperature spectra of DCC are due to stratospheric CO2, Ozone and Methane. In the channels with weighting functions below the stratosphere the brightness temperature is typically 205 K, with a characteristic 1 to 2.5 K drop between 1000 and 750 cm-1, equivalent to a 2-4 % drop in emissivity. This is likely due to the presence of cirrus (ice) particles. Some of this analysis of DCC can be extended using past and future operational sounders in polar orbit.

temperature↗

Source and Chemistry of Hydroxymethanesulfonate (HMS) in Fairbanks, Alaska

Fairbanks, Alaska is a subarctic city with fine-particle (PM 2.5 ) concentrations that exceed air quality regulations in winter due to weak dispersion caused by strong atmospheric inversions, local emissions, and the unique chemistry occurring under the cold and dark conditions. Here we report on observations from the winters of 2020 and 2021, motivated by our pilot study which showed exceptionally high concentrations of fine particle hydroxy methane sulfonate (HMS) or related sulfur (IV) species (e.g., sulfite and bisulfite). We deployed an online Particle-Into-Liquid Sampler-Ion Chromatography (PILS-IC) in conjunction with a suite of instruments to determine HMS precursors (HCHO, SO 2 ) and aerosol composition in general, with the goal to characterize the sources and sinks of HMS in wintertime Fairbanks. PM 2.5 HMS comprised a significant fraction of PM 2.5 sulfur (26-41%) and overall PM 2.5 mass concentration (2.8-6.8%) during pollution episodes, substantially higher than what has been observed in other regions, likely due to the exceptionally low temperatures. HMS peaked in January, with lower concentrations in December and February, resulting from changes in precursors as well as meteorological conditions. Strong correlations with inorganic sulfate and organic mass during pollution events suggest HMS is linked to processes responsible for poor air quality episodes. These findings demonstrate unique aspects of air pollution formation in cold and humid atmospheres.

Fine-particle↗

Carbon monoxide and methane in the North American Arctic and Subarctic troposphere - July-August 1988

Enhanced concentrations of CH4 in the unpolluted atmospheric mixed layer over both Arctic and subarctic tundra landscapes are documented here using data from the NASA Arctic Boundary Layer Expedition (ABLE 3A). The CH4 concentration gradients were determined mainly by interactions of biogenic emission from wet tundra and turbulent mixing proceses. The gradient were most frequently associated with intrusion of upper tropospheric or stratospheric air into the midtroposphere, emissions from forest and tundra fires, and long-range transport of enhanced concentration of these gases from unidentified sources. Summertime haze layers exhibited midtropospheric enhancements of CH4 similar to those measured in winter Arctic events. The observations confirm the importance of Arctic and Subarctic wetland environments as a regional source of global atmospheric CH4.

Harriss, Robert C.↗

Research in planetary astronomy and operation of the 2.2-meter telescope

The turn-around in the secular change in brightness of Pluto was detected, the planet is now beginning to brighten. The spectral signature was found of an ammonia bearing compound in the surface ices of Europa. Specific Io volcanic hotspots were detected from infrared photometry of the mutual events of the Jovian satellites. The polarized emission from the volcanic hotspots on Io was discovered and the locations of those hotspots were determined. The orbit of Charon was refined from speckle observations of the Pluto-Charon system. The spectral properties of liquid nitrogen-methane mixtures with reference to the infrared spectrum of Triton were studied. Major progress was made in modeling asteroid lightcurves from a modern theory of photometric properties of the asteroid surfaces. Several additional olivine-rich asteroids from near-infrared spectrophotometry were discovered. Important photometric, spectroscopic, narrow-band imaging data on Comet P/Halley was acquired, along with Schmidt photographs of Comet P/Halley and its tail.

Hall, D. N. B.↗