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We report progress in assessing the feasibility of a new satellite-based laser-sounding instrument to measure CO2 concentrations in the lower troposphere from space.
The Instrumentation Working Group compiled a summary of measurement techniques applicable to gas turbine engine aerosol precursors and particulates. An assessment was made of the limits, accuracy, applicability, and technology readiness of the various techniques. Despite advances made in emissions characterization of aircraft engines, uncertainties still exist in the mechanisms by which aerosols and particulates are produced in the near-field engine exhaust. To adequately assess current understanding of the formation of sulfuric acid aerosols in the exhaust plumes of gas turbine engines, measurements are required to determine the degree and importance of sulfur oxidation in the turbine and at the engine exit. Ideally, concentrations of all sulfur species would be acquired, with emphasis on SO2 and SO3. Numerous options exist for extractive and non-extractive measurement of SO2 at the engine exit, most of which are well developed. SO2 measurements should be performed first to place an upper bound on the percentage of SO2 oxidation. If extractive and non-extractive techniques indicate that a large amount of the fuel sulfur is not detected as SO2, then efforts are needed to improve techniques for SO3 measurements. Additional work will be required to account for the fuel sulfur in the engine exhaust. Chemical Ionization Mass Spectrometry (CI-MS) measurements need to be pursued, although a careful assessment needs to be made of the sampling line impact on the extracted sample composition. Efforts should also be placed on implementing non-intrusive techniques and extending their capabilities by maximizing exhaust coverage for line-of-sight measurements, as well as development of 2-D techniques, where feasible. Recommendations were made to continue engine exit and combustor measurements of particulates. Particulate measurements should include particle size distribution, mass fraction, hydration properties, and volatile fraction. However, methods to ensure that unaltered samples are obtained need to be developed. Particulate speciation was also assigned a high priority for quantifying the fractions of carbon soot, PAH, refractory materials, metals, sulfates, and nitrates. High priority was also placed on performing a comparison of particle sizing instruments. Concern was expressed by the workshop attendees who routinely make particulate measurements about the variation in number density measured during in-flight tests by different instruments. In some cases, measurements performed by different groups of researchers during the same flight tests showed an order of magnitude variation. Second priority was assigned to measuring concentrations of odd hydrogen and oxidizing species. Since OH, HO2, H2O2, and O are extremely reactive, non-extractive measurements are recommended. A combination of absorption and fluorescence is anticipated to be effective for OH measurements in the combustor and at the engine exit. Extractive measurements of HO2 have been made in the stratosphere, where the ambient level of OH is relatively low. Use of techniques that convert HO2 to OH for combustor and engine exit measurements needs to be evaluated, since the ratio of HO2/OH may be 1% or less at both the combustor and engine exit. CI-MS might be a viable option for H2O2, subject to sampling line conversion issues. However, H2O2 is a low priority oxidizing species in the combustor and at the engine exit. Two candidates for atomic oxygen measurements are Resonance Enhanced Multi-Photon Ionization (REMPI) and Laser-Induced Fluorescence (LIF). Particulate measurement by simultaneous extractive and non-extractive techniques was given equal priority to the oxidizer measurements. Concern was expressed over the ability of typical ground test sampling lines to deliver an unaltered sample to a remotely located instrument. It was suggested that the sampling probe and line losses be checked out by attempting measurements using an optical or non-extractive technique immediately upstream of the sampling probe. This is a possible application for Laser Induced Incandescence (LII) as a check on the volume fraction of soot. Optical measurements of size distribution are not well developed for ultrafine particles less than about 20 nm in diameter, so a non-extractive technique for particulate size distribution cannot be recommended without further development. Carbon dioxide measurements need to be made to complement other extractive measurement techniques. CO2 measurements enable conversion of other species concentrations to emission indices. Carbon monoxide, which acts as a sink for oxidizing species, should be measured using non-extractive techniques. CO can be rapidly converted to CO2 in extractive probes, and a comparison between extractive and non-extractive measurements should be performed. Development of non-extractive techniques would help to assess the degree of CO conversion, and might be needed to improve the concentration measurement accuracy. Measurements of NO(x) will continue to be critical due to the role of NO and NO2 in atmospheric chemistry, and their influence on atmospheric ozone. Time-resolved measurements of temperature, velocity, and species concentrations were included on the list of desired measurement. Thermocouples are typically adequate for engine exit measurements. PIV and LDV are well established for obtaining velocity profiles. The techniques are listed in the accompanying table; are divided into extractive and non-extractive techniques. Efforts were made to include a measurement uncertainty for each technique. An assessment of the technology readiness was included.
Measurements of temperature and CO2 concentration using dual-pump coherent anti-Stokes Raman scattering, (CARS) are described. The measurements were performed in laboratory flames,in a room-temperature gas cell, and on an engine test stand at the U.S. Air Force Research Laboratory, Wright-Patterson Air Force Base. A modeless dye laser, a single-mode Nd:YAG laser, and an unintensified back-illuminated charge-coupled device digital camera were used for these measurements. The CARS measurements were performed on a single-laser-shot basis. The standard deviations of the temperatures and CO2 mole fractions determined from single-shot dual-pump CARS spectra in steady laminar propane/air flames were approximately 2 and 10% of the mean values of approximately 2000 K and 0.10, respectively. The precision and accuracy of single-shot temperature measurements obtained from the nitrogen part of the dual-pump CARS system were investigated in detail in near-adiabatic hydrogen/air/CO2 flames. The precision of the CARS temperature measurements was found to be comparable to the best results reported in the literature for conventional two-laser, single-pump CARS. The application of dual-pump CARS for single-shot measurements in a swirl-stabilized combustor fueled with JP-8 was also demonstrated.
Trace gases and their isotopic ratios in planetary atmospheres offer important but subtle clues as to the origins of a planet's atmosphere, hydrology, geology, and potential for biology. An orbiting laser remote sensing instrument is capable of measuring trace gases on a global scale with unprecedented accuracy, and higher spatial resolution that can be obtained by passive instruments. We have developed an active sensing instrument for the remote measurement of trace gases in planetary atmospheres (including Earth). The technique uses widely tunable, seeded optical parametric generation (OPG) to measure methane, CO2, water vapor, and other trace gases in the near and mid-infrared spectral regions. Methane is a strong greenhouse gas on Earth and it is also a potential biogenic marker on Mars and other planets. Methane in the Earth's atmosphere survives for a shorter time than CO2 but its impact on climate change can be larger than CO2. Methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but recent observations indicate that methane levels may be on the rise. Increasing methane concentrations may trigger a positive feedback loop and a subsequent runaway greenhouse effect, where increasing temperatures result in increasing methane levels. The NRC Decadal Survey recognized the importance of global observations of greenhouse gases and called for simultaneous CH4, CO, and CO2 measurements but also underlined the technological limitations for these observations. For Mars, methane measurements are of great interest because of its potential as a strong biogenic marker. A remote sensing instrument that can measure day and night over all seasons and latitudes can identify and localize sources of biogenic gas plumes produced by subsurface chemistry or biology, and aid in the search for extra-terrestrial life. It can identify the dynamics of methane generation over time and latitude and identify future lander mission sites for more detailed in-situ analysis. In this paper we report on remote sensing measurements of methane using a high peak power, widely tunable optical parametric generator (OPG) operating at 3.3 micron and 1.65 micron. The OPG is pumped by a passively q-switched single frequency laser (3ns, 5KHz, 50uJ) and seeded by a diode laser. The spectral width of both signal and idler of seeded OPG is nearly Fourier transform limited. The output of seeded OPG is single frequency with high spectral purity and is widely tunable. Both 1650 nm and 3300 nm can be generated with a conversion efficiency of more than 30%. We have demonstrated detection of methane at 3274 nm and 1650 nm in a cell and also performed open path atmospheric measurements of methane at the same wavelengths. Finally, we were able to demonstrate simultaneous detection of methane at 3270.4 nm and CO2 at 1578.2 nm. In this paper we will discuss the OPG performance and atmospheric open path measurement results.
A mechanistic understanding of the global carbon cycle requires quantification of terrestrial ecosystem CO2 fluxes at regional scales. In this paper, we analyze the potential of a Doppler DIAL system to make flux measurements of atmospheric CO2 using the eddy-covariance and boundary layer budget methods and present results from a ground based experiment. The goal of this study is to put CO2 flux point measurements in a mesoscale context. In June 2007, a field experiment combining a 2-m Doppler Heterodyne Differential Absorption Lidar (HDIAL) and in-situ sensors of a 447-m tall tower (WLEF) took place in Wisconsin. The HDIAL measures simultaneously: 1) CO2 mixing ratio, 2) atmosphere structure via aerosol backscatter and 3) radial velocity. We demonstrate how to synthesize these data into regional flux estimates. Lidar-inferred fluxes are compared with eddy-covariance fluxes obtained in-situ at 396m AGL from the tower. In cases where the lidar was not yet able to measure the fluxes with acceptable precision, we discuss possible modifications to improve system performance.
The net CO2 assimilation (A) response to intercellular CO2 concentration (Ci) is a fundamental measurement in photosynthesis and plant physiology research. The conventional A/Ci protocols rely on steady-state measurements and take 15-40 minute per measurement, limiting data resolution or biological replication. Additionally, there are several CO2 protocols employed across the literature, without clear consensus as to the optimal protocol or systematic biases in their estimations. We compared the non-steady state Dynamic Assimilation Technique (DAT) protocol and the three most used CO2 protocols in steady-state measurements, and tested whether different CO2 protocols lead to systematic differences in estimations of the biochemical limitations to photosynthesis.
Plant functional traits such as photosynthetic capacity are critical parameters for terrestrial biosphere models. However, their spatial and temporal characteristics are still poorly represented. In this study, we used satellite observations of sun-induced fluorescence (SIF) to estimate top-of-canopy photosynthetic capacity (maximum carboxylation rate, V(sub cmax) at a reference temperature of 25 deg C) for crops, which was in turn utilized to simulate regional gross primary production (GPP). We first estimate the key parameter, V(sub cmax), in the widely-used FvCB photosynthesis model using field measurements of CO2 and water fluxes during 2007-2012 at seven crop eddy covariance flux sites over the US Corn Belt. The results showed that satellite far-red SIF retrievals have a stronger link to V(sub cmax) at the seasonal scale (R(squared)=0.70 for C4 and R(squared)=0.63 for C3 crop) as compared with widely-used vegetation indices. We calibrate an empirical model linking V(sub cmax) with SIF that was used to estimate spatially and temporally varying crop V(sub cmax) for the US Corn Belt region. The resulting V(sub cmax) maps are used together with meteorological data from MERRA reanalysis data and vegetation structural parameters derived from the satellite- based spectral reflectance data to constrain the Soil-Canopy Observation of Photosynthesis and Energy (SCOPE) balance model in order to estimate regional crop GPP. Our results show a substantial improvement in the seasonal and spatial patterns of cropland GPP when compared with crop yield inventory data. The evaluation with tall tower atmospheric CO2 measurements further supports our estimation of spatiotemporal V(sub cmax) from space-borne SIF. Considering that SIF has a direct link to photosynthetic activity, our findings highlight the potential to infer regional V(sub cmax) using remotely sensed SIF data and to use this information for a better quantification of regional cropland carbon cycles.
We have previously demonstrated a pulsed direct detection IPDA lidar to measure range and the column concentration of atmospheric CO2. The lidar measures the atmospheric backscatter profiles and samples the shape of the 1,572.33 nm CO2 absorption line. We participated in the ASCENDS science flights on the NASA DC-8 aircraft during August 2011 and report here lidar measurements made on four flights over a variety of surface and cloud conditions near the US. These included over a stratus cloud deck over the Pacific Ocean, to a dry lake bed surrounded by mountains in Nevada, to a desert area with a coal-fired power plant, and from the Rocky Mountains to Iowa, with segments with both cumulus and cirrus clouds. Most flights were to altitudes >12 km and had 5-6 altitude steps. Analyses show the retrievals of lidar range, CO2 column absorption, and CO2 mixing ratio worked well when measuring over topography with rapidly changing height and reflectivity, through thin clouds, between cumulus clouds, and to stratus cloud tops. The retrievals shows the decrease in column CO2 due to growing vegetation when flying over Iowa cropland as well as a sudden increase in CO2 concentration near a coal-fired power plant. For regions where the CO2 concentration was relatively constant, the measured CO2 absorption lineshape (averaged for 50 s) matched the predicted shapes to better than 1% RMS error. For 10 s averaging, the scatter in the retrievals was typically 2-3 ppm and was limited by the received signal photon count. Retrievals were made using atmospheric parameters from both an atmospheric model and from in situ temperature and pressure from the aircraft. The retrievals had no free parameters and did not use empirical adjustments, and >70% of the measurements passed screening and were used in analysis. The differences between the lidar-measured retrievals and in situ measured average CO2 column concentrations were <1.4 ppm for flight measurement altitudes >6 km.
Precise stable isotope measurements of the CO2 in the martian atmosphere have the potential to provide important constraints for our understanding of the history of volatiles, the carbon cycle, current atmospheric processes, and the degree of water/rock interaction on Mars. There have been several different measurements by landers and Earth based systems performed in recent years that have not been in agreement. In particular, measurements of the isotopic composition of martian atmospheric CO2 by the Thermal and Evolved Gas Analyzer (TEGA) instrument on the Mars Phoenix Lander and the Sample Analysis at Mars (SAM) instrument on the Mars Science Laboratory (MSL) are in stark disagreement. This work attempts to use measurements of mass 45 and mass 46 of martian atmospheric CO2 by the SAM and TEGA instruments to search for agreement as a first step towards reaching a consensus measurement that might be supported by data from both instruments.
The 2007 National Research Council (NRC) Decadal Survey on Earth Science and Applications from Space recommended Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) as a mid-term, Tier II, NASA space mission. ITT Exelis, formerly ITT Corp., and NASA Langley Research Center have been working together since 2004 to develop and demonstrate a prototype Laser Absorption Spectrometer for making high-precision, column CO2 mixing ratio measurements needed for the ASCENDS mission. This instrument, called the Multifunctional Fiber Laser Lidar (MFLL), operates in an intensity-modulated, continuous-wave mode in the 1.57- micron CO2 absorption band. Flight experiments have been conducted with the MFLL on a Lear-25, UC-12, and DC-8 aircraft over a variety of different surfaces and under a wide range of atmospheric conditions. Very high-precision CO2 column measurements resulting from high signal-to-noise (great than 1300) column optical depth measurements for a 10-s (approximately 1 km) averaging interval have been achieved. In situ measurements of atmospheric CO2 profiles were used to derive the expected CO2 column values, and when compared to the MFLL measurements over desert and vegetated surfaces, the MFLL measurements were found to agree with the in situ-derived CO2 columns to within an average of 0.17% or approximately 0.65 ppmv with a standard deviation of 0.44% or approximately 1.7 ppmv. Initial results demonstrating ranging capability using a swept modulation technique are also presented.
Profiling of atmospheric carbon dioxide (CO2) is important for understanding the natural carbon cycle on Earth and its influence on global warming and climate change. Differential absorption lidar is a powerful remote sensing technique used for profiling and monitoring atmospheric constituents. Recently there has been an interest to apply this technique, at the 2 m wavelength, for investigating atmospheric CO2. This drives the need for high quality detectors at this wavelength. Although 2 m detectors are commercially available, the quest for a better detector is still on. The detector performance, regarding quantum efficiency, gain and associated noise, affects the DIAL signal-to-noise ratio and background signal, thereby influencing the instrument sensitivity and dynamic range. Detectors based on the III-V based compound materials shows a strong potential for such application. In this paper the detector requirements for a long range CO2 DIAL profiles will be discussed. These requirements were compared to newly developed III-V compound infrared detectors. The performance of ternary InGaSb pn junction devices will be presented using different substrates, as well as quaternary InGaAsSb npn structure. The performance study was based on experimental characterization of the devices dark current, spectral response, gain and noise. The final results are compared to the current state-of-the-art InGaAs technology. Npn phototransistor structure showed the best performance, regarding the internal gain and therefore the device signal-to-noise ratio. 2-micrometers detectivity as high as 3.9 x 10(exp 11) cmHz(sup 1/2)/W was obtained at a temperature of -20 C and 4 V bias voltage. This corresponds to a responsivity of 2650 A/W with about 60% quantum efficiency.
We report a fiber-based, pulsed laser seeder system that rapidly switches among 6 wavelengths across atmospheric carbon dioxide (CO2) absorption line near 1572.3 nm for measurements of global CO2 mixing ratios to 1-ppmv precision. One master DFB laser diode has been frequency-locked to the CO2 line center using a frequency modulation technique, suppressing its peak-to-peak frequency drifts to 0.3 MHz at 0.8 sec averaging time over 72 hours. Four online DFB laser diodes have been offset-locked to the master laser using phase locked loops, with virtually the same sub-MHz absolute accuracy. The 6 lasers were externally modulated and then combined to produce the measurement pulse train.
Double-pulsed 2-micron integrated path differential absorption (IPDA) lidar is well suited for atmospheric CO2 remote sensing. The IPDA lidar technique relies on wavelength differentiation between strong and weak absorbing features of the gas normalized to the transmitted energy. In the double-pulse case, each shot of the transmitter produces two successive laser pulses separated by a short interval. Calibration of the transmitted pulse energies is required for accurate CO2 measurement. Design and calibration of a 2-micron double-pulse laser energy monitor is presented. The design is based on an InGaAs pin quantum detector. A high-speed photo-electromagnetic quantum detector was used for laser-pulse profile verification. Both quantum detectors were calibrated using a reference pyroelectric thermal detector. Calibration included comparing the three detection technologies in the single-pulsed mode, then comparing the quantum detectors in the double-pulsed mode. In addition, a self-calibration feature of the 2-micron IPDA lidar is presented. This feature allows one to monitor the transmitted laser energy, through residual scattering, with a single detection channel. This reduces the CO2 measurement uncertainty. IPDA lidar ground validation for CO2 measurement is presented for both calibrated energy monitor and self-calibration options. The calibrated energy monitor resulted in a lower CO2 measurement bias, while self-calibration resulted in a better CO2 temporal profiling when compared to the in situ sensor.
The vertical CO2 flux in the atmospheric boundary layer (ABL) is investigated with a Doppler differential absorption lidar (DIAL). The instrument was operated next to the WLEF instrumented tall tower in Park Falls, Wisconsin during three days and nights in June 2007. Profiles of turbulent CO2 mixing ratio and vertical velocity fluctuations are measured by in-situ sensors and Doppler DIAL. Time and space scales of turbulence are precisely defined in the ABL. The eddy-covariance method is applied to calculate turbulent CO2 flux both by lidar and in-situ sensors. We show preliminary mean lidar CO2 flux measurements in the ABL with a time and space resolution of 6 h and 1500 m respectively. The flux instrumental errors decrease linearly with the standard deviation of the CO2 data, as expected. Although turbulent fluctuations of CO2 are negligible with respect to the mean (0.1 %), we show that the eddy-covariance method can provide 2-h, 150-m range resolved CO2 flux estimates as long as the CO2 mixing ratio instrumental error is no greater than 10 ppm and the vertical velocity error is lower than the natural fluctuations over a time resolution of 10 s.
Vibrational relaxation measurements in carbon dioxide using induced infrared fluorescence technique
Global atmospheric CO2 measurements are essential to resolving significant discrepancies in our understanding of the global carbon budget and, hence, humankind's role in global climate change. The science measurement requirements for CO2 are extremely demanding (precision approx. 0.3%). No atmospheric chemical species has ever been measured from space with this precision. We are developing a novel application of a Fabry-Perot interferometer to detect spectral absorption of reflected sunlight by CO2 and O2 in the atmosphere. Preliminary design studies indicate that the method will be able to achieve the sensitivity and signal-to-noise detection required to measure column CO2 at the target specification. The objective of this program is to construct a prototype instrument for deployment on an aircraft to test the instrument performance and our ability to retrieve the data in the real atmosphere. To date we have assembled a laboratory bench system to begin testing the optical and electronic components. We are also measuring signal and noise levels in actual sunlight to evaluate component performance.
Global atmospheric CO2 measurements are essential to resolving significant discrepancies in our understanding of the global carbon budget and, hence, humankind's role in global climate change. The science measurement requirements for CO2 are extremely demanding (precision is less than .3%). No atmospheric chemical species has ever been measured from space with this precision. We are developing a novel application of a Fabry-Perot interferometer to detect spectral absorption of reflected sunlight by CO2 and O2 in the atmosphere. Preliminary design studies indicate that the method will be able to achieve the sensitivity and signal-to-noise detection required to measure column CO2 at the target specification. The objective of this program is to construct a prototype instrument for deployment on an aircraft to test the instrument performance and our ability to retrieve the data in the real atmosphere. To date we have assembled a laboratory bench system to begin testing the optical and electronic components. We are also undertaking some measurements of signal and noise levels for actual sunlight reflecting from the ground in order to evaluate the potential of some components to meet the exacting requirements of this measurement.
In order to increase our knowledge of the Martian polar caps, an improved understanding of the behavior of both frozen H2O and CO2 in different parts of the electromagnetic spectrum is needed. The thermal microwave part of the spectrum has received relatively little attention compared to the visible and infrared wavelengths. A simple experiment to measure the brightness temperature of frozen CO2 was first performed in the winter of 1998 using a 35 GHz radiometer. in experiments performed during the winter of 1999 and 2000, passive microwave radiation emanating from within layers of manufactured CO2 (dry ice) crystals was again measured with a 35 GHz handheld radiometer. Both large (0.8 cm) and small (0.3 cm) cylindrical-shaped dry ice pellets, at a temperature of 197 K (-76 C), were measured. A 1 sq m plate of aluminum sheet metal was positioned beneath the dry ice so that microwave emissions from the underlying soil layers would be minimized. Non-absorbing foam was positioned around the sides of the plate in order to keep the dry ice in place and to assure that the incremental deposits were level. Thirty-five GHz measurements of this plate were made through the dry ice deposits in the following way. Layers of dry ice were built up and measurements were repeated for the increasing CO2 pack. First, 7 cm of large CO2 pellets were poured onto the sheet metal plate, then an additional 7 cm were added, and finally, 12 cm were added on top of the 14 cm base. Hand-held 35 GHz measurements were made each time the thickness of the deposit was increased. The same process was repeated for the smaller grain pellets. Furthermore, during the past winter, 35 GHz measurements were taken of a 25 kg (27 cm x 27 cm x 27 cm) solid cube Of CO2, which was cut in half and then re-measured. Additional information is contained in the original extended abstract.