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At least 37 records · Page 2

Remote Sensing of Tropospheric Pollution from Space

We review the progress of tropospheric trace gas observations and address the need for additional measurement capabilities as recommended by the National Academy of Science (NAS, 2007). Tropospheric measurements from current and earlier instruments show pollution in the Northern Hemisphere as a result of fossil fuel burning and a strong seasonal dependence with the largest amounts of photochemically-generated ozone in summer. At low latitudes, where photon flux is stronger throughout the year, trace gas concentrations are driven by the abundance of the emissions, where the largest source, biomass burning, is readily seen in carbon monoxide measurements, but lightning and biogenic trace gases may also contribute to trace gas variability. Although substantive progress has been achieved in seasonal and global mapping of a few tropospheric trace gases, satellite trace-gas observations with considerably better temporal and spatial resolution are essential to forecasting air quality at scales required by policy-makers. The concurrent use of atmospheric composition measurements for both scientific and operational purposes is a new paradigm for the atmospheric chemistry community. The examples presented illustrate both the promise and challenge of merging satellite information with in situ observations in state-of-the-art data assimilation models.

Fishman, Jack↗

Tropospheric trace gases

Trace gas concentrations in the atmosphere reflect in part the overall metabolism of the biosphere, and in part the broad range of human activities such as agriculture, production of industrial chemicals, and combustion of fossil fuels and biomass. There is compelling evidence that the composition of the atmosphere is now changing. Observed trends in trace gas levels are reviewed and implications for the chemistry of the atmosphere are discussed. Throughout the discussion, particular emphasis is given to those species which are now increasing in the atmosphere.

Gammon, R.↗

BOREAS TGB-5 CO2, CH4 and CO Chamber Flux Data Over the NSA

The BOReal Ecosystem-Atmosphere Study Trace Gas Biogeochemistry (BOREAS TGB-5) team collected a variety of trace gas concentration and flux measurements at several NSA sites. This data set contains carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO) chamber flux measurements conducted in 1994 at upland forest sites that experienced stand-replacement fires. These measurements were acquired to understand the impact of fires on soil biogeochemistry and related changes in trace gas exchange in boreal forest soils. Relevant ancillary data, including data concerning the soil temperature, solar irradiance, and information from nearby un-burned control sites, are included to provide a basis for modeling the regional impacts of fire and climate changes on trace gas biogeochemistry. The data are provided in tabular ASCII files.

Burke, Roger↗

Carbon monoxide mixing ratio inference from gas filter radiometer data

A new algorithm has been developed which permits, for the first time, real time data reduction of nadir measurements taken with a gas filter correlation radiometer to determine tropospheric carbon monoxide concentrations. The algorithm significantly reduces the complexity of the equations to be solved while providing accuracy comparable to line-by-line calculations. The method is based on a regression analysis technique using a truncated power series representation of the primary instrument output signals to infer directly a weighted average of trace gas concentration. The results produced by a microcomputer-based implementation of this technique are compared with those produced by the more rigorous line-by-line methods. This algorithm has been used in the reduction of Measurement of Air Pollution from Satellites, Shuttle, and aircraft data.

Wallio, H. A.↗

Effects of engine emissions from high-speed civil transport aircraft: A two-dimensional modeling study, part 1

The AER two-dimensional chemistry-transport model is used to study the effect on stratospheric ozone (O3) from operations of supersonic and subsonic aircraft. The study is based on six emission scenarios provided to AER. The study showed that: (1) the O3 response is dominated by the portion of the emitted nitrogen compounds that is entrained in the stratosphere; (2) the entrainment is a sensitive function of the altitude at which the material is injected; (3) the O3 removal efficiency of the emitted material depends on the concentrations of trace gases in the background atmosphere; and (4) evaluation of the impact of fleet operations in the future atmosphere must take into account the expected changes in trace gas concentrations from other activities. Areas for model improvements in future studies are also discussed.

Ko, Malcolm K. W.↗

Implications of AAOE observations for proposed chemical explanations of the seasonal and interannual behavior of Antarctic ozone

Model simulations were used to investigate the seasonal and interannual behavior of ozone for different choices of initial odd nitrogen concentration in July and different assumptions on the heterogeneous reactions, with particular consideration given to the possible contribution of chlorine chemistry to the ozone hole phenomenon. The numerical experiments were selected based on the simulations of the observed trace gas concentrations during the Airborne Antarctic Ozone Experiment in 1987. In all cases considered, the catalytic cycle associated with the formation and photolysis of Cl2O2 could account for more than half of the photochemical removal of O3 within the Antarctic vortex through mid-September. The reaction of BrO with ClO, which accounts for 15-20 percent of O3 removal in the same period, tends to play a more important role toward the end of September, when the concentration of ClO is expected to decrease. No simple relationship was found between the increase in chlorine lavel and the interannual decrease in Antarctic O3.

Ko, M. K. W.↗

Sensitivity of N2O, CFCl3, and CF2Cl2 two-dimensional distributions to O2 absorption cross sections

A good test of the transport and ultraviolet radiation treatment for any model can be based on the consideration of the three gases N2O, CFCl3 (F-11), and CF2Cl2 (F-12). Attention is given to a two-dimensional model which makes it possible to study changes in seasonal and latitudinal distributions which result from O2 cross-section changes. A latitude-dependent ozone decrease has already been predicted by two-dimensional models for chlorofluoromethane (CFM) release. For this reason, it is of interest to determine if a strong latitude-dependent change is detectable in the CFM profiles. One-dimensional models have pointed toward a trend of decreased trace gas concentrations in correlation with decreased O2 cross sections. The O2 cross sections between 180 and 230 nm are changed within a range of experimentlly allowed values. It is found that lower O2 absorption cross sections lead to larger photodissociation rates for the trace gases F-11, F-12, and N2O.

Jackman, C. H.↗

Atmospheric trace gases - Trends and distributions over the last decade

Concentrations of the halocarbons CCl3F (F-11), CCl2F2 (F-12), CCl4, and CH3CCl3, methane (CH4), and nitrous oxide (N2O) over the decade between 1975 and 1985 are reported, based on measurements taken every January at the South Pole and in the Pacific Northwest. The concentrations of F-11, F-12, and CH3CCl3 in both hemispheres are now more than twice their concentrations 10 years ago. However, the annual rates of increase of F-11, F-12, and CH3CCl3 are now considerably slower than earlier in the decade, reflecting in part the effects of a ban on their nonessential uses. Continued increases in these trace gas concentrations may warm the earth and deplete the stratospheric ozone layer, which may cause widespread climatic changes and affect global habitability.

Rasmussen, R. A.↗

Evaluating models of climate and forest vegetation

Understanding how the biosphere may respond to increasing trace gas concentrations in the atmosphere requires models that contain vegetation responses to regional climate. Most of the processes ecologists study in forests, including trophic interactions, nutrient cycling, and disturbance regimes, and vital components of the world economy, such as forest products and agriculture, will be influenced in potentially unexpected ways by changing climate. These vegetation changes affect climate in the following ways: changing C, N, and S pools; trace gases; albedo; and water balance. The complexity of the indirect interactions among variables that depend on climate, together with the range of different space/time scales that best describe these processes, make the problems of modeling and prediction enormously difficult. These problems of predicting vegetation response to climate warming and potential ways of testing model predictions are the subjects of this chapter.

Clark, James S.↗

Evaluation of the 7-km GEOS-5 Nature Run

This report documents an evaluation by the Global Modeling and Assimilation Office (GMAO) of a two-year 7-km-resolution non-hydrostatic global mesoscale simulation produced with the Goddard Earth Observing System (GEOS-5) atmospheric general circulation model. The simulation was produced as a Nature Run for conducting observing system simulation experiments (OSSEs). Generation of the GEOS-5 Nature Run (G5NR) was motivated in part by the desire of the OSSE community for an improved high-resolution sequel to an existing Nature Run produced by the European Centre for Medium-Range Weather Forecasts (ECMWF), which has served the community for several years. The intended use of the G5NR in this context is for generating simulated observations to test proposed observing system designs regarding new instruments and their deployments. Because NASA's interest in OSSEs extends beyond traditional weather forecasting applications, the G5NR includes, in addition to standard meteorological components, a suite of aerosol types and several trace gas concentrations, with emissions downscaled to 10 km using ancillary information such as power plant location, population density and night-light information. The evaluation exercise described here involved more than twenty-five GMAO scientists investigating various aspects of the G5NR performance, including time mean temperature and wind fields, energy spectra, precipitation and the hydrological cycle, the representation of waves, tropical cyclones and midlatitude storms, land and ocean surface characteristics, the representation and forcing effects of clouds and radiation, dynamics of the stratosphere and mesosphere, and the representation of aerosols and trace gases. Comparisons are made with observational data sets when possible, as well as with reanalyses and other long model simulations. The evaluation is broad in scope, as it is meant to assess the overall realism of basic aspects of the G5NR deemed relevant to the conduct of OSSEs. However, because of the relatively short record and other practical considerations, these comparisons cannot provide a definitive, statistically sound assessment of all model deficiencies, or guarantee the G5NR's suitability for all OSSE applications. Differences between the observed and simulated behavior also must be judged in the context of basic internal atmospheric variability which can introduce variations that are not necessarily controlled by the prescribed sea surface temperatures used in generating the G5NR. The results show that the G5NR performs well as measured by the majority of metrics applied in this evaluation. Particular benefits derived from the 7-km resolution of G5NR include realistic representations of extreme weather events in both the tropics and extratropics including tropical cyclones, Nor'easters and mesoscale convective complexes; improved representation of the diurnal cycle of precipitation over land; well-resolved surface-atmosphere interactions such as katabatic wind flows over Antarctica and Greenland; and resolution of orographically generated gravity waves that propagate into the upper atmosphere and influence the large scale circulation. Obvious deficiencies in the G5NR include a "splitting" of the inter-tropical convergence zone, which leads to a weaker-than-observed Hadley circulation and related deficiencies in the depiction of stationary wave patterns. Also, while the G5NR captures global cloud features and radiative effects well in general, close comparison with observations reveals higher-than-observed cloud brightness, likely due to an overabundance of cloud condensate; less distinct cloud minima in subtropical subsidence zones, consistent with a weak Hadley circualtion; and too few near-coastal marine stratocumulus clouds.

GEOS-5↗

Positive water vapour feedback in climate models confirmed by satellite data

It has recently been suggested that GCMs used to evaluate climate change overestimate the greenhouse effect due to increased concentrations of trace gases in the atmosphere. Here, new satellite-generated water vapor data are used to compare summer and winter moisture values in regions of the middle and upper troposphere that have previously been difficult to observe with confidence. It is found that, as the hemispheres warm, increased convection leads to increased water vapor above 500 mbar in approximate quantitative agreement with results from current climate models. The same conclusion is reached by comparing the tropical western and eastern Pacific regions. Thus, water vapor feedback is not overestimated in models and should amplify the climate response to increased trace-gas concentrations.

Rind, D.↗

In-Flight Performance of the Ozone Monitoring Instrument

The Dutch-Finnish Ozone Monitoring Instrument (OMI) is an imaging spectrograph flying on NASA's EOS Aura satellite since 15 July 2004. OMI is primarily used to map trace-gas concentrations in the Earth's atmosphere, obtaining mid-resolution (0.4-0.6 nm) ultraviolet-visible (UV- VIS; 264-504 nm) spectra at multiple (30-60) simultaneous fields of view. Assessed via various approaches that include monitoring of radiances from selected ocean, land ice and cloud areas, as well as measurements of line profiles in the solar spectra, the instrument shows low optical degradation and high wavelength stability over the mission lifetime. In the regions relatively free from the slowly unraveling "row anomaly" (RA) the OMI irradiances have degraded by 3- 8 %, while radiances have changed by 1-2 %. The long-term wavelength calibration of the instrument remains stable to 0.005-0.020 nm.

ultraviolet↗

Electronic Trap-State Modulation in Sm-Doped SnO 2 Nanofibers Enables Ultrasensitive Hydrogen Sensing

The demand for sub-ppm hydrogen (H 2 ) sensing is growing across emerging applications such as environmental monitoring, breath-based disease diagnostics, and early-stage battery failure detection. However, achieving reliable ppb-level detection with chemiresistive metal oxide sensors remains challenging. At trace gas concentrations, resistance modulation is often insufficient, particularly in the absence of noble metal catalysts. Here, we report samarium-doped tin dioxide (Sm-SnO 2 ) nanofibers in which electronic trap-state modulation is exploited to enable ultrasensitive hydrogen sensing. The 2 at% Sm-doped SnO 2 nanofibers exhibited markedly enhanced H 2 sensitivity, achieving clear detection down to 25 ppb H 2 at 200 °C, with a theoretical limit of detection of 4.5 ppb, placing this material among the most sensitive noble-metal-free SnO 2 -based H 2 sensors reported to date. Mechanistic investigations through X-ray photoelectron spectroscopy and electron energy loss spectroscopy revealed that Sm 3+ doping introduces deep trap states associated with charge-compensating defect complexes. These states reduce free carrier density, increase baseline resistance, and enable trap-assisted charge release during H 2 exposure, thereby amplifying the sensing response. Trap-state engineering via rare-earth doping, exemplified by Sm-SnO 2 , provides an effective pathway for achieving ppb-level hydrogen detection in noble-metal-free chemiresistive sensors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Removal of trace gases can both increase and decrease cloud droplet formation

Aerosols consist of liquid or solid particles dispersed in a gas. Aerosol measurements generally rely on drying the particles before quantifying their physicochemical properties. This drying can potentially remove semivolatile compounds from the particles. Here, we show size-resolved cloud condensation nuclei (CCN) measurements quantifying the hygroscopicity parameter in the presence and absence of a denuder. The denuder efficiently removed alkanes and weakly functionalized acids, aldehydes, and alcohols with fewer than 10 carbon atoms from the gas phase. Denuding organic compounds perturbed the CCN-derived hygroscopicity parameter by up to 50%. Denuding either rendered the particles more or less CCN active, and the direction of the effect depended on sample relative humidity and trace gas concentration. The effect was weakest in early spring and strongest in late spring and summer. The measurements demonstrate an unexpectedly strong coupling between the particle and gas phase, influencing CCN activity through either volatilization or surface adsorption, or both.

54 ENVIRONMENTAL SCIENCES↗

Clouds and wet removal as causes of variability in the trace-gas composition of the marine troposphere

A modeling study of the effects of clouds and wet removal on the chemistry of the remote marine troposphere is described. Using a time-dependent model with parameterized vertical transport to calculate trace-gas concentrations, it is found that large variations in key species (e.g., HNO3, H2CO, and H2O2) result from simulations of sporadic rainfall, changes in cloud cover, and external inputs such as surface NO sources. Depending on the frequency and intensity of an event, the effects of these perturbations may persist for several days, thereby invalidating assumptions of photochemical equilibrium in the interpretation of measurements. Long-term integrations with fixed boundary conditions and regularly occurring cloud and rain episodes demonstrate a strong sensitivity of the mean concentration of longer-lived soluble gases to precipitation frequency but also confirm the validity of using properly chosen parameterizations of wet removal in steady state calculations.

Thompson, A. M.↗

Technology needs assessment of an atmospheric observation system for tropospheric research missions, part 1

The technology advancements needed to implement the atmospheric observation satellite systems for air quality research were identified. Tropospheric measurements are considered. The measurements and sensors are based on a model of knowledge objectives in atmospheric science. A set of potential missions and attendant spacecraft and sensors is postulated. The results show that the predominant technology needs will be in passive and active sensors for accurate and frequent global measurements of trace gas concentration profiles.

Alvarado, D. R.↗

Development and operation of a real-time data acquisition system for the NASA, Langley Research Center Differential Absorption Lidar

The capabilities of the DIAL data acquisition system (DAS) for the remote measurement of atmospheric trace gas concentrations from ground and aircraft platforms were extended through the purchase and integration of other hardware and the implementation of improved software. An operational manual for the current system is presented. Hardware and peripheral device registers are outlined only as an aid in debugging any DAS problems which may arise.

Butler, C.↗

Development and operation of a real-time data acquisition system for the NASA-LaRC differential absorption lidar

Computer hardware and software of the NASA multipurpose differential absorption lidar (DIAL) sysatem were improved. The NASA DIAL system is undergoing development and experimental deployment for remote measurement of atmospheric trace gas concentration from ground and aircraft platforms. A viable DIAL system was developed with the capability of remotely measuring O3 and H2O concentrations from an aircraft platform. Test flights were successfully performed on board the NASA/Goddard Flight Center Electra aircraft from 1980 to 1984. Improvements on the DIAL data acquisition system (DAS) are described.

Butler, C.↗