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NASA NTRS1994

Direct measurements of tropospheric ozone using TOMS data

Fishman and Larsen have proposed a new algorithm, called 'tropospheric residual method,' which retrieves the climatological tropospheric ozone by using SAGE (Stratospheric Aerosol and Gas Experiment) and TOMS (Total Ozone Mapping Spectrometer) data. In this paper, we will examine the feasibility of detection for tropospheric ozone using only TOMS data. From a case study over the Atlantic Ocean off the coast of west Africa, it has been found that total ozone in the archived TOMS data has been overestimated over a region of marine-stratocumulus clouds.

Hudson, Robert D.↗
NASA NTRS1994

Use of radon and cosmogenic radionuclides as indicators of exchange between troposphere and stratosphere

This research grant covered participation in the operational phase of NASA's Stratosphere-Troposphere Exchange Project (STEP), a multi-agency airborne science program conducted aboard NASA U-2 and ER-2 high altitude research aircraft. The primary goals of STEP were to investigate the mechanisms of irreversible movement of mass, trace gases, and aerosols from the troposphere into the stratosphere, and to explain the observed dryness of the stratosphere. Three flight experiments were conducted to address these questions: two extratropical experiments, in 1984 and 1986, and a tropical experiment, in 1987. The cosmogenic radionuclides Be-7 and P-32, produced in the stratosphere by cosmic rays, and Rn-222 (radon), emitted from continental soils, were well-suited as tracers of intra-stratospheric air mass movements, and to follow episodes of troposphere to stratosphere exchange. Measurements of Be-7 and P-32 were made in all three STEP experiments. Measurements of radon were made in the tropical experiment only. The equipment worked well, and produced a valuable data set in support of the STEP objectives, as indicated by the 'quick-look' results outlined.

Kritz, Mark A.↗
NASA NTRS1994

A Monte Carlo study of photochemical model uncertainties affecting the calculation of subsonic perturbations in the upper troposphere

Monte Carlo methods are frequently applied to the evaluation of uncertainties in models with multiple inputs that themselves have associated imprecisions. In the case of photochemical models used to evaluate changes in O3 or OH, inputs analyzed include rate coefficients measured in the laboratory, and chemical and physical constituents measured in the atmosphere. The Monte Carlo method was used with the 1-dimensional GSFC tropospheric photochemical model to examine uncertainty propagation to calculation of NO(x) and the major oxidants (O3, OH) in the upper troposphere. In all cases chemical kinetics inputs are varied and the NO(x) perturbation of a subsonic fleet is simulated. A series of model runs is used to explore sensitivities of model-computed parameters to other parameters: heterogeneous processes, the uncertainty in upper tropospheric H2O vapor measurements, aircraft emissions at different latitudes.

Thompson, Anne M.↗
NASA NTRS1995

Study of tropospheric correction for intercontinental GPS common-view time transfer

Current practice is to incorporate general empirical models of the troposphere, which depend only on the station height and the elevation of the satellite, in GPS time receivers used for common-view time transfer. Comparisons of these models with a semi-empirical model based on weather measurements show differences of several nanoseconds. This paper reports on a study of tropospheric correction during GPS common-view time transfer over a short baseline of about 700 km, and three long baselines of 6400 km, 9000 km and 9600 km. It is shown that the use of a general empirical model of the troposphere within a region where the climate is similar does not affect time transfer by more than a few hundreds of picoseconds. For the long distance links, differences between the use of a general empirical model and the use of a semi-empirical model reach several nanoseconds.

Lewandowski, Wlodzimierz W.↗
NASA NTRS1994

Low to middle tropospheric profiles and biosphere/troposphere fluxes of acidic gases in the summertime Canadian taiga

We report features of acidic gases in the troposphere from 9 to 5000 m altitude above ground over the Canadian taiga in the summer of 1990. The measurements were conducted at a 30-m meteorological tower and from the NASA Wallops Electra aircraft as part of the joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B Northern Wetland Studies (NOWES). We sampled air for acidic gases using the mist chamber collector coupled with subsequent analysis using ion chromatography. At the tower we collected samples at two heights during a 13-day period, including diurnal studies. Using eddy flux and profile data, we estimated the biosphere/troposphere fluxes of nitric, formic, and acetic acids and sulfur dioxide. For the organic acids, emissions from the taiga in the afternoon hours and deposition during the predawn morning hours were observed. The flux intensities alone were however not high enough to explain the observed changes in mixing ratios. The measured deposition fluxes of nitric acid were high enough to have a significant influence on its mixing ratio in the boundary layer. On three days we measured vertical profiles of nitric, formic, and acetic acids through the lower to midtroposphere. We found that the chemical composition of the troposphere was extremely heterogenous. Pronounced layers of polluted air were readily apparent from our measurements. Local photochemical production and episodic long-range transport of trace components, originating from biomass burning and possibly industrial emissions, appear to have a strong influence on the composition of the troposphere and biosphere/troposphere fluxes of acidic gases at this site.

Klemm, O.↗
NASA NTRS1994

Summertime tropospheric ozone distributions over central and eastern Canada

Ozone measurements were obtained between the surface and the 6-km altitude on aircraft flights over central and eastern Canada during the summer 1990 NASA Global Tropospheric Experiment Arctic Boundary Layer Expedition (GTE/ABLE 3B). Tropospheric O3 budgets for these regions were observed to be highly variable and significantly impacted by long-range transport and regional scale air mass modification processes. For example, integrated O3 abundance below 5-km altitude averaged 40% and 30% greater in air masses influenced by anthropogenic sources and biomass burning, respectively, than in background (polar) air. Conversely, aged air transported from subtropical areas of the Pacific at times reduced O3 abundance in this height interval by up to 20%. Though intrusion of anthropogenic air was infrequent during the experiment period, the influence of biomass-burning emissions was particularly notable as two thirds of the flights sampled air influenced by plumes from fires burning in Alaska and western Canada. The impinging pollution, both natural and anthropogenic, not only elevated O3 levels directly but also was a source of reactive nitrogen (and nonmethane hydrocarbons) which generally increases the tropospheric lifetime of O3 via moderation of photochemical destruction rates.

Anderson, B. E.↗
NASA NTRS1993

Transport and residence times of tropospheric aerosols inferred from a global three-dimensional simulation of Pb-210

A global three-dimensional model is used to investigate the transport and tropospheric residence time of Pb-210, an aerosol tracer produced in the atmosphere by radioactive decay of Rn-222 emitted from soils. The model uses meteorological input with 4 deg x 5 deg horizontal resolution and 4-hour temporal resolution from the Goddard Institute for Space Studies general circulation model (GCM). It computes aerosol scavenging by convective precipitation as part of the wet convective mass transport operator in order to capture the coupling between vertical transport and rainout. Scavenging in convective precipitation accounts for 74% of the global Pb-210 sink in the model; scavenging in large-scale precipitation accounts for 12%, and scavenging in dry deposition accounts for 14%. The model captures 63% of the variance of yearly mean Pb-210 concentrations measured at 85 sites around the world with negligible mean bias, lending support to the computation of aerosol scavenging. There are, however, a number of regional and seasonal discrepancies that reflect in part anomalies in GCM precipitation. Computed residence times with respect to deposition for Pb-210 aerosol in the tropospheric column are about 5 days at southern midlatitudes and 10-15 days in the tropics; values at northern midlatitudes vary from about 5 days in winter to 10 days in summer. The residence time of Pb-210 produced in the lowest 0.5 km of atmosphere is on average four times shorter than that of Pb-210 produced in the upper atmosphere. Both model and observations indicate a weaker decrease of Pb-210 concentrations between the continental mixed layer and the free troposphere than is observed for total aerosol concentrations; an explanation is that Rn-222 is transported to high altitudes in wet convective updrafts, while aerosols and soluble precursors of aerosols are scavenged by precipitation in the updrafts. Thus Pb-210 is not simply a tracer of aerosols produced in the continental boundary layer, but also of aerosols derived from insoluble precursors emitted from the surface of continents. One may draw an analogy between Pb-210 and nitrate, whose precursor NO(sub x) is sparingly soluble, and explain in this manner the strong correlation observed between nitrate and Pb-210 concentrations over the oceans.

Balkanski, Yves J.↗
NASA NTRS1993

Airborne brightness temperature measurements of the polar winter troposphere as part of the Airborne Arctic Stratosphere Experiment 2 and the effect of brightness temperature variations on the diabatic heating in the lower stratosphere

In this paper we report radiometric measurements of tropospheric brightness temperatures obtained during the AASE 2 experiment. These measurements represent the first attempt to characterize effective radiative temperatures as seen from above the troposphere during the Arctic winter. The reported measurements include brightness temperatures at 6.7 and 10.5 microns as seen from the NASA DC-8 aircraft flying at about 11 km altitude. We also present radiative transfer calculations to estimate the effect of tropospheric brightness temperature on the lower stratospheric heating rates. Because of the recent massive eruption of the Pinatubo volcano, we also discuss the effects of a volcanic aerosol layer. It is concluded that small particles like the volcanic aerosol or polar stratospheric clouds (PSCs) type 1 do not affect stratospheric heating rates by much; on the other hand, larger particles, PSCs types 2 and 3, may have significant effects on heating rates and consequently on dynamics of the lower stratosphere. The dynamical effects of local stratospheric temperature variations are briefly discussed.

Valero, Francisco P. J.↗
NASA NTRS1994

Origin of tropospheric NO(x) over subarctic eastern Canada in summer

The original of NO(X) in the summertime troposphere over subarctic eastern Canada is investigated by photochemical modeling of aircraft and ground-based measurements from the Arctic Boundary Layer Expedition (ABLE 3B). It is found that decomposition of peroxyacetyl nitrate (PAN) can account for most of the NO(X) observed between the surface and 6.2 km altitude (aircraft ceiling). Forest fires represent the principal source of PAN in the region, implying the same origin for NO(X). There is, however, evidence for an unidentified source of NO(X) in occasional air masses subsiding from the upper troposphere. Isoprene emissions from boreal forests maintain high NO(X) concentrations in the continental boundary layer over eastern Canada by scavenging OH and NO3, thus slowing down conversion of NO(X) to HNO3, both in the daytime and at night. This effect is partly compensated by the production of CH3CO3 radicals during isoprene oxidation, which slows down the decomposition of PAN subsiding from the free troposphere. The peroxy radical concentrations estimated from concurrent measurements of NO and NO2 concentrations during ABLE 3B are consistent with values computed from our photochemical model below 4 km, but model values are low at higher altitudes. The discrepancy may reflect either a missing radical source in the model or interferences in the NO2 measurement.

Fan, S.-M↗
NASA NTRS1995

Variability of moisture in the upper troposphere as inferred from TOVS satellite observations and the ECMWF model analyses in 1989

Large-scale variability of moisture in the upper troposphere is examined using TIROS (Television Infrared Observation Satellite) Operational Vertical Sounder (TOVS) satellite observations and European Centre for Medium-Range Weather Forecasts (ECMWF) model analyses from 1989 in the latitude band from 40 deg N to 40 S. To compare these dissimilar datasets, upwelling radiances were computed for the 6-7 micrometer water vapor band from the ECMWF temperature and moisture analyses, and these computed radiances were compared to the corresponding TOVS satellite observations. The ECMWF-based radiances reproduce the general locations and seasonal cycle of the TOVS-observed moisture features, particularly after an improved convective parameterization scheme was adopted by ECMWF in May 1989. However, the ECMWF analysis scheme still results in much milder lateral moisture gradients and seasonal contrasts than indicated by the TOVS observations. Seasonally, the upper troposphere in each hemisphere dries in winter and moistens in summer, but there are regions in each hemisphere that run counter to this seasonal trend, apparently depending on continental- and monsoon-scale dynamics. Dynamically, the TOVS-observed regions of significant subtropical dryness are correlated with persistent subsidence indicated by ECMWF 300-mb vertical velocity analyses. The TOVS radiance observations indicate large variations in space and time of the upper-tropospheric moisture field, which are not fully captured by the ECMWF analyses.

Salathe, Eric P., Jr.↗
NASA NTRS1993

An intercomparison of aircraft instrumentation for tropospheric measurements of sulfur dioxide

As part of the NASA Tropospheric Chemistry Program, a series of field intercomparisons have been conducted to evaluate the state-of-the art for measuring key tropospheric species. One of the objectives of the third intercomparison campaign in this series, Chemical Instrumentation Test and Evaluation 3 (CITE 3), was to evaluate instrumentation for making reliable tropospheric aircraft measurements of sulfur dioxide, dimethyl sulfide, hydrogen sulfide, carbon disulfide, and carbonyl sulfide. This paper reports the results of the intercomparisons of five sulfur dioxide measurement methods ranging from filter techniques, in which samples collected in flight are returned to the laboratory for analyses (chemiluminescent or ion chromatographic), to near real-time, in-flight measurements via gas chromatographic, mass spectrometric, and chemiluminescent techniques. All techniques showed some tendency to track sizeable changes in ambient SO2 such as those associated with altitude changes. For SO2 mixing ratios in the range of 200 pptv to a few ppbv, agreement among the techniques varies from about 30% to several orders of magnitude, depending upon the pair of measurements intercompared. For SO2 mixing ratios less than 200 pptv, measurements from the techniques are uncorrelated. In general, observed differences in the measurement of standards do not account for the flight results. The CITE 3 results do not unambiguously identify one or more of the measurement techniques as providing valid or invalid SO2 measurements, but identify the range of 'potential' uncertainty in SO2 measurements reported by currently available instrumentation and as measured under realistic aircraft environments.

Gregory, Gerald L.↗
NASA NTRS1996

Tropospheric Modeling Improvement

The work performed under this contract provides for the improvement of modeling of troposphere propagation delay in VLBI data, defining of required accuracy of ancillary data type(s) to measure tropospheric behavior, and to develop a clear correspondence between tropospheric behavior and the quality of geodetic VLBI measurements.

Knight, Curtis A.↗
NASA NTRS1996

The effect of aperture averaging upon tropospheric delay fluctuations seen with a DSN antenna

The spectrum of tropospheric delay fluctuations expected for a DSN antenna at time scales less than 100 s has been calculated. A new feature included in these calculations is the effect of aperture averaging, which causes a reduction in delay fluctuations on time scales less than the antenna wind speed crossing time, approximately equal to 5-10 s. On time scales less than a few seconds, the Allan deviation sigma(sub y)(Delta(t)) varies as (Delta(t))(sup +1), rather than sigma(sub y)(Delta(t)) varies as (Delta(t))(exp -1/6) without aperture averaging. Due to thermal radiometer noise, calibration of tropospheric delay fluctuations with water vapor radiometers will not be possible on time scales less than approximately 10 s. However, the tropospheric fluctuation level will be small enough that radio science measurements with a spacecraft on time scales less than a few seconds will be limited by the stability of frequency standards and/or other nontropospheric effects.

Linfield, R.↗
NASA NTRS1996

Tropospheric Modeling Improvement

The work performed under this contract provides for the improvement of modeling of troposphere propagation delay in Very Long Baseline Interferometry (VLBI) data, defining of required accuracy of ancillary data type(s) to measure tropospheric behavior and to develop a clear correspondence between tropospheric behavior and the quality of geodetic VLBI measurements.

Knight, Curtis A.↗
NASA NTRS1997

Adaptation of an In Situ Ground-Based Tropospheric OH/HO2 Instrument for Aircraft Use

In-situ HO(x) (OH and HO2) measurements are an essential part of understanding the photochemistry of aircraft exhaust in the atmosphere. HO(x) affects the partitioning of nitrogen species in the NO(y) family. Its reactions are important sources and sinks for tropospheric ozone, thus providing a link between the NO(x) in aircraft exhaust and tropospheric ozone. OH mixing ratios are enhanced in aircraft wakes due to the photolysis of the HONO that is made close to the engine. Measurements of HO(x) in aircraft wakes, along with NO(x) measurements, thus provides a constraint on chemical models of the engine combustion and exhaust. The development of the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS) is reported. We designed, developed, and successfully flew this instrument. It was part of the instrument complement on board the NASA DC-8 during SUCCESS, which took place in Kansas in April and May, 1996. ATHOS has a limit-of-detection for OH (S/N = 2) of 10(exp 5) OH molecules cm(exp -3) in less than 150 seconds. While this sensitivity is about 2-3 times less than the initial projections in the proposal, it is more than adequate for good measurements of OH and HO2 from the planetary boundary layer to the stratosphere. Our participation in SUCCESS was to be engineering test flights for ATHOS; however, the high-quality measurements we obtained are being used to study HO(x) photochemistry in contrails, clouds, and the clear air.

Brune, William H.↗
NASA NTRS1993

Airborne Brightness Temperature Measurements of the Polar Winter Troposphere as Part of the Airborne Arctic Stratosphere Experiment 2 and the Effect of Brightness Temperature Variations on the Diabatic Heating in the Lower Stratosphere

In this paper we report radiometric measurements of tropospheric brightness temperatures obtained during the AASE 2 experiment. These measurements represent the first attempt to characterize effective radiative temperatures as seen from above the troposphere during the Arctic winter. The reported measurements include brightness temperatures at 6.7 and 10.5 micrometers as seen from the NASA DC-8 aircraft flying at about 11 km altitude. We also present radiative transfer calculations to estimate the effect of tropospheric brightness temperature on the lower stratospheric heating rates. Because of the recent massive eruption of the Pinatubo volcano, we also discuss the effects of a volcanic aerosol layer. It is concluded that small particles like the volcanic aerosol or PSCs type 1 do not affect stratospheric heating rates by much; on the other hand, larger particles, PSCs types 2 and 3, may have significant effects on heating rates and consequently on dynamics of the lower stratosphere. The dynamical effects of local stratospheric temperature variations are briefly discussed.

Valero, Francisoco P. J.↗
NASA NTRS1996

The Effect of Aperture Averaging Upon Tropospheric Delay Fluctuations Seen with a DSN Antenna

The spectrum of tropospheric delay fluctuations expected for a DSN antenna at time scales less than 100 s has been calculated. A new feature included in these calculations is the effect of aperture averaging, which causes a reduction in delay fluctuations on time scales less than the antenna wind speed crossing time, approx. equal to 5-10 s. On time scales less than a few seconds, the Allan deviation sigma(y)(Delta(t)) is proportional to (Delta(t))(exp +1), rather than sigma(y)(Delta(t)) proportional to (Delta(t))(exp -1/6) without aperture averaging. Due to thermal radiometer noise, calibration of tropospheric delay fluctuations with water vapor radiometers will not be possible on time scales less than approx. equal to 10 s. However, the tropospheric fluctuation level will be small enough that radio science measurements with a spacecraft on time scales less than a few seconds will be limited by the stability of frequency standards and/or other nontropospheric effects.

Linfield, R.↗
NASA NTRS1998

Upper tropospheric water vapor: A field campaign of two Raman lidars, Airborne hygrometers, and Radiosondes

Water vapor in the atmosphere plays an important role in radiative transfer and the process of radiative balance so critical for understanding global change. It is the principal ingredient in cloud formation, one of the most difficult atmospheric processes to model, and the most variable component of the Earth-atmosphere albedo. And as a free molecule, it is the most active infrared absorber and emitter, thus, the most important greenhouse gas. The radiative impact of water vapor is important at all levels of the atmosphere. Even though moisture decreases by several orders-of-magnitude from the Earth's surface to the tropopause, recent research has shown that, from a radiative standpoint, a small percentage change in water vapor at any level is nearly equivalent. Therefore accurate and precise measurements of this important atmospheric constituent are needed at all levels to evaluate the full radiative impact. The need for improved measurements in the upper troposphere is particularly important because of the generally hostile (very dry and cold) conditions encountered. Because of the importance of water vapor to the understanding of radiative transfer, the Department of Energy's Atmospheric Radiation Measurements (ARM) program initiated a series of measurement campaigns at the Cloud And Radiation Testbed (CART) site in Oklahoma, especially focused on atmospheric water vapor. Three water vapor intensive observation period (water vapor IOP) campaigns were planned. Two of the water vapor IOP campaigns have been completed: the first IOP was held during the fall of 1996 with a focus on boundary layer water vapor measurements, and the second was conducted during the fall of 1997 with a focus on both boundary layer moisture e and moisture in the upper troposphere. This paper presents a review of the intercomparisons of water vapor measurements in the upper troposphere aquired during the second water vapor IOP. Data to be presented include water vapor measurements ements from: two Raman Lidars, the NASA Goddard Scanning Raman Lidar (SRL) and the CART Raman Lidar (CARL), a number of Vaisala radiosondes launched during the IOP campaign, and a dew point hygrometer flown on the University of North Dakota Cessna Citation Aircraft.

Melfi, S. Harvey↗