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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↗

NASA NTRS1998

Lidar Measurements of Tropospheric Wind Profiles with the Double Edge Technique

Research has established the importance of global tropospheric wind measurements for large scale improvements in numerical weather prediction. In addition, global wind measurements provide data that are fundamental to the understanding and prediction of global climate change. These tasks are closely linked with the goals of the NASA Earth Science Enterprise and Global Climate Change programs. NASA Goddard has been actively involved in the development of direct detection Doppler lidar methods and technologies to meet the wind observing needs of the atmospheric science community. A variety of direct detection Doppler wind lidar measurements have recently been reported indicating the growing interest in this area. Our program at Goddard has concentrated on the development of the edge technique for lidar wind measurements. Implementations of the edge technique using either the aerosol or molecular backscatter for the Doppler wind measurement have been described. The basic principles have been verified in lab and atmospheric lidar wind experiments. The lidar measurements were obtained with an aerosol edge technique lidar operating at 1064 nm. These measurements demonstrated high spatial resolution (22 m) and high velocity sensitivity (rms variances of 0.1 m/s) in the planetary boundary layer (PBL). The aerosol backscatter is typically high in the PBL and the effects of the molecular backscatter can often be neglected. However, as was discussed in the original edge technique paper, the molecular contribution to the signal is significant above the boundary layer and a correction for the effects of molecular backscatter is required to make wind measurements. In addition, the molecular signal is a dominant source of noise in regions where the molecular to aerosol ratio is large since the energy monitor channel used in the single edge technique measures the sum of the aerosol and molecular signals. To extend the operation of the edge technique into the free troposphere we have developed a variation of the edge technique called the double edge technique. In this paper a ground based aerosol double edge lidar is described and the first measurements of wind profiles in the free troposphere obtained with this lidar will be presented.

Gentry, Bruce M.↗

NASA NTRS1998

Impact of Tropospheric Aerosol Absorption on Ozone Retrieval from buv Measurements

The impact of tropospheric aerosols on the retrieval of column ozone amounts using spaceborne measurements of backscattered ultraviolet radiation is examined. Using radiative transfer calculations, we show that uv-absorbing desert dust may introduce errors as large as 10% in ozone column amount, depending on the aerosol layer height and optical depth. Smaller errors are produced by carbonaceous aerosols that result from biomass burning. Though the error is produced by complex interactions between ozone absorption (both stratospheric and tropospheric), aerosol scattering, and aerosol absorption, a surprisingly simple correction procedure reduces the error to about 1%, for a variety of aerosols and for a wide range of aerosol loading. Comparison of the corrected TOMS data with operational data indicates that though the zonal mean total ozone derived from TOMS are not significantly affected by these errors, localized affects in the tropics can be large enough to seriously affect the studies of tropospheric ozone that are currently undergoing using the TOMS data.

Torres, O.↗

NASA NTRS1996

A Demonstration of Precise Calibration of Tropospheric Delay Fluctuations with Water Vapor Radiometers

The ability of water vapor radiometers (WVRs) to calibrate changes in tropospheric delay was demonstrated during very long baseline radio interferometer (VLBI) observations at Goldstone, California. WVR measurements reduced the observed VLBI delay variations over a 13 hr period by a factor of approx. = 2.5. When applied to shorter time scales, a approx. = 50% reduction in 100-700 s delay variations was achieved during conditions of high tropospheric activity. Thermal WVR noise precluded calibration of short time scale delay fluctuations during quiet tropospheric conditions.

Teitelbaum, L. P.↗

NASA NTRS1998

A Multi-Instrument Approach for Characterizing the Vertical Structure of Aerosol Properties: Case Studies in the Pacific Basin Troposphere

During February/March 1994, a series of aircraft-based aerosol measurements were carried out in the Pacific Basin troposphere using a differential absorption lidar system deployed by NASA Langley, and optical spectrometer probes and a wire-impactor system operated by NASA Ames. A modified Klett inversion algorithm was applied to extract altitude profiles of aerosol backscattering from the IR lidar signal. The algorithm that we have designed for this purpose utilizes the in situ aerosol measurements to normalize the lidar profile at the aircraft altitude and to supply the lidar ratio as a function of height. The lidar-derived aerosol backscattering coefficients were then compared to the backscattering coefficients calculated from the in situ measurements. During several local aircraft descents, we found good agreement between the remote lidar and in situ results for the absolute value of the aerosol backscattering coefficient and its altitude variation only when we allowed for several layers with different aerosol refractive indices. The agreement validates our lidar calibration method and provides an indication of the variation in aerosol refractive index as a function of altitude. Two of the three case studies performed in this paper reveal layers of anthropogenic aerosols transported long distances into the Pacific Basin troposphere. A third case implies the existence of a layer of dustlike aerosol particles in the lower troposphere, most likely of Asian origin.

Redemann, J.↗

NASA NTRS1999

Seasonal and Interannual Variabilities in Tropical Tropospheric Ozone

This paper presents a detailed characterization of seasonal and interannual variability in tropical tropospheric column ozone (TCO). TCO time series are derived from 20 years (1979-1998) of total ozone mapping spectrometer (TOMS) data using the convective cloud differential (CCD) method. Our study identifies three regions in the tropics with distinctly different zonal characteristics related to seasonal and interannual variability. These three regions are the eastern Pacific, Atlantic, and western Pacific. Results show that in both the eastern and western Pacific seasonal-cycle variability of northern hemisphere (NH) TCO exhibits maximum amount during NH spring whereas largest amount in southern hemisphere (SH) TCO occurs during SH spring. In the Atlantic, maximum TCO in both hemispheres occurs in SH spring. These seasonal cycles are shown to be comparable to seasonal cycles present in ground-based ozonesonde measurements. Interannual variability in the Atlantic region indicates a quasi-biennial oscillation (QBO) signal that is out of phase with the QBO present in stratospheric column ozone (SCO). This is consistent with high pollution and high concentrations of mid-to-upper tropospheric O3-producing precursors in this region. The out of phase relation suggests a UV modulation of tropospheric photochemistry caused by the QBO in stratospheric O3. During El Nino events there is anomalously low TCO in the eastern Pacific and high values in the western Pacific, indicating the effects of convectively-driven transport of low-value boundary layer O3 (reducing TCO) and O3 precursors including H2O and OH. A simplified technique is proposed to derive high-resolution maps of TCO in the tropics even in the absence of tropopause-level clouds. This promising approach requires only total ozone gridded measurements and utilizes the small variability observed in TCO near the dateline. This technique has an advantage compared to the CCD method because the latter requires high-resolution footprint measurements of both reflectivity and total ozone in the presence of tropopause-level cloud tops.

Ziemke, J. R.↗

NASA NTRS1997

Western Pacific Tropospheric Ozone and Potential Vorticity: Implications for Asian Pollution

Tropospheric ozone (03) cross sections measured with lidar from a DC-8 aircraft over the western Pacific correspond closely with potential vorticity (PV). Both are transported from the middle latitude stratosphere, although this is not the only source of 03, and both have sinks in the tropical boundary layer. 03 and PV are good indicators of photochemical and transport process interactions. In summer, some Asian pollution, raised by convection to the upper troposphere, passes southward into the tropics and to the Southern Hemisphere. In winter, subsidence keeps the pollution at low altitudes where it moves over the ocean towards the Inter-Tropical Convergence Zone (ITCZ), with photochemical destruction and secondary pollutant generation occurring en route. Convection raises this modified air to the upper troposphere, where some re may enter the stratosphere. Thus winter Asian pollution may at have a smaller direct influence on the global atmosphere than it would if injected at other longitudes and seasons.

Browell, Edward V.↗