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All sourcesNASA NTRSDOE OSTI
NASA NTRS1987

Airborne intercomparison of nitric oxide measurement techniques

Results from an airborne intercomparison of techniques to measure tropospheric levels of nitric oxide (NO) are discussed. The intercomparison was part of the National Aeronautics and Space Administration's Global Tropospheric Experiment and was conducted during missions flown in the fall of 1983 and spring of 1984. Instruments intercompared included a laser-induced fluorescence (LIF) system and two chemiluminescence instruments (CL). NO mixing ratios from below 5 pptv (parts per trillion by volume) to greater than 100 pptv were reported, with the majority less than 20 pptv. Good correlation was observed between the measurements reported by the CL and LIF techniques. The general level of agreement observed for the ensemble of measurements obtained during the two missions provides the basis from which one can conclude that equally 'valid' measurements of background levels of NO can be expected from either CL or LIF instruments. At the same time the periods of disagreement that were observed between the CL and LIF instruments as well as between the two CL instruments highlight the difficulty of obtaining reliable measurements with NO mixing ratios in the 5-20 pptv range and emphasize the vigilance that should be maintained in future NO measurements.

Hoell, James M., Jr.↗
NASA NTRS1991

Temperature sensitivity of differential absorption lidar measurements of water vapor in the 720-nm region

Recently measured properties of water vapor (H2O) absorption lines have been used in calculations to evalute the temperature sensitivity of differential absorption lidar (Dial) H2O measurements. This paper estimates the temperature sensitivity of H2O lines in the 717-733-nm region for both H2O mixing ratio and number density measurements, and discusses the influence of the H2O line ground state energies E-double-prime, the H2O absorption linewidths, the linewidth temperature dependence parameter, and the atmospheric temperature and pressure variations with altitude and location on the temperature sensitivity calculations. Line parameters and temperature sensitivity calculations for 67 H2O lines in the 720-nm band are given which can be directly used in field experiments. Water vapor lines with E-double-prime values in the 100-300/cm range were found to be optimum for Dial measurements of H2O number densities, while E-double-prime values in the 250-500/cm range were found to be optimum for H2O mixing ratio measurements.

Browell, Edward V.↗
NASA NTRS2015

Formaldehyde Production from Isoprene Oxidation Across NOx Regimes

The chemical link between isoprene and formaldehyde (HCHO) is a strong, non-linear function of NOx (= 27 NO + NO2). This relationship is a linchpin for top-down isoprene emission inventory verification from orbital HCHO column observations. It is also a benchmark for overall mechanism performance with regard to VOC oxidation. Using a comprehensive suite of airborne in situ observations over the Southeast U.S., we quantify HCHO production across the urban-rural spectrum. Analysis of isoprene and its major first-generation oxidation products allows us to define both a "prompt" yield of HCHO (molecules of HCHO produced per molecule of freshly-emitted isoprene) and the background HCHO mixing ratio (from oxidation of longer-lived hydrocarbons). Over the range of observed NOx values (roughly 0.1 - 2 ppbv), the prompt yield increases by a factor of 3 (from 0.3 to 0.9), while background HCHO increases by more than a factor of 2 (from 1.5 to 3.3 ppbv). We apply the same method to evaluate the performance of both a global chemical transport model (AM3) and a measurement-constrained 0-D chemical box model. Both models reproduce the NOx dependence of the prompt HCHO yield, illustrating that models with updated isoprene oxidation mechanisms can adequately capture the link between HCHO and recent isoprene emissions. On the other hand, both models under-estimate background HCHO mixing ratios, suggesting missing HCHO precursors, inadequate representation of later-generation isoprene degradation and/or under-estimated hydroxyl radical concentrations. Moreover, we find that the total organic peroxy radical production rate is essentially independent of NOx, as the increase in oxidizing capacity with NOx is largely balanced by a decrease in VOC reactivity. Thus, the observed NOx dependence of HCHO mainly reflects the changing fate of organic peroxy radicals.

VOC↗
NASA NTRS1981

Comparison of the Nimbus-4 BUV ozone data with the Ames two-dimensional model

Predictions by the Ames two-dimensional model of altitude, latitude and seasonal variations in ozone distribution are compared with the first two years of Nimbus 4 backscattered ultraviolet (BUV) measurements in a preliminary attempt at model verification. The ozone observations consist of mixing ratios on the 1-, 2-, 5-, and 10-mbar pressure surfaces zonally and time averaged to obtain seasonal means for 1970 and 1971. The model is based on chemical reaction and photolysis rate constants recommended by the NASA Panel for Data Evaluation (1979), diurnally averaged for latitudes from 80 deg N to 80 deg S and altitudes from 0 to 60 km with 5 deg horizontal and 2.5 km vertical grid spacings. The large altitude, latitude and seasonal variations observed in the data are found to agree well with model predictions. Examination of the sensitivity of the model predictions to various assumed parameters indicates that improvements in agreement may be obtained by variations of the odd chlorine mixing ratio, odd-nitrogen level and transport parameters.

Borucki, W. J.↗
NASA NTRS2020

Characterizing 15 Years of Saharan-like, Dry, Well-Mixed Air Layers in North Africa

The Saharan Air Layer (SAL) is a dry, well-mixed layer (WML) of warm and sometimes dusty air of nearly constant water vapor mixing ratio generated by the intense surface heating and strong, dry convection in the Sahara Desert, which has notable downstream impacts on the surface energy balance, organized convective system development, seasonal precipitation, and air quality. Characterizing both WMLs and SALs from the existing rawinsonde network has proven challenging because of its sparseness and inconsistent data reporting. Spurred on by this challenge, we previously created a detection methodology and supporting software to automate the identification and characterization of WMLs from multiple data sources including rawinsondes, remote sensing platforms, and model products. We applied our algorithm to each dataset at both its native and at a common (most coarse data product) vertical resolution to detect WMLs and their characteristics (temperature, mixing ratio, AOD, etc.) at each of the 53 rawinsonde launch sites in north Africa.

Nicholls, Stephen D.↗
NASA NTRS2011

Analysis of Oxygen Spectral Lines in the 1.27 Micron Band for the ASCENDS Mission

The ASCENDS mission requires simultaneous laser remote sensing of CO2 and O2 in order to convert CO2 column number densities to average column CO2 mixing ratios (XCO2). As such, the CO2 column number density and the O2 column number density will be utilized to derive the average XCO2 column. NASA Langley Research Center, working with its partners, is developing O2 lidar technology in the 1.26-1.27- m band for surface pressure measurements. The O2 model optical depth calculation is very sensitive to knowledge of the transmitted wavelengths and to the choice of Voigt input parameters. Modeling using the HITRAN database is being carried out to establish the evolution of candidate O2 absorption lines as a function of atmospheric parameters such as altitude, temperature, and pressure. Preliminary results indicate limitations of the Voigt profile and the need to utilize more advanced models which take into account line mixing, line narrowing, and speed dependence. In this paper, we evaluate alternative lineshape models to establish the optimum lineshapes which better account for the variability of individual O2 absorption lines at various atmospheric conditions. The combination of our modeling efforts with accurate laboratory measurements is anticipated to aid in achieving the desired CO2 mixing ratio measurement accuracy requirement of for the ASCENDS mission.

Pliutau, Denis↗
DOE OSTI2021

Chemical Composition of Outbursting Comet C/2015 ER61 (PanSTARRS)

Comet C/2015 ER61 (PanSTARRS) is a long-period Oort cloud comet whose favorable approach to the inner parts of the solar system in 2017 April–May enabled us to characterize its primary volatile composition using the iSHELL spectrograph mounted on the 3 m NASA Infrared Telescope Facility (IRTF) on Maunakea, Hawaii. We used three iSHELL settings (covering ~2.8–5.2 μm) to sample fluorescent emissions from H{sub 2}O, OH, CH{sub 3}OH, HCN, C{sub 2} H{sub 2}, NH{sub 3}, CO, CH{sub 4}, C{sub 2}H{sub 6}, H{sub 2}CO, and OCS on multiple dates ranging from UT 2017 April 15 (shortly after its April 4 outburst) to May 13, nearly 30 days before the detection of its double nucleus. Our observations also offered the opportunity to obtain sensitive 3σ upper limits for cyanoacetylene (HC{sub 3}N). We report rotational temperatures (T{sub rot}), production rates (Qs), abundance (mixing) ratios (relative to H{sub 2}O and C{sub 2}H{sub 6}), and spatial distributions in the coma. ER61 exhibits variability in production rates of many species on short (day-to-day) and long (pre- versus post-perihelion) timescales. The relative abundances of these volatile species remained consistent within uncertainties during our pre-perihelion observations but tended to decrease during our post-perihelion observations (with the exception of CH{sub 3}OH and HCN). The short-timescale variability in the production rates of these volatiles could be due to diurnal effects (over the course of the rotation of the nucleus) and/or the effect of its outburst. The decrease in the production rates and hence the mixing ratios in some volatiles in post-perihelion dates could be due to the presence of seasonal effects in ER61.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1980

Comparison of the Nimbus-4 BUV ozone data with the Ames two-dimensional model

A comparison is made of the first two years of Nimbus 4 backscattered ultraviolet (BUV) ozone measurements with the predictions of the Ames two dimensional model. The ozone observations used consist of the mixing ratio on the 1, 2, 5, and 10 mb pressure surfaces. The data are zone and time averaged to obtain seasonal means for 1970 and 1971 and are found to show strong and repeatable meridional and seasonal dependencies. The model used for comparison with the observations extends from 80 N to 80 S latitude and from altitudes of 0 to 60 km with 5 deg horizontal grid spacing and 2.5 km vertical grid spacing. Chemical reaction and photolysis rates are diurnally averaged and the photodissociation rates are corrected for the effects of scattering. The large altitude, latitude, and seasonal changes in the ozone data agree with the model predictions. Model predictions of the sensitivity of the comparisons to changes in the assumed mixing ratios of water vapor, odd nitrogen, and odd chlorine, as well as to changes in the ambient temperature and transport parameters are also shown.

Borucki, W. J.↗
NASA NTRS2009

Turbulent CO2 Flux Measurements by Lidar: Length Scales, Results and Comparison with In-Situ Sensors

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.

Gilbert, Fabien↗
NASA NTRS2003

Factors Affecting the Evolution of Hurricane Erin and the Distributions of Hydrometeors: Role of Microphysical Processes

Fine-resolution simulations of Hurricane Erin 2001 are conducted using the Penn State University/National Center for Atmospheric Research mesoscale model version 3.5 to investigate the role of thermodynamic, boundary layer and microphysical processes in Erin's growth and maintenance, and their effects on the horizontal and vertical distributions of hydrometeors. Through comparison against radar, radiometer, and dropsonde data collected during the Convection and Moisture Experiment 4, it is seen that realistic simulations of Erin are obtained provided that fine resolution simulations with detailed representations of physical processes are conducted. The principle findings of the study are as follows: 1) a new iterative condensation scheme, which limits the unphysical increase of equivalent potential temperature associated with most condensation schemes, increases the horizontal size of the hurricane, decreases its maximum rainfall rate, reduces its intensity, and makes its eye more moist; 2) in general, microphysical parameterization schemes with more categories of hydrometeors produce more intense hurricanes, larger hydrometeor mixing ratios, and more intense updrafts and downdrafts; 3) the choice of coefficients describing hydrometeor fall velocities has as big of an impact on the hurricane simulations as does choice of microphysical parameterization scheme with no clear relationship between fall velocity and hurricane intensity; and 4) in order for a tropical cyclone to adequately intensify, an advanced boundary layer scheme (e.g., Burk-Thompson scheme) must be used to represent boundary layer processes. The impacts of varying simulations on the horizontal and vertical distributions of different categories of hydrometeor species, on equivalent potential temperature, and on storm updrafts and downdrafts are examined to determine how the release of latent heat feedbacks upon the structure of Erin. In general, all simulations tend to overpredict precipitation rate and hydrometeor mixing ratios. The ramifications of these findings for quantitative precipitation forecasts (QPFs) of tropical cyclones are discussed.

McFarquhar, Greg M.↗
DOE OSTI2025

Measurement report: Extreme heat and wildfire emissions enhance volatile organic compounds in a temperate forest

Climate extremes are projected to cause unprecedented deviations in the emission and transformation of volatile organic compounds (VOCs), which trigger feedback mechanisms that will impact the atmospheric oxidation and formation of aerosols and clouds. However, the response of VOCs to future conditions such as extreme heat and wildfire events is still uncertain. This study explored the modification of the mixing ratio and distribution of several anthropogenic and biogenic VOCs in a temperate oak–hickory–juniper forest as a response to increased temperature and transported biomass burning plumes. A chemical ionization mass spectrometer was deployed on a tower at a height of 32 m in rural central Missouri, United States, for the continuous and in situ measurement of VOCs from June to August of 2023. The maximum observed temperature in the region was 38 °C, and during multiple episodes the temperature remained above 32 °C for several hours. Biogenic VOCs such as isoprene and monoterpene followed closely the temperature daily profile but at varying rates, whereas anthropogenic VOCs were insensitive to elevated temperature. During the measurement period, wildfire emissions were transported to the site and substantially increased the mixing ratios of acetonitrile and benzene, which are produced from burning of biomass. An in-depth analysis of the mass spectra revealed more than 250 minor compounds, such as formamide and methylglyoxal. Extreme heat and presence of wildfire plumes modified the overall volatility, reactivity, O : C, and H : C ratios of the extended list of VOCs. The calculated OH reactivities during extreme temperature condition and transport of biomass burning plumes were 106.37±4.27 and 106.22±5.15 s −1 , respectively, which are substantially higher than background level of 98.78±1.16 s −1 . Multivariate analysis also clustered the compounds into five factors, which highlighted the sources of the unaccounted-for VOCs. Ultimately, results here underscore the effect of extreme heat and wildfire emissions on the overall chemical properties VOC in a temperate forest.

Salvador, Christian Mark [Oak Ridge National Labor↗
NASA NTRS1994

Uniqueness of a solution of a steady state photochemical problem: Applications to Mars

Based on the conservation of chemical elements in chemical reactions, a rule is proved that the number of boundary conditions given by densities and/or non-zero velocities should not be less than the number of chemical elements in the system, and the components given by densities and velocities should include all elements in the system. Applications of this rule to Mars are considered. It is proved that a problem of CO2-H2O chemistry in the lower and middle atmosphere of Mars, say, in the range of 0-80 km does not have an unique solution, if only CO2 and H2O densities are given at the lower boundary, while all other boundary conditions are fluxes. Two models of this type are discussed. These models fit the same boundary conditions, are balanced with a relative uncertainty of 10(exp -4) for H2, and predict the O2, CO, and H2 mixing ratios which differ by order of magnitude. One more species density, e.g. that of O2, should be specified at the boundary to obtain the unique solution. The situation is better if the upper boundary is extended to the exobase where thermal escape velocities of H and H2 can be specified. However, in this case, either oxygen nonthermal escape rate or the O2 density at the surface should be given as the boundary condition. Two models of Mars' photochemistry, with and without nitrogen chemistry, are considered. The oxygen nonthermal escape rate of 1.2 x 10(exp 8) cm(exp -2) s(exp -1) is given at 240 km and is balanced with the total hydrogen escape rate within uncertainty of 1 percent for both models. Both models fit the measured O2 and CO mixing ratios, the O3 line absorption at 9.6 microns, and the O2 1.27 microns dayglow within the uncertainties of the measured values; although, the model without nitrogen chemistry fits better.

Krasnopolsky, V. A.↗
DOE OSTI2021

Statistical Characterization of Temperature and Pressure Vertical Profiles for the Analysis of Laser Heterodyne Radiometry Data

The statistical analysis of historic pressure and temperature profiles from radiosonde launches for use in the fitting of molecular oxygen line shapes is presented. As the O 2 mixing ratio is nearly constant throughout the lower atmosphere, only variations in pressure and temperature profiles will affect the fit of observed O 2 features in Laser Heterodyne Radiometry (LHR) spectra. Radiosonde temperature and pressure data are extracted from the Integrated Global Radiosonde Archive (IGRA) for a given station, date, and launch time. Data may be extracted for a single launch, for the same date over several years, and/or within a window centered on a target date. The temperature and pressure profiles are further characterized by the statistical variation in coefficients of polynomial fits in altitude. The properties of the probability distributions for each coefficient are used to constrain fits of O 2 line shapes through Nelder–Mead optimization. The refined temperature and pressure profiles are then used in the retrieval of vertically resolved mixing ratios for greenhouse gases (GHGs) measured in the same instrument. In continuous collections, each vertical profile determination may be treated as a Bayesian prior to inform subsequent measurements and provide an estimate of uncertainties.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Profiling the molecular destruction rates of temperature and humidity as well as the turbulent kinetic energy dissipation in the convective boundary layer

A simultaneous deployment of Doppler, temperature, and water-vapor lidars is able to provide profiles of molecular destruction rates and turbulent kinetic energy (TKE) dissipation in the convective boundary layer (CBL). Horizontal wind profiles and profiles of vertical wind, temperature, and moisture fluctuations are combined, and transversal temporal autocovariance functions (ACFs) are determined for deriving the dissipation and molecular destruction rates. These are fundamental loss terms in the TKE as well as the potential temperature and mixing ratio variance equations. These ACFs are fitted to their theoretical shapes and coefficients in the inertial subrange. Error bars are estimated by a propagation of noise errors. Sophisticated analyses of the ACFs are performed in order to choose the correct range of lags of the fits for fitting their theoretical shapes in the inertial subrange as well as for minimizing systematic errors due to temporal and spatial averaging and micro- and mesoscale circulations. We demonstrate that we achieve very consistent results of the derived profiles of turbulent variables regardless of whether 1 or 10 s time resolutions are used. We also show that the temporal and spatial length scales of the fluctuations in vertical wind, moisture, and potential temperature are similar with a spatial integral scale of ≈160 m at least in the mixed layer (ML). The profiles of the molecular destruction rates show a maximum in the interfacial layer (IL) and reach values of ϵ m ≃ 7 x 10 -4 g 2 kg −2 s −1 for mixing ratio and ϵ θ ≃ 1.6 x 10 -3 K 2 s −1 for potential temperature. In contrast, the maximum of the TKE dissipation is reached in the ML and amounts to ≃ 10 -2 m 2 s −3 . We also demonstrate that the vertical wind ACF coefficient k w ∝ $\overline{w'^{2}}$ and the TKE dissipation ϵ ∝ ($\overline{w'^{2}}$) 3/2 . For the molecular destruction rates, we show that ϵ m ∝ $\overline{m'^{2}}$ ($\overline{w'^{2}}$) 1/2 and ϵ θ ∝ $\overline{θ'^{2}}$ ($\overline{w'^{2}}$) 1/2 . These equations can be used for parameterizations of ϵ, ϵ m , and ϵ θ . All noise error bars are derived by error propagation and are small enough to compare the results with previous observations and large-eddy simulations. The results agree well with previous observations but show more detailed structures in the IL. Consequently, the synergy resulting from this new combination of active remote sensors enables the profiling of turbulent variables such as integral scales, variances, TKE dissipation, and the molecular destruction rates as well as deriving relationships between them. The results can be used for the parameterization of turbulent variables, TKE budget analyses, and the verification of large-eddy simulations.

dissipation rate↗
DOE OSTI2026

Improved method for temporally interpolating radiosonde profiles in the convective boundary layer

A significantly improved technique for temporally interpolating radiosonde (RS) profiles of potential temperature and water vapor mixing ratio in the planetary boundary layer during daytime is introduced. The key innovation of this technique is its operation on a height grid normalized with the planetary boundary layer height. This study utilized a three-month dataset of three-hourly soundings from the Atmospheric Radiation Measurement Facility's Southern Great Plains site. The technique was evaluated for convective boundary layer cases, with the necessary boundary layer height data obtained from a ground-based infrared spectrometer. A total of 79 comparisons were conducted between reference soundings and interpolated profiles that did and did not employ height normalization. The results demonstrated a substantial improvement in the representation of interpolated profiles using the new technique, characterized by enhanced correlation, improved amplitude representation, and reduced bias for potential temperature, as well as improved correlation and reduced bias for water vapor mixing ratio.

convective boundary layer↗
DOE OSTI2022

The Impact of Nonzenith Elevation Angles on Ground-Based Infrared Thermodynamic Retrievals

Observing thermodynamic profiles within the planetary boundary layer is essential to understanding and predicting atmospheric phenomena because of the significant exchange of sensible and latent heat between the land and atmosphere within that layer. The Atmospheric Emitted Radiance Interferometer (AERI) is a ground-based infrared spectrometer used to obtain the vertical profiles of temperature and water vapor mixing ratio. Most AERIs are only capable of zenith views, although the Marine AERI (M-AERI) has a design that allows it to view various elevation angles. In this study, we quantify the improvement in the information content and accuracy of the retrieved profiles when nonzenith angles are included, as is common with microwave radiometer profilers. The impacts of the additional scan angles are quantified through both a synthetic study and with M-AERI observations from the ARM Cloud Aerosol Precipitation Experiment (ACAPEX) campaign. Furthermore, the simulation study shows that low elevation angles contain more information content for temperature whereas high elevation angles have more information content for water vapor. Outside of very humid environments, the addition of low elevation angles also results in lower root-mean-square errors when compared with high angles for both temperature and water vapor mixing ratio, although this is primarily a result of averaging multiple observations together to reduce instrument noise. Real-world results from the ACAPEX dataset indicate similar results as were found for the simulation study, although not all predicted benefits are realized because of the small sample size and observational uncertainties.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2017

Surface Ozone in the Colorado Northern Front Range and the Influence of Oil and Gas Development During FRAPPE/DISCOVER-AQ in Summer 2014

High mixing ratios of ozone (O3) in the northern Front Range (NFR) of Colorado are not limited to the urban Denver area but were also observed in rural areas where oil and gas activity is the primary source of O3 precursors. On individual days, oil and gas O3 precursors can contribute in excess of 30 ppb to O3 growth and can lead to exceedances of the EPA O3 National Ambient Air Quality Standard. Data used in this study were gathered from continuous surface O3 monitors for June-August 2013-2015 as well as additional flask measurements and mobile laboratories that were part of the FRAPPE/DISCOVER-AQ field campaign of July-August 2014. Overall observed O3 levels during the summer of 2014 were lower than in 2013, likely due to cooler and damper weather than an average summer. This study determined the median hourly surface O3 mixing ratio in the NFR on summer days with limited photochemical production to be approximately 45-55 ppb. Mobile laboratory and flask data collected on three days provide representative case studies of different O3 formation environments in and around Greeley, Colorado. Observations of several gases (including methane, ethane, CO, nitrous oxide) along with O3 are used to identify sources of O3 precursor emissions. A July 23 survey demonstrated low O3 (45-60 ppb) while August 3 and August 13 surveys recorded O3 levels of 75-80 ppb or more. August 3 exemplifies influence of moderate urban and high oil and gas O3 precursor emissions. August 13 demonstrates high oil and gas emissions, low agricultural emissions, and CO measurements that were well correlated with ethane from oil and gas, suggesting an oil and gas related activity as a NOx and O3 precursor source. Low isoprene levels indicated that they were not a significant contributor to O3 precursors measured during the case studies.

Pollution↗
NASA NTRS2001

Stratospheric Age Spectra and Mean Ages from In Situ Observations of Carbon Dioxide

In situ observations of CO2 obtained from 1992 through 2000 using the NASA ER-2 aircraft and high-altitude balloons show that seasonal and interannual variations in CO2 mixing ratios propagate from the troposphere into the lower stratosphere via the tropical tropopause, along with the long-term trend due to fossil fuel combustion. These signals spread laterally and vertically, providing detailed quantitative information about the transport history of sampled air. We have used these data to derive age spectra and mean ages that can be compared with results from models of the stratospheric circulation. For an air parcel at a point in the stratosphere, the age spectrum is defined as the probability distribution function for transit times from the tropical tropopause for each fluid element comprising the parcel. The mean age is the average transit time, corresponding to the first moment of the age spectrum. Age spectra have been derived for altitudes below approximately 20 km for the tropics and for northern midlatitudes where there is sufficient data and where the amplitudes of the seasonal and interannual oscillations in CO2 mixing ratios are large enough to be detected. Tropical age spectra are narrow, with seasonal variation indicating faster ascent during northern winter, consistent with a circulation driven by breaking of extratropical waves. The midlatitude CO2 data are consistent with bimodal age spectra, which could result from a subtropical "barrier" to horizontal exchange over a substantial altitude region. Seasonally resolved mean ages are available with nearly pole-to-pole coverage below 20 km and in the tropics and at middle and high northern latitudes up to the maximum altitude reached by the balloons (approximately 30 km). At ER-2 altitudes, steep meridional gradients in mean age are observed in the subtropics. Between 20 and 30 km, midlatitude air is approximately 2 years older than tropical air at the same altitude. The oldest air sampled was in the Arctic polar vortex with a mean age of .5 plus or minus 0.5 years. This value is much younger than mean ages inferred from simultaneous and previous observations of SF6 in the Arctic vortex, providing evidence for a mesospheric sink for SF6. The mean age in the midlatitude middle stratosphere (approximately 25-32 km) is nearly constant with respect to altitude at 5 plus or minus 0.5 years. Comparison with earlier balloon observations of CO2 dating back to the 1970s shows that the mean age of air in this region has been relatively invariant over the last 25 years.

Andrews, Arlyn E.↗