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In this paper we evaluate new retrievals of the deuterium content of water vapor from the Aqua Atmospheric InfraRed Sounder (AIRS), with aircraft measurements of HDO and H2O from the ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) field mission. Single-footprint AIRS radiances are processed with an optimal estimation algorithm that provides vertical profiles of the HDO∕H2O ratio, characterized uncertainties and instrument operators (i.e., averaging kernel matrix). These retrievals are compared to vertical profiles of the HDO∕H2O ratio from the Oregon State University Water Isotope Spectrometer for Precipitation and Entrainment Research (WISPER) on the ORACLES NASA P-3B Orion aircraft. Measurements were taken over the southeastern Atlantic Ocean from 31 August to 25 September 2016. HDO∕H2O is commonly reported in δD notation, which is the fractional deviation of the HDO∕H2O ratio from the standard reference ratio. For collocated measurements, the satellite instrument operator (averaging kernels and a priori constraint) is applied to the aircraft profile measurements. We find that AIRS δD bias relative to the aircraft is well within the estimated measurement uncertainty. In the lower troposphere, 1000 to 800 hPa, AIRS δD bias is −6.6 ‰ and the root-mean-square (rms) deviation is 20.9 ‰, consistent with the calculated uncertainty of 19.1 ‰. In the mid-troposphere, 800 to 500 hPa, AIRS δD bias is −6.8 ‰ and rms 44.9 ‰, comparable to the calculated uncertainty of 25.8 ‰.

This study presents a simulated simultaneous retrieval of mass mean cloud ice particle effective diameter, ice water content, water vapor, and temperature profiles using a combination of a 94‐GHz cloud radar and multifrequency (118, 183, 240, 310, 380, 664, and 850 GHz) millimeter‐ and submillimeter‐wave radiometers from a space platform. The retrieval capabilities and uncertainties of the combined radar and microwave radiometers are quantified. We show that this combined active and passive remote sensing approach with SmallSat technologies addresses a gap in the current state‐of‐the‐art remote sensing measurements of ice cloud properties, especially deriving vertical profiles of ice cloud particle sizes in the atmosphere together with the ambient thermodynamic conditions. Therefore, this new approach can serve as a plausible candidate for future missions that target cloud and precipitation processes to improve weather forecasts and climate predictions.

Remote imaging spectroscopy's role in Earth science will grow in the coming decade as a series of globe-spanning spectroscopy missions launch from NASA, ESA, and other agencies. The nature of remote imaging spectroscopy will change, advancing from short regional studies to address global multi-year questions. The diversity of data will also grow with exposure to a wider range of biomes and atmospheric conditions. To execute these new investigations we must reconcile diverse observing conditions to derive consistent global maps. To this end, rigorous uncertainty quantification and propagation enables an optimal synthesis of data accounting for observing conditions and data quality. Understanding data uncertainties is also important for principled hypothesis testing, information content assessment, and informed decision making by end users. We survey prior efforts in uncertainty quantification for imaging spectroscopy, and describe methods for validating the accuracy of uncertainty predictions. We conclude with a discussion of remaining challenges and promising avenues for future research. © (2020) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.

The evolution of the Amazon forest is tightly coupled to its terrestrial water balance (evapotranspiration minus precipitation, or ET-P), as an increase in ET-P reduces soil moisture, increasing water stress. However, large differences of ~ 50% between current monthly estimates of ET-P make it challenging to confidently quantify its spatio-temporal distribution and evolution. Here, we show that new satellite observations of the HDO/H2O ratio of water vapor, spanning 2003 to 2020, constrain estimates of the Amazon water balance with monthly precision of ~ 20%. The HDO/H2O ratio of water vapor is sensitive to the difference between ET and P, rather than to either flux alone, because lighter isotopes preferentially evaporate and heavier isotopes preferentially condense. Consequently, variable bias and sensitivity errors that result from combining different ET and precipitation products are minimized with this proxy. Our analysis demonstrates these data can quantify the spatial patterns of Amazon water balance from monthly to interannual time scales.

Atmospheric isotopologues of water vapor (e.g., HDO) are important tracers for understanding Earth’s hydrological cycles. Most remote sensing measurements of these isotopologues, however, are colum...

Remote spectroscopy of terrestrial ecosystems generally falls into one of two categories: UV, Visible and ShortWave InfraRed (VSWIR) methods measuring reflected solar illumination, and Thermal InfraRed (TIR) methods measuring radiation emitted from the Earth's surface. Both interpret the measured radiance with inversion algorithms that estimate surface reflectance, emissivity, surface temperatures, and the atmospheric state. However, the two regimes have traditionally used independent inversion methods. Here we present the first simultaneous inversion of the upwelling radiance spectrum from the UV through the VSWIR and the Thermal Infrared. Maximum A Posteriori estimation determines the surface and atmosphere state that is most consistent with measured radiance across the entire range. We find that the complementary information in the two intervals improves estimates of atmospheric properties, surface emissivity, and surface temperature. Posterior uncertainty is 40% lower in surface temperature and 60% in air temperature. Spurious correlations between atmospheric and surface state are also reduced, with 90% lower correlated uncertainty between total column water vapor and both surface and air temperature. Temperature-emissivity separation also improves, with a 33% reduction in correlated posterior uncertainty between the parameters. We demonstrate the method on coincident data from the Classic Airborne Visible Infrared Imaging Spectrometer (AVIRIS-C) operating in the VSWIR range, and the Hyperspectral Thermal Emission Spectrometer (HyTES) in the TIR range, during flights on NASA's high-altitude ER-2 aircraft. Measurements spanning 0.4 to 12 microns can improve estimates of surface and atmospheric properties, significantly advancing studies in terrestrial ecosystems, geology, agriculture, and urban management.

In this paper we evaluate new retrievals of the deuterium content of water vapor from the Aqua Atmospheric InfraRed Sounder (AIRS) with aircraft measurements of HDO and H2O from the ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) field mission. Single footprint AIRS radiances are processed with an optimal estimation algorithm that provides a vertical profile of the HDO/H2O ratio, characterized uncertainties, and instrument operators (or averaging kernel matrix). These retrievals are compared to vertical profiles of the HDO/H2O from the Oregon State University Water Isotope Spectrometer for Precipitation and Entrainment Research (WISPER) on the ORACLES NASA P-3B Orion aircraft. Measurements were taken over the Southeast Atlantic Ocean from 31 August to 25 September 2016. HDO/H2O is commonly reported in delta-D notation, which is the fractional deviation of the HDO/H2O ratio from the standard reference ratio. For collocated measurements, the satellite operator (averaging kernels and a priori constraint) is applied to the aircraft profile measurements. We find that AIRS delta-D bias relative to the aircraft is well within the estimated measurement uncertainty. In the lower troposphere, 1000 to 800 hPa, AIRS delta-D bias is −6.6‰ and the Root Mean Square (RMS) deviation is 20.9‰, consistent with the calculated uncertainty of 19.1‰. In the mid-troposphere, 800 to 500 hPa, AIRS delta-D bias is 6.8‰ and RMS 44.9‰, comparable to the calculated uncertainty of 25.8‰.

Single-pixel tropospheric retrievals of HDO and H2O concentrations are retrieved from Atmospheric Infrared Sounder (AIRS) radiances using the optimal estimation algorithm developed for the Aura Tropospheric Emission Spectrometer (TES) project. We evaluate the error characteristics and vertical sensitivity of AIRS measurements corresponding to 5 d of TES data (or five global surveys) during the Northern Hemisphere summers between 2006 and 2010 (∼600 co-located comparisons per day). We find that the retrieval characteristics of the AIRS deuterium content measurements have similar vertical resolution in the middle troposphere as TES but with slightly less sensitivity in the lowermost troposphere, with a typical degrees of freedom (DOFS) in the tropics of 1.5. The calculated measurement uncertainty is ∼30 ‰ (parts per thousand relative to the deuterium composition of ocean water) for a tropospheric average between 750 and 350 hPa, the altitude region where AIRS is most sensitive, compared to ∼15 ‰ for the TES data. Comparison with the TES data also indicates that the uncertainty of a single target AIRS HDO ∕ H2O measurement is ∼30 ‰. Comparison of AIRS and TES data between 30∘ S and 50∘ N indicates that the AIRS data are biased low by ∼-2.6 ‰ with a latitudinal variation of ∼7.8 ‰. This latitudinal variation is consistent with the accuracy of TES data compared to in situ measurements, suggesting that both AIRS and TES have similar accuracy.

The EOS (Earth Observing System) Aura Tropospheric Emission Spectrometer (TES) retrieves the atmospheric HDO / H2O ratio in the mid-to-lower troposphere as well as the planetary boundary layer. TES observations of water vapor and the HDO isotopologue have been compared with nearly coincident in situ airborne measurements for direct validation of the TES products. The field measurements were made with a commercially available Picarro L1115-i isotopic water analyzer on aircraft over the Alaskan interior boreal forest during the three summers of 2011 to 2013. TES special observations were utilized in these comparisons. The TES averaging kernels and a priori constraints have been applied to the in situ data, using version 5 (V005) of the TES data. TES calculated errors are compared with the standard deviation (1σ) of scan-to-scan variability to check consistency with the TES observation error. Spatial and temporal variations are assessed from the in situ aircraft measurements. It is found that the standard deviation of scan-to-scan variability of TES δD is ±34.1‰ in the boundary layer and ± 26.5‰ in the free troposphere. This scan-to-scan variability is consistent with the TES estimated error (observation error) of 10–18‰ after accounting for the atmospheric variations along the TES track of ±16‰ in the boundary layer, increasing to ±30‰ in the free troposphere observed by the aircraft in situ measurements. We estimate that TES V005 δD is biased high by an amount that decreases with pressure: approximately +123‰ at 1000 hPa, +98‰ in the boundary layer and +37‰ in the free troposphere. The uncertainty in this bias estimate is ±20‰. A correction for this bias has been applied to the TES HDO Lite Product data set. After bias correction, we show that TES has accurate sensitivity to water vapor isotopologues in the boundary layer.

[1] TES (Tropospheric Emission Spectrometer) nadir and MLS (Microwave Limb Sounder) limb measurements from the Aura satellite are used to jointly estimate an atmospheric carbon monoxide (CO) profile with extended vertical range compared to profiles retrieved from the individual measurement. We describe the algorithms, the processing procedures, the prototyping results, and the evaluations for this new joint product. TES and MLS “stand-alone” CO profile retrievals are largely complementary, with TES being largely sensitive to lower to middle troposphere while MLS measures CO in the upper troposphere and above. We pair TES nadir and MLS limb tangent locations within 6–8 min and within 220 km. The paired radiance measurements of the two instruments in each location are optimally combined to retrieve a single CO profile along with other trace gases whose signal interferes with that from CO. This combined CO profile has a vertical resolution and vertical range that is an improvement over the two stand-alone products, especially in the upper troposphere/lower stratosphere. For example, the degrees of freedom for signal (DOFS) between surface and 50 hPa for TES alone are

The NASA ER-2 aircraft sampled the lower stratosphere over North America during the field mission for the NASA Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS). This study reports observations of convectively influenced air parcels with enhanced water vapor in the overworld stratosphere over the summertime continental United States and investigates three case studies in detail. Water vapor mixing ratios greater than 10 ppmv, which is much higher than the background 4 to 6 ppmv of the overworld stratosphere, were measured by the JPL Laser Hygrometer (JLH Mark2) at altitudes between 16.0 and 17.5 km (potential temperatures of approximately 380 to 410 K). Overshooting cloud tops (OTs) are identified from a SEAC4RS OT detection product based on satellite infrared window channel brightness temperature gradients. Through trajectory analysis, we make the connection between these in situ water measurements and OT. Back trajectory analysis ties enhanced water to OT 1 to 7 days prior to the intercept by the aircraft. The trajectory paths are dominated by the North American monsoon (NAM) anticyclonic circulation. This connection suggests that ice is convectively transported to the overworld stratosphere in OT events and subsequently sublimated; such events may irreversibly enhance stratospheric water vapor in the summer over Mexico and the United States. A regional context is provided by water observations from the Aura Microwave Limb Sounder (MLS).

We compare Tropospheric Emission Spectrometer (TES) versions 3 and 4, V003 and V004, respectively, nadir-stare ozone profiles with ozonesonde profiles from the Arctic Intensive Ozonesonde Network Study (ARCIONS, http://croc.gsfc.nasa.gov/arcions/ during the Arctic Research on the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field mission. The ozonesonde data are from launches timed to match Aura's overpass, where 11 coincidences spanned 44° N to 71° N from April to July 2008. Using the TES "stare" observation mode, 32 observations are taken over each coincidental ozonesonde launch. By effectively sampling the same air mass 32 times, comparisons are made between the empirically-calculated random errors to the expected random errors from measurement noise, temperature and interfering species, such as water. This study represents the first validation of high latitude (>70°) TES ozone. We find that the calculated errors are consistent with the actual errors with a similar vertical distribution that varies between 5% and 20% for V003 and V004 TES data. In general, TES ozone profiles are positively biased (by less than 15%) from the surface to the upper-troposphere (~1000 to 100 hPa) and negatively biased (by less than 20%) from the upper-troposphere to the lower-stratosphere (100 to 30 hPa) when compared to the ozonesonde data. Lastly, for V003 and V004 TES data between 44° N and 71° N there is variability in the mean biases (from −14 to +15%), mean theoretical errors (from 6 to 13%), and mean random errors (from 9 to 19%).

The composition of residual particles from evaporated cirrus ice crystals near the tropical tropopause as well as unfrozen aerosols were measured with a single particle mass spectrometer. Subvisible cirrus residuals were predominantly composed of internal mixtures of neutralized sulfate with organic material and were chemically indistinguishable from unfrozen sulfate-organic aerosols. Ice residuals were also similar in size to unfrozen aerosol. Heterogeneous ice nuclei such as mineral dust were not enhanced in these subvisible cirrus residuals. Biomass burning particles were depleted in the residuals. Cloud probe measurements showing low cirrus ice crystal number concentrations were inconsistent with conventional homogeneous freezing. Recent laboratory studies provide heterogeneous nucleation scenarios that may explain tropopause level subvisible cirrus formation.

Water vapor mixing ratio retrieval using the Howard University Raman lidar is presented with emphasis on three aspects: (i) comparison of the lidar with collocated radiosondes and Raman lidar, (ii) investigation of the relationship between atmospheric state variables and the relative performance of the lidar and sonde (in particular, their poor agreement), and (iii) comparison with satellite-based measurements. The measurements were acquired during the Water Vapor Validation Experiment Sondes/Satellites 2006 campaign. Ensemble averaging of water vapor mixing ratio data from 10 nighttime comparisons with Vaisala RS92 radiosondes shows, on average, an agreement within ±10%, up to ∼8 km. A similar analysis of lidar-to-lidar data of over 700 profiles revealed an agreement to within 20% over the first 7 km (10% below 4 km). A grid analysis, defined in the temperature–relative humidity space, was developed to characterize the lidar–radiosonde agreement and quantitatively localizes regions of strong and weak correlations as a function of altitude, temperature, or relative humidity. Three main regions of weak correlation emerge: (i) regions of low relative humidity and low temperature, (ii) regions of moderate relative humidity at low temperatures, and (iii) regions of low relative humidity at moderate temperatures. Comparison of Atmospheric Infrared Sounder and Tropospheric Emission Sounder satellite retrievals of moisture with those of Howard University Raman lidar showed a general agreement in the trend, but the satellites miss details in atmospheric structure because of their low resolution. A relative difference of about ±20% is usually found between lidar and satellite measurements for the coincidences available.

One consequence of the evidence-based practice movement is the proliferation of manualized interventions. Clinicians voice a number of concerns about the use of treatment manuals. These include concerns that manuals impede the therapeutic relationship and discourage flexibility in addressing the individual needs of clients. One manualized intervention called parent—child interaction therapy (PCIT) has shown exceptional promise in the treatment of child behavioral problems. PCIT is a parent-mediated behavioral intervention aimed at reducing externalizing behaviors in children by changing parenting practices. The manual includes session scripts for clinicians, a proscribed sequence of intervention activities, and checklists for clinicians and parents to document that intervention is completed in the prescribed manner. Three cases are presented in which clients vary by personal characteristics and individual needs. Case descriptions reveal how this manualized intervention was adapted successfully to address the needs of a variety of families. Implications for therapeutic relationship are also discussed.

Persistent contrails are a common feature of the upper troposphere. We describe two methods for intercomparing and evaluating RHi measurements in a persistent contrail with calculated or expected values. The methods were applied to measurements made in the upper troposphere on board an NASA WB-57F aircraft while sampling its own contrail. Included in the analysis are measurements of water vapor pressure, temperature, ice particle number and size, and nitric oxide (NO). The systematic use of these contrail-sampling methods in future studies will improve our understanding of contrail microphysics and the performance of fast-response water and temperature measurements.

Measurements are presented that were acquired from the National Aeronautics and Space Administration (NASA) DC-8 aircraft during an intensive 3-day study of Tropical Storm/Hurricane Humberto on 22, 23, and 24 September 2001. Particle size distributions, particle image information, vertical velocities, and single- and dual-wavelength Doppler radar observations were obtained during repeated sampling of the eyewall and outer eye regions. Eyewall sampling temperatures ranged from −22° to −57°C and peak updraft velocities from 4 to 15 m s−1. High concentrations of small ice particles, in the order 50 cm−3 and above, were observed within and around the updrafts. Aggregates, some larger than 7 mm, dominated the larger sizes. The slope of the fitted exponential size distributions λ was distinctly different close to the eye than outside of that region. Even at low temperatures, λ was characteristic of warm temperature growth (λ < 30 cm−1) close to the eye and characteristic of low temperature growth outside of it as well (λ > 100 cm−1). The two modes found for λ are shown to be consistent with observations from nonhurricane ice cloud layers formed through deep convection, but differ markedly from ice cloud layers generated in situ. It is shown that the median, mass-weighted, terminal velocities derived for the Humberto data and from the other datasets are primarily a function of λ. Microphysical measurements and dual wavelength radar observations are used together to infer and interpret particle growth processes. Rain in the lower portions of the eyewall extended up to the 6- or 7-km level. In the outer eye regions, aggregation progressed downward from between 8.5 and 11.9 km to the melting layer, with some graupel noted in rainbands. Homogeneous ice nucleation is implicated in the high concentrations of small ice particles observed in the vicinity of the updrafts.

Airborne in situ measurements over the eastern Pacific Ocean in January 2004 have revealed a new category of nitric acid (HNO3)-containing particles in the tropical lower stratosphere. These particles are most likely composed of nitric acid trihydrate (NAT). They were intermittently observed in a narrow layer above the tropopause (18±0.1 km) and over a broad geographic extent (>1100 km). In contrast to the background liquid sulfate aerosol, these particles are solid, much larger (1.7-4.7 µm vs.0.1µm in diameter), and significantly less abundant (-4 cm-3 vs.10 cm-3). Microphysical trajectory models suggest that the NAT particles grow over a 6-14 day period in supersaturated air that remains close to the tropical tropopause and might be a common feature in the tropics. The small number density of these particles implies a highly selective or slow nucleation process. Understanding the formation of solid NAT particles in the tropics could improve our understanding of stratospheric nucleation processes and, therefore, dehydration and denitrification.

Recent in situ measurements at tropical tropopause temperatures as low as 187 K indicate supersaturations with respect to ice exceeding 100% with little or no ice present. In contrast, models used to simulate cloud formation near the tropopause assume a supersaturation threshold for ice nucleation of about 65% based on laboratory measurements of aqueous aerosol freezing. The high supersaturations reported here, along with cloud simulations assuming a plausible range of temperature histories in the sampled air mass, indicate that the vast majority of aerosols in the air sampled on this flight must have had supersaturation thresholds for ice nucleation exceeding 100% (i.e. near liquid water saturation at these temperatures). Possible explanations for this high threshold are that (1) the expressions used for calculating vapor pressure over supercooled water at low temperatures give values are at least 20% too low, (2) organic films on the aerosol surfaces reduce their accommodation coefficient for uptake of water, resulting in aerosols with more concentrated solutions when moderate-rapid cooling occurs and correspondingly inhibited homogeneous freezing, and (3) if surface freezing dominates, organic coatings may increase the surface energy of the ice embryo/vapor interface resulting in suppressed ice nucleation. Simulations of in situ cloud formation in the tropical tropopause layer (TTL) throughout the tropics indicate that if decreased accommodation coefficients and resulting high thresholds for ice nucleation prevailed throughout the tropics, then the calculated occurrence frequency and areal coverage of TTL cirrus would be significantly suppressed. However, the simulations also show that even if in situ TTL cirrus form only over a very small fraction of the tropics in the western Pacific, enough air passes through them due to rapid horizontal transport such that they can still effectively freeze-dry air entering the stratosphere. The TTL cirrus simulations show that even if very large supersaturations are required for ice nucleation, these large supersaturations should occur very rarely.

We use in situ measurements of CO obtained in the tropics from 1995 to 1997 on the NASA ER-2 aircraft and a simple photochemical model to calculate the elapsed time between the entry of air into the stratosphere and the observation, which we define as the photochemical age of the air. Assuming this age represents the transit time of the air mass from a boundary at 390 K to its measured altitude, we calculate boundary condition values of CO 2 derived from in situ measurements of this species from 400 to 480 K. We validate the approach by comparing these CO 2 boundary values with an independent representation of the boundary condition from observations of CO 2 in air that had recently entered the stratosphere (as indicated by simultaneous measurements of N 2 O, CO, and potential temperature). For five of the six flights, differences between CO 2 boundary condition values determined using the photochemical age of the air and those derived from independent measurements can be accounted for with isentropic mixing of midlatitude stratospheric air into the tropics. Having validated the photochemical ages of the sampled stratospheric air, we use the same analysis of in situ water data to provide water vapor boundary condition values that constrain the seasonal cycle of water vapor entering the stratosphere. On the basis of these constraints we evaluate the seasonal cycle of entry-level water vapor derived from tropical tropopause temperatures from the radiosonde network between 10°S and 10°N. We conclude that while average saturation mixing ratios provide a suitable boundary condition for water vapor entering the stratosphere, the uncertainties in saturation mixing ratios derived from radiosonde temperatures and the lack of coverage prevents distinguishing between ascent preferentially occurring over the western equatorial Pacific or throughout the tropics. With the assumption that vertical diffusion and midlatitude mixing have a negligible effect on the calculated age, ascent velocities can be inferred from the photochemical ages. These ascent velocities show a seasonal cycle that is inconsistent with our current understanding of the dynamics driving the stratospheric circulation and with independent estimates of tropical vertical ascent rates.

Observations in the 1999-2000 Arctic winter stratosphere show the most severe and extensive denitrification ever observed in the northern hemisphere. Denitrification was inferred from in situ measurements conducted during high-altitude aircraft flights between January and March 2000. Average removal of more than 60% of the reactive nitrogen reservoir (NO y ) was observed in air masses throughout the core of the Arctic vortex. Denitrification was observed at altitudes between 16 and 21 km, with the most severe denitrification observed at 20 to 21 km. Nitrified air masses were also observed, primarily at lower altitudes. These results show that denitrification in the Arctic lower stratosphere can approach the severity and extent of that previously observed only in the Antarctic.

Nitrous oxide (N 2 O) and methane (CH 4 ) were measured in the upper troposphere and lower stratosphere by multiple instruments aboard the NASA ER-2 aircraft during the 1995-1996 Stratospheric Tracers of Atmospheric Transport (STRAT) and 1997 Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) campaigns. Differences between coincidental, in situ measurements are examined to evaluate the agreement and variability in the agreement between these instruments during each flight. Mean N 2 O measurement differences for each flight were much smaller than limits calculated from quoted values of N 2 O measurement accuracy and for all but two flights were ≤8.7 ppb (3.5%). Mean CH 4 measurement differences for flights were similarly much smaller than calculated limits and for all but three flights were ≤65 ppb (4.4%). Typical agreement between instruments during flights averaged 6.2 ppb (2.5%) for N 2 O and 43 ppb (2.9%) for CH 4 . In contrast, for about half of the flights, the variability of N 2 O and CH 4 measurement differences exceeded limits calculated from quoted values of measurement precision. The typical measurement difference variability (1σ) during a flight averaged ±8.0 ppb (3.2%) for N 2 O and ±43 ppb (2.9%) for CH 4 . For some flights, large differences or variations in differences are attributable to the poor measurement accuracy or precision of one instrument. It is demonstrated that small offsets between the computer clocks of these instruments can result in significant differences between their coincidental N 2 O and CH 4 data, especially when there is high spatial variability in tracer abundance along a flight track.

We use the correlation between CH(sub 4) and N(sub 2)O as measured during the POLARIS campaign in spring 1997 to estimate the degree of mixing between descended air masses from the vortex and air masses from mid-latitudes.

A suite of compounds with a wide range of photochemical lifetimes (3 months to several decades) was measured in the tropical and midlatitude upper troposphere and lower stratosphere during the Stratospheric Tracers of Atmospheric Transport (STRAT) experiment (fall 1995 and winter, summer, and fall 1996) and the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) deployment in late summer 1997. These species include various chlorofluorocarbons, hydrocarbons, halocarbons, and halons measured in whole air samples and CO measured in situ by tunable diode laser spectroscopy. Mixing ratio profiles of long-lived species in the tropical lower stratosphere are examined using a one-dimensional (1-D) photochemical model that includes entrainment from the extratropical stratosphere and is constrained by measured concentrations of OH. Profiles of tracers found using the 1-D model agree well with all the observed tropical profiles for an entrainment time scale of 8.5 -4 +6 months, independent of altitude between potential temperatures of 370 and 500 K. The tropical profile of CO is used to show that the annually averaged ascent rate profile, on the basis of a set of radiative heating calculations, is accurate to approximately ±44%, a smaller uncertainty than found by considering the uncertainties in the radiative model and its inputs. Tropical profiles of ethane and C 2 Cl 4 reveal that the concentration of Cl is higher than expected on the basis of photochemical model simulations using standard gas phase kinetics and established relationships between total inorganic chlorine and CFC-11. Our observations suggest that short-lived organic chlorinated compounds and HCI carried across the tropical tropopause may provide an important source of inorganic chlorine to the tropical lower stratosphere that has been largely unappreciated in previous studies. The entrainment timescale found here is considerably less than the value found by a similar study that focused on observations obtained in the lower stratosphere during 1994. Several possible explanations for this difference are discussed.

In situ measurements of CO were made in the upper troposphere and lower stratosphere (7–21 km altitude) with the Jet Propulsion Laboratory (JPL) Aircraft Laser Infrared Absorption Spectrometer (ALIAS) on 58 flights of the NASA ER-2 aircraft from October 1995 through September 1997, between 90°N and 3°S latitude. Measured upper tropospheric CO was variable and typically ranged between 55 and 115 ppb, except for higher values over Alaska during summer 1997. Tropical stratospheric CO ranged from 58 ± 5 ppb at the tropopause to 12 ± 2 ppb above 20 km, having similar profiles in all seasons of the year. The tropical profile is reproduced by a simple Lagrangian box model of tropical ascent using measured CH4 and OH concentrations, Cl and O(^1D) concentrations from a photochemical model, and diabatic heating rates from a radiative heating model. From measured CO, quasi-horizontal mixing between the tropical and mid-latitude lower stratosphere is inferred to be rapid in the region between 400 K and 450 K potential temperature (altitudes less than 20 km).

To investigate secular changes in CO and CH_4, we examined monthly means of tropospheric measurements made from samples collected at 19 fixed sites in the National Oceanic and Atmospheric Administration (NOAA) Climate Monitoring and Diagnostics Laboratory (CMDL) global cooperative flask sampling network. The CH_4 data are available for the period 1984–1995. A somewhat shorter time series is available for CO (1989–1995). The data were analyzed to extract a consistent pattern of change in time and in latitude. The most important preliminary finding is that the patterns of CO and CH_4 change appear to resemble that of biomass burning. That is, there is maximum change during local spring in both northern and southern hemispheres. If we attribute a significant part of the change in CH_4 trend (3–6 ppb/yr) to biomass burning, the corresponding change in CO is approximately 2–5 ppb/yr. This would explain the bulk of the observed change in CO (4–7 ppb/yr).

Methane (CH4), molecular hydrogen (H2), and water vapor (H2O) were measured concurrently on board the NASA ER-2 aircraft during the 1995–1996 Stratospheric Tracers of Atmospheric Transport (STRAT) and 1997 Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) campaigns. Correlations between these three main hydrogen reservoirs in the northern extratropical lower stratosphere are examined to evaluate H2O production from CH4 and H2 oxidation. The expected ratio of stratospheric H2O production (PH2O)to CH4 destruction (LCH4) = −1.973±0.003 is calculated from an evaluation of CH4 and H2 oxidation reactions and the relationship between H2 and CH4 mixing ratios measured during STRAT. Correlations between H2O and CH4 were tight and linear only for air masses with mean ages ≥3.8 years, restricting this analysis predominantly to latitudes between 40° and 90°N and potential temperatures between 470 and 540 K. The mean observed ΔH2O/CH4 (−2.15±0.18) is in statistical agreement with the expected PH2O/LCH4. The annual mean stratospheric entry mixing ratio for H2O calculated from this slope is 4.0 ± 0.3 ppm. The quantity H2O + 2·CH4 is quasi-conserved at 7.4 ± 0.5 ppm in older air masses in the northern extratropical lower stratosphere. Significant departure of H2O + 2·CH4 from the mean value is a sensitive indicator of processes which influence H2O without affecting CH4, such as dehydration in a polar vortex or near the tropical tropopause. No significant trend is observed in ER-2 aircraft data for H2O + 2·CH4 in the lower stratosphere from 1993 through 1997.

Simultaneous in situ measurements of N_2O and CH_4 were made with a tunable diode laser spectrometer (ALIAS II) aboard the Observations from the Middle Stratosphere (OMS) balloon platform from New Mexico, Alaska, and Brazil during 1996 and 1997. We find different compact relationships of CH_4 with N_2O in the tropics and extra-tropics because mixing is slow between these regions. Transport into the extra-tropics from the tropics or the polar vortex leads to deviations from the normal compact relationship. We use measured N_2O and CH_4 and a simple model to quantify entrainment of mid-latitude stratospheric air into the tropics. The entrainment time scale is estimated to be 16 (+17, −8) months for altitudes between 20 and 28 km. The fraction of tropical air entrained from the extra-tropical stratosphere is 50% (+18%, −30%) at 20 km, increasing to 78% (+11%, −19%) at 28 km.

In situ measurements of hydrochloric acid (HCI) concentrations in the lower stratosphere from 1991 to 1996 reveal that its abundance relative to that of total inorganic chlorine (CIy) has evolved upwards from HCI/CIy=40% in late 1991 to 70% in 1996.

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (theta approximately 450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(y)) had also been removed, with layers of enhanced NO(y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (approximately 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 micrometers) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range Transport of theta is estimated to have been dehydrated in this event.

The concentrations of the hydrogen radicals OH and HO 2 in the middle and upper troposphere were measured simultaneously with those of NO, O 3 , CO, H 2 O, CH 4 , non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O 3 in this region of the atmosphere. Comparison of the measured concentrations of OH and HO 2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HO x required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production of O 3 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO 2 and NO) is calculated to be about 1 part per billion by volume each day. This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more O 3 than expected.

The AquaVIT-1 Intercomparison of Atmospheric Water Vapor Measurement Techniques was conducted at the aerosol and cloud simulation chamber AIDA at the Karlsruhe Institute of Technology, Germany, in October 2007. The overall objective was to intercompare state-of-the-art and prototype atmospheric hygrometers with each other and with independent humidity standards under controlled conditions. This activity was conducted as a blind intercomparison with coordination by selected referees. The effort was motivated by persistent discrepancies found in atmospheric measurements involving multiple instruments operating on research aircraft and balloon platforms, particularly in the upper troposphere and lower stratosphere where water vapor reaches its lowest atmospheric values (less than 10 ppm). With the AIDA chamber volume of 84 m3, multiple instruments analyzed air with a common water vapor mixing ratio, either by extracting air into instrument flow systems, locating instruments inside the chamber, or sampling the chamber volume optically. The intercomparison was successfully conducted over 10 days during which pressure, temperature, and mixing ratio were systematically varied (50 to 500 hPa, 185 to 243 K, and 0.3 to 152 ppm). In the absence of an accepted reference instrument, the reference value was taken to be the ensemble mean of a core subset of the measurements. For these core instruments, the agreement between 10 and 150 ppm of water vapor is considered good with variation about the reference value of about ±10% (±1σ). In the region of most interest between 1 and 10 ppm, the core subset agreement is fair with variation about the reference value of ±20% (±1σ). The upper limit of precision was also derived for each instrument from the reported data. These results indicate that the core instruments, in general, have intrinsic skill to determine unknown water vapor mixing ratios with an accuracy of at least ±20%. The implication for atmospheric measurements is that the substantially larger differences observed during in-flight intercomparisons stem from other factors associated with the moving platforms or the non-laboratory environment. The success of AquaVIT-1 provides a template for future intercomparison efforts with water vapor or other species that are focused on improving the analytical quality of atmospheric measurements on moving platforms.

We present a climatology of O3, CO, and H2O for the upper troposphere and lower stratosphere (UTLS), based on a large collection of high-resolution research aircraft data taken between 1995 and 2008. To group aircraft observations with sparse horizontal coverage, the UTLS is divided into three regimes: the tropics, subtropics, and the polar region. These regimes are defined using a set of simple criteria based on tropopause height and multiple tropopause conditions. Tropopause-referenced tracer profiles and tracer-tracer correlations show distinct characteristics for each regime, which reflect the underlying transport processes. The UTLS climatology derived here shows many features of earlier climatologies. In addition, mixed air masses in the subtropics, identified by O3-CO correlations, show two characteristic modes in the tracer-tracer space that are a result of mixed air masses in layers above and below the tropopause (TP). A thin layer of mixed air (1–2 km around the tropopause) is identified for all regions and seasons, where tracer gradients across the TP are largest. The most pronounced influence of mixing between the tropical transition layer and the subtropics was found in spring and summer in the region above 380 K potential temperature. The vertical extent of mixed air masses between UT and LS reaches up to 5 km above the TP. The tracer correlations and distributions in the UTLS derived here can serve as a reference for model and satellite data evaluation.

[1] Comparisons of Tropospheric Emission Spectrometer (TES) water vapor retrievals with in situ measurements are presented. Global comparisons of TES water vapor retrievals with nighttime National Centers for Environmental Prediction RS90/RS92 radiosondes show a small (

[1] The Tropospheric Emission Spectrometer (TES) is an infrared, high-resolution Fourier transform spectrometer which was launched onboard NASA's Aura satellite in 2004 and is providing global, vertically resolved measurements of ozone in the troposphere. TES version 2 (V002) data profiles have been validated in the troposphere and lower stratosphere by way of comparison to ozonesondes and aircraft measurements. TES measurements also have sensitivity throughout the stratosphere, and therefore TES ozone profiles can be integrated to determine the total and stratospheric column in addition to the tropospheric column ozone values. In this work we compare the ozone in the stratosphere measured by TES to observations from the Microwave Limb Sounder (MLS) instrument in order to show the quality of the TES measurements in the stratosphere. We also compare the determination of a total column value for ozone based on the TES profiles to the column measured by the Ozone Monitoring Instrument (OMI). The TES tropospheric ozone column value is also calculated from the TES profiles and compared with column values determined from ozonesonde data. Column measurements are useful because the errors are markedly reduced from errors at the profile levels and can be used to assess both biases and quality of the TES ozone retrievals. TES observations of total or partial column ozone compare well with the other instruments but tend toward higher values than the other measurements. Specifically, TES is higher than OMI by ∼10 Dobson units (DU) for the total ozone column. TES measures higher values in the stratosphere (above 100 hPa) by ∼3 DU and measures higher ozone column values (∼4 DU) in the troposphere than ozonesondes. While the strength of the TES nadir ozone product is the vertical resolution it provides in the troposphere, a tropospheric column value derived from TES have utility in analyses using or validating tropospheric ozone residual products.

[1] The validation of version 2.2 (v2.2) H2O measurements from the Earth Observing System (EOS) Microwave Limb Sounder (Aura MLS) on the Aura satellite are presented. Results from comparisons made with Aqua Atmospheric Infrared Sounder (AIRS), Vaisala radiosondes, frost point hygrometer, and WB57 aircraft hygrometers are presented. Comparisons with the Aura MLS v1.5 H2O, Goddard global modeling and assimilation office Earth Observing System analyses (GEOS-5) are also discussed. For H2O mixing ratios less than 500 ppmv, the MLS v2.2 has an accuracy better than 25% between 316 and 147 hPa. The precision is 65% at 316 hPa that reduces to 25% at 147 hPa. This performance is better than expected from MLS measurement systematic error analyses. MLS overestimates H2O for mixing ratios greater than 500 ppmv which is consistent with a scaling error in either the calibrated or calculated MLS radiances. The validation of the accuracy of MLS v2.2 H2O from 121 to 83 hPa which is expected to be better than 15% cannot be confirmed at this time because of large disagreements among the hygrometers used in the AVE campaigns. The precision of the v2.2 H2O from 121 to 83 hPa is 10–20%. The vertical resolution is 1.5–3.5 km depending on height. The horizontal resolution is 210 × 7 km2 along and perpendicular to the Aura orbit track, respectively. Relative humidity is calculated from H2O and temperature. The precision, accuracy, and spatial resolution are worse than for H2O.

In situ observations in a tropical subvisible cirrus cloud during the Costa Rica Aura Validation Experiment on 2 February 2006 show the presence of condensed-phase nitric acid. The cloud was observed near the tropopause at altitudes of 16.3–17.7 km in an extremely cold (183–191 K) and dry (.lt. 5 ppm H2O) air mass. Relative humidities with respect to ice ranged from 150–250% throughout most of the cloud. Optical particle measurements indicate the presence of ice crystals as large as 90 μm in diameter. Condensed HNO3/H2O molar ratios observed in the cloud particles were 1–2 orders of magnitude greater than ratios observed previously in cirrus clouds at similar HNO3 partial pressures. Nitric acid trihydrate saturation ratios were 10 or greater during much of the cloud encounter, indicating that HNO3 may be present in the cloud particles as a stable condensate and not simply physically adsorbed on or trapped in the particles

[1] Validation of Tropospheric Emission Spectrometer (TES) tropospheric CO profiles with in situ CO measurements from the Differential Absorption CO Measurement (DACOM) instrument during the Intercontinental Chemical Transport Experiment (INTEX)-B campaigns in March to May 2006 are presented. For each identified DACOM CO profile, one to three TES CO profiles are selected closest in location to the small area that the DACOM profile covers. The time differences between the comparison profiles are within 2 hours. The DACOM CO vertical profiles are adjusted by applying nearest coincident TES averaging kernels and the a priori profiles. This step accounts for the effect of the vertical resolution of the TES CO retrievals and removes the influence of the a priori assumptions in the comparisons. Comparison statistics for data taken near Houston in March 2006 show good agreement between TES and the adjusted DACOM CO profiles in the lower and middle troposphere with a correlation coefficient of 0.87. On average, the TES CO volume mixing ratio profile is 0–10% lower than the adjusted DACOM CO profile from the lower to middle troposphere. This is within the 10–20% standard deviations of the TES or DACOM CO profiles taken in the Houston area. The comparisons of TES and DACOM CO profiles near Hawaii and Anchorage in April to May 2006 are not as good. In these regions the aircraft DACOM CO profiles are characterized by plumes or enhanced CO layers, consistent with known features in the tracer fields due to transpacific transport of polluted air parcels originating from East Asia. Although TES observations over the Pacific region also show localized regions of enhanced CO, the coincidence criteria for obtaining good comparisons with aircraft measurements are challenging. The meaning of validation comparisons in profile portions where TES retrievals have little sensitivity is addressed. Examinations of characteristic parameters in TES retrievals are important in data applications.

[1] The Tropospheric Emission Spectrometer (TES) on the Earth Observing System (EOS)-Aura spacecraft measures global profiles of atmospheric ozone with vertical resolution of 6–7 km in the troposphere for the nadir view. For a first validation of TES ozone measurements we have compared TES-retrieved ozone profiles to ozonesondes from fall, 2004. In some cases the ozonesonde data are from dedicated launches timed to match the Aura overpass, while other comparisons are performed with routine data available from the Southern Hemisphere Additional Ozonesonde (SHADOZ) archive and World Ozone and Ultraviolet Data Center (WOUDC) data archives. We account for TES measurement sensitivity and vertical resolution by applying the TES-averaging kernel and constraint to the ozonesonde data before differencing the profiles. Overall, for V001 data, TES ozone profiles are systematically higher than sondes in the upper troposphere but compare well in the lower troposphere, with respect to estimated errors. These comparisons show that TES is able to detect relative variations in the coarse vertical structure of tropospheric ozone.

SUMMARYWhat are the mechanisms of multifunctionality, i.e. the use of the same peripheral structures for multiple behaviors? We studied this question using the multifunctional feeding apparatus of the marine mollusk Aplysia californica, in which the same muscles mediate biting (an attempt to grasp food) and swallowing (ingestion of food). Biting and swallowing responses were compared using magnetic resonance imaging of intact, behaving animals and a three-dimensional kinematic model. Biting is associated with larger amplitude protractions of the grasper (radula/odontophore) than swallowing, and smaller retractions. Larger biting protractions than in swallowing appear to be due to a more anterior position of the grasper as the behavior begins, a larger amplitude contraction of protractor muscle I2, and contraction of the posterior portion of the I1/I3/jaw complex. The posterior I1/I3/jaw complex may be context-dependent, i.e. its mechanical context changes the direction of the force it exerts. Thus, the posterior of I1/I3 may aid protraction near the peak of biting, whereas the entire I1/I3/jaw complex acts as a retractor during swallowing. In addition, larger amplitude closure of the grasper during swallowing allows an animal to exert more force as it ingests food. These results demonstrate that differential deployment of the periphery can mediate multifunctionality.

[1] We present global, vertical profile estimates of the HDO/H2O ratio from the Tropospheric Emission Spectrometer (TES) on the Earth Observing System (EOS) Aura satellite. We emphasize in this paper the estimation approach and error characterization, which are critical to determining the very small absolute concentration of HDO relative to H2O and its uncertainty. These estimates were made from TES nadir-viewing (downlooking) thermal infrared spectral radiances observed on 20 September 2004. Profiles of HDO and H2O are simultaneously estimated from the observed radiances and a profile of the ratio is then calculated. This simultaneous, or “joint,” estimate is regularized with an a priori covariance matrix that includes expected correlations between HDO and H2O. This approach minimizes errors in the profile of the HDO/H2O ratio that are due to overlapping HDO and H2O spectroscopic lines. Under clear-sky conditions in the tropics, TES estimates of the HDO/H2O ratio are sensitive to the distribution of the actual ratio between the surface and about 300 hPa with peak sensitivity at 700 hPa. The sensitivity decreases with latitude through its dependence on temperature and water amount. We estimate a precision of approximately 1% to 2% for the ratio of the HDO/H2O tropospheric densities; however, there is possibly a bias of approximately 5% in the ratio due to the HDO spectroscopic line strengths. These global observations clearly show increased isotopic depletion of water vapor at higher latitudes as well as increased depletion in the upper troposphere versus the lower troposphere.

Convective systems are an important mechanism in the transport of boundary layer air into the upper troposphere. The Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) campaign, in July 2002, was developed as a comprehensive atmospheric mission to improve knowledge of subtropical cirrus systems and their roles in regional and global climate. In situ measurements of carbon monoxide (CO), water vapor (H20v), and total water (H20t) aboard NASA's . WB-57F aircraft and CO aboard the U.S. Navy's Twin Otter aircraft were obtained to study the role of convective transport. Three flights sampled convective outflow on 11, 16 and 29 July found varying degrees of CO enhancement relative to the fiee troposphere. A cloud-resolving model used the in situ observations and meteorological fields to study these three systems. Several methods of filtering the observations were devised here using ice water content, relative humidity with respect to ice, and particle number concentration as a means to statistically sample the model results to represent the flight tracks. A weighted histogram based on ice water content observations was then used to sample the simulations for the three flights. In addition, because the observations occurred in the convective outflow cirrus and not in the storm cores, the model was used to estimate the maximum CO within the convective systems. In general, anvil-level air parcels contained an estimated 20-40% boundary layer air in the analyzed storms.

[1] High-resolution (1 Hz at true airspeeds near 200 m s−1) observations of methane, ozone, water vapor, and temperature taken between the surface and 18 km from the WB57F aircraft near San Jose, Costa Rica (10°N, 84°W), are used to examine processes influencing the maintenance of these profiles. There was a clearly defined thermal tropopause on each of the eight profiles, accompanied by structure on methane-ozone scatterplots on the five profiles having methane observations. There was a well-defined decrease in methane mixing ratio between approximately 12 and 15 km in each of these five profiles, 2–5 km beneath the thermal tropopause, correlated with sharp changes in water vapor and equivalent potential temperature. The methane observations are interpreted as meaning that air is recirculated between the lower stratosphere and the upper tropical troposphere. At the point on each vertical profile where the water vapor had its minimum value, the air was never saturated or apparently supersaturated, although apparent supersaturation with respect to ice was observed in vertically extensive, near-adiabatic layers with tops some 200–300 m below the water vapor minimum on all profiles. One of the profiles also exhibited apparent supersaturation above its water vapor minimum, near 18 km. We examine the decrease in water vapor to minimal values as a four-stage process in which its mixing ratio was lowered from ∼10 to ∼3 ppmv, consider the role of solar and thermal evaporation of the smaller ice particles in the final stage of the dehydration process, and correlate features separating near-adiabatic layers above 150 hPa pressure altitude with local sea surface temperatures.

[1] This paper provides an initial assessment of the accuracy of the Atmospheric Infrared Sounder (AIRS) water vapor retrievals from 500 to 100 mbar. AIRS satellite measurements are compared with accurate aircraft (NASA WB57) and balloon in situ water vapor measurements obtained during the NASA Pre-Aura Validation Experiment (Pre-AVE) in Costa Rica during Jan. 2004. AIRS retrieval (each pressure level of a single footprint) of water vapor amount agrees with the in situ measurements to ∼25% or better if matched closely in time (1 hr) and space (50–100 km). Both AIRS and in situ measurements observe similar significant variation in moisture amount over a two-day period, associated with large-scale changes in weather patterns.