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A Study of Cirrus Clouds and Aerosols in the Upper Troposphere using Models and Satellite Data

This report is the final report for the Cooperative Agreement NCC2-1213. It is a compilation of publications produced under this Cooperative Agreement and conference presentations. The tasks for the Aerosol Physical Chemistry Model for the Upper Troposphere include: Task 1: To compare APCM predictions against the SUCCESS data and other aircraft campaigns and to investigate the role of aerosol composition on cirrus cloud nucleation; Task 2: To study the seasonal evolution and spatial distribution of upper-tropospheric tropical and polar cirrus; Task 3: To investigate CLAES cirrus data with other complementary (TOGA-COARE and CEPEX) data. Tasks for Upper Tropospheric Cirrus Clouds include: Task 1: Assemble 3-hourly (or more frequent) meteorological satellite data fiom geostationary satellites to obtain a global, or nearly global, dataset of infiared brightness temperatures as a function of time for airborne experimental periods; Task 2: Explore methods to improve the cloud top altitude distributions calculated fiom meteorological satellite data. This will focus on linlung the 6.5 micron channel geostationary brightness temperatures and the 10.5 micron brightness temperatures; Task 3: Explore methods to differentiate convective fiom stratiform cloudiness; Task 4: Perform trajectory analyses using an existing trajectory modeling package that links the cloud data with air mass histories; Task 5: Apply techniques from tasks 1 through 4 to provide meteorological support to the CRYSTAL-FACE mission, both in its preparation and deployment phases. The report include four published articles and two slide presentations.

Bergstrom, Robert W.↗

New Perspectives from Satellite and Profile Observations on Tropospheric Ozone over Africa and the Adjacent Oceans: An Indian-Atlantic Ocean Link to tbe "Ozone Paradox"

In the past few years, tropospheric ozone observations of Africa and its adjacent ocenas have been greatly enhanced by high resolution (spatial and temporal) satellite measurements and profile data from aircraft (MOZAIC) and balloon-borne (SHADOZ) soundings. These views have demonstrated for the first time the complexity of chemical-dynamical interactions over the African continent and the Indian and Atlantic Oceans. The tropical Atlantic "ozone paradax" refers to the observation that during the season of maximum biomass burning in west Africa north of the Intertropical Convergence Zone (ITCZ), the highest tropospheric ozone total column occurs south of the ITCZ over the tropical Atlantic. The longitudinal view of tropospheric ozone in the southern tropics from SHADOZ (Southern Hemisphere Additional Ozonesondes) soundings shown the persistence of a "zonal-wave one" pattern that reinforces the "ozone paradox". These ozone features interact with dynamics over southern and northern Africa where anthropogenic sources include the industrial regions of the South African Highveld and Mideastern-Mediterranean influences, respectively. Our newest studies with satellites and soundings show that up to half the ozone pollution over the Atlantic in the January-March "paradox" period may originate from south Asian pollution. Individual patches of pollurion over the Indian Ocean are transported upward by convective mixing and are enriched by pyrogenic, biogenic sources and lightning as they cross Africa and descend over the Atlantic. In summary, local sources, intercontinental import and export and unique regional transport patterns put Africa at a crossroads of troposheric ozone influences.

Thompson, Anne M.↗

Influence of isentropic transport on seasonal ozone variations in the lower stratosphere and subtropical upper troposphere

The isentropic cross-tropopause ozone transport has been estimated in both hemispheres in 1999 based on the potential vorticity mapping of Stratospheric Aerosol and Gas Experiment 11 ozone measurements and contour advection calculations using the NASA Goddard Space Flight Center Global and Modeling Assimilation Office analysis. The estimated net isentropic stratosphere-to-troposphere ozone flux is approx.118 +/- 61 x 10(exp9)kg/yr globally within the layer between 330 and 370 K in 1999; 60% of it is found in the Northern Hemisphere, and 40% is found in the Southern Hemisphere. The monthly average ozone fluxes are strongest in summer and weakest in winter in both hemispheres. The seasonal variations of ozone in the lower stratosphere (LS) and upper troposphere (UT) have been analyzed using ozonesonde observations from ozonesonde stations in the extratropics and subtropics, respectively. It is shown that observed ozone levels increase in the UT over subtropical ozonesonde stations and decrease in the LS over extratropical stations in late spring/early summer and that the ozone increases in the summertime subtropical UT are unlikely to be explained by photochemical ozone production and diabatic transport alone. We conclude that isentropic transport is a significant contributor to ozone levels in the subtropical upper troposphere, especially in summer.

Jing, P.↗

Solar-stratosphere-troposphere interaction as a mechanism of solar influence on climate

We will briefly review recent studies showing that stratospheric disturbances propagate to the troposphere and that UV variability affects the atmospheric circulation in the stratosphere and troposphere in a coherent fashion. We will outline a mechanism by which solar-stratosphere-troposphere interaction may influence climate and discuss a simple model that includes the basic elements of this mechanism.

sun climate↗

Exploring the Production of NOx by Lightning and Its Impact on Tropospheric Ozone

Our quantitative understanding of free tropospheric (FT) chemistry is quite poor. State-of-the-art regional air quality models (e.g., US EPA's CMAQ) perform very poorly in simulating FT chemistry, with Uniform ozone around 70 ppb throughout the FT in summer, while ozonesonde data show much higher levels of ozone and much spatial-temporal structure. Such models completely neglect lightning-NOx (LNOx) emissions (the most significant source of NOx in the FT), and also contain large uncertainties in the specifications of intercontinental transport, stratosphere-troposphere exchange (STE) and PBLFT exchange (PFTE). Global air chemistry models include LNOx, but in very crude fashion, with the frequency and distribution of lightning being based on modeled cloud parameters (hence large uncertainty), lightning energetics being assumed to be constant for all flashes (literature value, while in reality there is at least a two-orders of magnitude variability from flash-to-flash), and the production of NOx in the surrounding heated air, per Joule of heating, being assumed to be constant also (literature value, while in fact it is a non-linear function of the dissipated heat and local air density, p). This situation is commonly blamed on paucity of pertinent observational data, but for the USA, there is now a wealth of surface- and satellite-based data of lightning available to permit much improved observation-based estimation of LNOx emissions. In the FT, such NOx has a long residence time, and also the ozone production efficiency from NOx there is considerably higher than in the PBL. It is, therefore, of critical importance in FT chemistry. This paper will describe the approach and data products of an ongoing NSSTC project aimed at a much-improved quantification of not only LNOx production on the scale of continental USA based on local and regional lightning observations, but also of intercontinental transport, STE and PFTE, all in upgraded simulations of tropospheric transport and chemistry. In our approach for LNOx, (a) we utilize continuous observed lightning information from the NLDN ground network and from satellite imagers (OTD and LIS) to quantify lightning frequency and distribution at the spatial-temporal scales of models such as CMAQ; (b) we develop new methodologies to quantify flash-specific lightning energy dissipation as heat (epsilon) using data from the research-grade lightning measurement facility at NASA-KSC, and to parameterize epsilon based on regional lightning monitoring data (ground- and satellite-based); and, (c) we develop a new parameterization of NOx production as a function of epsilon and rho. Based on such observation-based information, we are working to develop a gridded, episodic LNOx emissions inventory for the USA for use in models like CMAQ. We are also developing approaches for global(MOZART)- regional(CMAQ) chemistry coupling to improve intercontinental transport and STE. Finally, we are developing new methodologies for assimilation of satellite-observed (GOES) clouds into meteorological modeling (MM5), to improve PFTE and to optimize co-location of cloud convection and observed lightning. We will incorporate these improvements in CMAQ simulations over the USA to better understand FT processes and chemistry, and its impact on ground-level ozone.

Gillani, Noor↗

Study Pollution Impacts on Upper-Tropospheric Clouds with Aura, CloudSat, and CALIPSO Data

This viewgraph presentation reviews the impact of pollution on clouds in the Upper Troposphere. Using the data from the Aura Microwave Limb Sounder (MLS), CloudSat, CALIPSO the presentation shows signatures of pollution impacts on clouds in the upper troposphere. The presentation demonstrates the complementary sensitivities of MLS , CloudSat and CALIPSO to upper tropospheric clouds. It also calls for careful analysis required to sort out microphysical changes from dynamical changes.

radar↗

Dial Measurements of Free-Tropospheric Ozone Profiles in Huntsville, AL

A tropospheric ozone DIfferential Absorption Lidar (DIAL) system has been developed jointly by NASA and the University of Alabama at Huntsville (UAH). Two separated Nd:YAG pumped dye laser systems produce the laser pulses with wavelengths of 285 and 291 nm at 20 Hz frequency. The receiver is a Newtonian telescope with a 40 cm primary and a two-channel aft optics unit. The detection system currently uses photon counting to facilitate operations at the maximum achievable altitude. This lidar measures free-tropospheric ozone profiles between 4-10 km at Regional Atmospheric Profiling Laboratory for Discovery (RAPCD) in UAH campus (ASL 206 m) under both daytime and nighttime conditions. Frequent coincident ozonesonde flights and theoretical calculations provide evidence to indicate the retrieval accuracy ranges from approx.5% at 4 km to approx.60% at 10 km with 750-m vertical resolution and 30-minute integration. Three Hamamatsu 7400 PMTs and analog detection technique will be added on the current system to extend the measurement to approx.100 m above ground to monitor the PBL and lower tropospheric ozone variations.

Newchurch, Mike↗

Remote Sensing of Tropospheric Pollution from Space

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

Fishman, Jack↗

Development of an Airborne Molecular Direct Detection Doppler Lidar for Tropospheric Wind Profiling

Global measurement of tropospheric winds is a key measurement for understanding atmospheric dynamics and improving numerical weather prediction. Global wind profiles remain a high priority for the operational weather community and also for a variety of research applications including studies of the global hydrologic cycle and transport studies of aerosols and trace species. In addition to space based winds, high altitude airborne Doppler lidar systems flown on research aircraft, UAV's or other advanced sub-orbital platforms would be of great scientific benefit for studying mesoscale dynamics and storm systems such as hurricanes. The Tropospheric Wind Lidar Technology Experiment (TWiLiTE) is a three year program to advance the technology readiness level of the key technologies and subsystems of a molecular direct detection wind lidar system by validating them, at the system level, in an integrated airborne lidar system. The TWiLiTE Doppler lidar system is designed for autonomous operation on the WB57, a high altitude aircraft operated by NASA Johnson. The WE357 is capable of flying well above the midlatitude tropopause so the downward looking lidar will measure complete profiles of the horizontal wind field through the lower stratosphere and the entire troposphere. The completed system will have the capability to profile winds in clear air from the aircraft altitude of 18 km to the surface with 250 m vertical resolution and < 3 mis velocity accuracy. Progress in technology development and status of the instrument design will be presented.

Gentry, Bruce↗

Sensitivity of Photolysis Frequencies and Key Tropospheric Oxidants in a Global Model to Cloud Vertical Distributions and Optical Properties

As a follow-up study to our recent assessment of the radiative effects of clouds on tropospheric chemistry, this paper presents an analysis of the sensitivity of such effects to cloud vertical distributions and optical properties in a global 3-D chemical transport model (GEOS4-Chem CTM). GEOS-Chem was driven with a series of meteorological archives (GEOS1-STRAT, GEOS-3 and GEOS-4) generated by the NASA Goddard Earth Observing System data assimilation system, which have significantly different cloud optical depths (CODs) and vertical distributions. Clouds in GEOS1-STRAT and GEOS-3 have more similar vertical distributions while those in GEOS-4 are optically much thinner in the tropical upper troposphere. We find that the radiative impact of clouds on global photolysis frequencies and hydroxyl radical (OH) is more sensitive to the vertical distribution of clouds than to the magnitude of column CODs. Model simulations with each of the three cloud distributions all show that the change in the global burden of O3 due to clouds is less than 5%. Model perturbation experiments with GEOS-3, where the magnitude of 3-D CODs are progressively varied by -100% to 100%, predict only modest changes (<5%) in global mean OH concentrations. J(O1D), J(NO2) and OH concentrations show the strongest sensitivity for small CODs and become insensitive at large CODs due to saturation effects. Caution should be exercised not to use in photochemical models a value for cloud single scattering albedo lower than about 0.999 in order to be consistent with the current knowledge of cloud absorption at the UV wavelength. Our results have important implications for model intercomparisons and climate feedback on tropospheric photochemistry.

Liu, Hongyu↗

Mechanisms for the Intraseasonal Variability of Tropospheric Ozone over the Indian Ocean during the Winter Monsoon

We synthesize daily sonde (vertical) information and daily satellite (horizontal) information to provide an empirical description of ozone origins over the northern Indian Ocean during the INDOEX (Indian Ocean Experiment) field campaign (February-March 1999). This area is shown to be a significant portion of the "high-ozone tropics". East-west O3 features and their flow are identified, and ozone origins are compared to other tropical regions, using water vapor as a second tracer. In the study period, multiple processes contribute to O3 column enhancements, their importance varying strongly by latitude: (1) Low-altitude O3 pollution over the northern Indian Ocean mainly originates from the Indian subcontinent and is traceable to high emission areas. Convective activity south of Sri Lanka helps direct ozone outflow from the northern Indian subcontinent. (2) Middle tropospheric O3 maxima over the northern Indian Ocean originate from various sources, often transitioning within a few hours. Convective venting of Asian pollutants can add 20-30 ppbv to the middle troposphere at 5degN-10degN, alternating with stratospheric influence. (3) A number of cases suggest that strong mixing-in of stratospheric air along the subtropical jet raised tropospheric O3 in early March by approx.40-50 ppbv, especially poleward of approx. 10degN. (4) Influences of lightning and large-scale biomass burning were not strong during this period, in contrast to the situation in Africa and the South Atlantic or locally in Southeast Asia. This work illustrates successes and limitations in approaches to synthesizing disparate information on trace-gas distributions taken from satellite retrieval products and ozonesondes.

Chatfield, R. b.↗

An Overview of the NASA Spring/Summer 2008 Arctic Campaign - ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites)

ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) is a major NASA led airborne field campaign being performed in the spring and summer of 2008 at high latitudes (http://cloud1.arc.nasa.gov/arctas/). ARCTAS is a part of the International Polar Year program and its activities are closely coordinated with multiple U. S. (NOAA, DOE), Canadian, and European partners. Observational data from an ensemble of aircraft, surface, and satellite sensors are closely integrated with models of atmospheric chemistry and transport in this experiment. Principal NASA airborne platforms include a DC-8 for detailed atmospheric composition studies, a P-3 that focuses on aerosols and radiation, and a B-200 that is dedicated to remote sensing of aerosols. Satellite validation is a central activity in all these platforms and is mainly focused on CALIPSO, Aura, and Aqua satellites. Major ARCTAS themes are: (1) Long-range transport of pollution to the Arctic including arctic haze, tropospheric ozone, and persistent pollutants such as mercury; (2) Boreal forest fires and their implications for atmospheric composition and climate; (3) Aerosol radiative forcing from arctic haze, boreal fires, surface-deposited black carbon, and other perturbations; and (4) Chemical processes with focus on ozone, aerosols, mercury, and halogens. The spring deployment (April) is presently underway and is targeting plumes of anthropogenic and biomass burning pollution and dust from Asia and North America, arctic haze, stratosphere-troposphere exchange, and ozone photochemistry involving HOx and halogen radicals. The summer deployment (July) will target boreal forest fires and summertime photochemistry. The ARCTAS mission is providing a critical link to enhance the value of NASA satellite observations for Earth science. In this talk we will discuss the implementation of this campaign and some preliminary results.

Jacob, Daniel J.↗

The Seasonal Response of Titan's Troposphere and Stratosphere

The radiative response of Titan's atmosphere varies by several orders of magnitude with altitude. This presents an interesting situation in which most of the stratosphere----at least that part above 100km is characterized by radiative relaxation times that are short compared to the length of a Titan season, and the troposphere and tropopause region by times that are larger than seasonal timescales. Consistent with this, Cassini CIRS spectra indicate stratospheric temperatures at 100-170 kin that are 20-30 K cooler at high northern latitudes in winter than those at equatorial and southern latitudes. Given the expectation that the situation will largely reverse in southern winter, the observed large meridional contrast is likely indicative of the expected seasonal variation at polar latitudes in both hemispheres. CIRS spectra do not as easily yield temperatures below 100 km in the lower stratosphere and tropopause region, because of the contribution of heterogeneously distributed aerosols and condensates to the infrared opacity. However, Cassini radio occultations probe both the stratosphere and troposphere, and below 80 km they show the thermal contrast with latitude to be muted, e.g,, approx.5 K near the tropopause at 40-50 km and approx.3 K just above the surface. This is consistent with the large radiative relaxation times at these altitudes and with efficient meridional heat transport. What is curious is the manner in which temperatures in the north winter polar atmosphere make the transition between the troposphere and lower stratosphere, where seasonal variations are relatively small, and higher altitudes, where they are large. Temperatures at all latitudes sounded by the radio occultations exhibit similar behavior in the lower stratosphere, increasing with altitude. Between 80 and 100 kin, however, the temperatures at high northern latitudes exhibit a sudden drop with increasing altitude, producing the meridional contrast in the upper stratosphere described above. While the radiative relaxation time associated with infrared gaseous coolants decreases with altitude in the stratosphere, it is not likely to account for the abrupt transition observed. Possible mechanisms for this transition are discussed, including the presence of an optically thick. cloud at thermal-infrared wavelengths.

Flasar, F. M.↗

Recent Biomass Burning in the Tropics and Related Changes in Tropospheric Ozone

Biomass burning is an important source of chemical precursors of tropospheric ozone. In the tropics, biomass burning produces ozone enhancements over broad regions of Indonesia, Africa, and South America including Brazil. Fires are intentionally set in these regions during the dry season each year to clear cropland and to clear land for human/industrial expansion. In Indonesia enhanced burning occurs during dry El Nino conditions such as in 1997 and 2006. These burning activities cause enhancement in atmospheric particulates and trace gases which are harmful to human health. Measurements from the Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) from October 2004-November 2008 are used to evaluate the effects of biomass burning on tropical tropospheric ozone. These measurements show sizeable decreases approx.15-20% in ozone in Brazil during 2008 compared to 2007 which we attribute to the reduction in biomass burning. Three broad biomass burning regions in the tropics (South America including Brazil, western Africa, and Indonesia) were analyzed in the context of OMI/MLS measurements and the Global Modeling Initiative (GMI) chemical transport model developed at Goddard Space Flight Center. The results indicate that the impact of biomass burning on ozone is significant within and near the burning regions with increases of approx.10-25% in tropospheric column ozone relative to average background concentrations. The model suggests that about half of the increases in ozone from these burning events come from altitudes below 3 km. Globally the model indicates increases of approx.4-5% in ozone, approx.7-9% in NO, (NO+NO2), and approx.30-40% in CO.

Ziemke↗

The Structure and Dynamics of Titan's Middle Atmosphere and Troposphere

Titan, after Venus, is the second example in the solar system of an atmosphere with a global cyclostrophic circulation. The origin and maintenance of these superrotating atmospheres is not well understood, but Titan has a strong seasonal modulation in the middle atmosphere, and the seasonal changes in the winds may offer clues. The pole in winter and early spring is characterized by temperatures 20-30 K cooler at 140-170 km than those at low latitudes, and strong circumpolar winds as high as 190 m/s at 200- 250 km. At these levels the polar region is characterized by enhanced concentrations of several organic gases, and also detectable condensates. All this suggests that the polar vortex provides a mixing barrier between winter polar and lower-latitude air masses, analogous to the polar ozone holes on Earth. Because the concentrations of organic gases increase with altitude in the middle atmosphere, the observed enhancements suggest subsidence over the winter pole. Consistent with this are the observed temperatures approximately 200 K at the winter-polar stratopause (280 km), making it the warmest part of the atmosphere. The warm stratopause likely results from adiabatic heating associated with the subsidence. Recent observations in late northern winter and early spring indicate that the warm anomaly at the winter-polar stratopause is weakening;. In contrast to the middle atmosphere, latitude contrasts in tropospheric temperatures are muted. During the northern winter season, they were approximately 5 K at the tropopause and 3 K or less near the surface, being coldest at high northern latitudes. This is understandable in terms of the long radiative relaxation times in the troposphere, compared to times that are much shorter than a season in the upper stratosphere and higher. Curiously, the transition between the small meridional contrast (and presumably seasonal variations) in temperatures observed in the troposphere and the large variations observed at higher altitudes occurs abruptly above 80 km. Here the temperatures in the lower stratosphere, generally increasing with altitude, exhibit a sudden drop with increasing altitude at high northern latitudes, producing the contrast between low and high northern winter latitudes in the upper stratosphere described above. While the radiative relaxation time associated with infrared gaseous coolants decreases with altitude in the stratosphere, the abrupt transition suggests the presence of an optically thick condensate at thermal-infrared wavelengths. Near the surface, temperature lapse rates are adiabatic over the lowest 2 km, with the suggestion of a nocturnal stable inversion over the lowest 200 m in radio-occultation soundings near the morning terminator. At mid and high latitudes in both winter and summer hemispheres, the profiles are more statically stable (i.e., subadiabatic). This is most pronounced in the winter hemisphere.

Flasar, F.M.↗

Southern Hemisphere Carbon Monoxide Inferannual Variability Observed by Terra/Measurement of Pollution in the Troposphere (MOPITT)

Biomass burning is an annual occurrence in the tropical southern hemisphere (SH) and represents a major source of regional pollution. Vegetation fires emit carbon monoxide (CO), which due to its medium lifetime is an excellent tracer of tropospheric transport. CO is also one of the few tropospheric trace gases currently observed from satellite and this provides long-term global measurements. In this paper, we use the 5 year CO data record from the Measurement Of Pollution In The Troposphere (MOPITT) instrument to examine the inter-annual variability of the SH CO loading and show how this relates to climate conditions which determine the intensity of fire sources. The MOPITT observations show an annual austral springtime peak in the SH zonal CO loading each year with dry-season biomass burning emissions in S. America, southern Africa, the Maritime Continent, and northwestern Australia. Although fires in southern Africa and S. America typically produce the greatest amount of CO, the most significant inter-annual variation is due to varying fire activity and emissions from the Maritime Continent and northern Australia. We find that this variation in turn correlates well with the El Nino Southern Oscillation precipitation index. Between 2000 and 2005, emissions were greatest in late 2002 and an inverse modeling of the MOPITT data using the MOZART chemical transport model estimates the southeast Asia regional fire source for the year August 2002 to September 2003 to be 52 Tg CO. Comparison of the MOPITT retrievals and NOAA surface network measurements indicate that the latter do not fully capture the inter-annual variability or the seasonal range of the CO zonal average concentration due to biases associated with atmospheric and geographic sampling.

Edwards, D. P.↗

Applications of OMI Tropospheric NO(Sub 2) Data: Air Quality Trends in the US and Lightning NO(x) Source Strength

This talk will be presented in two parts: 1) an analysis of tropospheric column NO2 trends in the eastern half of the United States over the period 2005 to 2009 and 2) estimation of lightning NO(x) production rates based on OMI observations and lightning flash rate data. The air quality trends in the eastern US will be determined for specific subregions using tropospheric column NO2 data from OMI for 2005 through 2008 and from GOME-2 for 2007 through 2009. This period is characterized by significant NO(x) emission reductions at power plants within most of this region. The air quality trends will be compared with those estimated from continuous emission monitoring data from the power plants compiled by the US Environmental Protection Agency. OMI NO2 data have also been used to estimate lightning NOx production per flash in selected storms near Costa Rica and Panama during the 2007 NASA TC4 field campaign and over the continental US, Gulf of Mexico, and western Atlantic during the summers of 2005 and 2006. The lightning signal is extracted from the OMI data through a custom retrieval in which an NO2 profile representative of convective outflow is used in the airmass factor calculation and the background NO2 column is subtracted from the tropospheric column. When combined with NO(x)/NO2 ratios from the NASA GMT model and observed flash rates, the resulting estimates of NO(x) production per flash are comparable to those estimated obtained from analyses of aircraft data and cloud-resolving modeling.

Pickering, Kenneth↗

Can Vertical Profiles of Tropospheric Methane on Titan Be Derived from Radio-Occultation Soundings?

The intensity of the received signal at Earth in the radio occultations of Titan is attenuated both by refractive defocusing and pressure-induced absorption from N2-N2 and CH4-N2 pairs. Because the absorption strength is different for the two sets of pairs, matching the retrieved absorptivity profile can in principle yield the vertical variation in gaseous methane in the troposphere. There are two factors that make this difficult. The first is the propagation of noise in the phase and amplitude of the received signal in the absorption retrieval. The phase data is first inverted to retrieve vertical profiles of refractivity, from which the refractive defocusing is calculated. This is then subtracted from the observed. intensity attenuation of the received signal to generate a profile of atmospheric absorption. The second problem is the uncertainty in the pressure-induced absorption coefficients. Laboratory data at radio wavelengths is only available near room temperature (see, e.g., [1] for N2-N2), and the extrapolation to the low temperatures in Titan's troposphere is not well established. Ab initio calculations by Borysow et al. [2, 3] provide absorption coefficients at low temperatures and long wavelengths, but their accuracy has come into question. We present examples from Cassini radio occultations of Titan to illustrate the difficulties. For methane mole fractions in the lower troposphere comparable to that inferred from the Huygens probe (approximately 0.05), it will be difficult to separate the contributions of N2-N2 collisions from those of N2-CH4, collisions to the retrieved absorption. However, higher concentrations of CH4 and/or a higher signal-to-noise ratio from a future uplink experiment could result in a successful separation of the two components. However, key to this are highly accurate estimates of the absorption from a combination of laboratory measurements at love temperatures and long wavelengths, and possibly improved theoretical calculations.

Flasar, F. Michael↗