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NASA NTRS2003

Climate Impacts on Tropospheric Ozone and Hydroxyl

Climate change may influence tropospheric ozone and OH via several main pathways: (1) altering chemistry via temperature and humidity changes, (2) changing ozone and precursor sources via surface emissions, stratosphere-troposphere exchange, and light- ning, and (3) affecting trace gas sinks via the hydrological cycle and dry deposition. We report results from a set of coupled chemistry-climate model simulations designed to systematically study these effects. We compare the various effects with one another and with past and projected future changes in anthropogenic and natural emissions of ozone precursors. We find that white the overall impact of climate on ozone is probably small compared to emission changes, some significant seasonal and regional effects are apparent. The global effect on hydroxyl is quite large, however, similar in size to the effect of emission changes. Additionally, we show that many of the chemistry-climate links that are not yet adequately modeled are potentially important.

Shindell, Drew T.↗
NASA NTRS2003

Elevated Ozone in the Troposphere over the Atlantic and Pacific Oceans in the Northern Hemisphere

Tropospheric column ozone (TCO) is derived from differential measurements of total column ozone from Nimus-7 and Earth Probe TOMS, and stratospheric column ozone from the Microwave Limb Sounder instrument on the Upper Atmospheric Research Satellite. It is shown that TCO during summer months over the Atlantic and Pacific Oceans at northern mid-latitudes is about the same (50-60 Dobson Units) as over the continents of North America, Europe and Asia, where surface emissions of nitrogen oxides from industrial sources, biomass and biofuel burning and biogenic emissions are significantly larger. This nearly uniform zonal variation in TCO is modulated by surface topography of the Rocky and Himalayan mountains and Tibetan Plateau where TCO is reduced by 20-30 Dobson Units. The zonal characteristics of TCO derived from satellite measurements are well simulated by a global chemical transport model called MOZART-2 (Model of Ozone and Related Chemical Tracers, version 2). The model results are analyzed to delineate the relative importance of various processes contributing to observed zonal characteristics of TCO, and they are shown that the surface emission of NOx contributes about 50% of the TCO at northern mid-latitudes, especially over the continents of North America, Europe and Asia. The result of TCO derived from TOMS and the analysis from MOZART-2 indicate that TCO is a very useful tool to study tropospheric O3 pollution resulting from surface emissions of pollutants.

Chandra, S.↗
NASA NTRS2003

Extratropical Stratosphere-Troposphere Mass Exchange

Global net mass flux between the troposphere and the stratosphere can be computed simply by estimating the heating rate along the 380K isentropic surface and the time rate of change of the lower most stratosphere (region between the tropopause and 380K). Given the net tropopause mass flux and the cross tropopause diabatic flux, the residual adiabatic mass flux can be estimated. These fluxes have been computed using three different meteorological data sets, the FVGCM and two assimilation data sets, FVDAS, and UKMO, using the 3.5 PVU defined tropopause. For all three data sets, the extratropical diabatic flux across the tropopause is generally to be larger than the net flux cross tropopause flux implying that there is a net extra-tropical adiabatic flux of air from the troposphere into the middle world stratosphere. This adiabatic flux is four to five times larger than the flux into the stratosphere across the tropical tropopause. For the FVDAS, the tropopause diabatic flux is smaller than UKMO as a result of colder tropopause temperatures. The difference in the diabatic mass fluxes by almost a factor of two between the two data assimilation meteorological analyses is much larger than the interannual variability in the UKMO or FVGCM data sets. Compared to radiosonde estimated tropopause temperatures, both data assimilation tropopause temperatures are warm biased due to a low bias in the tropopause heights. These comparisons point to the PV determination of the tropopause height as the source of the differences in the mass fluxes.

Schoeberl, Mark↗
NASA NTRS2004

Balloon Borne Soundings of Water Vapor, Ozone and Temperature in the Upper Tropospheric and Lower Stratosphere as Part of the Second SAGE III Ozone Loss and Validation Experiment (SOLVE-2)

The main goal of our work was to provide in situ water vapor and ozone profiles in the upper troposphere and lower stratosphere as reference measurements for the validation of SAGE III water vapor and ozone retrievals. We used the NOAA/CMDL frost point hygrometer and ECC ozone sondes on small research balloons to provide continuous profiles between the surface and the mid stratosphere. The NOAA/CMDL frost point hygrometer is currently the only lightweight balloon borne instrument capable of measuring water vapor between the lower troposphere and middle stratosphere. The validation measurements were based in the arctic region of Scandinavia for northern hemisphere observations and in New Zealand for southern hemisphere observations and timed to coincide with overpasses of the SAGE III instrument. In addition to SAGE III validation we also tried to coordinate launches with other instruments and studied dehydration and transport processes in the Arctic stratospheric vortex.

Voemel, Holger↗
NASA NTRS2004

Observations of the Upper Tropospheric Water Vapor Feedback in UARS MLS and HALOE Data

One of the biggest uncertainties in climate science today concerns the water vapor feedback. Most GCMs hold relative humidity fixed as the climate changes, which provides a strong positive feedback to warming due from anthropogenic greenhouse gas emissions. Some in the community, on the other hand, have speculated that tropospheric specific humidity will remain fixed as the climate changes. Observational studies have attempted to resolve this disagreement, but the results have been inconclusive, and few of the studies have focused on the upper troposphere (UT). This is a significant oversight: the surface temperature is especially sensitive to changes in water vapor in the UT owing to the cold temperatures found there. We present an analysis of UARS MLS and HALOE water vapor measurements at 21 5 hPa. We find strong evidence that the water vapor feedback in the UT is positive, but not as strong as fixed relative humidity scenarios. This suggests that GCMs are overestimating the sensitivity of the climate.

Dessler, A. E.↗
NASA NTRS2004

Variability in Tropical Tropospheric Ozone as Observed by SHADOZ

The SHADOZ (Southern Hemisphere Additional Ozonesondes) ozone sounding network was initiated in 1998 to improve the coverage of tropical in-situ ozone measurements for satellite validation, algorithm development and related process studies. Over 2000 soundings have been archived at the central website, , for 12 stations: Ascension Island; Nairobi and Malindi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil; Paramaribo, Surinam. Some results to date indicate reliability of the measurement and highly variable interactions between ozone and tropical meteorology. For example: 1. By using ECC sondes with similar procedures, 5-10% accuracy and precision (1-sigma) of the sonde total ozone measurement was achieved [Thompson et al., 2003al; 2. Week-to-week variability in tropospheric ozone is so great that statistics are frequently not Gaussian and most stations vary up to a factor of 3 in column amount over the course of a year [Thompson et al., 2002b]. 3. Longitudinal variability in tropospheric ozone profiles is a consistent feature, with a 10- 15 DU column-integrated difference between Atlantic and Pacific sites; this is the cause of the zonal wave-one feature in total ozone [Shiotani, 1992]. The ozone record from Paramaribo, Surinam (6N, 55W) is a marked contrast to southern tropical ozone because Surinam is often north of the Intertropical Convergence Zone. Interpretations of SHADOZ time-series and approaches to classification suggested by SHADOZ data over Africa and the Indian Ocean will be described.

Thompson, Anne M.↗
NASA NTRS1997

Temperature lapse rate and methane in Titan's troposphere

We have reanalyzed the Voyager radio occultation data for Titan, examining two alternative approaches to methane condensation. In one approach, methane condensation is facilitated by the presence of nitrogen because nitrogen lowers the condensation level of a methane/nitrogen mixture. The resulting enhancement in methane condensation lowers the upper limit on surface relative humidity of methane obtained from the Voyager occultation data from 0.7 to 0.6. We conclude that in this case the surface relative humidity of methane lies between 0.08 and 0.6, with values close to 0.6 indicated. In the other approach, methane is allowed to become supersaturated and reaches 1.4 times saturation in the troposphere. In this case, surface humidities up to 100% are allowed by the Voyager occultation data, and thus the upper limit must be set by other considerations. We conclude that if supersaturation is included, then the surface relative humidity of methane can be any value greater than 0.08--unless a deep ocean is present, in which case the surface relative humidity is limited to less than 0.85. Again, values close to 0.6 are indicated. Overall, the tropospheric lapse rate on Titan appears to be determined by radiative equilibrium. The lapse rate is everywhere stable against dry convection, but is unstable to moist convection. This finding is consistent with a supersaturated atmosphere in which condensation-and hence moist convection-is inhibited.

Methane/analysis↗
NASA NTRS2004

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

We investigated the isotopic fractionation of CH4 and hydrogen (H2) in the stratosphere by incorporating isotope-specific rate coefficients into the Lawrence Livermore National Laboratory (LLNL) 2D model and comparing the model results with new observations from the NASA ER-2 aircraft (funded through a separate task under the Upper Atmosphere Research Program). The model results reveal that fractionation which occurs in the stratosphere has a significant influence on isotope compositions in the free troposphere, an important point which had previously been ignored, unrecognized or unquantified for many long-lived trace gases, including CH4 and H2 which we have focused our efforts on to date. Our analyses of the model results and new isotope observations have also been used to test how well the kinetic isotope effects are known, at least to within the uncertainties in model chemistry and transport. Overall, these results represent an important step forward in our understanding of isotope fractionation in the atmosphere and demonstrate that stratospheric isotope fractionation cannot be ignored in modeling studies which use isotope observations in the troposphere to infer the global budgets of CH4 (an important greenhouse gas) and of H2 (a gas whose atmospheric budget must be better quantified, particularly before a large human perturbation from fuel cell use is realized). Our analyses of model results and observations from the NASA ER-2 aircraft are briefly summarized separately below for CH4, H2, and H2O and for the contribution of these modeling studies to date to our understanding of isotope fractionation for N2O, CO2, and O3 as well.

Boering, Kristie A.↗
NASA NTRS2003

Global and Regional Decreases in Tropospheric Oxidants from Photochemical Effects of Aerosols

We evaluate the sensitivity of tropospheric OH, O3, and O3 precursors to photochemical effects of aerosols not usually included in global models: (1) aerosol scattering and absorption of ultraviolet radiation and (2) reactive uptake of HO', NO2, and NO3. Our approach is to couple a global 3-D model of tropospheric chemistry (GEOS- CHEM) with aerosol fields from a global 3-D aerosol model (GOCART). Reactive uptake by aerosols is computed using reaction probabilities from a recent review (gamma(sub HO2) = 0.2, gamma(sub NO2) = 10(exp -4), gamma(sub NO3) = l0(exp -3). Aerosols decrease the O3 - O((sup 1)D) photolysis frequency by 5-20% at the surface throughout the Northern Hemisphere (largely due to mineral dust) and by a factor of 2 in biomass burning regions (largely due to black carbon). Aerosol uptake of HO2 accounts for 10-40% of total HOx radical ((triple bonds)OH + peroxy) loss in the boundary layer over polluted continental regions (largely due to sulfate and organic carbon) and for more than 70% over tropical biomass burning regions (largely due to organic carbon). Uptake of NO2 and NO3 accounts for 10-20% of total HNO3 production over biomass burning regions and less elsewhere. Annual mean OH concentrations decrease by 9% globally and by 5-35% in the boundary layer over the Northern Hemisphere. Simulated CO increases by 5- 15 ppbv in the remote Northern Hemisphere, improving agreement with observations. Simulated boundary layer O3 decreases by 15- 45 ppbv over India during the biomass burning season in March and by 5-9 ppbv over northern Europe in August, again improving comparison with observations. We find that particulate matter controls would increase surface O3 over Europe and other industrial regions.

Martin, Randall V.↗
NASA NTRS2004

Tropospheric Wind Monitoring During Day-of-Launch Operations for NASA's Space Shuttle Program

The Environments Group at the National Aeronautics and Space Administration's Marshall Space Flight Center monitors the winds aloft above Kennedy Space Center (KSC) in support of the Space Shuttle Program day-of-launch operations. Assessment of tropospheric winds is used to support the ascent phase of launch. Three systems at KSC are used to generate independent tropospheric wind profiles prior to launch; 1) high resolution jimsphere balloon system, 2) 50-MHz Doppler Radar Wind Profiler (DRWP) and 3) low resolution radiosonde system. All independent sources are compared against each other for accuracy. To assess spatial and temporal wind variability during launch countdown each jimsphere profile is compared against a design wind database to ensure wind change does not violate wind change criteria.

Decker, Ryan↗
NASA NTRS2004

First Global Maps of Stratospheric and Tropospheric NO2 from OMI

The Ozone Monitoring Instrument (OMI) was launched successfully in July 2004, as one of four instruments on the EOS Aura satellite. OMI makes hyperspectral measurements that are used to retrieve column densities of critical trace gases, including formaldehyde, BrO, SO2 and NO2 . We present the first results from the OM1 operational NO2 algorithm and demonstrate its ability to retrieve the tropospheric and stratospheric components of NO2. The DOAS method is used to determine slant column densities, and initial air mass factors (AMFs) are used. to give initial estimates of the vertical column densities (VCDs). VCDs from up to 15 consecutive orbits are collected, and a spatial filtering technique is applied to extract the synoptic-scale features characteristic of the stratospheric, field. features to be evidence of tropospheric excess NO2 , and apply an AMF appropriate to polluted conditions, to obtain an improved retrieval of the NO2 total VCD. We describe the assumptions underlying the algorithm in detail, and show global maps of NO2 VCDs, based on the first operational data from OMI.

Bucsela, Eric J.↗
NASA NTRS2004

Tropospheric Wind Monitoring During Day-of-Launch Operations for National Aeronautics and Space Administration's Space Shuttle Program

The Environments Group at the National Aeronautics and Space Administration's Marshall Space Flight Center (NASA/MSFC) monitors the winds aloft at Kennedy Space Center (KSC) during the countdown for all Space Shuttle launches. Assessment of tropospheric winds is used to support the ascent phase of launch. Three systems at KSC are used to generate independent tropospheric wind profiles prior to launch; 1) high resolution Jimsphere balloon system, 2) 50-MHz Doppler Radar Wind Profiler (DRWP) and 3) low resolution radiosonde system. Data generated by the systems are used to assess spatial and temporal wind variability during launch countdown to ensure wind change observed does not violate wind change criteria constraints.

Decker, Ryan K.↗
NASA NTRS2004

Surface-Satellite Measurements for Atmospheric Radiative Transfer (SMART)and Chemical, Optical and Microphysical Measurements of In-Situ Troposphere (COMMIT) Research Activities

The GSFC SMART consists of a suite of remote sensing instruments, including many commercially available radiometers, spectrometer, interferometer, and three in-house developed inskuments: micro-pulse lidar (MPL), scanning microwave radiometer (SMiR), and sun-sky-surface photometer (S(sup 3)). SMART cover the spectral range from UV to microwave, and passive to active remote sensing. This is to enrich the EOS-like research activities (i.e., EOS validation, innovative investigations, and long-term local environmental observations). During past years, SMART has been deployed in many NASA supported field campaigns to collocate with satellite nadir overpass for intercomparisons, and for initializing model simulations. Built on the successful experience of SMART, we are currently developing a new ground-based in-situ sampling package, COMMIT, including measurements of trace gases (CO, SO2, NOx, and O3,) concentrations, fine/coarse particle sizers and chemical composition, single- and three-wavelength nephelometers, and surface meteorological probes. COMMIT is built for seeking a relationship between surface in-situ measurements and boundary layer characteristics. This is to enrich EOS-like research on removing boundary layer signal from the entire column from space observation - to deduce the stable (less variability) free-troposphere observations. The COMMIT will try its best to link the chemical, microphysical, and optical properties of the boundary layer with radiation. The next major activities for SMART-COMMIT are scheduled for 2004-2006 in BASE-ASIA and EAST-AIRE. The expected close collaboration of BASE-ASIA with various research projects in Asia (i.e., ABC in South Asia, led by Ramanathan et al.; EAST-AIRE in East Asia, led by Li et al.; and APEX in Northeast Asia, led by Nakajima et al.) will definitely provide a better understanding of the impact of the biomass burning and air pollutants on regional-to-global climate, hydrological and carbon cycles, and tropospheric chemistry in Asia.

Tsay, Si-Chee↗
NASA NTRS2003

Stratospheric-Tropospheric Interaction and the 2002 Ozone Hole

The 2002 ozone hole was remarkable for its small size and early break-up. This small size resulted from a series of wave events over the course of the 2002 winter. The major event of the 2002 winter was the major warming in late September 2002. This warming resulted from an extremely strong wave event that propagated out of the troposphere, reversed the zonal mean flow, and warmed the polar vortex. This late-September event was the culmination of a series of large wave events which occurred over the course of the 2002 winter. These waves collectively warmed the vortex and decelerated the stratospheric flow. In this talk, we will trace the origin of these wave events, and we will also analyze the feedback of the large disruption of the stratospheric flow on the troposphere.

Newman, Paul A.↗
NASA NTRS2004

The Satellite View of Extra-Tropical Stratosphere-Troposphere Exchange and the UT/LS

This talk will review satellite studies which have helped define the UT/LS and stratosphere-troposphere exchange. Satellites have provided a global perspective but have had limited temporal and spatial measurements for stratosphere-troposphere exchange (STE) studies. Nonetheless, long lived tracer measurements from satellites can be used as proxies for age-of-air can thus provide estimates of mixing and transport processes in the UT/LS. These measurements can be compared to model estimates of the mean age-of-air and trace gas fluxes providing an important model diagnostic. With the launch of EOS Aura, the potential for satellite trace gas measurements of the lower-most stratosphere and STE is significantly improved, and Aura s mission will be briefly described.

Schoeberl, Mark R.↗
NASA NTRS2004

Insights into Tropospheric Ozone from the INTEX Ozonesonde Network Study (IONS)

Ozone profile data from soundings integrate models, aircraft and other ground-based measurements for better interpretation of atmospheric chemistry and dynamics. A well-designed network of ozonesonde stations, with consistent sampling, can answer questions not possible with short campaigns or current satellite technology. The SHADOZ (Southern Hemisphere Additional Ozonesondes) project, for example, has led to these findings about tropical ozone: definition of the zonal tropospheric wave-one pattern in equatorial ozone, characterization of the "Atlantic ozone paradox" and establishment of a link between tropical Atlantic and Indian Ocean pollution. Building on the SHADOZ concept, a short-term ozone network was formed in July-August 2004 to coordinate ozonesonde launches during the ICARTT/INTEX/NEAQS (International Consortium on Atmospheric Research on Transport and Transformation)/Intercontinental Transport Experiment/New England Air Quality Study. In IONS (INTEX Ozonesonde Network Study), more than 250 soundings, with daily frequency at half the sites, were launched from eleven North American stations and an oceanographic ship in the Gulf of Maine. Although the goal was to examine pollution influences under stable high-pressure systems and transport associated with "warm conveyor belt" flows, the INTEX study region was dominated by a series of weak frontal system that mixed aged pollution with stratospheric ozone in the middle troposphere. Deconvoluting ozone sources provides new insights into ozone in the transition between mid-latitude and polar air.

Thompson, Anne M.↗
NASA NTRS2005

Interannual Variations in Tropical Upper-Tropospheric Humidity: Understanding Tropical Convective and Dynamical Processes

Uncertainty remains as to what extent variability in mid to upper tropospheric moisture, especially over the tropics, behaves as constant relative humidity during interannual climate variations associated with ENSO. Systematic variations in HIRS 6.7 micron and MLS 205 GHz suggest that dry subtropical regions evolving during warm SST events depress relative humidity, but the interpretation of these events is still uncertain. Additional specific concerns have to do with regional signatures of convective processes: How does the origin of dry air in the eastern subtropical N. Pacific differ in ENSO warm versus cold years? The dynamics of Rossby wave forcing by convective heating, subtropical jet stream dynamics, and dynamics driven subsidence all come into play here. How variations in precipitating ice hydrometeors from tropical anvils relate to variations in UTH is also a subject of debate? Do variations in precipitating ice, cloud cover and water vapor behavior show any support for the Iris-hypothesis mechanism? Here we examine historical records of SSM/T-2 data to gain a better physical understanding of the effects of deep convective moisture sources and dynamically-induced vertical circulations on UTH. These high frequency microwave measurements (183.3 GHz) take advantage of far less sensitivity to cloud hydrometeors than the 6.7 micron data to yield a record of upper tropospheric relative humidity. Furthermore, signatures of precipitating ice from these channels facilitate comparisons to TRMM hydrometeors detected by radar. In analyzing these observations, we isolate water vapor and temperature change components that affect brightness temperatures and the inferred relative humidity. Trajectory modeling is also used to understand interannual humidity anomalies in terms of outflow fbm convective regions and history of diabatically-driven sinking which modifies relative humidity.

Robertson, Franklin R.↗
NASA NTRS2005

How well can we Measure the Vertical Profile of Tropospheric Aerosol Extinction?

The recent Department of Energy Atmospheric Radiation Measurement (ARM) Aerosol Intensive Operations Period (MOP, May 2003) yielded one of the best measurement sets obtained to-date to assess our ability to measure the vertical profile of ambient aerosol extinction sigma(sub ep)(lambda) in the lower troposphere. During one month, a heavily instrumented aircraft with well characterized aerosol sampling ability carrying well proven and new aerosol instrumentation, devoted most of the 60 available flight hours to flying vertical profiles over the heavily instrumented ARM Southern Great Plains (SGP) Climate Research Facility (CRF). This allowed us to compare vertical extinction profiles obtained from 6 different instuments: airborne Sun photometer (AATS-14), airborne nephelometer/absorption photometer, airborne cavity ring-down system, ground-based Raman lidar and 2 ground-based elastic backscatter lidars. We find the in-situ measured sigma(sub ep)(lambda) to be lower than the AATS-14 derived values. Bias differences are 0.002 - 0.004 K/m equivalent to 12-17% in the visible, or 45% in the near-infrared. On the other hand, we find that with respect to AATS-14, the lidar sigma(sub ep)(lambda) are higher. An unnoticed loss of sensitivity of the Raman lidar had occurred leading up to AIOP and we expect better agreement from the recently restored system looking at the collective results from 6 field campaigns conducted since 1996, airborne in situ measurements of sigma(sub ep)(lambda) tend to be biased slightly low (17% at visible wavelengths) when compared to airborne Sun photometer sigma(sub ep)(lambda). On the other hand, sigma(sub ep)(lambda) values derived from lidars tend to have no or positive biases. From the bias differences we conclude that the typical systematic error associated with measuring the tropospheric vertical profile of the ambient aerosol extinction with current state of-the art instrumentation is 15-20% at visible wavelengths and potentially larger in the UV and near-infrared.

Schmid, Beat↗