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NASA NTRS2001

Advanced Global Atmospheric Gases Experiment (AGAGE)

AGAGE comprises continuous high frequency in-situ gas chromatographic FID/ECD measurements of two biogenic/anthropogenic gases (CH4, N2O) and five anthropogenic gases (CFCl3, CF2Cl2, CH3CCl3, CF2ClCFCl2, CCl4) which are carried out at five globally distributed sites (Ireland, California, Barbados, Samoa, Tasmania). Also, high frequency in-situ gas-chromatographic mass spectrometric measurements of about 30 species including chlorofluorocarbon replacements and many natural halocarbons are made at two sites (Ireland, Tasmania), and will soon begin at the other three sites. Finally, high frequency in-situ gas chromatographic HgO-RD measurements of CO and H2 are performed at two sites (Ireland, Tasmania). The goal is quantitative determination of the sources, sinks, and circulation of these environmentally important gases.

Prinn, Ronald G.↗

NASA NTRS2001

Studies of Tropical/Mid-Latitude Exchange Using UARS Observations

At the time this proposal was submitted, recent publications had suggested an important role for transport of midlatitude air into the tropical lower stratosphere. Most of these studies had employed data that gave only a time-averaged picture, making it difficult to determine the nature of the transport processes responsible for the observed behavior. We proposed to analyze observations of long-lived trace gases, such as nitric acid, methane, nitrous oxide, and chlorofluorocarbons, made from the Upper Atmosphere Research Satellite, to investigate the seasonal behavior of mixing between the midlatitudes and tropics. We planned to construct probability distributions of the concentrations of these species over small altitude ranges and to compare them to expectations based on modeled mean concentrations and knowledge of instrument precision. Differences from expectation were to be analyzed with respect to meteorological parameters to determine whether wave activity may have induced apparent mixing.

Avallone, Linnea↗

NASA NTRS2002

Ozone Layer Observations

The US National Aeronautics and Space Administration (NASA) has been monitoring the ozone layer from space using optical remote sensing techniques since 1970. With concern over catalytic destruction of ozone (mid-1970s) and the development of the Antarctic ozone hole (mid-1980s), long term ozone monitoring has become the primary focus of NASA's series of ozone measuring instruments. A series of TOMS (Total Ozone Mapping Spectrometer) and SBUV (Solar Backscatter Ultraviolet) instruments has produced a nearly continuous record of global ozone from 1979 to the present. These instruments infer ozone by measuring sunlight backscattered from the atmosphere in the ultraviolet through differential absorption. These measurements have documented a 15 Dobson Unit drop in global average ozone since 1980, and the declines in ozone in the antarctic each October have been far more dramatic. Instruments that measure the ozone vertical distribution, the SBUV and SAGE (Stratospheric Aerosol and Gas Experiment) instruments for example, show that the largest changes are occurring in the lower stratosphere and upper troposphere. The goal of ozone measurement in the next decades will be to document the predicted recovery of the ozone layer as CFC (chlorofluorocarbon) levels decline. This will require a continuation of global measurements of total column ozone on a global basis, but using data from successor instruments to TOMS. Hyperspectral instruments capable of measuring in the UV will be needed for this purpose. Establishing the relative roles of chemistry and dynamics will require instruments to measure ozone in the troposphere and in the stratosphere with good vertical resolution. Instruments that can measure other chemicals important to ozone formation and destruction will also be needed.

McPeters, Richard↗

NASA NTRS2003

Monitoring of Observation Errors in the Assimilation of Satellite Ozone Data

The stratospheric ozone layer protects life on Earth from the harmful effects of solar ultravioiet radiation. The ozone layer is currently in a fragile state because of depletion caused by man-made chemicals, especially chlorofluorocarbons. The state of the ozone layer is being monitored and evaluated by scientific experts around the world, in order to help policy makers assess the impacts of international protocols that control the production and release of ozone depleting chemicals. Scientists use a variety ozone measurements and models in order to form a comprehensive picture about the current state of the ozone layer, and to predict the future behavior (expected to be a recovery, as the abundance of the depleting chemicals decreases). Among the data sets used, those from satellite-borne instruments have the advantage of providing a wealth of information about the ozone distribution over most of the globe. Several instruments onboard American and international satellites make measurements of the properties of the atmosphere, from which atmospheric ozone amounts are estimated; long-term measurement programs enable monitoring of trends in ozone. However, the characteristics of satellite instruments change in time. For example, the instrument lenses through which measurements are made may deteriorate over time, or the satellite orbit may drift so that measurements over each location are made later and later in the day. These changes may increase the errors in the retrieved ozone amounts, and degrade the quality of estimated ozone amounts and of their variability. Our work focuses on combining the satellite ozone data with global models that capture atmospheric motion and ozone chemistry, using advanced statistical techniques: this is known as data assimilation. Our method provides a three-dimensional global ozone distribution that is consistent with both the satellite measurements and with our understanding of processes (described in the models) that control ozone distribution. Through the monitoring of statistical properties of the agreement between the data and the model, this approach also enables us to detect changes in the quality of ozone data retrieved from satellite-borne instrument measurements. This paper demonstrates that calculations of the changes in satellite data quality, and the impact these changes on the estimates of the global ozone distribution, can assist in maintaining the uniform quality of the satellite ozone data throughout the lifetime of these instruments, thus contributing to our understanding of long-term ozone change.

Stajner, Ivanka↗

NASA NTRS2006

On detecting a trend in the residual circulation from observations of column HCl

The troposphere is the part of the atmosphere where people live. The troposphere goes up to about 12 km above the earth over places at middle latitudes like Washington, D.C. The next layer of air up in the atmosphere is called the stratosphere. The tropopause separates the troposphere and stratosphere. Most of the ozone in the atmosphere is in the stratosphere where it protects people from the harmful rays in sunlight. Near the earth s surface, ozone is a pollutant. In general, air travels from the troposphere to the stratosphere through upward motion in the tropics. Most of the air comes back down to the troposphere at middle latitudes. The so-called "stratospheric residual circulation" moves the air in the stratosphere from the tropics to the middle latitudes. In this way, the amount of air that moves out of the stratosphere into the troposphere at middle latitudes depends on the strength of the residual circulation. This overturning of the atmosphere is important as it brings chemicals produced by the activities of people into the stratosphere. Most notable are chlorofluorocarbons (CFCs) that destroy stratospheric ozone. The transport of air out of the stratosphere removes ozone-destroying chemicals, but also brings ozone into the troposphere.

Olsen, M. A.↗

NASA NTRS1995

Kinetics of FO2 with NO, NO2, O3, CH4, and C2H6

The presence of fluorine containing compounds (e.g. HF and COF2) in the Earth's atmosphere is thought to be due solely to the decomposition of man-made chemicals such as chlorofluorocarbons and hydrofluorocarbons. The effect on atmosphere ozone of reactive fluorine-containing intermediates produced during CFC and HFC decomposition has attracted significant interest recently.

fluorine compounds atmospheric gasses ozone mass s↗

NASA NTRS2007

Variations in Stratospheric Inorganic Chlorine Between 1991 and 2006

So how quickly will the ozone hole recover? This depends on how quickly the chlorine content (Cl2) of the atmosphere will decline. The ozone hole forms over the Antarctic each southern spring (September and October). The extremely small ozone amounts in the ozone hole are there because of chemical reactions of ozone with chlorine. This chlorine originates largely from industrially produced chlorofluorocarbon (CFC) compounds. An international agreement, the Montreal Protocol, is drastically reducing the amount of chlorine-containing compounds that we are releasing into the atmosphere. To be able to attribute changes in stratospheric ozone to changes in chlorine we need to know the distribution of atmospheric chlorine. However, due to a lack of continuous observations of all the key chlorine gases, producing a continuous time series of stratospheric chlorine has not been achieved to date. We have for the first time devised a technique to make a 17-year time series for stratospheric chlorine that uses the long time series of HCl observations made from several space borne instruments and a neural network. The neural networks allow us to both inter-calibrate the various HCl instruments and to infer the total amount of atmospheric chlorine from HCl. These new estimates of Cl, provide a much needed critical test for current global models that currently predict significant differences in both Cl(sub y) and ozone recovery. These models exhibit differences in their projection of the recovery time and our chlorine content time series will help separate the good from the bad in these projections.

Lary, D. J.↗

NASA NTRS2007

Short- and Medium-term Atmospheric Effects of Very Large Solar Proton Events

Long-term variations in ozone have been caused by both natural and humankind related processes. In particular, the humankind or anthropogenic influence on ozone from chlorofluorocarbons and halons (chlorine and bromine) has led to international regulations greatly limiting the release of these substances. These anthropogenic effects on ozone are most important in polar regions and have been significant since the 1970s. Certain natural ozone influences are also important in polar regions and are caused by the impact of solar charged particles on the atmosphere. Such natural variations have been studied in order to better quantify the human influence on polar ozone. Large-scale explosions on the Sun near solar maximum lead to emissions of charged particles (mainly protons and electrons), some of which enter the Earth's magnetosphere and rain down on the polar regions. "Solar proton events" have been used to describe these phenomena since the protons associated with these solar events sometimes create a significant atmospheric disturbance. We have used the National Center for Atmospheric Research (NCAR) Whole Atmosphere Community Climate Model (WACCM) to study the short- and medium-term (days to a few months) influences of solar proton events between 1963 and 2005 on stratospheric ozone. The four largest events in the past 45 years (August 1972; October 1989; July 2000; and October-November 2003) caused very distinctive polar changes in layers of the Earth's atmosphere known as the stratosphere (12-50 km; -7-30 miles) and mesosphere (50-90 km; 30-55 miles). The solar protons connected with these events created hydrogen- and nitrogen- containing compounds, which led to the polar ozone destruction. The hydrogen-containing compounds have very short lifetimes and lasted for only a few days (typically the duration of the solar proton event). On the other hand, the nitrogen-containing compounds lasted much longer, especially in the Winter. The nitrogen oxides were predicted to increase substantially due to these solar events and led to mid- to upper polar stratospheric ozone decreases of over 20%. These WACCM results generally agreed with satellite measurements. Both WACCM and measurements showed enhancements of nitric acid, dinitrogen pentoxide, and chlorine nitrate, which were indirectly caused by these solar events. Solar proton events were shown to cause a significant change in the polar stratosphere and need to be considered in understanding variations during years of strong solar activity.

Jackman, Charles H.↗

NASA NTRS2008

Stratospheric Ozone in the Post-CFC Era

Vertical and latitudinal changes in the stratospheric ozone in the post-chlorofluorocarbon (CFC) era are investigated using simulations of the recent past and the 21st century with a coupled chemistry-climate model. Model results reveal that, in the 2060s when the stratospheric halogen loading is projected to return to its 1980 values, the extratropical column ozone is significantly higher than that in 1975-1984, but the tropical column ozone does not recover to 1980 values. Upper and lower stratospheric ozone changes in the post- CFC era have very different patterns. Above 15 hPa ozone increases almost latitudinally uniformly by 6 Dobson Unit (DU), whereas below 15 hPa ozone decreases in the tropics by 8 DU and increases in the extratropics by up to 16 DU. The upper stratospheric ozone increase is a photochemical response to greenhouse gas induced strong cooling, and the lower stratospheric ozone changes are consistent with enhanced mean advective transport due to a stronger Brewer-Dobson circulation. The model results suggest that the strengthening of the Brewer-Dobson circulation plays a crucial role in ozone recovery and ozone distributions in the post-CFC era.

Li, Feng↗

NASA NTRS2008

The GEOS Chemistry Climate Model: Comparisons to Satellite Data

The Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) has been developed by combining the atmospheric chemistry and transport modules developed over the years at Goddard and the GEOS general circulation model, also developed at Goddard. We will compare model simulations of ozone, and the minor constituents that affect ozone, for the period around 1980 with newly released revised data from the Limb Infrared Monitor of the Stratosphere (LIMS) instrument on Nimbus 4. We will also compare model simulations for the period of the early 2000s with the data from the Microwave Limb Sounder (MLS) and the High Resolution Dynamic Limb Sounder (HRDLS) on the Aura satellite. We will use these comparisons to examine the performance of the model for the present atmosphere and for the change that has occurred during the last 2 decades of ozone loss due to chlorine and bromine compounds released from chlorofluorocarbons and halons.

Stolarski, Richard S.↗

NASA NTRS2008

The Long-term Middle Atmospheric Influence of Very Large Solar Proton Events

Long-term variations in ozone have been caused by both natural and humankind related processes. The humankind or anthropogenic influence on ozone originates from the chlorofluorocarbons and halons (chlorine and bromine) and has led to international regulations greatly limiting the release of these substances. Certain natural ozone influences are also important in polar regions and are caused by the impact of solar charged particles on the atmosphere. Such natural variations have been studied in order to better quantify the human influence on polar ozone. Large-scale explosions on the Sun near solar maximum lead to emissions of charged particles (mainly protons and electrons), some of which enter the Earth's magnetosphere and rain down on the polar regions. "Solar proton events" have been used to describe these phenomena since the protons associated with these solar events sometimes create a significant atmospheric disturbance. We have used the National Center for Atmospheric Research (NCAR) Whole Atmosphere Community Climate Model (WACCM) to study the long-term (> few months) influences of solar proton events from 1963 through 2004 on stratospheric ozone and temperature. There were extremely large solar proton events in 1972, 1989,2000,2001, and 2003. These events caused very distinctive polar changes in layers of the Earth's atmosphere known as the stratosphere (12-50 km; -7-30 miles) and mesosphere (50-90 km; 30-55 miles). The solar protons connected with these events created hydrogen- and nitrogen-containing compounds, which led to the polar ozone destruction. The nitrogen-containing compounds, called odd nitrogen, lasted much longer than the hydrogen-containing compounds and led to long-lived stratospheric impacts. An extremely active period for these events occurred in the five-year period, 2000- 2004, and caused increases in odd nitrogen which lasted for several months after individual events. Associated stratospheric ozone decreases of >lo% were calculated to last for up to five months past the largest events. However, the computed total column ozone and stratospheric temperature changes connected with the solar events were not found to be statistically significant. Thus, solar proton events do not likely contribute significantly to measured total column ozone fluctuations and stratospheric temperature changes.

Jackman, Charles H.↗

NASA NTRS2008

Fiber-Optic Determination of N2, O2, and Fuel Vapor in the Ullage of Liquid-Fuel Tanks

A fiber-optic sensor system has been developed that can remotely measure the concentration of molecular oxygen (O2), nitrogen (N2), hydrocarbon vapor, and other gases (CO2, CO, H2O, chlorofluorocarbons, etc.) in the ullage of a liquid-fuel tank. The system provides an accurate and quantitative identification of the above gases with an accuracy of better than 1 percent by volume (for O2 or N2) in real-time (5 seconds). In an effort to prevent aircraft fuel tank fires or explosions similar to the tragic TWA Flight 800 explosion in 1996, OBIGGS are currently being developed for large commercial aircraft to prevent dangerous conditions from forming inside fuel tanks by providing an inerting gas blanket that is low in oxygen, thus preventing the ignition of the fuel/air mixture in the ullage. OBIGGS have been used in military aircraft for many years and are now standard equipment on some newer large commercial aircraft (such as the Boeing 787). Currently, OBIGGS are being developed for retrofitting to existing commercial aircraft fleets in response to pending mandates from the FAA. Most OBIGGS use an air separation module (ASM) that separates O2 from N2 to make nitrogen-enriched air from compressed air flow diverted from the engine (bleed air). Current OBIGGS systems do not have a closed-loop feedback control, in part, due to the lack of suitable process sensors that can reliably measure N2 or O2 and at the same time, do not constitute an inherent source of ignition. Thus, current OBIGGS operate with a high factor-of-safety dictated by process protocol to ensure adequate fuel-tank inerting. This approach is inherently inefficient as it consumes more engine bleed air than is necessary compared to a closed-loop controlled approach. The reduction of bleed air usage is important as it reduces fuel consumption, which translates to both increased flight range and lower operational costs. Numerous approaches to developing OBIGGS feedback-control sensors have been under development by many research groups and companies. However, the direct measurement of nitrogen (N2) is a challenge to most OBIGGS ullage sensors (such as tunable diode laser absorption) as they cannot measure N2 directly but depend on the measurement of oxygen (O2). The problem with a singular measure of O2, is that as the concentration (number density) of O2 decreases due to the inerting process or due to lower pressures from high altitudes, the precision and accuracy of the O2 measurement decreases. However, measuring O2 density in combination with N2 density (which is more abundant in air and in a N2-inerted fuel tank) can provide a much more accurate and reliable determination of the OBIGGS efficacy.

Nguyen, Quang-Viet↗

NASA NTRS2010

Selection of Environmentally Friendly Solvents for the Extravehicular Mobility Unit Secondary Oxygen Pack Cold Trap Testing

Freon-113(TradeMark) has been used as a chemistry lab sampling solvent at NASA/JSC for EMU (extravehicular Mobility Unit) SOP (Secondary Oxygen Pack) oxygen testing Cold Traps utilized at the USA (United Space Alliance) Houston facility. Similar testing has occurred at the HSWL (Hamilton Sundstrand Windsor Locks) facility. A NASA Executive Order bans the procurement of all ODS (ozone depleting substances), including Freon-113 by the end of 2009. In order to comply with NASA direction, HSWL began evaluating viable solvents to replace Freon-113 . The study and testing effort to find Freon-113 replacements used for Cold Trap sampling is the subject of this paper. Test results have shown HFE-7100 (a 3M fluorinated ether) to be an adequate replacement for Freon-113 as a solvent to remove and measure the non-volatile residue collected in a Cold Trap during oxygen testing. Furthermore, S-316 (a Horiba Instruments Inc. high molecular weight, non-ODS chlorofluorocarbon) was found to be an adequate replacement for Freon-113 as a solvent to reconstitute non-volatile residue removed from a Cold Trap during oxygen testing for subsequent HC (hydrocarbon) analysis via FTIR (Fourier Transform Infrared Spectroscopy).

Steele, John↗

NASA NTRS2010

Multi-decade Measurements of the Long-Term Trends of Atmospheric Species by High-Spectral-Resolution Infrared Solar Absorption Spectroscopy

Solar absorption spectra were recorded for the first time in 5 years with the McMath Fourier transform spectrometer at the US National solar Observatory on Kitt Peak in southern Arizona, USA (31.91 N latitude, 111.61 W longitude, 2.09 km altitude). The solar absorption spectra cover 750-1300 and 1850-5000 cm(sup -1) and were recorded on 20 days during March-June 2009. The measurements mark the continuation of a long-term record of atmospheric chemical composition measurements that have been used to quantify seasonal cycles and long-term trends of both tropospheric and stratospheric species from observations that began i 1977. Fits to the measured spectra have been performed, and they indicate the spectra obtained since return to operational status are nearly free of channeling and the instrument line shape function is well reproduced taking into account the measurement parameters. We report updated time series measurements of total columns for six atmospheric species and their analysis for seasonal cycles and long-term trends. An sn example, the time series fit shows a decrease in the annual increase rate i Montreal-Protocol-regulated chlorofluorocarbon CCL2F2 from 1.51 plus or minus 0.38% yr(sup -1) at the beginning of the time span to -1.54 plus or minus 1.28 yr(sup -1) at the end of the time span, 1 sigma, and hence provides evidence for the impact of those regulations on the trend.

Rinsland, Curtis P.↗

NASA NTRS2010

Options to Accelerate Ozone Recovery: Ozone and Climate Benefits

The humankind or anthropogenic influence on ozone primarily originated from the chlorofluorocarbons and halons (chlorine and bromine). Representatives from governments have met periodically over the years to establish international regulations starting with the Montreal Protocol in 1987, which greatly limited the release of these ozone-depleting substances (DDSs). Two global models have been used to investigate the impact of hypothetical reductions in future emissions of ODSs on total column ozone. The investigations primarily focused on chlorine- and bromine-containing gases, but some computations also included nitrous oxide (N2O). The Montreal Protocol with ODS controls have been so successful that further regulations of chlorine- and bromine-containing gases could have only a fraction of the impact that regulations already in force have had. if all anthropogenic ODS emissions were halted beginning in 2011, ozone is calculated to be higher by about 1-2% during the period 2030-2100 compared to a case of no additional ODS restrictions. Chlorine- and bromine-containing gases and nitrous oxide are also greenhouse gases and lead to warming of the troposphere. Elimination of N 20 emissions would result in a reduction of radiative forcing of 0.23 W/sq m in 2100 than presently computed and destruction of the CFC bank would produce a reduction in radiative forcing of 0.005 W/sq m in 2100. This paper provides a quantitative way to consider future regulations of the CFC bank and N 20 emissions

Fleming, E. L.↗

NASA NTRS2009

Stratospheric Ozone in the Post-CFC Era

Vertical and latitudinal changes in the stratospheric ozone in the post-chlorofluorocarbon (CFC) era are investigated using simulations of the recent past and the 21st century with a coupled chemistry-climate model. Model results reveal that, in the 2060s when the stratospheric halogen loading is projected to return to its 1980 values, the extratropical column ozone is significantly higher than that in 1975-1984, but the tropical column ozone does not recover to 1980 values. Upper and lower stratospheric ozone changes in the post-CFC era have very different patterns. Above 15 hPa ozone increases almost latitudinally uniformly by 6 Dobson Unit (DU), whereas below 15 hPa ozone decreases in the tropics by 8 DU and increases in the extratropics by up to 16 DU. The upper stratospheric ozone increase is a photochemical response to greenhouse gas induced strong cooling, and the lower stratospheric ozone changes are consistent with enhanced mean advective transport due to a stronger Brewer-Dobson circulation. The model results suggest that the strengthening of the Brewer-Dobson circulation plays a crucial role in ozone recovery and ozone distributions in the post-CFC era.

Li, F.↗

NASA NTRS2005

Chemical Loss of Polar Ozone: Present Understanding and Remaining Uncertainties

Not long after the discovery of the Antarctic ozone hole, it was established that halogen compounds, supplied to the atmosphere mainly by anthropogenic activities, are the primary driver of polar ozone loss. We will briefly review the chemical mechanisms that cause polar ozone loss and the early evidence showing the key role played by anthropogenic halogens. Recently, stratospheric halogen loading has leveled off, due to adherence to the Montreal Protocol and its amendments that has essentially banned CFCs (chlorofluorocarbons) and other halocarbons. We will describe recent reports of the first stage of recovery of the Antarctic ozone hole (e.g., a statistically significant slowing of the downward trend), associated with the leveling off of stratospheric halogens. Despite this degree of understanding, we will discuss the tendency of photochemical models to underestimate the observed rate of polar ozone loss and a hypothesis that has recently been put forth that might resolve this discrepancy. Finally, we will briefly discuss chemical loss of Arctic ozone, which

climate change↗

NASA NTRS2010

Atmospheric CO2: Principal Control Knob Governing Earth's Temperature

Ample physical evidence shows that carbon dioxide (CO2) is the single most important climate-relevant greenhouse gas in Earth s atmosphere. This is because CO2, like ozone, N2O, CH4, and chlorofluorocarbons, does not condense and precipitate from the atmosphere at current climate temperatures, whereas water vapor can and does. Noncondensing greenhouse gases, which account for 25% of the total terrestrial greenhouse effect, thus serve to provide the stable temperature structure that sustains the current levels of atmospheric water vapor and clouds via feedback processes that account for the remaining 75% of the greenhouse effect. Without the radiative forcing supplied by CO2 and the other noncondensing greenhouse gases, the terrestrial greenhouse would collapse, plunging the global climate into an icebound Earth state.

Lacis, Andrew A.↗