UV Absorption Cross Sections of Nitrous Oxide (N2O) and Carbon Tetrachloride (CCl4) Between 210 and 350 K and the Atmospheric Implications

NASA Technical Reports Server (NTRS)

Carlon, Nabilah Rontu; Papanastasiou, Dimitrios K.; Fleming, Eric L.; Jackman, Charles H.; Newman, Paul A.; Burkholder, James B.

2010-01-01

Absorption cross sections of nitrous oxide (N2O) and carbon tetrachloride (CCl4) are reported at five atomic UV lines (184.95, 202.548, 206.200, 213.857, and 228.8 nm) at 27 temperatures in the range 210-350 K. In addition, UV absorption spectra of CCl4 are reported between 200-235 nm as a function of temperature (225-350 K). The results from this work are critically compared with results from earlier studies. For N2O, the present results are in good agreement with the current JPL recommendation enabling a reduction in the estimated uncertainty in the N2O atmospheric photolysis rate. For CCl4, the present cross section results are systematically greater than the current recommendation at the reduced temperatures most relevant to stratospheric photolysis. The new cross sections result in a 5-7% increase in the modeled CCl4 photolysis loss, and a slight decrease in the stratospheric lifetime, from 51 to 50 years, for present day conditions. The corresponding changes in modeled inorganic chlorine and ozone in the stratosphere are quite small. A CCl4 cross section parameterization for use in 37 atmospheric model calculations is presented.

Biospheric-atmospheric coupling on the early Earth

NASA Technical Reports Server (NTRS)

Levine, J. S.

1991-01-01

Theoretical calculations performed with a one-dimensional photochemical model have been performed to assess the biospheric-atmospheric transfer of gases. Ozone reached levels to shield the Earth from biologically lethal solar ultraviolet radiation (220-300 nm) when atmospheric oxygen reached about 1/10 of its present atmospheric level. In the present atmosphere, about 90 percent of atmospheric nitrous oxide is destroyed via solar photolysis in the stratosphere with about 10 percent destroyed via reaction with excited oxygen atoms. The reaction between nitrous oxide and excited oxygen atoms leads to the production of nitric oxide in the stratosphere, which is responsible for about 70 percent of the global destruction of oxygen in the stratosphere. In the oxygen/ozone deficient atmosphere, solar photolysis destroyed about 100 percent of the atmospheric nitrous oxide, relegating the production of nitric oxide via reaction with excited oxygen to zero. Our laboratory and field measurements indicate that atmospheric oxygen promotes the biogenic production of N2O and NO via denitrification and the biogenic production of methane by methanogenesis.

Laboratory Investigations of Stratospheric Halogen Chemistry

NASA Technical Reports Server (NTRS)

Wine, Paul H.; Nicovich, J. Michael; Stickel, Robert E.; Hynes, Anthony J.

1997-01-01

A final report for the NASA-supported project on laboratory investigations of stratospheric halogen chemistry is presented. In recent years, this project has focused on three areas of research: (1) kinetic, mechanistic, and thermochemical studies of reactions which produce weakly bound chemical species of atmospheric interest; (2) development of flash photolysis schemes for studying radical-radical reactions of stratospheric interest; and (3) photochemistry studies of interest for understanding stratospheric chemistry. The first section of this paper contains a discussion of work which has not yet been published. All subsequent chapters contain reprints of published papers that acknowledge support from this grant.

Molecular beam studies of stratospheric photochemistry

NASA Astrophysics Data System (ADS)

Moore, Teresa Anne

1998-12-01

Photochemistry of chlorine oxide containing species plays a major role in stratospheric ozone depletion. This thesis discusses two photodissociation studies of the key molecules ClONO2 and ClOOCl which were previously thought to only produce Cl-atom (ozone depleting) products at wavelengths relevant to the stratosphere. The development of a molecular beam source of ClOOCl and the photodissociation dynamics of the model system Cl2O are also discussed. In the first chapter, the photochemistry of ClONO2 is examined at 308 nm using the technique of photofragment translational spectroscopy. Two primary decomposition pathways, leading to Cl + NO3 and ClO + NO2, were observed, with a lower limit of 0.33 for the relative yield of ClO. The angular distributions for both channels were anisotropic, indicating that the dissociation occurs within a rotational period. Chapter two revisits the photodissociation dynamics of Cl2O at 248 and 308 nm, on which we had previously reported preliminary findings. At 248 nm, three distinct dissociation pathways leading to Cl + ClO products were resolved. At 308 nm, the angular distribution was slightly more isotropic that previously reported, leaving open the possibility that Cl2O excited at 308 nm lives longer than a rotational period. Chapter three describes the development and optimization of a molecular beam source of ClOOCl. We utilized pulsed laser photolysis of ClA2O to generate ClO radicals, and cooled the cell to promote three body recombination to form ClOOCl. The principal components in the beam were Cl2, Cl2O, and ClOOCl. In the fourth chapter, the photodissociation dynamics of ClOOCl are investigated at 248 and 308 nm. We observed multiple dissociation pathways which produced ClO + ClO and 2Cl + O2 products. The relative Cl:ClO product yields are 1.0:0.13 and 1.0:0.20 for ClOOCl photolysis at 248 and 308 nm, respectively. The upper limit for the relative yield of the ClO + ClO channel was 0.19 at 248 nm and 0.31 at 308 nm. These results substantially confirm the current assumption but decrease somewhat the efficiency of the ClOOCl ozone-depleting catalytic cycle. At 248 nm, ClOOCl photolysis exhibited novel dissociation dynamics which appeared to depend on the symmetry of the excited state.

Development of atmospheric N2O isotopomers model based on a chemistry-coupled atmospheric general circulation model

NASA Astrophysics Data System (ADS)

Ishijima, K.; Toyoda, S.; Sudo, K.; Yoshikawa, C.; Nanbu, S.; Aoki, S.; Nakazawa, T.; Yoshida, N.

2009-12-01

It is well known that isotopic information is useful to qualitatively understand cycles and constrain sources of some atmospheric species, but so far there has been no study to model N2O isotopomers throughout the atmosphere from the troposphere to the stratosphere, including realistic surface N2O isotopomers emissions. We have started to develop a model to simulate spatiotemporal variations of the atmospheric N2O isotopomers in both the troposphere and the stratosphere, based on a chemistry-coupled atmospheric general circulation model, in order to obtain more accurate quantitative understanding of the global N2O cycle. For surface emissions of the isotopomers, combination of EDGAR-based anthropogenic and soil fluxes and monthly varying GEIA oceanic fluxes are factored, using isotopic values of global total sources estimated from firn-air analyses based long-term trend of the atmospheric N2O isotopomers. Isotopic fractionations in chemical reactions are considered for photolysis and photo-oxidation of N2O in the stratosphere. The isotopic fractionation coefficients have been employed from studies based on laboratory experiments, but we also will test the coefficients determined by theoretical calculations. In terms of the global N2O isotopomer budgets, precise quantification of the sources is quite challenging, because even the spatiotemporal variabilities of N2O sources have never been adequately estimated. Therefore, we have firstly started validation of simulated isotopomer results in the stratosphere, by using the isotopomer profiles obtained by balloon observations. N2O concentration profiles are mostly well reproduced, partly because of realistic reproduction of dynamical processes by nudging with reanalysis meteorological data. However, the concentration in the polar vortex tends to be overestimated, probably due to relatively coarse wave-length resolution in photolysis calculation. Such model features also appear in the isotopomers results, which are almost underestimated, relative to the balloon observations, although the concentration is well simulated. The tendency has been somewhat improved by incorporating another photolysis scheme with slightly higher wave-length resolution into the model. From another point of view, these facts indicate that N2O isotopomers can be used for validation of the stratospheric photochemical calculations in model, because of very high sensitivity of the isotopomer ratio values to some settings such as the wave-length resolution in the photochemical scheme.Therefore, N2O isotopomers modeling seems to be not only useful for validation of the fractionation coefficients and of isotopic characterization of sources, but also have the possibility to be an index especially for precision in the stratospheric photolysis in model.

A kinetics investigation of several reactions involving chlorine containing compounds

NASA Technical Reports Server (NTRS)

Davis, D. D.

1978-01-01

The technique of flash photolysis-resonance fluorescence was utilized to study nine reactions of stratospheric importance. The tropospheric degradation reactions of seven halogenated hydrocarbons were studied to assess their possible influx into the stratosphere. There are reactions of either Cl, OH, or O(3P) species with hydrogenated species, O3 or chlorinated compounds. Apart from the kinetic measurements, the quantum yield for the production of O(1D) from O3 in the crucial wavelength region of 293 to 316.5 nm was studied by utilizing a narrow wavelength laser as the photolysis source. The product formation was monitored by measuring the fluorescence of NO2 formed through O(1D) reaction with N2O followed by NO reaction with O3 to give NO2.

Visible and near-ultraviolet spectroscopy at Thule AFB (76.5 N) from January 28 - February 15, 1988

NASA Technical Reports Server (NTRS)

Mount, G. H.; Sanders, R. W.; Jakoubek, R. O.; Schmeltekopf, A. L.; Solomon, S.

1988-01-01

Near-ultraviolet and visible spectrographs identical to those employed at McMurdo Station, Antarctica (77.8 S) during the austral spring seasons of 1986 and 1987 were used to study the stratosphere above Thule, Greenland (76.5 N) during early spring, 1988. Observations were carried out both at night using the direct moon as a light source, and during the day by collecting the scattered light from the zenith sky when solar zenith angles were less than about 94.5 degrees. Excellent meteorological conditions prevailed in the troposphere and stratosphere at Thule. Surface weather was extremely clear over most of the period, facilitating measurements of the direct light from the moon. The lower stratospheric arctic polar vortex was located very near Thule throughout the observing period, and temperature at the 30 mbar level were typically below -80 C above Thule, according to the National Meteorological Center daily analyses. Thus conditions were favorable for polar stratospheric cloud formation above Thule. Total column ozone abundances were about 350 to 400 Dobson units, and did not suggest a clear temporal trend over the observing period. Stratospheric nitrogen dioxide measurements were complicated by the presence of a large component of tropospheric pollution on many occasions. Stratospheric nitrogen dioxide could be identified on most days using the absorption in the scattered light from the zenith sky, which greatly enhances the stratospheric airmass while suppressing the tropospheric contribution. These measurements suggest that the total vertical column abundance of nitrogen dioxide present over Thule in February was extremely low, sometimes as low as 3 x 10 to the 14th per sq cm. The abundance of nitrogen dioxide increased systemically from about 3 x 10 to the 14th in late January to 1.0 x 10 to the 15th per sq cm in mid-February, perhaps because of photolysis of N2O5 in the upper part of the stratosphere, near 25 to 35 km.

Flash photolysis resonance fluorescence investigation of the reaction of O /P-3/ atoms with ClONO2

NASA Technical Reports Server (NTRS)

Kurylo, M. J.

1977-01-01

The rate constant for the reaction of O (P-3) atoms with ClONO2 at 10 torr total pressure is assessed over the temperature range 225-273 K by the flash photolysis resonance fluorescence technique. The data, taken together with results given by Molina et al. (1977), have been used to formulate an Arrhenius expression suitable for stratospheric modeling applications. Comparison of the rate of ClONO2 destruction via the oxygen atom reaction with the solar photolysis rate shows that chemical reaction accounts for less than 15% of the CLONO2 removal at altitudes between 20 and 30 km.

New photolysis system for NO2 measurements in the lower stratosphere

NASA Technical Reports Server (NTRS)

Gao, R. S.; Keim, E. R.; Woodbridge, E. L.; Ciciora, S. J.; Proffitt, M. H.; Thompson, T. L.; Mclaughlin, R. J.; Fahey, D. W.

1994-01-01

A new system for NO2 detection has been developed for use on the NASA ER-2 aircraft. The system converts NO2 to NO using UV photolysis with the NO product subsequently detected with an on-board chemiluminescence detector. The new system is compact, light weight, has high time resolution (approximately 1 s), and is significantly more efficient then some previous designs. Details of the system design and airborne performance are discussed.

Laboratory studies of stratospheric bromine chemistry: Kinetics of the reactions of bromine monoxide with nitrogen dioxide and atomic oxygen

NASA Astrophysics Data System (ADS)

Thorn, Robert Peyton

A laser flash photolysis - long path absorption - technique has been employed to study the kinetics of the reaction BrO+NO2+M(k(sub 16)) yields products as a function of temperature (248-346 K), pressure (16-800 Torr), and buffer gas identity (N2, CF4). 351 nm photolysis of NO2/Br2/N2 mixtures generated BrO. The BrO decay in the presence of excess NO2 was followed by UV absorption at 338.3 nm. The reaction is in the falloff regime between third and second order over the entire range of conditions investigated. This is the first study where temperature dependent measurements of k(sub 16)(P,T) have been reported at pressures greater than 12 Torr; hence, these results help constrain choices of k(sub 16)(P,T) for use in modeling stratospheric BrO(x) chemistry. The kinetics of the important stratospheric reaction BrO+O(P-3)(k(sub 14)) yields Br+O2 in N2 buffer gas have been studied as a function of temperature (233-328 K) and pressure (25-150 Torr) using a novel dual laser flash photolysis/long path absorption/resonance fluorescence technique. 248 nm pulsed laser photolysis of Br2/O3/N2 mixtures produces O atoms in excess over Br2. After a delay sufficient for BrO to be generated, a 532 nm laser pulse photolysis a small fraction of the O3 to generate O(P-3). The decay of O(P-3) in the presence of an excess, known concentration of BrO, as determined by UV absorption at 338.3 nm and by numerical simulation, is then followed by time-resoved atomic resonance fluorescence spectroscopy. The experimental results have shown the reaction kinetics to be independent of pressure, to increase with decreasing temperature, and to be faster than suggested by the only previous (indirect) measurement. The resulting Anhenius expression for k(sub 14)(T) is k(sub 14)(T) = 1.64 x 10(exp -11) exp(263/T) cm(exp 3) molecule(exp-1)s(exp -1). The absolute accuracy of k(sub 14)(T) at any temperature within the range studied is estimated to be +/- 25%. Possible kinetic interferences from production of vibrationally or electronically excited O2 are discussed. The effect of the faster reaction rate coefficients that are reported for the BrO + NO2 + M and BrO + O(P-3) reactions upon bromine partitioning and ozone depletion in the stratosphere is discussed.

Direct observation of ClO from chlorine nitrate photolysis. [as mechanism of polar ozone depletion

NASA Technical Reports Server (NTRS)

Minton, Timothy K.; Nelson, Christine M.; Moore, Teresa A.; Okumura, Mitchio

1992-01-01

Chlorine nitrate photolysis has been investigated with the use of a molecular beam technique. Excitation at both 248 and 193 nanometers led to photodissociation by two pathways, ClONO2 yields ClO + NO2 and ClONO2 yields Cl + NO3, with comparable yields. This experiment provides a direct measurement of the ClO product channel and consequently raises the possibility of an analogous channel in ClO dimer photolysis. Photodissociation of the ClO dimer is a critical step in the catalytic cycle that is presumed to dominate polar stratospheric ozone destruction. A substantial yield of ClO would reduce the efficiency of this cycle.

Detection of stratospheric N2O5 by infrared remote sounding

NASA Technical Reports Server (NTRS)

Toon, G. C.; Farmer, C. B.; Norton, R. H.

1986-01-01

Measurements of N2O5 absorption (1230 and 1260 per cm) in infrared spectra were carried out using the Atmospheric Trace Molecule Spectroscopy (ATMOS) instruments on board Spacelab 3. The detection of stratospheric N2O5, a temporary reservoir species whose photolysis products catalyze ozone destruction, was confirmed. Preliminary analysis of spectra recorded at sunrise on 1 May 1985 indicates a peak volume mixing ratio of 1.6 x 10 the -9th at 35 km an altitude of 35 km, or a broad concentration peak pf 4 x 10 to the 8th molecules per cu cm between 21 and 35 km. Absorption was not detected in spectra measured at sunset due to the depletion of N2O5 by photolysis during the day. The volume mixing ratio profile of N2O5 between 0 and 75 km altitude is reproduced in graphic form.

Pressure and temperature dependence kinetics study of the NO + BrO yielding NO2 + Br reaction - Implications for stratospheric bromine photochemistry

NASA Technical Reports Server (NTRS)

Watson, R. T.; Sander, S. P.; Yung, Y. L.

1979-01-01

The reactivity of NO with BrO radicals over a wide range of pressure (100-700 torr) and temperature (224-398 K) is investigated using the flash photolysis-ultraviolet absorption technique. The flash photolysis system consists of a high-pressure xenon arc light source, a reaction cell/gas filter/flash lamp combination, and a 216.5 half-meter monochromator/polychromator/spectrography for wavelength selectivity. The details of the reaction and its corresponding Arrhenius expression are identified. The results are compared with previous measurements, and atmospheric implications of the reaction are discussed. The NO + BrO yielding NO2 + Br reaction is shown to be important in controlling the concentration ratios of BrO/Br and BrO/HBr in the stratosphere, but this reaction does not affect the catalytic efficiency of BrOx in ozone destruction.

A flash photolysis resonance fluorescence investigation of the reaction OH + CH3CCl3 yields H2O + CH2CCl3. [in troposphere

NASA Technical Reports Server (NTRS)

Kurylo, M. J.; Anderson, P. C.; Klais, O.

1979-01-01

The absolute rate constant for the reaction OH + CH3CCl3 yields H2O + CH2CCl3 was determined by the flash photolysis resonance fluorescence method from 253 to 363K. The use of the Arrhenius equation with atmospheric observational data on methyl chloroform nearly doubles the predicted tropospheric OH reaction sink strength for the removal of atmospheric gases whose lifetimes are controlled by OH. The increased use of methyl chloroform instead of the restricted trichloroethylene focused attention to its role in stratospheric ozone depletion, producing modeling analyses to determine the amount of released methyl chloroform which reaches the stratosphere. Since the primary atmospheric loss of CH3CCl3 is considered by reaction with OH radicals, these data are used to compute an average tropospheric OH concentration and the strength of the 'global tropospheric OH reaction sink'.

Interactive Photochemistry in Earth System Models to Assess Uncertainty in Ozone and Greenhouse Gases. Final report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Prather, Michael J.; Hsu, Juno; Nicolau, Alex

Atmospheric chemistry controls the abundances and hence climate forcing of important greenhouse gases including N 2O, CH 4, HFCs, CFCs, and O 3. Attributing climate change to human activities requires, at a minimum, accurate models of the chemistry and circulation of the atmosphere that relate emissions to abundances. This DOE-funded research provided realistic, yet computationally optimized and affordable, photochemical modules to the Community Earth System Model (CESM) that augment the CESM capability to explore the uncertainty in future stratospheric-tropospheric ozone, stratospheric circulation, and thus the lifetimes of chemically controlled greenhouse gases from climate simulations. To this end, we have successfullymore » implemented Fast-J (radiation algorithm determining key chemical photolysis rates) and Linoz v3.0 (linearized photochemistry for interactive O 3, N 2O, NO y and CH 4) packages in LLNL-CESM and for the first time demonstrated how change in O2 photolysis rate within its uncertainty range can significantly impact on the stratospheric climate and ozone abundances. From the UCI side, this proposal also helped LLNL develop a CAM-Superfast Chemistry model that was implemented for the IPCC AR5 and contributed chemical-climate simulations to CMIP5.« less

Simulation of Aerosols and Chemistry with a Unified Global Model

NASA Technical Reports Server (NTRS)

Chin, Mian

2004-01-01

This project is to continue the development of the global simulation capabilities of tropospheric and stratospheric chemistry and aerosols in a unified global model. This is a part of our overall investigation of aerosol-chemistry-climate interaction. In the past year, we have enabled the tropospheric chemistry simulations based on the GEOS-CHEM model, and added stratospheric chemical reactions into the GEOS-CHEM such that a globally unified troposphere-stratosphere chemistry and transport can be simulated consistently without any simplifications. The tropospheric chemical mechanism in the GEOS-CHEM includes 80 species and 150 reactions. 24 tracers are transported, including O3, NOx, total nitrogen (NOy), H2O2, CO, and several types of hydrocarbon. The chemical solver used in the GEOS-CHEM model is a highly accurate sparse-matrix vectorized Gear solver (SMVGEAR). The stratospheric chemical mechanism includes an additional approximately 100 reactions and photolysis processes. Because of the large number of total chemical reactions and photolysis processes and very different photochemical regimes involved in the unified simulation, the model demands significant computer resources that are currently not practical. Therefore, several improvements will be taken, such as massive parallelization, code optimization, or selecting a faster solver. We have also continued aerosol simulation (including sulfate, dust, black carbon, organic carbon, and sea-salt) in the global model to cover most of year 2002. These results have been made available to many groups worldwide and accessible from the website http://code916.gsfc.nasa.gov/People/Chin/aot.html.

Continuous Lidar Monitoring of Polar Stratospheric Clouds at the South Pole

NASA Technical Reports Server (NTRS)

Campbell, James R.; Welton, Ellsworth J.; Spinhirne, James D

2009-01-01

Polar stratospheric clouds (PSC) play a primary role in the formation of annual ozone holes over Antarctica during the austral sunrise. Meridional temperature gradients in the lower stratosphere and upper troposphere, caused by strong radiative cooling, induce a broad dynamic vortex centered near the South Pole that decouples and insulates the winter polar airmass. PSC nucleate and grow as vortex temperatures gradually fall below equilibrium saturation and frost points for ambient sulfate, nitrate, and water vapor concentrations (generally below 197 K). Cloud surfaces promote heterogeneous reactions that convert stable chlorine and bromine-based molecules into photochemically active ones. As spring nears, and the sun reappears and rises, photolysis decomposes these partitioned compounds into individual halogen atoms that react with and catalytically destroy thousands of ozone molecules before they are stochastically neutralized. Despite a generic understanding of the ozone hole paradigm, many key components of the system, such as cloud occurrence, phase, and composition; particle growth mechanisms; and denitrification of the lower stratosphere have yet to be fully resolved. Satellite-based observations have dramatically improved the ability to detect PSC and quantify seasonal polar chemical partitioning. However, coverage directly over the Antarctic plateau is limited by polar-orbiting tracks that rarely exceed 80 degrees S. In December 1999, a NASA Micropulse Lidar Network instrument (MPLNET) was first deployed to the NOAA Earth Systems Research Laboratory (ESRL) Atmospheric Research Observatory at the Amundsen-Scott South Pole Station for continuous cloud and aerosol profiling. MPLNET instruments are eye-safe, capable of full-time autonomous operation, and suitably rugged and compact to withstand long-term remote deployment. With only brief interruptions during the winters of 2001 and 2002, a nearly continuous data archive exists to the present.

Laboratory Studies of Stratospheric Bromine Chemistry: Kinetics of the Reactions of Bromine Monoxide with Nitrogen Dioxide and Atomic Oxygen.

NASA Astrophysics Data System (ADS)

Thorn, Robert Peyton, Jr.

A laser flash photolysis - long path absorption technique has been employed to study the kinetics of the reaction rm BrO + NO_2 + M{k _{16}atopto} products as a function of temperature (248-346 K), pressure (16 -800 Torr), and buffer gas identity (rm N _2,CF_4). 351 nm photolysis of rm NO_2/Br_2/N_2 mixtures generated BrO. The BrO decay in the presence of excess NO_2 was followed by UV absorption at 338.3 nm. The reaction is in the falloff regime between third and second order over the entire range of conditions investigated. This is the first study where temperature dependent measurements of k_{16} (P,T) have been reported at pressures greater than 12 Torr; hence, these results help constrain choices of k_{16}(P,T) for use in modeling stratospheric BrO_{rm x} chemistry. The kinetics of the important stratospheric reaction rm BrO+O(^3P)_sp{to }{k_{14}}Br+O_2 in N_2 buffer gas have been studied as a function of temperature (233-328 K) and pressure (25 -150 Torr) using a novel dual laser flash photolysis/long path absorption/resonance fluorescence technique. 248 nm pulsed laser photolysis of rm Br_2/O _3/N_2 mixtures produces O atoms in excess over Br_2. After a delay sufficient for BrO to be generated, a 532 nm laser pulse photolyses a small fraction of the O_3 to generate O(^3P). The decay of O(^3P) in the presence of an excess, known concentration of BrO, as determined by UV absorption at 338.3 nm and by numerical simulation, is then followed by time-resolved atomic resonance fluorescence spectroscopy. The experimental results have shown the reaction kinetics to be independent of pressure, to increase with decreasing temperature, and to be faster than suggested by the only previous (indirect) measurement. The resulting Anhenius expression for k_{14}(T) is given below.rm k_{14 }(T) = 1.64times 10^{-11} exp (263/T) cm^3 molecule ^{-1} s^{-1} The absolute accuracy of k_{14 }(T) at any temperature within the range studied is estimated to be +/-25%. Possible kinetic interferences from production of vibrationally or electronically excited O_2 are discussed. The effect of the faster reaction rate coefficients that are reported for the rm BrO + NO_2 + M and BrO + O(^3P) reactions upon bromine partitioning and ozone depletion in the stratosphere is discussed.

Tests of halogen photochemistry using in situ measurements of ClO and BrO in the lower polar stratosphere

NASA Astrophysics Data System (ADS)

Avallone, Linnea M.; Toohey, Darin W.

2001-05-01

In situ observations of the halogen oxides ClO and BrO made from the NASA ER-2 during the Airborne Arctic Stratospheric Expedition (AASE) I and II missions are used to test current understanding of photochemical parameters. Measurements of ClO obtained during AASE I in the dark perturbed polar vortex are analyzed with respect to temperature to derive the equilibrium expression for the ClO/Cl2O2 system. Assuming photochemical steady state and complete activation of chlorine (ClO + 2Cl2O2 = Cly), observations of ClO made during AASE II are used to derive the photolysis rate of Cl2O2. The photolysis rate derived from atmospheric observations is compared to J values calculated with a photochemical model and various values for the absorption cross section of Cl2O2. The photolysis rate calculated with the cross section of Huder and DeMore [1995] is shown to be systematically too small, while those of Burkholder et al. [1990] and Cox and Hayman [1988] are too large to be consistent with atmospheric observations. Observations of BrO made during AASE II indicate that our understanding of the inorganic bromine budget in the polar regions is incomplete. A possible role for the adduct BrOOCl is investigated.

Reactions of chlorine nitrate with HCl and H2O. [ozone controlling chemistry in stratosphere

NASA Technical Reports Server (NTRS)

Hatakeyama, Shiro; Leu, Ming-Taun

1986-01-01

The kinetics of the reactions of chlorine nitrate with HCl and H2O are characterized using a static photolysis/Fourier transform infrared spectrophotometer apparatus. For the homogeneous gas-phase reaction with HCl, an upper limit for the rate constant of less than 8.4 x 10 to the -21st, and for the reaction with H2O, a limit of less than 3.4 x 10 to the -21st cu cm/molecule per s, were obtained at 296 + or - 2 K. The yield of HNO3 is almost unity in both cases, and no synergistic effect is noted between HCl and H2O. The kinetic behavior of the reaction with H2O is well described by simple first-order kinetics, while the behavior of the reaction with HCl is described in terms of the Langmuir adsorption isotherm.

Electronic state spectroscopy by high-resolution vacuum ultraviolet photoabsorption, He(I) photoelectron spectroscopy and ab initio calculations of ethyl acetate

NASA Astrophysics Data System (ADS)

Śmialek, Malgorzata A.; Łabuda, Marta; Guthmuller, Julien; Hubin-Franskin, Marie-Jeanne; Delwiche, Jacques; Hoffmann, Søren Vrønning; Jones, Nykola C.; Mason, Nigel J.; Limão-Vieira, Paulo

2016-06-01

The high-resolution vacuum ultraviolet photoabsorption spectrum of ethyl acetate, C4H8O2, is presented over the energy range 4.5-10.7 eV (275.5-116.0 nm). Valence and Rydberg transitions and their associated vibronic series observed in the photoabsorption spectrum, have been assigned in accordance with new ab initio calculations of the vertical excitation energies and oscillator strengths. Also, the photoabsorption cross sections have been used to calculate the photolysis lifetime of this ester in the upper stratosphere (20-50 km). Calculations have also been carried out to determine the ionisation energies and fine structure of the lowest ionic state of ethyl acetate and are compared with a newly recorded photoelectron spectrum (from 9.5 to 16.7 eV). Vibrational structure is observed in the first photoelectron band of this molecule for the first time.

Toluene Valence and Rydberg Excitations as Studied by ab initio Calculations and Vacuum Ultraviolet (VUV) Synchrotron Radiation.

PubMed

Serralheiro, C; Duflot, D; da Silva, F Ferreira; Hoffmann, S V; Jones, N C; Mason, N J; Mendes, B; Limão-Vieira, P

2015-08-27

The electronic spectroscopy of isolated toluene in the gas phase has been investigated using high-resolution photoabsorption spectroscopy in the 4.0-10.8 eV energy range, with absolute cross-section measurements derived. We present the first set of ab initio calculations (vertical energies and oscillator strengths), which we use in the assignment of valence and Rydberg transitions of the toluene molecule. The spectrum reveals several new features not previously reported in the literature, with particular relevance to 7.989 and 8.958 eV, which are here tentatively assigned to the π*(17a') ← σ(15a') and 1π*(10a″) ← 1π(14a') transitions, respectively. The measured absolute photoabsorption cross sections have been used to calculate the photolysis lifetime of toluene in the upper stratosphere (20-50 km).

On the turnaround of stratospheric ozone trends deduced from the reevaluated Umkehr record of Arosa, Switzerland

NASA Astrophysics Data System (ADS)

Zanis, P.; Maillard, E.; Staehelin, J.; Zerefos, C.; Kosmidis, E.; Tourpali, K.; Wohltmann, I.

2006-11-01

In this work, we investigate the issue of the turnaround in ozone trends of the recently homogenized Umkehr ozone record of Arosa, Switzerland, which is the longest Umkehr data set, extending from 1956 to date, using different statistical methods. All methods show statistically significant negative ozone trends from 1970 to 1995 in the upper stratosphere (above 32.6 km) throughout the course of the year as well as in the lower stratosphere (below 23.5 km) mainly during winter to spring, which can be partially attributed to dynamical changes. Over the recent period (1996-2004) the year-round trends in the lower stratosphere become positive and are more positive during the winter to spring period. The results also show changes in upper stratospheric ozone trends after 1996, which are, however, not statistically significant at 95% if aerosol correction is applied on the retrieved data. This lack of significant trend changes during the recent period in the upper stratosphere is regionally coherent with recent results derived from upper stratospheric ozone data recorded by lidars, microwave radiometers, and satellite instruments at an adjacent location. Although the positive change in trends after 1996 both for upper and lower stratospheric ozone is in line with the reduction of the emissions of ozone-depleting substances from the successful implementation of the Montreal Protocol and its amendments, we recommend, because of lack of significance for the upper stratospheric trends, repeating this analysis in a few years in order to overcome ambiguous results for documentation of the turnaround of upper stratospheric ozone.

Sensitivity of Polar Stratospheric Ozone Loss to Uncertainties in Chemical Reaction Kinetics

NASA Technical Reports Server (NTRS)

Kawa, S. Randolph; Stolarksi, Richard S.; Douglass, Anne R.; Newman, Paul A.

2008-01-01

Several recent observational and laboratory studies of processes involved in polar stratospheric ozone loss have prompted a reexamination of aspects of our understanding for this key indicator of global change. To a large extent, our confidence in understanding and projecting changes in polar and global ozone is based on our ability to simulate these processes in numerical models of chemistry and transport. The fidelity of the models is assessed in comparison with a wide range of observations. These models depend on laboratory-measured kinetic reaction rates and photolysis cross sections to simulate molecular interactions. A typical stratospheric chemistry mechanism has on the order of 50- 100 species undergoing over a hundred intermolecular reactions and several tens of photolysis reactions. The rates of all of these reactions are subject to uncertainty, some substantial. Given the complexity of the models, however, it is difficult to quantify uncertainties in many aspects of system. In this study we use a simple box-model scenario for Antarctic ozone to estimate the uncertainty in loss attributable to known reaction kinetic uncertainties. Following the method of earlier work, rates and uncertainties from the latest laboratory evaluations are applied in random combinations. We determine the key reactions and rates contributing the largest potential errors and compare the results to observations to evaluate which combinations are consistent with atmospheric data. Implications for our theoretical and practical understanding of polar ozone loss will be assessed.

Photochemistry of Saturn's Atmosphere. 1; Hydrocarbon Chemistry and Comparisons with ISO Observations

NASA Technical Reports Server (NTRS)

Moses, Julianne I.; Bezard, Bruno; Lellouch, Emmanuel; Gladstone, G. Randall; Feuchtgruber, Helmut; Allen, Mark

2000-01-01

To investigate the details of hydrocarbon photochemistry on Saturn, we have developed a one-dimensional diurnally averaged model that couples hydrocarbon and oxygen photochemistry, molecular and eddy diffusion, radiative transfer, and condensation. The model results are compared with observations from the Infrared Space Observatory (ISO) to place tighter constraints on molecular abundances, to better define Saturn's eddy diffusion coefficient profile, and to identify important chemical schemes that control the abundances of the observable hydrocarbons in Saturn's upper atmosphere. From the ISO observations, we determine that the column 12 densities of CH3, CH3C2H, and C4H2 above 10 mbar are 4 (sup +2) (sub -1.5) x 10 (exp 13) cm (sup -2), (1.1 plus or minus 0.3) x 10 (exp 15) cm (exp -2), and (1.2 plus or minus 0.3) x 10 (exp 14) cm (sup -2), respectively. The observed ISO emission features also indicate C2H2 mixing ratios of 1.2 (sup +0.9) (sub -0.6) x 10 (exp -6) at 0.3 mbar and (2.7 plus or minus 0.8) x 10 (exp -7) at 1.4 mbar, and a C2H6 mixing ratio of (9 plus or minus 2.5) x 10 (exp -6) at 0.5 mbar. Upper limits are provided for C2H4, CH2CCH2, C3H8, and C6H2 sensitivity of the model results to variations in the eddy diffusion coefficient profile, the solar flux, the CH4 photolysis branching ratios, the atomic hydrogen influx, and key reaction rates are discussed in detail. We find that C4H2 and CH3C2H are particularly good tracers of important chemical processes and physical conditions in Saturn's upper atmosphere, and C2H6 is a good tracer of the eddy diffusion coefficient in Saturn's lower stratosphere. The eddy diffusion coefficient must be smaller than approximately 3 x 10 (exp 4) sq cm s (sup -1) at pressures greater than 1 mbar in order to reproduce the C2H6 abundance inferred from ISO observations. The eddy diffusion coefficients in the upper stratosphere could be constrained by observations of CH3 radicals if the low-temperature chemistry of CH3 were better understood. We also discuss the implications of our modeling for aerosol formation in Saturn's lower stratosphere-diacetylene, butane, and water condense between approximately 1 and 300 mbar in our model and will dominate stratospheric haze formation at nonauroral latitudes. Our photochemical models will be useful for planning observational sequences and for analyzing data from the upcoming Cassini mission.

Toward a Better Quantitative Understanding of Polar Stratospheric Ozone Loss

NASA Technical Reports Server (NTRS)

Frieler, K.; Rex, M.; Salawitch, R. J.; Canty, T.; Streibel, M.; Stimpfle, R. M.; Pfeilsticker, K.; Dorf, M.; Weisenstein, D. K.; Godin-Beekmann, S.

2006-01-01

Previous studies have shown that observed large O3 loss rates in cold Arctic Januaries cannot be explained with current understanding of the loss processes, recommended reaction kinetics, and standard assumptions about total stratospheric chlorine and bromine. Studies based on data collected during recent field campaigns suggest faster rates of photolysis and thermal decomposition of ClOOCl and higher stratospheric bromine concentrations than previously assumed. We show that a model accounting for these kinetic changes and higher levels of BrO can largely resolve the January Arctic O3 loss problem and closely reproduces observed Arctic O3 loss while being consistent with observed levels of ClO and ClOOCl. The model also suggests that bromine catalyzed O3 loss is more important relative to chlorine catalyzed loss than previously thought.

Pressure-Dependent Yields and Product Branching Ratios in the Broadband Photolysis of Chlorine Nitrate

NASA Technical Reports Server (NTRS)

Nickolaisen, Scott L.; Sander, Stanley P.; Friedl, Randall R.

1996-01-01

The photolysis of chlorine nitrate was studied using broadband flash photolysis coupled with long-path ultraviolet-visible absorption spectroscopy. Branching ratios for the Cl + NO3 and ClO + NO2 product channels were determined from time-dependent measurements of ClO and NO3 concentrations. Yields of the ClO and NO3 products displayed a dependence on the bath gas density and the spectral distribution of the photolysis pulse. Product yields decreased with increasing bath gas density regardless of the spectral distribution of the photolysis pulse; however, the decrease in product yield was much more pronounced when photolysis was limited to longer wavelengths. For photolysis in a quartz cell (lambda > 200 nm) the yield decreased by a factor of 2 over the pressure 10-100 Torr. In a Pyrex cell (lambda > 300 nm), the yield decreased by a factor of 50 over the same pressure range. When photolysis was limited to lambda > 350 nm, the yield decreased by a factor of 250. Branching ratios for the photolysis channels [ClONO2 + h.nu yields ClO + NO2 (1a) and ClONO2 + h.nu yields Cl + NO3 (lb)] were determined from the relative ClO and NO3 product yields at various pressures. Although the absolute product yield displayed a pressure dependence, the branching between the two channels was independent of pressure. The relative branching ratios (assuming negligible contributions from other channels) are 0.61 +/- 0.20 for channel 1a and 0.39 +/- 0.20 for channel lb for photolysis with lambda > 200 nm and 0.44 +/- 0.08 for channel 1a and 0.56 +/- 0.08 for channel 1b for photolysis with lambda > 300 nm. The implications of these results for the chemistry of the lower stratosphere are discussed.

Improved ACE-FTS observations of carbon tetrachloride (CCl4)

NASA Astrophysics Data System (ADS)

Harrison, Jeremy; Chipperfield, Martyn; Boone, Chris; Bernath, Peter

2016-04-01

The Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS), on board the SCISAT satellite, has been recording solar occultation spectra through the Earth's atmosphere since 2004 and continues to take measurements with only minor loss in performance. ACE-FTS time series are available for a range of chlorine 'source' gases, including CCl3F (CFC-11), CCl2F2 (CFC-12), CHF2Cl (HCFC-22), CH3Cl and CCl4. Recently there has been much community interest in carbon tetrachloride (CCl4), a substance regulated by the Montreal Protocol because it leads to the catalytic destruction of stratospheric ozone. Estimated sources and sinks of CCl4 remain inconsistent with observations of its abundance. Satellite observations of CCl4 in the stratosphere are particularly useful in validating stratospheric loss (photolysis) rates; in fact the atmospheric loss of CCl4 is essentially all due to photolysis in the stratosphere. However, the latest ACE-FTS v3.5 CCl4 retrieval is biased high by ˜ 20-30%. A new ACE-FTS retrieval scheme utilising new laboratory spectroscopic measurements of CCl4 and improved microwindow selection has recently been developed. This improves upon the v3.5 retrieval and resolves the issue of the high bias; this new scheme will form the basis for the upcoming v4 processing version of ACE-FTS data. This presentation will outline the improvements made in the retrieval, and a subset of data will be compared with modelled CCl4 distributions from SLIMCAT, a state-of-the-art three-dimensional chemical transport model. The use of ACE-FTS data to evaluate the modelled stratospheric loss rate of CCl4 will also be discussed. The evaluated model, which also includes a treatment of surface soil and ocean sinks, will then be used to quantify current uncertainties in the global budget of CCl4.

A new approach to Ozone Depletion Potential (ODP) estimation

NASA Astrophysics Data System (ADS)

Portmann, R. W.; Daniel, J. S.; Yu, P.

2017-12-01

The Ozone Depletion Potential (ODP) is given by the time integrated global ozone loss of an ozone depleting substance (ODS) relative to a reference ODS (usually CFC-11). The ODP is used by the Montreal Protocol (and subsequent amendments) to inform policy decisions on the production of ODSs. Since the early 1990s, ODPs have usually been estimated using an approximate formulism that utilizes the lifetime and the fractional release factor of the ODS. This has the advantage that it can utilize measured concentrations of the ODSs to estimate their fractional release factors. However, there is a strong correlation between stratospheric lifetimes and fractional release factors of ODSs and that this can introduce uncertainties into ODP calculations when the terms are estimated independently. Instead, we show that the ODP is proportional to the average global ozone loss per equivalent chlorine molecule released in the stratosphere by the ODS loss process (which we call the Γ factor) and, importantly, this ratio varies only over a relatively small range ( 0.3-1.5) for ODPs with stratospheric lifetimes of 20 to more than 1,000 years. The Γ factor varies smoothly with stratospheric lifetime for ODSs with loss processes dominated by photolysis and is larger for long-lived species, while stratospheric OH loss processes produce relatively small Γs that are nearly independent of stratospheric lifetime. The fractional release approach does not accurately capture these relationships. We propose a new formulation that takes advantage of this smooth variation by parameterizing the Γ factor using ozone changes computed using the chemical climate model CESM-WACCM and the NOCAR two-dimensional model. We show that while the absolute Γ's vary between WACCM and NOCAR models, much of the difference is removed for the Γ/ΓCFC-11 ratio that is used in the ODP formula. This parameterized method simplifies the computation of ODPs while providing enhanced accuracy compared to the fractional release method and it can be used to estimate many ODPs given information on chemical reaction rates and photolysis processes.

The Response of ClO Radical Concentrations to Variations in NO2 Radical Concentrations in the Lower Stratosphere

NASA Technical Reports Server (NTRS)

Stimpfle, R. M.; Koplow, J. P.; Cohen, R. C.; Kohn, D. W.; Wennberg, P. O.; Judah, D. M.; Toohey, D. W.; Avallone, L. M.; Anderson, J. G.; Salawitch, R. J.

1994-01-01

The response of ClO concentrations to changes in NO2 concentrations has been inferred from simultaneous observations of [ClO], [NO], [NO2] and [O3] in the mid-latitude lower stratosphere. This analysis demonstrates that [ClO] is inversely correlated with [NO2], consistent with formation and photolysis of [ClONO2]. A factor of ten range in the concentration of NO2 was sampled (0.1 to 1 x 10(exp 9) mol/cc), with a comparable range in the ratio of [ClO] to total available inorganic chlorine (1% <= [ClO]/[Cl(sub y)] <= 5%). This analysis leads to an estimate of [ClONO2]/[Cl(sub y)] = 0.12 (x/divided by 2), in the mid-latitude, lower-stratospheric air masses sampled.

Dynamic-Chemical Coupling of the Upper Troposphere and Lower Stratosphere Region

NASA Technical Reports Server (NTRS)

Grewe, Volker; Shindell, Drew T.; Reithmeier, Christian

2000-01-01

The importance of the interaction of chemistry and dynamics in the upper troposphere and lower stratosphere for chemical species like ozone is investigated using two chemistry-climate models. Species emitted in the upper troposphere, like NOx (=NO+NO2) by lightning or aircraft, have the chance to be transported into the lowermost stratosphere. Trajectory calculations suggest that the main transport pathway runs via the Inter Tropical Convergence Zone, across the tropical tropopause and then to higher latitudes, i.e. into the lowermost stratosphere. Longer lifetimes of NOx in the lower stratosphere yield an accumulation of NO. there, which feeds back on upper troposphere chemistry. This effect has been estimated for lightning NO. emissions and reveals a contribution of at least 25% to 40% to the total northern hemisphere mid-latitude lightning increase of either NOx and ozone.

Valence and ionic lowest-lying electronic states of ethyl formate as studied by high-resolution vacuum ultraviolet photoabsorption, He(I) photoelectron spectroscopy, and ab initio calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Śmiałek, M. A., E-mail: smialek@pg.gda.pl; Łabuda, M.; Guthmuller, J.

2014-09-14

The highest resolution vacuum ultraviolet photoabsorption spectrum of ethyl formate, C{sub 2}H{sub 5}OCHO, yet reported is presented over the wavelength range 115.0–275.5 nm (10.75–4.5 eV) revealing several new spectral features. Valence and Rydberg transitions and their associated vibronic series, observed in the photoabsorption spectrum, have been assigned in accordance with new ab initio calculations of the vertical excitation energies and oscillator strengths. Calculations have also been carried out to determine the ionization energies and fine structure of the lowest ionic state of ethyl formate and are compared with a newly recorded He(I) photoelectron spectrum (from 10.1 to 16.1 eV). Newmore » vibrational structure is observed in the first photoelectron band. The photoabsorption cross sections have been used to calculate the photolysis lifetime of ethyl formate in the upper stratosphere (20–50 km)« less

NF3: UV Absorption Spectrum Temperature Dependence and the Atmospheric and Climate Forcing Implications

NASA Technical Reports Server (NTRS)

Papadimitriou, Vassileios C.; McGillen, Max R.; Fleming, Eric L.; Jackman, Charles H.; Burkholder, James B.

2013-01-01

Nitrogen trifluoride (NF3) is an atmospherically persistent greenhouse gas that is primarily removed by UV photolysis and reaction with O((sup 1)D) atoms. In this work, the NF3 gas-phase UV absorption spectrum, sigma(delta,T), was measured at 16 wavelengths between 184.95 and 250 nm at temperatures between 212 and 296 K. A significant spectrum temperature dependence was observed in the wavelength region most relevant to atmospheric photolysis (200-220 nm) with a decrease in sigma(210 nm,T) of approximately 45 percent between 296 and 212 K. Atmospheric photolysis rates and global annually averaged lifetimes of NF3 were calculated using the Goddard Space Flight Center 2-D model and the sigma(delta,T) parameterization developed in this work. Including the UV absorption spectrum temperature dependence increased the stratospheric photolysis lifetime from 610 to 762 years and the total global lifetime from 484 to 585 years; the NF3 global warming potentials on the 20-, 100-, and 500-year time horizons increased less than 0.3, 1.1, and 6.5 percent to 13,300, 17,700, and 19,700, respectively.

Laser Flash Photolysis Studies of Radical-Radical Reaction Kinetics: The O((sup 3)P(sub J)) + BrO Reaction

NASA Technical Reports Server (NTRS)

Thorn, R. P.; Cronkhite, J. M.; Nicovich, J. M.; Wine, P. H.

1997-01-01

A novel dual laser flash photolysis-long path absorption-resonance fluorescence technique has been employed to study the kinetics of the important stratospheric reaction 0((sup 3)P(sub j)) + Br yields(k1) BrO((sup 2)P(sub J)) + O2 as a function of temperature (231-328 K) and pressure (25-150 Torr) in N2 buffer gas. The experimental approach preserves the principal advantages of the flash photolysis method, i.e., complete absence of surface reactions and a wide range of accessible pressures, but also employs techniques which are characteristic of the discharge flow method, namely chemical titration as a means for deducing the absolute concentration of a radical reactant and use of multiple detection axes. We find that k1 is independent of pressure, and that the temperature dependence of k1 is adequately described by the Arrhenius expression k1(T) = 1.91 x 10(exp -11)(230/J) cu cm/ molecule.s; the absolute accuracy of measured values for k1 is estimated to vary from +/- 20 percent at at T approximately 230 K to +/- 30 percent at T approximately 330 K. Our results demonstrate that the O((sup 3)P(sub j)) + BrO rate coefficient is significantly faster than previously 'guesstimated,' and suggest that the catalytic cycle with the O((sup 3)P(sub j)) + BrO reaction as its rate-limiting step is the dominant stratospheric BrO(x), odd-oxygen destruction cycle at altitudes above 24 km.

The Remarkable 2003--2004 Winter and Other Recent Warm Winters in the Arctic Stratosphere Since the Late 1990s

NASA Technical Reports Server (NTRS)

Manney, Gloria L.; Kruger, Kirstin; Sabutis, Joseph L.; Sena, Sara Amina; Pawson, Steven

2005-01-01

The 2003-2004 Arctic winter was remarkable in the approximately 50-year record of meteorological analyses. A major warming beginning in early January 2004 led to nearly 2 months of vortex disruption with high-latitude easterlies in the middle to lower stratosphere. The upper stratospheric vortex broke up in late December, but began to recover by early January, and in February and March was the strongest since regular observations began in 1979. The lower stratospheric vortex broke up in late January. Comparison with 2 previous years, 1984-1985 and 1986-1987, with prolonged midwinter warming periods shows unique characteristics of the 2003-2004 warming period: The length of the vortex disruption, the strong and rapid recovery in the upper stratosphere, and the slow progression of the warming from upper to lower stratosphere. January 2004 zonal mean winds in the middle and lower stratosphere were over 2 standard deviations below average. Examination of past variability shows that the recent frequency of major stratospheric warmings (7 in the past 6 years) is unprecedented. Lower stratospheric temperatures were unusually high during 6 of the past 7 years, with 5 having much lower than usual potential for polar stratospheric cloud (PSC) formation and ozone loss (nearly none in 1998-1999, 2001-2002, and 2003-2004, and very little in 1997-1998 and 2000-2001). Middle and upper stratospheric temperatures, however, were unusually low during and after February. The pattern of 5 of the last 7 years with very low PSC potential would be expected to occur randomly once every 850 years. This cluster of warm winters, immediately following a period of unusually cold winters, may have important implications for possible changes in interannual variability and for determination and attribution of trends in stratospheric temperatures and ozone.

The response of C1O radical concentrations to variations in NO2 radical concentrations in the lower stratosphere

NASA Technical Reports Server (NTRS)

Stimfle, R. M.; Koplow, J. P.; Cohen, R. C.; Kohn, D. W.; Wennberg, P. O.; Judah, D. M.; Toohey, D. W.; Avallone, L. M.; Anderson, J. G.; Salawitch, R. J.

1994-01-01

The respose of ClO concentrations to changes in NO2 concentrations has been inferred from simultaneous observations of (ClO), (NO), (NO2) and (O3) in the midlatitude lower stratosphere. This analysis demonstrates that (ClO) is inversely correlated with (NO2), consistent with formation and photolysis of (ClONO2). A factor of ten range in the concentration if NO2 was sampled (0.1 to 1 x 10(exp 9) mol/cu cm), with a comparable range in the ratio of (ClO) to total available inorganic chlorine (1% less than or equal to (ClO)/(Cl(sub y)) less than or equal to 5%. This analysis leads to an estimate of (ClONO2)/(Cl(sub y)) = 0.12 (x/2), in the mid-latitude, lower-stratospheric air masses sampled.

Observed and Modeled HOCl Profiles in the Midlatitude Stratosphere: Implication for Ozone Loss

NASA Technical Reports Server (NTRS)

Kovalenko, L. J.; Jucks, K. W.; Salawitch, R. J.; Toon, G. C.; Blavier, J. F.; Johnson, D. G.; Kleinbohl, A.; Livesey, N. J .; Margitan, J. J.; Pickett, H. M.;

Lower-Stratospheric Control of the Frequency of Sudden Stratospheric Warming Events

NASA Astrophysics Data System (ADS)

Martineau, Patrick; Chen, Gang; Son, Seok-Woo; Kim, Joowan

2018-03-01

The sensitivity of stratospheric polar vortex variability to the basic-state stratospheric temperature profile is investigated by performing a parameter sweep experiment with a dry dynamical core general circulation model where the equilibrium temperature profiles in the polar lower and upper stratosphere are systematically varied. It is found that stratospheric variability is more sensitive to the temperature distribution in the lower stratosphere than in the upper stratosphere. In particular, a cold lower stratosphere favors a strong time-mean polar vortex with a large daily variability, promoting frequent sudden stratospheric warming events in the model runs forced with both wavenumber-1 and wavenumber-2 topographies. This sensitivity is explained by the control exerted by the lower-stratospheric basic state onto fluxes of planetary-scale wave activity from the troposphere to the stratosphere, confirming that the lower stratosphere can act like a valve for the upward propagation of wave activity. It is further shown that with optimal model parameters, stratospheric polar vortex climatology and variability mimicking Southern and Northern Hemisphere conditions are obtained with both wavenumber-1 and wavenumber-2 topographies.

The Remarkable 2003-2004 Winter and Other Recent Warm Winters in the Arctic Stratosphere Since the Late 1990s

NASA Technical Reports Server (NTRS)

Manney, Gloria L.; Krueger, Kirstin; Sabutis, Joseph L.; Sena, Sara Amina; Pawson, Steven

2004-01-01

The 2003-2004 Arctic winter was remarkable in the 40-year record of meteorological analyses. A major warming beginning in early January 2004 led to nearly two months of vortex disruption with high-latitude easterlies in the middle to lower stratosphere. The upper stratospheric vortex broke up in late December, but began to recover by early January, and in February and March was the strongest since regular observations began in 1979. The lower stratospheric vortex broke up in late January. Comparison with two previous years, 1984-1985 and 1986-1987, with prolonged mid-winter warming periods shows unique characteristics of the 2003-2004 warming period: The length of the vortex disruption, the strong and rapid recovery in the upper stratosphere, and the slow progression of the warming from upper to lower stratosphere. January 2004 zonal mean winds in the middle and lower stratosphere were over two standard deviations below average. Examination of past variability shows that the recent frequency of major stratospheric warmings (seven in the past six years) is unprecedented. Lower stratospheric temperatures were unusually high during six of the past seven years, with five having much lower than usual potential for PSC formation and ozone loss (nearly none in 1998-1999, 2001-2002 and 2003-2004, and very little in 1997-1998 and 2000-2001). Middle and upper stratospheric temperatures, however, were unusually low during and after February. The pattern of five of the last seven years with very low PSC potential would be expected to occur randomly once every approximately 850 years. This cluster of warm winters, immediately following a period of unusually cold winters, may have important implications for possible changes in interannual variability and for determination and attribution of trends in stratospheric temperatures and ozone.

Long-term trends in stratospheric ozone, temperature, and water vapor over the Indian region

NASA Astrophysics Data System (ADS)

Thankamani Akhil Raj, Sivan; Venkat Ratnam, Madineni; Narayana Rao, Daggumati; Venkata Krishna Murthy, Boddam

2018-01-01

We have investigated the long-term trends in and variabilities of stratospheric ozone, water vapor and temperature over the Indian monsoon region using the long-term data constructed from multi-satellite (Upper Atmosphere Research Satellite (UARS MLS and HALOE, 1993-2005), Aura Microwave Limb Sounder (MLS, 2004-2015), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER, 2002-2015) on board TIMED (Thermosphere Ionosphere Mesosphere Energetics Dynamics)) observations covering the period 1993-2015. We have selected two locations, namely, Trivandrum (8.4° N, 76.9° E) and New Delhi (28° N, 77° E), covering northern and southern parts of the Indian region. We also used observations from another station, Gadanki (13.5° N, 79.2° E), for comparison. A decreasing trend in ozone associated with NOx chemistry in the tropical middle stratosphere is found, and the trend turned to positive in the upper stratosphere. Temperature shows a cooling trend in the stratosphere, with a maximum around 37 km over Trivandrum (-1.71 ± 0.49 K decade-1) and New Delhi (-1.15 ± 0.55 K decade-1). The observed cooling trend in the stratosphere over Trivandrum and New Delhi is consistent with Gadanki lidar observations during 1998-2011. The water vapor shows a decreasing trend in the lower stratosphere and an increasing trend in the middle and upper stratosphere. A good correlation between N2O and O3 is found in the middle stratosphere (˜ 10 hPa) and poor correlation in the lower stratosphere. There is not much regional difference in the water vapor and temperature trends. However, upper stratospheric ozone trends over Trivandrum and New Delhi are different. The trend analysis carried out by varying the initial year has shown significant changes in the estimated trend.

Nitrogen and Oxygen Photochemistry following SL9

NASA Technical Reports Server (NTRS)

Moses, Julianne I.; Allen, Mark; Gladstone, G. Randall

1995-01-01

The collision of Shoemaker Levy 9 (SL9) with Jupiter caused many new molecular species to be deposited in the Jovian stratosphere. We use a photochemical model to follow the evolution of the impact derived species. Our results regarding the nitrogen and oxygen compounds are presented here. NH3 photolysis initiates the nitrogen photochemistry. Much of the nitrogen ends up in N2, nitrogen-sulfur compounds, and HCN, but NH3 and nitriles such as C2H3CN may also exist in observable quantities for a year or so after the impacts. Oxygen species survive for a long time in the Jovian stratosphere. The only major oxygen containing compounds that exhibit dramatic changes in the lower stratosphere in the first year following the impacts are SO, SO2, and OCS - H2O, CO2, and CO are comparatively stable. We discuss the important photochemical processes operating on the nitrogen and oxygen species in the Jovian stratosphere, make prediction concerning the temporal variation of the major species, and identify molecules that might act as good tracers for atmospheric dynamics.

Analysis of Present Day and Future OH and Methane Lifetime in the ACCMIP Simulations

NASA Technical Reports Server (NTRS)

Voulgarakis, A.; Naik, V.; Lamarque, J. -F.; Shindell, D. T.; Young, P. J.; Prather, M. J.; Wild, O.; Field, R. D.; Bergmann, D.; Cameron-Smith P.;

The role of meteoric smoke in the Earth s environment

NASA Astrophysics Data System (ADS)

Plane, J.

An average of about 120 tonnes of interplanetary dust is believed to enter the earth's atmosphere each day. At least 55% of this ablates completely into atoms and ions, mostly between 70 and 110 km. Meteoric ablation is the source of the layers of metal atoms (Na, Fe etc.) that occur globally in the upper mesosphere; these layers are observed routinely by ground-based resonance lidars. This paper is concerned with the subsequent fate of the meteoric metals, and other constituents such as sulfur. The laboratory programme at the University of East Anglia studies the reactions that metallic species are likely to undergo in this region of the atmosphere. The resulting rate coefficients and photolysis cross sections are then used in atmospheric models. Once these models can satisfactorily reproduce the characteristic features of the mesospheric metal layers (as is the case for Na and Fe), they can then be used to predict the condensation of metal-containing species (oxides, hydroxides, carbonates) into nanometer-sized dust particles, known as "meteoric smoke". This paper will discuss the role of this smoke in providing condensation nuclei for noctilucent clouds in the upper mesosphere, forming sulphuric acid particles in the stratospheric Junge layer, and fertilizing the Fe-deficient Southern Ocean.

A method for establishing a long duration, stratospheric platform for astronomical research

NASA Astrophysics Data System (ADS)

Fesen, Robert; Brown, Yorke

2015-10-01

During certain times of the year at middle and low latitudes, winds in the upper stratosphere move in nearly the opposite direction than the wind in the lower stratosphere. Here we present a method for maintaining a high-altitude balloon platform in near station-keeping mode that utilizes this stratospheric wind shear. The proposed method places a balloon-borne science platform high in the stratosphere connected by a lightweight, high-strength tether to a tug vehicle located in the lower or middle stratosphere. Using aerodynamic control surfaces, wind-induced aerodynamic forces on the tug can be manipulated to counter the wind drag acting on the higher altitude science vehicle, thus controlling the upper vehicle's geographic location. We describe the general framework of this station-keeping method, some important properties required for the upper stratospheric science payload and lower tug platforms, and compare this station-keeping approach with the capabilities of a high altitude airship and conventional tethered aerostat approaches. We conclude by discussing the advantages of such a platform for a variety of missions with emphasis on astrophysical research.

Annual variations of water vapor in the stratosphere and upper troposphere observed by the Stratospheric Aerosol and Gas Experiment II

NASA Technical Reports Server (NTRS)

Mccormick, M. P.; Chiou, E. W.; Mcmaster, L. R.; Chu, W. P.; Larsen, J. C.; Rind, D.; Oltmans, S.

1993-01-01

Data collected by the Stratospheric Aerosol and Gas Experiment II are presented, showing annual variations of water vapor in the stratosphere and the upper troposphere. The altitude-time cross sections of water vapor were found to exhibit annually repeatable patterns in both hemispheres, with a yearly minimum in water vapor appearing in both hemispheres at about the same time, supporting the concept of a common source for stratospheric dry air. A linear regression analysis was applied to the three-year data set to elucidate global values and variations of water vapor ratio.

Lidar investigations of ozone in the upper troposphere - lower stratosphere: technique and results of measurements

NASA Astrophysics Data System (ADS)

Romanovskii, Oleg A.; Nevzorov, Alexey A.; Nevzorov, Alexey V.; Kharchenko, Olga V.

2018-04-01

The main aim of the research is to develop the technique for laser remote ozone sensing in the upper troposphere - lower stratosphere by differential absorption method for temperature and aerosol correction and analysis of measurement results. The authors have determined wavelengths, promising to measure ozone profiles in the upper troposphere - lower stratosphere. We present the results of DIAL measurements of the vertical ozone distribution at the Siberian lidar station in Tomsk. The recovered ozone profiles were compared with IASI satellite data and Kruger model.

Atmospheric Removal of Very Long-lived Greenhouse Gases in the Mesosphere

NASA Astrophysics Data System (ADS)

Totterdill, A.; Kovacs, T.; Gomez Martin, J.; FENG, W.; Chipperfield, M.; Plane, J. M.

2013-12-01

Chlorofluorocarbons are known to have serious ozone depleting and global warming potentials. Perfluorinated compounds such as SF6, NF3, SF5CF3 and CF3CF2Cl which have very long lifetimes (ranging from a few centuries to over 3000 years) are too stable to affect stratospheric ozone but do have among the highest per molecule radiative forcing of any greenhouse pollutant, making them extremely potent greenhouse gases. Due to the stability of these gases in the lower atmosphere, mesospheric loss processes could significantly reduce their estimated atmospheric lifetimes and hence, overall climate impact. Potential sinks include reactions with metals and energetic particles such as electrons or short wavelength photons already present in the upper atmosphere. The metals, in this instance iron, sodium or potassium, are produced by meteoric ablation, while background and energetic electrons have the continuous source of photoionization and auroral precipitation, respectively. In this study we investigate the removal potentials of four very long lived gases (SF6, NF3, SF5CF3 and CF3CF2Cl). First, by four metals (Fe, Mg, Na and K), where rate coefficients are measured using the Fast Flow Tube and Pulsed Laser Flash Photolysis / Laser Induced Fluorescence techniques. Second, removal by electron attachment was investigated using a quadrupole mass spectrometer. measurements. Third, Lyman-alpha (121.56 nm) photolysis was measured in a VUV absorption cell. The resulting removal rate coefficients are currently being input into the Whole Atmosphere Community Climate Model (WACCM) to obtain lifetime measurements for these species.

Observations of a stratospheric depletion and annual mean interhemispheric gradient in the atmospheric Ar/N2 ratio from the HIPPO Global campaign

NASA Astrophysics Data System (ADS)

Bent, J. D.; Keeling, R. F.; Stephens, B. B.; Wofsy, S. C.; Daube, B. C.; Kort, E. A.; Pittman, J. V.; Jimenez-Pizarro, R.; Santoni, G.

2014-12-01

The atmospheric Ar/N2 ratio varies on a seasonal basis due to temperature-dependent solubility changes in the surface ocean. Low signal:noise ratios, limited vertical coverage, and sampler-sampler offsets have historically hampered characterization of vertical and inter-hemispheric gradients. We present data from the HIPPO Global campaign (2009-11) showing that Ar/N2 and interannually-detrended N2O correlate well in the lower stratosphere, suggesting that, as stratospheric air ages and loses N2O to photolysis and photo-oxidation, it also gradually loses argon to gravity as the heavier atom preferentially "rains out" of the air parcel. The HIPPO Ar/N2 data from the lower troposphere also resolve seasonal cycles in each hemisphere, as well as a gradient in the annual mean between hemispheres, with higher values in the southern hemisphere. The HIPPO cycles and inter-hemispheric gradient are in good agreement with data from surface stations.

Signals of El Niño Modoki in the tropical tropopause layer and stratosphere

NASA Astrophysics Data System (ADS)

Xie, F.; Li, J.; Tian, W.; Feng, J.

2012-02-01

The effects of El Niño Modoki events on the tropical tropopause layer (TTL) and on the stratosphere were investigated using European Center for Medium Range Weather Forecasting (ECMWF) reanalysis data, satellite observations from the Aura satellite Microwave Limb Sounder (MLS), oceanic El Niño indices, and general climate model outputs. El Niño Modoki events tend to depress convective activities in the western and eastern Pacific but enhance convective activities in the central and northern Pacific. Consequently, during Modoki events, negative water vapor anomalies occur in the western and eastern Pacific upper troposphere, whereas there are positive anomalies in the central and northern Pacific upper troposphere. The spatial patterns of the outgoing longwave radiation (OLR) and upper tropospheric water vapor anomalies exhibit a tripolar form. The empirical orthogonal function (EOF) analysis of the OLR and upper tropospheric water vapor anomalies reveals that canonical El Niño events are associated with the leading mode of the EOF, while El Niño Modoki events correspond to the second mode. El Niño Modoki activities tend to moisten the lower and middle stratosphere, but dry the upper stratosphere. It was also found that the canonical El Niño signal can overlay linearly on the QBO signal in the stratosphere, whereas the interaction between the El Niño Modoki and QBO signals is non-linear. Because of these non-linear interactions, El Niño Modoki events have a reverse effect on high latitudes stratosphere, as compared with the effects of typical Modoki events, i.e. the northern polar vortex is stronger and colder but the southern polar vortex is weaker and warmer during El Niño Modoki events. However, simulations suggest that canonical El Niño and El Niño Modoki activities actually have the same influence on high latitudes stratosphere, in the absence of interactions between QBO and ENSO signals. The present results also reveal that canonical El Niño events have a greater impact on the high-latitude Northern Hemisphere stratosphere than on the high-latitude Southern Hemisphere stratosphere. However, El Niño Modoki events can more profoundly influence the high-latitude Southern Hemisphere stratosphere than the high-latitude Northern Hemisphere stratosphere.

Chemical Composition and Dynamics of the Upper Troposphere and the Lower Stratosphere: Overview of the Project

NASA Astrophysics Data System (ADS)

Sofieva, V. F.; Liu, C.; Huang, F.; Kyrola, E.; Liu, Y.; Ialongo, I.; Hakkarainen, J.; Zhang, Y.

2016-08-01

The DRAGON-3 cooperation study on the upper troposphere and the lower stratosphere (UTLS) is based on new satellite data and modern atmospheric models. The objectives of the project are: (i) assessment of satellite data on chemical composition in UTLS, (ii) dynamical and chemical structures of the UTLS and its variability, (iii) multi-scale variability of stratospheric ozone, (iv) climatology of the stratospheric aerosol layer and its variability, and (v) updated ozone climatology and its relation to tropopause/multiple tropopauses.In this paper, we present the main results of the project.

The Distribution of Hydrogen, Nitrogen, and Chlorine Radicals in the Lower Stratosphere: Implications for Changes in O3 due to Emission of NO(y) from Supersonic Aircraft

NASA Technical Reports Server (NTRS)

Salawitch, R. J.; Wofsy, S. C.; Wennberg, P. O.; Cohen, R. C.; Anderson, J. G.; Fahey, D. W.; Gao, R. S.; Keim, E. R.; Woodbridge, E. L.; Stimpfle, R. M.;

Stratospheric Response to Intraseasonal Changes in Incoming Solar Radiation

NASA Astrophysics Data System (ADS)

Garfinkel, Chaim; silverman, vered; harnik, nili; Erlich, caryn

2016-04-01

Superposed epoch analysis of meteorological reanalysis data is used to demonstrate a significant connection between intraseasonal solar variability and temperatures in the stratosphere. Decreasing solar flux leads to a cooling of the tropical upper stratosphere above 7hPa, while increasing solar flux leads to a warming of the tropical upper stratosphere above 7hPa, after a lag of approximately six to ten days. Late winter (February-March) Arctic stratospheric temperatures also change in response to changing incoming solar flux in a manner consistent with that seen on the 11 year timescale: ten to thirty days after the start of decreasing solar flux, the polar cap warms during the easterly phase of the Quasi-Biennal Oscillation. In contrast, cooling is present after decreasing solar flux during the westerly phase of the Quasi-Biennal Oscillation (though it is less robust than the warming during the easterly phase). The estimated composite mean changes in Northern Hemisphere upper stratospheric (~ 5hPa) polar temperatures exceed 8K, and are potentially a source of intraseasonal predictability for the surface. These changes in polar temperature are consistent with the changes in wave driving entering the stratosphere. Garfinkel, C.I., V. Silverman, N. Harnik, C. Erlich, Y. Riz (2015), Stratospheric Response to Intraseasonal Changes in Incoming Solar Radiation, J. Geophys. Res. Atmos., 120, 7648-7660. doi: 10.1002/2015JD023244.

Space Shuttle ice nuclei

NASA Astrophysics Data System (ADS)

Turco, R. P.; Toon, O. B.; Whitten, R. C.; Cicerone, R. J.

1982-08-01

Estimates are made showing that, as a consequence of rocket activity in the earth's upper atmosphere in the Shuttle era, average ice nuclei concentrations in the upper atmosphere could increase by a factor of two, and that an aluminum dust layer weighing up to 1000 tons might eventually form in the lower atmosphere. The concentrations of Space Shuttle ice nuclei (SSIN) in the upper troposphere and lower stratosphere were estimated by taking into account the composition of the particles, the extent of surface poisoning, and the size of the particles. Calculated stratospheric size distributions at 20 km with Space Shuttle particulate injection, calculated SSIN concentrations at 10 and 20 km altitude corresponding to different water vapor/ice supersaturations, and predicted SSIN concentrations in the lower stratosphere and upper troposphere are shown.

Long-term temperature observations from the troposphere to upper mesosphere over Mauna Loa, HI (19.5N, 155.6W) and Table Mountain, CA (34.4N, 117.7W) by JPL Lidars and nearby Radiosondes

NASA Astrophysics Data System (ADS)

Li, T.; Leblanc, T.; McDermid, S.; Wu, D. L.

2007-12-01

The JPL Rayleigh lidars at Mauna Loa Observatory (MLO), HI (19.5N, 155.6W) and Table Mountain Observatory (TMO), CA (34.4N, 117.7W) have been operated for the regular nighttime data acquisition of temperature since 1994 and 1989 respectively. Using the monthly mean temperature vertical profiles observed by the JPL lidars (35- 85km) and nearby radiosondes (5-30km), and with the linear regression analysis, we are able to extract the temperature trend, solar cycle, El Nino South Oscillation (ENSO), and Quasi-Biennial Oscillation (QBO) signals from the troposphere to upper mesosphere over MLO and TMO. The temperature trends show different behaviors at two sites, minor trend at MLO, but more negative trend at TMO. The solar cycle responses in temperature are generally positive above the middle stratosphere at both sites, but negative response at MLO and positive at TMO below. During the El Nino events, the warmer temperatures in the troposphere and upper mesosphere, and the colder temperatures in the stratosphere and lower mesosphere were observed at MLO and almost visa verse at TMO. The significant QBO oscillations were observed in the stratosphere with amplitudes of ~2-3K and with clearer downward phase progression at MLO than that at TMO. The mesospheric QBO near 75-85km is clearly present at both sites with amplitude of ~2K and with longer vertical wavelength than that in stratosphere. In addition, we calculated the GW variances using lidar temperature profiles with 30min and 1km resolutions in the upper stratosphere (38-50km) and lower mesosphere (50-62km), and nearby radiosondes in the lower stratosphere (18-30km). The monthly mean GW variances clearly show an annual oscillation with a maximum in the winter and minimum in the summer. The QBO signature could be clearly seen in the lower stratosphere. In the upper stratosphere, a longer period oscillation (~5-6 years) with maxima in 2000-2001 and 2006 was revealed to synchronize with the solar maximum and minimum. No clear signature of GW activity in the lower mesosphere could be associated to that in the upper stratosphere, suggesting that part of gravity waves may either dissipated or reflected when crossing the stratopause region.

Observed stratospheric downward reflection, and its relation to upward pulses of wave activity

NASA Astrophysics Data System (ADS)

Harnik, N.

2009-04-01

We examine the differences between observed stratospheric vertical wave reflection and wave absorption events, which differ in that the wave induced deceleration remains confined to upper levels in the former. The two types of events signify two types of stratospheric winter dynamics, associated with different downward coupling to the troposphere (Perlwitz and Harnik, 2004). Using time lag composites, we find that the main factor influencing which event will occur is the duration, in time, of the upward pulse of wave activity entering the stratosphere from the troposphere. Short pulses accelerate the flow at their trailing edge in the lower stratosphere while they decelerate it at upper levels, resulting in a vertical shear reversal, and corresponding downward reflection, while long pulses continue decelerating the vortex at progressively lower levels. The confinement of deceleration to upper levels for short wave forcing pulses is also found in an idealized model of an interaction between a planetary wave and the stratospheric vortex, though some aspects of the wave geometry evolution, and thus vertical reflection, are not captured realistically in the model. The results suggest the stratospheric influence on the type of wave interaction, in reality, is indirect - through a possible effect on the duration of upward wave fluxes through the tropopause.

The Tropical Upper Troposphere and Lower Stratosphere in the GEOS-2 GCM

NASA Technical Reports Server (NTRS)

Pawson, S.; Takacs, L.; Molod, A.; Nebuda, S.; Chen, M.; Rood, R.; Read, W. L.; Fiorino, M.

1999-01-01

The structure of the tropical upper troposphere and lower stratosphere in the GEOS-2 General Circulation Model (GCM) is discussed. The emphasis of this study is on the reality of monthly-mean temperature and water vapor distributions in the model, compared to reasonable observational estimates. It is shown that although the zonal-mean temperature is in good agreement with observations, the GCM supports an excessive zonal asymmetry near the tropopause compared to the ECMWF Reanalyses. In reality there is a QBO-related variability in the zonally averaged lower stratospheric temperature which is not captured by the model. The observed upper tropospheric temperature and humidity fields show variations related to those in the sea surface temperature, which are not incorporated in the GCM; nevertheless, there is some interannual variability in the GCM, indicating a component arising from internal processes. The model is too moist in the middle troposphere (500 hPa) but too dry in the upper troposphere, suggesting that there is too little vertical transport or too much drying in the GCM. Transport into the stratosphere shows a pronounced annual cycle, with drier air entering the tropical stratosphere when the tropopause is coldest in northern winter; while the alternating dry and moist air masses can be traced ascending through the tropical lower stratosphere, the progression of the anomalies is too rapid.

Natural variability of tropical upper stratospheric ozone inferred from the Atmosphere Explorer backscatter ultraviolet experiment

NASA Technical Reports Server (NTRS)

Frederick, J. E.; Abrams, R. B.; Dasgupta, R.; Guenther, B.

1981-01-01

Analysis of backscattered ultraviolet radiances observed at tropical latitudes by the Atmosphere Explorer-E satellite reveals both annual and semiannual cycles in upper stratospheric ozone. The annual variation dominates the signal at wavelengths which sense ozone primarily above 45 km while below this, to the lowest altitude sensed, 35 km, the semiannual component has comparable amplitude. Comparison of radiance measurements taken with the same instrument at solar minimum during 1976 and solar maximum in 1979 show no significant differences. This suggests that variations in upper stratospheric ozone over the solar cycle are small, although the data presently available do not allow a definite conclusion.

An upper limit for stratospheric hydrogen peroxide

NASA Technical Reports Server (NTRS)

Chance, K. V.; Traub, W. A.

1984-01-01

It has been postulated that hydrogen peroxide is important in stratospheric chemistry as a reservoir and sink for odd hydrogen species, and for its ability to interconvert them. The present investigation is concerned with an altitude dependent upper limit curve for stratospheric hydrogen peroxide, taking into account an altitude range from 21.5 to 38.0 km for January 23, 1983. The data employed are from balloon flight No. 1316-P, launched from the National Scientific Balloon Facility (NSBF) in Palestine, Texas. The obtained upper limit curve lies substantially below the data reported by Waters et al. (1981), even though the results are from the same latitude and are both wintertime measurements.

Impact of convection on stratospheric humidity and upper tropospheric clouds

NASA Astrophysics Data System (ADS)

Ueyama, R.; Schoeberl, M. R.; Jensen, E. J.; Pfister, L.; Avery, M. A.

2017-12-01

The role of convection on stratospheric water vapor and upper tropospheric cloud fraction is investigated using two sets of complementary transport and microphysical models driven by MERRA-2 and ERA-Interim meteorological analyses: (1) computationally efficient ensembles of forward trajectories with simplified cloud microphysics, and (2) one-dimensional simulations with detailed microphysics along back trajectories. Convective influence along the trajectories is diagnosed based on TRMM/GPM rainfall products and geostationary infrared satellite cloud-top measurements, with convective cloud-top height adjusted to match the CloudSat, CALIPSO, and CATS measurements. We evaluate and constrain the model results by comparison with satellite observations (e.g., Aura MLS, CALIPSO CALIOP) and high-altitude aircraft campaigns (e.g., ATTREX, POSIDON). Convection moistens the lower stratosphere by approximately 10-15% and increases the cloud fraction in the upper troposphere by 35-50%. Convective moistening is dominated by the saturating effect of parcels; convectively-lofted ice has a negligible impact on lower stratospheric humidity. We also find that the highest convective clouds have a disproportionately large impact on stratospheric water vapor because stratospheric relative humidity is low. Implications of these model results on the role of convection on present and future climate will be discussed.

Ozone Temperature Correlations in the Upper Stratosphere as a Measure of Chlorine Content

NASA Technical Reports Server (NTRS)

Stolarski, Richard S.; Douglass, Ann R.; Remsberg, Ellis E.; Livesey, Nathaniel J.; Gille, John C.

2012-01-01

We use data from the Nimbus-7 Limb Infrared Monitor of the Stratosphere (LIMS) for the 1978-1979 period together with data from the Upper Atmosphere Research Satellite Microwave Limb Sounder (UARS MLS) for the years 1993 to 1999, the Aura MLS for the years 2004 to 2011, and the Aura High Resolution Infrared Limb Sounder (HIRDLS) for the years 2005 to 2007 to examine ozone-temperature correlations in the upper stratosphere. Our model simulations indicate that the sensitivity coefficient of the ozone response to temperature (Delta ln(O3)/Delta.(l/T)) decreases as chlorine has increased in the stratosphere and should increase in the future as chlorine decreases. The data are in agreement with our simulation of the past. We also find that the sensitivity coefficient does not change in a constant-chlorine simulation. Thus the change in the sensitivity coefficient depends on the change in chlorine, but not on the change in greenhouse gases. We suggest that these and future data can be used to track the impact of chlorine added to the stratosphere and also to track the recovery of the stratosphere as chlorine is removed under the provisions of the Montreal Protocol.

Response of the dynamic and thermodynamic structure of the stratosphere to the solar cycle in the boreal winter

NASA Astrophysics Data System (ADS)

Shi, Chunhua; Gao, Yannan; Cai, Juan; Guo, Dong; Lu, Yan

2018-04-01

The response of the dynamic and thermodynamic structure of the stratosphere to the solar cycle in the boreal winter is investigated based on measurements of the solar cycle by the Spectral Irradiance Monitor onboard the SORCE satellite, monthly ERA-Interim Reanalysis data from the European Center for Medium-Range Weather Forecasts, the radiative transfer scheme of the Beijing Climate Center (BCC-RAD) and a multiple linear regression model. The results show that during periods of strong solar activity, the solar shortwave heating anomaly from the climatology in the tropical upper stratosphere triggers a local warm anomaly and strong westerly winds in mid-latitudes, which strengthens the upward propagation of planetary wave 1 but prevents that of wave 2. The enhanced westerly jet makes a slight adjustment to the propagation path of wave 1, but prevents wave 2 from propagating upward, decreases the dissipation of wave 2 in the extratropical upper stratosphere and hence weakens the Brewer-Dobson circulation. The adiabatic heating term in relation to the Brewer-Dobson circulation shows anomalous warming in the tropical lower stratosphere and anomalous cooling in the mid-latitude upper stratosphere.

The vertical distribution and origin of HCN in Neptune's atmosphere

NASA Technical Reports Server (NTRS)

Lellouch, Emmanuel; Romani, Paul N.; Rosenqvist, Jan

1994-01-01

Measurements and modeling of the (3-2) rotational line of hydrogen cyanide at 265.9 GHz in Neptune's atmosphere are presented. High signal-to-noise observations provide information on the HCN vertical distribution in Neptune's stratosphere. The HCN mixing ratio is found to be nearly uniform with height above the condensation level. Best fits occur for HCN distributions that have a slight increase with altitude. A least-squares analysis yields a mixing ratio of (3.2 +/- 0.8)10(exp -10) at 2 mbar and a mean mixing ratio scale height of 250(sup 750)(sub -110) km in the 0.1-3 mbar region. To interpret these results, we developed a photochemical model of HCN. HCN formation is initiated by the reaction between CH3 radicals, produced from methane photochemistry, and N atoms. The primary sink for HCN is condensation, with minor contributions from photolysis and chemical losses. Two possible sources of N atoms are investigated: (1) infall of N escaped from Triton's upper atmosphere, and (2) galactic cosmic ray (GCR) impact on internal N2. Given the uncertainties on (i) the transport and possible ionization of N in Neptune's magnetosphere, and the fate of N(+) reaching Neptune's upper atmosphere and (ii) the N2 mixing ratio in Neptune's deep atmosphere, we suggest that both sources of N atoms may significantly contibute to the formation of HCN.

On the Identification of Ozone Recovery

NASA Astrophysics Data System (ADS)

Stone, Kane A.; Solomon, Susan; Kinnison, Douglas E.

2018-05-01

As ozone depleting substances decline, stratospheric ozone is displaying signs of healing in the Antarctic lower stratosphere. Here we focus on higher altitudes and the global stratosphere. Two key processes that can influence ozone recovery are evaluated: dynamical variability and solar proton events (SPEs). A nine-member ensemble of free-running simulations indicates that dynamical variability dominates the relatively small ozone recovery signal over 1998-2016 in the subpolar lower stratosphere, particularly near the tropical tropopause. The absence of observed recovery there to date is therefore not unexpected. For the upper stratosphere, high latitudes (50-80°N/S) during autumn and winter show the largest recovery. Large halogen-induced odd oxygen loss there provides a fingerprint of seasonal sensitivity to chlorine trends. However, we show that SPEs also have a profound effect on ozone trends within this region since 2000. Thus, accounting for SPEs is important for detection of recovery in the upper stratosphere.

Global variations of zonal mean ozone during stratospheric warming events

NASA Technical Reports Server (NTRS)

Randel, William J.

1993-01-01

Eight years of Solar Backscatter Ultraviolet (SBUV) ozone data are examined to study zonal mean variations associated with stratospheric planetary wave (warming) events. These fluctuations are found to be nearly global in extent, with relatively large variations in the tropics, and coherent signatures reaching up to 50 deg in the opposite (summer) hemisphere. These ozone variations are a manifestation of the global circulation cells associated with stratospheric warming events; the ozone responds dynamically in the lower stratosphere to transport, and photochemically in the upper stratosphere to the circulation-induced temperature changes. The observed ozone variations in the tropics are of particular interest because transport is dominated by zonal-mean vertical motions (eddy flux divergences and mean meridional transports are negligible), and hence, substantial simplifications to the governing equations occur. The response of the atmosphere to these impulsive circulation changes provides a situation for robust estimates of the ozone-temperature sensitivity in the upper stratosphere.

Orography and the Boreal Winter Stratosphere: The Importance of the Mongolian Mountains

NASA Astrophysics Data System (ADS)

White, R. H.; Battisti, D. S.; Sheshadri, A.

2018-02-01

The impact of mountains on stratospheric circulation is explored using the Whole Atmosphere Community Climate Model. The "Mongolian mountains" decrease the boreal winter stratospheric jet strength by ˜1/3 and increase the frequency of major sudden stratospheric warmings from 0.08 year-1 to the observed 0.60 year-1. These changes are twice the magnitude of the impacts of the Tibetan plateau and Himalayas. Consistent with the decrease in the zonal jet, there is enhanced Eliassen-Palm flux convergence; this is predominantly from changes in wave propagation pathways through changes to the upper troposphere circulation, not from an increased amplitude of planetary waves reaching the stratosphere. The Mongolian mountains have the greater impact on upper tropospheric circulation due to their meridional location. The Rocky Mountains have no significant impact on the stratospheric jet. Changes in wave propagation in response to the Mongolian mountains are similar to those associated with major sudden stratospheric warming events in observations.

Analysis of data from spacecraft (stratospheric warmings)

NASA Technical Reports Server (NTRS)

1974-01-01

The details of the stratospheric warming processes as to time, area, and intensity were established, and the warmings with other terrestrial and solar phenomena occurring at satellite platform altitudes, or observable from satellite platforms, were correlated. Links were sought between the perturbed upper atmosphere (mesosphere and thermosphere) and the stratosphere that might explain stratospheric warmings.

Sulfate aerosols and polar stratospheric cloud formation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tolbert, M.A.

Before the discovery of the Antarctic ozone hole, it was generally assumed that gas-phase chemical reactions controlled the abundance of stratospheric ozone. However, the massive springtime ozone losses over Antarctica first reported by Farman et al in 1985 could not be explained on the basis of gas-phase chemistry alone. In 1986, Solomon et al suggested that chemical reactions occurring on the surfaces of polar stratospheric clouds (PSCs) could be important for the observed ozone losses. Since that time, an explosion of laboratory, field, and theoretical research in heterogeneous atmospheric chemistry has occurred. Recent work has indicated that the most importantmore » heterogeneous reaction on PSCs is ClONO[sub 2] + HCl [yields] Cl[sub 2] + HNO[sub 3]. This reaction converts inert chlorine into photochemically active Cl[sub 2]. Photolysis of Cl[sub 2] then leads to chlorine radicals capable of destroying ozone through very efficient catalytic chain reactions. New observations during the second Airborne Arctic Stratospheric Expedition found stoichiometric loss of ClONO[sub 2] and HCl in air processed by PSCs in accordance with reaction 1. Attention is turning toward understanding what kinds of aerosols form in the stratospheric, their formation mechanism, surface area, and specific chemical reactivity. Some of the latest findings, which underline the importance of aerosols, were presented at a recent National Aeronautics and Space Administration workshop in Boulder, Colorado.« less

Review of ultraviolet absorption cross sections of a series of alternative fluorocarbons

NASA Technical Reports Server (NTRS)

Molina, Mario J.

1990-01-01

Solar photolysis is likely to contribute to the stratospheric destruction of those alternative fluorocarbons (HFC's) which have two or more chlorine atoms bonded to the same carbon atom. Two of the eight HFC's considered here fall into this category, namely HFC-123 and HFC141b. For these two species there is good agreement among the various measurements of the ultraviolet cross sections in the wavelength region which is important for atmospheric photodissociation, that is, around 200 nm. There is also good agreement for HFC-124, HFC-22 and HFC-142b. These are the three species which contain one chlorine atom per molecule. The agreement in the measurements is poor for the other species, i.e., those that do not contain chlorine, except in so far as to corroborate that solar photolysis should be negligible relative to destruction by hydroxyl radicals.

Present state of knowledge of the upper atmosphere 1990: An assessment report

NASA Technical Reports Server (NTRS)

Watson, R. T.; Kurylo, M. J.; Prather, M. J.; Ormond, F. M.

1990-01-01

NASA is charged with the responsibility to report on the state of the knowledge of the Earth's upper atmosphere, particularly the stratosphere. Part 1 of this report, issued earlier this year, summarized the objectives, status, and accomplishments of the research tasks supported under NASA's Upper Atmosphere Research Program during the last two years. New findings since the last report to Congress was issued in 1988 are presented. Several scientific assessments of the current understanding of the chemical composition and physical structure of the stratosphere are included, in particular how the abundance and distribution of ozone is predicted to change in the future. These reviews include: a summary of the most recent international assessment of stratospheric ozone; a study of future chlorine and bromine loading of the atmosphere; a review of the photochemical and chemical kinetics data that are used as input parameters for the atmospheric models; a new assessment of the impact of Space Shuttle launches on the stratosphere; a summary of the environmental issues and needed research to evaluate the impact of the newly re-proposed fleet of stratospheric supersonic civil aircraft; and a list of the contributors to this report and the science assessments which have formed our present state of knowledge of the upper atmosphere and ozone depletion.

Space-Time Variations in Water Vapor as Observed by the UARS Microwave Limb Sounder

NASA Technical Reports Server (NTRS)

Elson, Lee S.; Read, William G.; Waters, Joe W.; Mote, Philip W.; Kinnersley, Jonathan S.; Harwood, Robert S.

1996-01-01

Water vapor in the upper troposphere has a significant impact on the climate system. Difficulties in making accurate global measurements have led to uncertainty in understanding water vapor's coupling to the hydrologic cycle in the lower troposphere and its role in radiative energy balance. The Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite is able to retrieve water vapor concentration in the upper troposphere with good sensitivity and nearly global coverage. An analysis of these preliminary retrievals based on 3 years of observations shows the water vapor distribution to be similar to that measured by other techniques and to model results. The primary MLS water vapor measurements were made in the stratosphere, where this species acts as a conserved tracer under certain conditions. As is the case for the upper troposphere, most of the stratospheric discussion focuses on the time evolution of the zonal mean and zonally varying water vapor. Stratospheric results span a 19-month period and tropospheric results a 36-month period, both beginning in October of 1991. Comparisons with stratospheric model calculations show general agreement, with some differences in the amplitude and phase of long-term variations. At certain times and places, the evolution of water vapor distributions in the lower stratosphere suggests the presence of meridional transport.

Gravity Waves and Mesospheric Clouds in the Summer Middle Atmosphere: A Comparison of Lidar Measurements and Ray Modeling of Gravity Waves Over Sondrestrom, Greenland

NASA Technical Reports Server (NTRS)

Gerrard, Andrew J.; Kane, Timothy J.; Eckermann, Stephen D.; Thayer, Jeffrey P.

2004-01-01

We conducted gravity wave ray-tracing experiments within an atmospheric region centered near the ARCLITE lidar system at Sondrestrom, Greenland (67N, 310 deg E), in efforts to understand lidar observations of both upper stratospheric gravity wave activity and mesospheric clouds during August 1996 and the summer of 2001. The ray model was used to trace gravity waves through realistic three-dimensional daily-varying background atmospheres in the region, based on forecasts and analyses in the troposphere and stratosphere and climatologies higher up. Reverse ray tracing based on upper stratospheric lidar observations at Sondrestrom was also used to try to objectively identify wave source regions in the troposphere. A source spectrum specified by reverse ray tracing experiments in early August 1996 (when atmospheric flow patterns produced enhanced transmission of waves into the upper stratosphere) yielded model results throughout the remainder of August 1996 that agreed best with the lidar observations. The model also simulated increased vertical group propagation of waves between 40 km and 80 km due to intensifying mean easterlies, which allowed many of the gravity waves observed at 40 km over Sondrestrom to propagate quasi-vertically from 40-80 km and then interact with any mesospheric clouds at 80 km near Sondrestrom, supporting earlier experimentally-inferred correlations between upper stratospheric gravity wave activity and mesospheric cloud backscatter from Sondrestrom lidar observations. A pilot experiment of real-time runs with the model in 2001 using weather forecast data as a low-level background produced less agreement with lidar observations. We believe this is due to limitations in our specified tropospheric source spectrum, the use of climatological winds and temperatures in the upper stratosphere and mesosphere, and missing lidar data from important time periods.

Middle Atmosphere Response to Different Descriptions of the 11-Year Solar Cycle in Spectral Irradiance in a Chemistry-Climate Model

NASA Technical Reports Server (NTRS)

Swartz, W. H.; Stolarski, R. S.; Oman, L. D.; Fleming, E. L.; Jackman, C. H.

2012-01-01

The 11-year solar cycle in solar spectral irradiance (SSI) inferred from measurements by the SOlar Radiation & Climate Experiment (SORCE) suggests a much larger variation in the ultraviolet than previously accepted. We present middle atmosphere ozone and temperature responses to the solar cycles in SORCE SSI and the ubiquitous Naval Research Laboratory (NRL) SSI reconstruction using the Goddard Earth Observing System chemistry-climate model (GEOS CCM). The results are largely consistent with other recent modeling studies. The modeled ozone response is positive throughout the stratosphere and lower mesosphere using the NRL SSI, while the SORCE SSI produces a response that is larger in the lower stratosphere but out of phase with respect to total solar irradiance above 45 km. The modeled responses in total ozone are similar to those derived from satellite and ground-based measurements, 3-6 Dobson Units per 100 units of 10.7-cm radio flux (F10.7) in the tropics. The peak zonal mean tropical temperature response 50 using the SORCE SSI is nearly 2 K per 100 units 3 times larger than the simulation using the NRL SSI. The GEOS CCM and the Goddard Space Flight Center (GSFC) 2-D coupled model are used to examine how the SSI solar cycle affects the atmosphere through direct solar heating and photolysis processes individually. Middle atmosphere ozone is affected almost entirely through photolysis, whereas the solar cycle in temperature is caused both through direct heating and photolysis feedbacks, processes that are mostly linearly separable. Further, the net ozone response results from the balance of ozone production at wavelengths less than 242 nm and destruction at longer wavelengths, coincidentally corresponding to the wavelength regimes of the SOLar STellar Irradiance Comparison Experiment (SOLSTICE) and Spectral Irradiance Monitor (SIM) on SORCE, respectively. A higher wavelength-resolution analysis of the spectral response could allow for a better prediction of the atmospheric response to arbitrary SSI variations.

A comparison of the structure and flow characteristics of the upper troposphere and stratosphere of the Northern and Southern Hemispheres

NASA Technical Reports Server (NTRS)

Adler, R. F.

1974-01-01

The general circulations of the Northern and Southern Hemispheres are compared with regard to the upper troposphere and stratosphere using atmospheric structure obtained from satellite, multi-channel radiance data. Specifically, the data are from the Satellite Infrared Spectrometer (SIRS) instrument aboard the Nimbus 3 spacecraft. The inter-hemispheric comparisons are based on two months of data (one summer month and one winter month) in each hemisphere. Topics studied include: mean meridional circulation in the Southern Hemisphere stratosphere; magnitude and distribution of tropospheric eddy heat flux; magnitudes of energy cycle components; and the relation of vortex structure to the breakdown climatology of the Antarctic stratospheric polar vortex.

A global analysis of the ozone deficit in the upper stratosphere and lower mesosphere

NASA Technical Reports Server (NTRS)

Eluszkiewicz, Janusz; Allen, Mark

1993-01-01

The global measurements of temperature, ozone, water vapor, and nitrogen dioxide acquired by the Limb Infrared Monitor of the Stratosphere (LIMS), supplemented by a precomputed distribution of chlorine monoxide, are used to test the balance between odd oxygen production and loss in the upper stratosphere and lower mesosphere. An efficient photochemical equilibrium model, whose validity is ascertained by comparison with the results from a fully time-dependent one-dimensional model at selected latitudes, is used in the calculations. The computed ozone abundances are systematically lower than observations for May 1-7, 1979, which suggests, contrary to the conclusions of other recent studies, a real problem in model simulations of stratospheric ozone.

Climatology of water vapor in the upper troposphere and lower stratosphere determined from Sage 2 observations

NASA Technical Reports Server (NTRS)

Chiou, Er-Woon; McCormick, M. P.

1994-01-01

The purpose of this paper is to present a vertically-resolved global climatology of water vapor in the upper troposphere and lower stratosphere based on multi-year SAGE 2 observations. Seasonally averaged zonal mean profiles are illustrated in terms of both mixing ration and relative humidity.

Temperature Trends in the Tropical Upper Troposphere and Lower Stratosphere: Connections with Sea Surface Temperatures and Implications for Water Vapor and Ozone

NASA Technical Reports Server (NTRS)

Garfinkel, C. I.; Waugh, D. W.; Oman, L. D.; Wang, L.; Hurwitz, M. M.

2013-01-01

Satellite observations and chemistry-climate model experiments are used to understand the zonal structure of tropical lower stratospheric temperature, water vapor, and ozone trends. The warming in the tropical upper troposphere over the past 30 years is strongest near the Indo-Pacific warm pool, while the warming trend in the western and central Pacific is much weaker. In the lower stratosphere, these trends are reversed: the historical cooling trend is strongest over the Indo-Pacific warm pool and is weakest in the western and central Pacific. These zonal variations are stronger than the zonal-mean response in boreal winter. Targeted experiments with a chemistry-climate model are used to demonstrate that sea surface temperature (hereafter SST) trends are driving the zonal asymmetry in upper tropospheric and lower stratospheric tropical temperature trends. Warming SSTs in the Indian Ocean and in the warm pool region have led to enhanced moist heating in the upper troposphere, and in turn to a Gill-like response that extends into the lower stratosphere. The anomalous circulation has led to zonal structure in the ozone and water vapor trends near the tropopause, and subsequently to less water vapor entering the stratosphere. The radiative impact of these changes in trace gases is smaller than the direct impact of the moist heating. Projected future SSTs appear to drive a temperature and water vapor response whose zonal structure is similar to the historical response. In the lower stratosphere, the changes in water vapor and temperature due to projected future SSTs are of similar strength to, though slightly weaker than, that due directly to projected future CO2, ozone, and methane.

Effective absorption cross sections and photolysis rates of anthropogenic and biogenic secondary organic aerosols

NASA Astrophysics Data System (ADS)

Romonosky, Dian E.; Ali, Nujhat N.; Saiduddin, Mariyah N.; Wu, Michael; Lee, Hyun Ji (Julie); Aiona, Paige K.; Nizkorodov, Sergey A.

2016-04-01

Mass absorption coefficient (MAC) values were measured for secondary organic aerosol (SOA) samples produced by flow tube ozonolysis and smog chamber photooxidation of a wide range of volatile organic compounds (VOC), specifically: α-pinene, β-pinene, β-myrcene, d-limonene, farnesene, guaiacol, imidazole, isoprene, linalool, ocimene, p-xylene, 1-methylpyrrole, and 2-methylpyrrole. Both low-NOx and high-NOx conditions were employed during the chamber photooxidation experiments. MAC values were converted into effective molecular absorption cross sections assuming an average molecular weight of 300 g/mol for SOA compounds. The upper limits for the effective photolysis rates of SOA compounds were calculated by assuming unity photolysis quantum yields and convoluting the absorption cross sections with a time-dependent solar spectral flux. A more realistic estimate for the photolysis rates relying on the quantum yield of acetone was also obtained. The results show that condensed-phase photolysis of SOA compounds can potentially occur with effective lifetimes ranging from minutes to days, suggesting that photolysis is an efficient and largely overlooked mechanism of SOA aging.

The maintenance of elevated active chlorine levels in the Antarctic lower stratosphere through HCl null cycles

NASA Astrophysics Data System (ADS)

Müller, Rolf; Grooß, Jens-Uwe; Mannan Zafar, Abdul; Robrecht, Sabine; Lehmann, Ralph

2018-03-01

The Antarctic ozone hole arises from ozone destruction driven by elevated levels of ozone destroying (active) chlorine in Antarctic spring. These elevated levels of active chlorine have to be formed first and then maintained throughout the period of ozone destruction. It is a matter of debate how this maintenance of active chlorine is brought about in Antarctic spring, when the rate of formation of HCl (considered to be the main chlorine deactivation mechanism in Antarctica) is extremely high. Here we show that in the heart of the ozone hole (16-18 km or 85-55 hPa, in the core of the vortex), high levels of active chlorine are maintained by effective chemical cycles (referred to as HCl null cycles hereafter). In these cycles, the formation of HCl is balanced by immediate reactivation, i.e. by immediate reformation of active chlorine. Under these conditions, polar stratospheric clouds sequester HNO3 and thereby cause NO2 concentrations to be low. These HCl null cycles allow active chlorine levels to be maintained in the Antarctic lower stratosphere and thus rapid ozone destruction to occur. For the observed almost complete activation of stratospheric chlorine in the lower stratosphere, the heterogeneous reaction HCl + HOCl is essential; the production of HOCl occurs via HO2 + ClO, with the HO2 resulting from CH2O photolysis. These results are important for assessing the impact of changes of the future stratospheric composition on the recovery of the ozone hole. Our simulations indicate that, in the lower stratosphere, future increased methane concentrations will not lead to enhanced chlorine deactivation (through the reaction CH4 + Cl → HCl + CH3) and that extreme ozone destruction to levels below ≈ 0.1 ppm will occur until mid-century.

A Long Data Record (1979-2003) of Stratospheric Ozone Derived from TOMS Cloud Slicing: Comparison with SAGE and Implications for Ozone Recovery

NASA Technical Reports Server (NTRS)

Ziemke, Jerry R.; Chandra, Sushil; Bhartia, Pawan K.

2004-01-01

It is generally recognized that Stratospheric Aerosols and Gas Experiment (SAGE) stratospheric ozone data have become a standard long-record reference field for comparison with other stratospheric ozone measurements. This study demonstrates that stratospheric column ozone (SCO) derived from total ozone mapping spectrometer (TOMS) Cloud Slicing may be used to supplement SAGE data as a stand-alone long- record reference field in the tropics extending to middle and high latitudes over the Pacific. Comparisons of SAGE I1 version 6.2 SCO and TOMS version 8 Cloud Slicing SCO for 1984-2003 exhibit remarkable agreement in monthly ensemble means to within 1-3 DU (1 - 1.5% of SCO) despite being independently-calibrated measurements. An important component of our study is to incorporate these column ozone measurements to investigate long-term trends for the period 1979-2003. Our study includes Solar Backscatter Ultraviolet (SBW) version 8 measurements of upper stratospheric column ozone (i.e., zero to 32 hPa column ozone) to characterize seasonal cycles and seasonal trends in this region, as well as the lower stratosphere and troposphere when combined with TOMS SCO and total column ozone. The trend analyses suggest that most ozone reduction in the atmosphere since 1979 in mid-to-high latitudes has occurred in the Lower stratosphere below approx. 25 km. The delineation of upper and lower stratospheric column ozone indicate that trends in the upper stratosphere during the latter half of the 1979-2003 period have reduced to near zero globally, while trends in the lower stratosphere have become larger by approx. 5 DU decade%om the tropics extending to mid-latitudes in both hemispheres. For TCO, the trend analyses suggest moderate increases over the 25-year time record in the extra-tropics of both hemispheres of around 4-6 DU (Northern Hemisphere) and 6-8 DU (Southern Hemisphere).

Stratospheric Ozone Response in Experiments G3 and G4 of the Geoengineering Model Intercomparison Project (GeoMIP)

NASA Technical Reports Server (NTRS)

Pitari, Giovanni; Aquila, Valentina; Kravitz, Ben; Watanabe, Shingo; Tilmes, Simone; Mancini, Eva; DeLuca, Natalia; DiGenova, Glauco

2013-01-01

Geoengineering with stratospheric sulfate aerosols has been proposed as a means of temporarily cooling the planet, alleviating some of the side effects of anthropogenic CO2 emissions. However, one of the known side effects of stratospheric injections of sulfate aerosols is a decrease in stratospheric ozone. Here we show results from two general circulation models and two coupled chemistry climate models that have simulated stratospheric sulfate aerosol geoengineering as part of the Geoengineering Model Intercomparison Project (GeoMIP). Changes in photolysis rates and upwelling of ozone-poor air in the tropics reduce stratospheric ozone, suppression of the NOx cycle increases stratospheric ozone, and an increase in available surfaces for heterogeneous chemistry modulates reductions in ozone. On average, the models show a factor 20-40 increase of the sulfate aerosol surface area density (SAD) at 50 hPa in the tropics with respect to unperturbed background conditions and a factor 3-10 increase at mid-high latitudes. The net effect for a tropical injection rate of 5 Tg SO2 per year is a decrease in globally averaged ozone by 1.1-2.1 DU in the years 2040-2050 for three models which include heterogeneous chemistry on the sulfate aerosol surfaces. GISS-E2-R, a fully coupled general circulation model, performed simulations with no heterogeneous chemistry and a smaller aerosol size; it showed a decrease in ozone by 9.7 DU. After the year 2050, suppression of the NOx cycle becomes more important than destruction of ozone by ClOx, causing an increase in total stratospheric ozone. Contribution of ozone changes in this experiment to radiative forcing is 0.23 W m-2 in GISS-E2-R and less than 0.1 W m-2 in the other three models. Polar ozone depletion, due to enhanced formation of both sulfate aerosol SAD and polar stratospheric clouds, results in an average 5 percent increase in calculated surface UV-B.

Model Sensitivity Studies of the Decrease in Atmospheric Carbon Tetrachloride

NASA Technical Reports Server (NTRS)

Chipperfield, Martyn P.; Liang, Qing; Rigby, Matt; Hossaini, Ryan; Montzka, Stephen A.; Dhomse, Sandip; Feng, Wuhu; Prinn, Ronald G.; Weiss, Ray F.; Harth, Christina M.;

Model sensitivity studies of the decrease in atmospheric carbon tetrachloride

NASA Astrophysics Data System (ADS)

Chipperfield, Martyn P.; Liang, Qing; Rigby, Matthew; Hossaini, Ryan; Montzka, Stephen A.; Dhomse, Sandip; Feng, Wuhu; Prinn, Ronald G.; Weiss, Ray F.; Harth, Christina M.; Salameh, Peter K.; Mühle, Jens; O'Doherty, Simon; Young, Dickon; Simmonds, Peter G.; Krummel, Paul B.; Fraser, Paul J.; Steele, L. Paul; Happell, James D.; Rhew, Robert C.; Butler, James; Yvon-Lewis, Shari A.; Hall, Bradley; Nance, David; Moore, Fred; Miller, Ben R.; Elkins, James W.; Harrison, Jeremy J.; Boone, Chris D.; Atlas, Elliot L.; Mahieu, Emmanuel

2016-12-01

Carbon tetrachloride (CCl4) is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this decrease is known to be slower than expected based on reported CCl4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (74 % of total), but a reported 10 % uncertainty in its combined photolysis cross section and quantum yield has only a modest impact on the modelled rate of CCl4 decay. This is partly due to the limiting effect of the rate of transport of CCl4 from the main tropospheric reservoir to the stratosphere, where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9 % of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (17 % of total) has the largest impact on modelled CCl4 decay due to its sizeable contribution to CCl4 loss and large lifetime uncertainty range (147 to 241 years). With an assumed CCl4 emission rate of 39 Gg year-1, the reference simulation with the best estimate of loss processes still underestimates the observed CCl4 (overestimates the decay) over the past 2 decades but to a smaller extent than previous studies. Changes to the rate of CCl4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 47 Gg year-1. Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the National Oceanic and Atmospheric Administration (NOAA) network are larger than from the Advanced Global Atmospheric Gases Experiment (AGAGE) network but have shown a steeper decreasing trend over the past 2 decades. These differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl4 sinks.

Mechanisms and Feedbacks Causing Changes in Upper Stratospheric Ozone in the 21st Century

NASA Technical Reports Server (NTRS)

Oman, Luke; Waugh, D. W.; Kawa, S. R.; Stolarski, R. S.; Douglass, A. R.; Newman, P. A.

2009-01-01

Stratospheric ozone is expected to increase during the 21st century as the abundance of halogenated ozone-depleting substances decrease to 1960 values. However, climate change will likely alter this "recovery" of stratospheric ozone by changing stratospheric temperatures, circulation, and abundance of reactive chemical species. Here we quantity the contribution of different mechanisms to changes in upper stratospheric ozone from 1960 to 2100 in the Goddard Earth Observing System Chemistry-Climate Model (GEOS CCM), using multiple linear regression analysis applied to simulations using either Alb or A2 greenhouse gas (GHG) scenarios. In both these scenarios upper stratospheric ozone has a secular increase over the 21st century. For the simulation using the Alb GHG scenario, this increase is determined by the decrease in halogen amounts and the greenhouse gas induced cooling, with roughly equal contributions from each mechanism. There is a larger cooling in the simulation using the A2 GHG scenario, but also enhanced loss from higher NOy and HOx concentrations, which nearly offsets the increase due to cooler temperatures. The resulting ozone evolutions are similar in the A2 and Alb simulations. The response of ozone due to feedbacks from temperature and HOx changes, related to changing halogen concentrations, are also quantified using simulations with fixed halogen concentrations.

Influence of sudden stratospheric warming and quasi biennial oscillation on western disturbance over north India

NASA Astrophysics Data System (ADS)

Remya, R.; Kottayil, Ajil; Mohanakumar, K.

2017-07-01

This study demonstrates the variability in Western Disturbance during the sudden stratospheric warming (SSW) period and its eventual influence on the north Indian weather pattern. The modulations in the north Indian winter under the two phases of the Quasi-biennial oscillation (QBO) during SSW periods are also examined. The analysis has been carried out by using the ERA interim reanalysis dataset for different pressure levels in the stratosphere and upper troposphere during the time period of 1980-2010. The daily minimum surface temperature data published by India Meteorological Department from 1969 to 2013 has been used for the analysis of temperature anomaly over north India during SSW. The period of intense stratospheric warming witnesses a downward propagation and intensification of kinetic energy from stratosphere to upper troposphere over the Mediterranean and Caspian Sea. When QBO is in easterly phase, the cooling over north India is much larger when compared to the westerly phase during instances of SSW. SSW coincident with the easterly phase of QBO causes an intensified subtropical jet over the mid-latitude regions. The modulation in circulation pattern in stratosphere and upper troposphere when ENSO occurs during SSW period is also analysed separately. This study provides the link among SSW, Western Disturbances and the north Indian cooling during winter season.

Evidence of Seasonally Dependent Stratosphere-Troposphere Exchange and Purging of Lower Stratospheric Aeroso from a Multi-Year Lidar Dataset

NASA Technical Reports Server (NTRS)

Menzies, R. T.; Tratt, D. M.

1994-01-01

Tropospheric and lower stratospheric aerosol backscatter data obtained from a calibrated backscatter lidar at Pasadena, California (34 deg N latitude)over the 1984-1993 period clearly indicate tightly coupled aerosol optical properties in the upper troposphere and lower stratosphere in the winter and early spring, due to the active mid-latitude stratospheric-tropospheric (ST) exchange processes occurring at this time of year.

Stratospheric ozone changes under solar geoengineering: implications for UV exposure and air quality

NASA Astrophysics Data System (ADS)

Nowack, Peer Johannes; Abraham, Nathan Luke; Braesicke, Peter; Pyle, John Adrian

2016-03-01

Various forms of geoengineering have been proposed to counter anthropogenic climate change. Methods which aim to modify the Earth's energy balance by reducing insolation are often subsumed under the term solar radiation management (SRM). Here, we present results of a standard SRM modelling experiment in which the incoming solar irradiance is reduced to offset the global mean warming induced by a quadrupling of atmospheric carbon dioxide. For the first time in an atmosphere-ocean coupled climate model, we include atmospheric composition feedbacks for this experiment. While the SRM scheme considered here could offset greenhouse gas induced global mean surface warming, it leads to important changes in atmospheric composition. We find large stratospheric ozone increases that induce significant reductions in surface UV-B irradiance, which would have implications for vitamin D production. In addition, the higher stratospheric ozone levels lead to decreased ozone photolysis in the troposphere. In combination with lower atmospheric specific humidity under SRM, this results in overall surface ozone concentration increases in the idealized G1 experiment. Both UV-B and surface ozone changes are important for human health. We therefore highlight that both stratospheric and tropospheric ozone changes must be considered in the assessment of any SRM scheme, due to their important roles in regulating UV exposure and air quality.

A molecular beam mass spectrometric study of the formation and photolysis of C(lc)lO dimer

NASA Technical Reports Server (NTRS)

Greene, Frank T.; Robaugh, David A.

1992-01-01

A study of the chlorine oxides present at temperatures and pressures typical of the Antarctic stratosphere was carried out. A series of low temperature flow reactors was constructed and used in conjunction with molecular beam mass spectrometric techniques to identify species and characterize their kinetic behavior at temperatures of -20 to -70 C and pressures of from 30 to 130 Torr. It was found that the gas phase chlorine-oxygen system was quite complex at low temperatures. ClO dimer was identified and found to be thermodynamically very stable under stratospheric conditions. It was also found that any system which contained ClO also contained a larger oxide. The oxide was identified as Cl2O3. A survey of possible higher oxides, which have been postulated as possible chlorine sinks in the stratosphere, was also carried out. The rate of formation of ClO dimer was measured as a function of temperature and pressure. Measurements were made of both the decay of ClO and the formation of the dimer. By comparing these rates it was determined that virtually all of the ClO was converted to the dimer under stratospheric conditions, and that the other ClO reactions were not important under these conditions.

The long-term evolution of hydrocarbons in Jupiter's stratosphere

NASA Astrophysics Data System (ADS)

Melin, Henrik; Fletcher, Leigh N.; Greathouse, Thomas K.; Giles, Rohini Sara; Sinclair, James; Orton, Glenn S.; Irwin, Patrick Gerard Joseph

2016-10-01

We present the global distribution of hydrocarbons in Jupiter's stratosphere using ground-based mid-infrared R~15,000 TEXES observations from the NASA Infrared Telescope Facility (IRTF), obtained between 2013 and 2016. Ethane and acetylene are the primary products of methane photolysis in Jupiter's stratosphere, and their spatial distribution can be used to trace atmospheric circulation and the lifetimes of chemical constituents. Zonal mean distributions of these species have been previously studied from the Voyager and Cassini spacecraft (Nixon et al., 2010, doi: 10.1016/j.pss.2010.05.008), but the TEXES dataset now provides the opportunity to track the evolution of the hydrocarbons from Earth (Fletcher et al., 2016, doi:10.1016/j.icarus.2016.06.008 ). Global spectral maps of methane, ethane and acetylene emission are used to characterize the temporal evolution of large scale features in Jupiter's stratosphere (0.5-20 mbar?), including: equator to pole contrasts driven by large-scale stratospheric overturning; mid-latitude bands of elevated hydrocarbon emission; small-scale wave phenomena driven by meteorological activity in the underlying troposphere; and the tropical changes in emission related to Jupiter's Quasi-Quadrennial Oscillation. The NEMESIS spectral inversion tool (Irwin et al., 2008, doi: 10.1016/j.jqsrt.2007.11.006) is used to derive stratospheric temperatures and hydrocarbon abundances from spatially-resolved spectra at 744, 819, and 1247 cm-1. We use these to investigate the changes in the vertical temperature and ethane and acetylene distributions over time, with the aim of providing the global and temporal context for Juno's exploration of the jovian atmosphere in 2016/17.

The Limb Infrared Monitor of the Stratosphere (LIMS) experiment

NASA Technical Reports Server (NTRS)

Russell, J. M.; Gille, J. C.

1978-01-01

The Limb Infrared Monitor of the Stratosphere is used to obtain vertical profiles and maps of temperature and the concentration of ozone, water vapor, nitrogen dioxide, and nitric acid for the region of the stratosphere bounded by the upper troposphere and the lower mesosphere.

A New Connection Between Greenhouse Warming and Stratospheric Ozone Depletion

NASA Technical Reports Server (NTRS)

Salawitch, R.

1998-01-01

The direct radiative effects of the build-up of carbon dioxide and other greenhouse gases have led to a gradual cooling of the stratosphere with largest changes in temperature occurring in the upper stratosphere, well above the region of peak ozone concentration.

Three-dimensional dynamical and chemical modelling of the upper atmosphere

NASA Technical Reports Server (NTRS)

Prinn, R. G.; Alyea, F. N.; Cunnold, D. M.

1976-01-01

Progress in coding a 3-D upper atmospheric model and in modeling the ozone perturbation resulting from the shuttle booster exhaust is reported. A time-dependent version of a 2-D model was studied and the sulfur cycle in the stratosphere was investigated. The role of meteorology in influencing stratospheric composition measurements was also studied.

Upper Tropospheric Ozone Between Latitudes 60S and 60N Derived from Nimbus 7 TOMS/THIR Cloud Slicing

NASA Technical Reports Server (NTRS)

Ziemke, Jerald R.; Chandra, Sushil; Bhartia, P. K.

2002-01-01

This study evaluates the spatial distributions and seasonal cycles in upper tropospheric ozone (pressure range 200-500 hPa) from low to high latitudes (60S to 60N) derived from the satellite retrieval method called "Cloud Slicing." Cloud Slicing is a unique technique for determining ozone profile information in the troposphere by combining co-located measurements of cloud-top, pressure and above-cloud column ozone. For upper tropospheric ozone, co-located measurements of Nimbus 7 Total Ozone Mapping Spectrometer (TOMS) above-cloud column ozone, and Nimbus 7 Temperature Humidity Infrared Radiometer (THIR) cloud-top pressure during 1979-1984 were incorporated. In the tropics, upper tropospheric ozone shows year-round enhancement in the Atlantic region and evidence of a possible semiannual variability. Upper tropospheric ozone outside the tropics shows greatest abundance in winter and spring seasons in both hemispheres with largest seasonal and largest amounts in the NH. These characteristics are similar to lower stratospheric ozone. Comparisons of upper tropospheric column ozone with both stratospheric ozone and a proxy of lower stratospheric air mass (i.e., tropopause pressure) from National Centers for Environmental Prediction (NCEP) suggest that stratosphere-troposphere exchange (STE) may be a significant source for the seasonal variability of upper tropospheric ozone almost everywhere between 60S and 60N except in low latitudes around 10S to 25N where other sources (e.g., tropospheric transport, biomass burning, aerosol effects, lightning, etc.) may have a greater role.

Stratospheric Temperature Changes: Observations and Model Simulations

NASA Technical Reports Server (NTRS)

Ramaswamy, V.; Chanin, M.-L.; Angell, J.; Barnett, J.; Gaffen, D.; Gelman, M.; Keckhut, P.; Koshelkov, Y.; Labitzke, K.; Lin, J.-J. R.

1999-01-01

This paper reviews observations of stratospheric temperatures that have been made over a period of several decades. Those observed temperatures have been used to assess variations and trends in stratospheric temperatures. A wide range of observation datasets have been used, comprising measurements by radiosonde (1940s to the present), satellite (1979 - present), lidar (1979 - present) and rocketsonde (periods varying with location, but most terminating by about the mid-1990s). In addition, trends have also been assessed from meteorological analyses, based on radiosonde and/or satellite data, and products based on assimilating observations into a general circulation model. Radiosonde and satellite data indicate a cooling trend of the annual-mean lower stratosphere since about 1980. Over the period 1979-1994, the trend is 0.6K/decade. For the period prior to 1980, the radiosonde data exhibit a substantially weaker long-term cooling trend. In the northern hemisphere, the cooling trend is about 0.75K/decade in the lower stratosphere, with a reduction in the cooling in mid-stratosphere (near 35 km), and increased cooling in the upper stratosphere (approximately 2 K per decade at 50 km). Model simulations indicate that the depletion of lower stratospheric ozone is the dominant factor in the observed lower stratospheric cooling. In the middle and upper stratosphere both the well-mixed greenhouse gases (such as CO) and ozone changes contribute in an important manner to the cooling.

Mixing and ageing in the polar lower stratosphere in winter 2015-2016

NASA Astrophysics Data System (ADS)

Krause, Jens; Hoor, Peter; Engel, Andreas; Plöger, Felix; Grooß, Jens-Uwe; Bönisch, Harald; Keber, Timo; Sinnhuber, Björn-Martin; Woiwode, Wolfgang; Oelhaf, Hermann

2018-05-01

We present data from winter 2015-2016, which were measured during the POLSTRACC (The Polar Stratosphere in a Changing Climate) aircraft campaign between December 2015 and March 2016 in the Arctic upper troposphere and lower stratosphere (UTLS). The focus of this work is on the role of transport and mixing between aged and potentially chemically processed air masses from the stratosphere which have midlatitude and low-latitude air mass fractions with small transit times originating at the tropical lower stratosphere. By combining measurements of CO, N2O and SF6 we estimate the evolution of the relative contributions of transport and mixing to the UTLS composition over the course of the winter. We find an increasing influence of aged stratospheric air partly from the vortex as indicated by decreasing N2O and SF6 values over the course of the winter in the extratropical lower and lowermost stratosphere between Θ = 360 K and Θ = 410 K over the North Atlantic and the European Arctic. Surprisingly we also found a mean increase in CO of (3.00 ± 1.64) ppbV from January to March relative to N2O in the lower stratosphere. We show that this increase in CO is consistent with an increased mixing of tropospheric air as part of the fast transport mechanism in the lower stratosphere surf zone. The analysed air masses were partly affected by air masses which originated at the tropical tropopause and were quasi-horizontally mixed into higher latitudes. This increase in the tropospheric air fraction partly compensates for ageing of the UTLS due to the diabatic descent of air masses from the vortex by horizontally mixed, tropospheric-influenced air masses. This is consistent with simulated age spectra from the Chemical Lagrangian Model of the Stratosphere (CLaMS), which show a respective fractional increase in tropospheric air with transit times under 6 months and a simultaneous increase in aged air from upper stratospheric and vortex regions with transit times longer than 2 years. We thus conclude that the lowermost stratosphere in winter 2015-2016 was affected by aged air from the upper stratosphere and vortex region. These air masses were significantly affected by increased mixing from the lower latitudes, which led to a simultaneous increase in the fraction of young air in the lowermost Arctic stratosphere by 6 % from January to March 2016.

Inorganic Iodine and Bromine in the Tropical Upper Troposphere/Lower Stratosphere Derived From Balloon Borne Observations

NASA Astrophysics Data System (ADS)

Dorf, M.; Butz, A.; Camy-Peyret, C.; Chipperfield, M.; Kreycy, S.; Kritten, L.; Prados-Roman, C.; Pfeilsticker, K.

2008-12-01

Due to the ozone destroying capabilities of bromine and iodine bearing compounds, the stratospheric budget of inorganic bromine and iodine is of major interest for modeling ozone depletion and assessing the future evolution of the ozone layer. In particular the contribution of very short lived substances (VSLS) to the bromine budget has recently been shown to enhance ozone depletion in mid-latitudes and polar regions. So far, iodine species have not been unambiguously detected in the stratosphere with upper limits for total inorganic iodine (Iy) of about 0.1 ppt. However, observations are sparse and mainly restricted to mid- and high-latitudes. Here, we assess the budget of iodine and bromine in the tropical Upper Troposphere/ Lower Stratosphere (UT/LS) where the halogen source gases enter the stratosphere and supply the stratosphere with halogen species. We report on two stratospheric balloon flights of the LPMA/DOAS (Limb Profile Monitor of the Atmosphere/Differential Optical Absorption Spectrometer) payload from a tropical station in northern Brazil (5°S, 43°W) in June 2005 and June 2008. There, the LPMA/DOAS payload conducted spectroscopic direct sun measurements in the UV/visible and infrared spectral range during balloon ascent and in solar occultation geometry. The LPMA/DOAS observations allow for the retrieval of IO and OIO from their absorption features in the visible spectral range. Neither species could be detected unambiguously with detection limits ranging between 0.01 and 0.2 ppt in the UT/LS. Constraining a stratospheric chemistry model by the inferred detection limits for IO and OIO, yields an upper limit for Iy of 0.1 to 0.3 ppt. Implications for stratospheric ozone are discussed on the basis of model studies. BrO is inferred from absorption bands in the UV spectral range yielding the first BrO vertical profile in the tropical UT/LS. For the balloon flight in June 2005, total inorganic bromine (Bry) is estimated to (21.5 ± 2.5) ppt in 4.5-year-old air using a stratospheric model constrained by measured BrO. We derive a total contribution of (5.2 ± 2.5) ppt from brominated VSLS and inorganic product gases to Bry. Tropospheric BrO was found to be < 1 ppt. Our results are compared to 3-D CTM SLIMCAT model runs.

Enhancements in lower stratospheric CH3CN observed by the upper atmosphere research Sattellite Microwave Limb Sounder following boreal forest fires

NASA Technical Reports Server (NTRS)

Livesey, N. J.; Fromm, M. D.; Waters, J. W.; Manney, G. L.; Santee, M. L.; Read, W. G.

2004-01-01

On 25 August 1992, the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite observed a significant enhancement in the abundance of lower stratospheric methyl cyanide (CH3CN) at 100??hPa (16??km altitude) in a small region off the east coast of Florida.

Upper Stratospheric Temperature Climatology Derived from SAGE II Observations: Preliminary Results

NASA Technical Reports Server (NTRS)

Wang, P.-H.; Cunnold, D. M.; Wang, H. J.; Chu, W. P.; Thomason, L. W.

2002-01-01

This study shows that the temperature information in the upper stratosphere can be derived from the SAGE II 385-mn observations. The preliminary results indicate that the zonal mean temperature increases with altitude below 50 km and decreases above 50 km. At 50 km, a regional maximum of 263 K is located in the tropics, and a minimum of 261 K occurs in the subtropics in both hemispheres. The derived long-term temperature changes from 1985 to 1997 reveal a statistically significant negative trend of -2 to -2.5 K/decade in the tropical upper stratosphere and about -2 K/decade in the subtropics near the stratopause. At latitudes poleward of 50, the results show a statistically significant positive trend of about 1 K/decade in the upper stratosphere. The preliminary results also show large annual temperature oscillations in the extratropics with a maximum amplitude of approx. 8 K located at about 44 km near 50 in both hemispheres during local summer. In addition, the semiannual oscillation is found to be a maximum in the tropics with a peak amplitude of approx. 3.3 K located at about 42 km during the equinox.

Investigation of Tropical Transport with UARS Data

NASA Technical Reports Server (NTRS)

Dunkerton, Timothy J.

1999-01-01

Measurements of trace constituents obtained by instruments aboard the Upper Atmosphere Research Satellite (UARS) have been used to study transport processes associated with the quasi-biennial oscillation, laterally propagating Rossby waves, and upward propagating Kelvin waves in the tropical and subtropical upper troposphere and stratosphere. Mean vertical motions, vertical diffusivities and in-mixing rates were inferred from observations of the 'tape recorder' signal in near-equatorial stratospheric water vapor. The effect of the quasi-biennial oscillation (QBO) on tracer distributions in the upper half of the stratosphere was seen in a spectacular 'staircase' pattern, predominantly in the winter hemisphere, revealing the latitudinally asymmetric nature of QBO transport due to induced mean meridional circulations and modulation of lateral mixing associated with planetary Rossby waves. The propagation of Rossby waves across the equator in the westerly phase of the QBO was seen in tracer fields and corroborating United Kingdom Meteorological Office (UKMO) analyses; a modeling study of the effect of these waves on typical QBO wind profiles was performed. Water vapor in the upper troposphere and lower stratosphere was found to exhibit signatures of the tropical intraseasonal oscillation (TIO) and faster Kelvin waves in the two regions, respectively.

Long-term Evolution of Upper Stratospheric Ozone at Selected Stations of the Network for the Detection of Stratospheric Change (NDSC)

NASA Technical Reports Server (NTRS)

Steinbrecht, W.; Claude, H.; Schoenenborn, F.; McDermid, I. S.; LeBlanc, T.; Godin, S.; Swart, D. P. J.; Meijer, Y. J.; Bodecker, G. E.; Connor, B. J.;

The Plunger Hypothesis: an overview of a new theory of stratosphere-troposphere dynamic coupling

NASA Astrophysics Data System (ADS)

Clark, S.; Baldwin, M. P.; Stephenson, D.

2015-12-01

I will demonstrate the advantages of a new method of quantifying polar stratosphere-troposphere coupling by considering large-scale movements of mass into and out of the polar stratosphere. This project aims to use these mass movements to explain pressure and temperature anomalies throughout the polar troposphere and lower stratosphere in the aftermath of extreme stratospheric events. We hypothesise that these mass movements are induced by deposition of momentum by breaking waves in the stratosphere, slowing the wintertime polar vortex, and so are associated with sudden stratospheric warmings (SSWs). Such a mass movement in the upper stratosphere acts to compress the polar atmosphere below it in the manner of a plunger. In this way the pressure anomaly in the upper polar stratosphere 'controls' the pressure and temperature anomalies below by adiabatic compression of the polar atmospheric column. Better understanding this method of control will allow us to use stratospheric data to improve medium-range forecasting ability in the troposphere. One of the key innovations featured in this project is considering pressure and temperature fields at fixed geopotential surfaces, allowing for the easy observation of mass movement into and out of a polar cap region (which we have defined as north of 65N) as a function of altitude. Reanalysis data considered in this manner demonstrates a relationship between tropospheric pressure anomalies and stratospheric anomalies in the polar cap, and so a way to predict tropospheric variability given stratospheric information. This work forms part of a three and a half year PhD project.

On the Climate Impacts of Upper Tropospheric and Lower Stratospheric Ozone

NASA Astrophysics Data System (ADS)

Xia, Yan; Huang, Yi; Hu, Yongyun

2018-01-01

The global warming simulations of the general circulation models (GCMs) are generally performed with different ozone prescriptions. We find that the differences in ozone distribution, especially in the upper tropospheric and lower stratospheric (UTLS) region, account for important model discrepancies shown in the ozone-only historical experiment of the Coupled Model Intercomparison Project Phase 5 (CMIP5). These discrepancies include global high cloud fraction, stratospheric temperature, and stratospheric water vapor. Through a set of experiments conducted by an atmospheric GCM with contrasting UTLS ozone prescriptions, we verify that UTLS ozone not only directly radiatively heats the UTLS region and cools the upper parts of the stratosphere but also strongly influences the high clouds due to its impact on relative humidity and static stability in the UTLS region and the stratospheric water vapor due to its impact on the tropical tropopause temperature. These consequences strongly affect the global mean effective radiative forcing of ozone, as noted in previous studies. Our findings suggest that special attention should be paid to the UTLS ozone when evaluating the climate effects of ozone depletion in the 20th century and recovery in the 21st century. UTLS ozone difference may also be important for understanding the intermodel discrepancy in the climate projections of the CMIP6 GCMs in which either prescribed or interactive ozone is used.

Studies of ClO and BrO reactions important in the polar stratosphere: Kinetics and mechanism of the ClO+BrO and ClO+ClO reactions

NASA Technical Reports Server (NTRS)

Friedl, Randall R.; Sander, Stanley P.

1988-01-01

The reactions, BrO + ClO yields Br + ClOO (1a) yields Br + OClO (1b) yields BrCl + O2 (1c) and ClO + ClO yields Cl + CiOO (2a) yields Cl + OClO (2b) yields Cl2 + O2 (2c) yields (ClO)2 (2d) have assumed new importance in explaining the unusual springtime depletion of ozone observed in the Antarctic stratosphere. The mechanisms of these reactions involve the formation of metastable intermediates which subsequently decompose through several energetically allowed products providing the motivation to study these reactions using both the discharge flow-mass spectrometric and flash photolysis - ultraviolet absorption techniques. These methods have also been used to explore aspects of the kinetics and spectroscopy of the ClO dimer.

Determination of hydrocarbon abundances and the strength of eddy mixing in the stratosphere of Neptune: Analysis of UVS solar occultation lightcurves

NASA Technical Reports Server (NTRS)

Bishop, James

1995-01-01

Work on completing our analysis of the Voyager UVS solar occultation data acquired during Neptune encounter is essentially complete, as testified by the attached poster materials. The photochemical modeling addresses the recent revision in branching ratios for radical production in the photolysis of methane at H Lyman alpha implied by the lab measurements of Mordaunt et al. (1993). The software generated in this effort has been useful for checking the degree to which photochemical models addressing other datasets (mainly infrared) are consistent with the UVS data. This work complements the UVS modeling results in that the IR data refer to deeper pressure levels; as regards the modeling of UVS data, the most significant result is the convincing support for the presence of a stagnant lower stratosphere. Evidence for strong dynamical (mixing) transport of minor constituents at shallower pressures is provided by the UVS data analysis.

Chemical Loss of Ozone in the Arctic Polar Vortex in the Winter of 1991-1992

NASA Technical Reports Server (NTRS)

Salawitch, R. J.; Wofsy, S. C.; Gottlieb, E. W.; Lait, L. R.; Newman, P. A.; Schoeberl, M. R.; Strahan, S. E.; Loewenstein, M.; Podolske, J. R.; Chan, K. R.;

Tracking the delayed response of the northern winter stratosphere to ENSO using multi reanalyses and model simulations

NASA Astrophysics Data System (ADS)

Ren, Rongcai; Rao, Jian; Wu, Guoxiong; Cai, Ming

2017-05-01

The concurrent effects of the El Niño-Southern Oscillation (ENSO) on the northern winter stratosphere have been widely recognized; however, the delayed effects of ENSO in the next winter after mature ENSO have yet to be confirmed in multi reanalyses and model simulations. This study uses three reanalysis datasets, a long-term fully coupled model simulation, and a high-top general circulation model to examine ENSO's delayed effects in the stratosphere. The warm-minus-cold composite analyses consistently showed that, except those quick-decaying quasi-biennial ENSO events that reverse signs during July-August-September (JAS) in their decay years, ENSO events particularly those quasi-quadrennial (QQ) that persist through JAS, always have a significant effect on the extratropical stratosphere in both the concurrent winter and the next winter following mature ENSO. During the concurrent winter, the QQ ENSO-induced Pacific-North American (PNA) pattern corresponds to an anomalous wavenumber-1 from the upper troposphere to the stratosphere, which acts to intensify/weaken the climatological wave pattern during warm/cold ENSO. Associated with the zonally quasi-homogeneous tropical forcing in spring of the QQ ENSO decay years, there appear persistent and zonally quasi-homogeneous temperature anomalies in the midlatitudes from the upper troposphere to the lower stratosphere until summer. With the reduction in ENSO forcing and the PNA responses in the following winter, an anomalous wavenumber-2 prevails in the extratropics. Although the anomalous wave flux divergence in the upper stratospheric layer is still dominated by wavenumber-1, it is mainly caused by wavenumber-2 in the lower stratosphere. However, the wavenumber-2 activity in the next winter is always underestimated in the model simulations, and wavenumber-1 activity dominates in both winters.

Irreversible transport in the stratosphere by internal waves of short vertical wavelength

NASA Technical Reports Server (NTRS)

Danielsen, Edwin F.; Hipskind, R. S.; Starr, Walter L.; Vedder, James F.; Gaines, Steven E.; Kley, Dieter; Kelley, Ken K.

1991-01-01

Measurements performed during stratospheric flights of the U-2 aircraft confirm that cross-jet transport is dominated by waves, not by large-scale circulations. Monotonic gradients of trace constituents normal to the jet axis, with upper stratospheric tracers increasing poleward and tropospheric tracers increasing equatorward, are augmented by large-scale confluence as the jet intensifies during cyclogenesis. These gradients are rotated, intensified, and significantly increased in areas as their mixing ratio surfaces are folded by the differential transport of a very low frequency transverse wave. The quasi-horizontal transport produces a laminar structure with stable layers rich in upper stratospheric tracers alternating vertically with less stable layers rich in tropospheric tracers. The transport proceeds toward irreversibility at higher frequency, shear-gravity waves extend the folding to smaller horizontal scales.

Vertical structure of stratospheric water vapour trends derived from merged satellite data

PubMed Central

Hegglin, M. I.; Plummer, D. A.; Shepherd, T. G.; Scinocca, J. F.; Anderson, J.; Froidevaux, L.; Funke, B.; Hurst, D.; Rozanov, A.; Urban, J.; von Clarmann, T.; Walker, K. A.; Wang, H. J.; Tegtmeier, S.; Weigel, K.

2017-01-01

Stratospheric water vapour is a powerful greenhouse gas. The longest available record from balloon observations over Boulder, Colorado, USA shows increases in stratospheric water vapour concentrations that cannot be fully explained by observed changes in the main drivers, tropical tropopause temperatures and methane. Satellite observations could help resolve the issue, but constructing a reliable long-term data record from individual short satellite records is challenging. Here we present an approach to merge satellite data sets with the help of a chemistry-climate model nudged to observed meteorology. We use the models' water vapour as a transfer function between data sets that overcomes issues arising from instrument drift and short overlap periods. In the lower stratosphere, our water vapour record extends back to 1988 and water vapour concentrations largely follow tropical tropopause temperatures. Lower and mid-stratospheric long-term trends are negative, and the trends from Boulder are shown not to be globally representative. In the upper stratosphere, our record extends back to 1986 and shows positive long-term trends. The altitudinal differences in the trends are explained by methane oxidation together with a strengthened lower-stratospheric and a weakened upper-stratospheric circulation inferred by this analysis. Our results call into question previous estimates of surface radiative forcing based on presumed global long-term increases in water vapour concentrations in the lower stratosphere. PMID:29263751

Vertical structure of stratospheric water vapour trends derived from merged satellite data.

PubMed

Hegglin, M I; Plummer, D A; Shepherd, T G; Scinocca, J F; Anderson, J; Froidevaux, L; Funke, B; Hurst, D; Rozanov, A; Urban, J; von Clarmann, T; Walker, K A; Wang, H J; Tegtmeier, S; Weigel, K

2014-01-01

Stratospheric water vapour is a powerful greenhouse gas. The longest available record from balloon observations over Boulder, Colorado, USA shows increases in stratospheric water vapour concentrations that cannot be fully explained by observed changes in the main drivers, tropical tropopause temperatures and methane. Satellite observations could help resolve the issue, but constructing a reliable long-term data record from individual short satellite records is challenging. Here we present an approach to merge satellite data sets with the help of a chemistry-climate model nudged to observed meteorology. We use the models' water vapour as a transfer function between data sets that overcomes issues arising from instrument drift and short overlap periods. In the lower stratosphere, our water vapour record extends back to 1988 and water vapour concentrations largely follow tropical tropopause temperatures. Lower and mid-stratospheric long-term trends are negative, and the trends from Boulder are shown not to be globally representative. In the upper stratosphere, our record extends back to 1986 and shows positive long-term trends. The altitudinal differences in the trends are explained by methane oxidation together with a strengthened lower-stratospheric and a weakened upper-stratospheric circulation inferred by this analysis. Our results call into question previous estimates of surface radiative forcing based on presumed global long-term increases in water vapour concentrations in the lower stratosphere.

Stratospheric HTO perturbations 1980-1983

NASA Astrophysics Data System (ADS)

Mason, A. S.

1985-02-01

Three perturbations of the stratospheric tritiated water burden have occurred. An atmospheric nuclear detonation in 1980 injected about 2.1 MCi. The massive eruptions of the volcano El Chichon may have contributed to a doubling of the removal rate in 1982. An unusually large wintertime exchange with the upper stratosphere may have occurred between 1982 and 1983.

Merged SAGE II, Ozone_cci and OMPS ozone profiles dataset and evaluation of ozone trends in the stratosphere

NASA Astrophysics Data System (ADS)

Tamminen, J.; Sofieva, V.; Kyrölä, E.; Laine, M.; Degenstein, D. A.; Bourassa, A. E.; Roth, C.; Zawada, D.; Weber, M.; Rozanov, A.; Rahpoe, N.; Stiller, G. P.; Laeng, A.; von Clarmann, T.; Walker, K. A.; Sheese, P.; Hubert, D.; Van Roozendael, M.; Zehner, C.; Damadeo, R. P.; Zawodny, J. M.; Kramarova, N. A.; Bhartia, P. K.

2017-12-01

We present a merged dataset of ozone profiles from several satellite instruments: SAGE II on ERBS, GOMOS, SCIAMACHY and MIPAS on Envisat, OSIRIS on Odin, ACE-FTS on SCISAT, and OMPS on Suomi-NPP. The merged dataset is created in the framework of European Space Agency Climate Change Initiative (Ozone_cci) with the aim of analyzing stratospheric ozone trends. For the merged dataset, we used the latest versions of the original ozone datasets. The datasets from the individual instruments have been extensively validated and inter-compared; only those datasets, which are in good agreement and do not exhibit significant drifts with respect to collocated ground-based observations and with respect to each other, are used for merging. The long-term SAGE-CCI-OMPS dataset is created by computation and merging of deseasonalized anomalies from individual instruments. The merged SAGE-CCI-OMPS dataset consists of deseasonalized anomalies of ozone in 10° latitude bands from 90°S to 90°N and from 10 to 50 km in steps of 1 km covering the period from October 1984 to July 2016. This newly created dataset is used for evaluating ozone trends in the stratosphere through multiple linear regression. Negative ozone trends in the upper stratosphere are observed before 1997 and positive trends are found after 1997. The upper stratospheric trends are statistically significant at mid-latitudes in the upper stratosphere and indicate ozone recovery, as expected from the decrease of stratospheric halogens that started in the middle of the 1990s.

Multimodel Assessment of the Factors Driving Stratospheric Ozone Evolution over the 21st Century

NASA Technical Reports Server (NTRS)

Oman, L. D.; Plummer, D. A.; Waugh, D. W.; Austin, J.; Scinocca, J. F.; Douglass, A. R.; Salawitch, R. J.; Canty, T.; Akiyoshi, H.; Bekki, S.;

The temperature dependence of the rate constant for the reaction of hydroxyl radicals with nitric acid

NASA Technical Reports Server (NTRS)

Kurylo, M. J.; Cornett, K. D.; Murphy, J. L.

1982-01-01

The rate constant for the reaction of hydroxyl radicals with nitric acid in the 225-443 K temperature range has been measured by means of the flash photolysis resonance fluorescence technique. Above 300 K, the rate constant levels off in a way that can only be explained by the occurrence of two reaction channels, of which one, operative at low temperatures, proceeds through the formation of an adduct intermediate. The implications of these rate constant values for stratospheric reaction constants is discussed.

Solar Radiation Measurements Onboard the Research Aircraft HALO

NASA Astrophysics Data System (ADS)

Lohse, I.; Bohn, B.; Werner, F.; Ehrlich, A.; Wendisch, M.

2014-12-01

Airborne measurements of the separated upward and downward components of solar spectral actinic flux densities for the determination of photolysis frequencies and of upward nadir spectral radiance were performed with the HALO Solar Radiation (HALO-SR) instrument package onboard the High Altitude and Long Range Research Aircraft (HALO). The instrumentation of HALO-SR is characterized and first measurement data from the Next-generation Aircraft Remote-Sensing for Validation Studies (NARVAL) campaigns in 2013 and 2014 are presented. The measured data are analyzed in the context of the retrieved microphysical and optical properties of clouds which were observed underneath the aircraft. Detailed angular sensitivities of the two optical actinic flux receivers were determined in the laboratory. The effects of deviations from the ideal response are investigated using radiative transfer calculations of atmospheric radiance distributions under various atmospheric conditions and different ground albedos. Corresponding correction factors are derived. Example photolysis frequencies are presented, which were sampled in the free troposphere and lower stratosphere over the Atlantic Ocean during the 2013/14 HALO NARVAL campaigns. Dependencies of photolysis frequencies on cloud cover, flight altitude and wavelength range of the photolysis process are investigated. Calculated actinic flux densities in the presence of clouds benefit from the measured spectral radiances. Retrieved cloud optical thicknesses and effective droplet radii are used as model input for the radiative transfer calculations. By comparison with the concurrent measurements of actinic flux densities the retrieval approach is validated. Acknowledgements: Funding by the Deutsche Forschungsgemeinschaft within the priority program HALO (BO 1580/4-1, WE 1900/21-1) is gratefully acknowledged.

Quantum yield for carbon monoxide production in the 248 nm photodissociation of carbonyl sulfide (OCS)

NASA Technical Reports Server (NTRS)

Zhao, Z.; Stickel, R. E.; Wine, P. H.

1995-01-01

Tunable diode laser absorption spectroscopy has been coupled with excimer laser flash photolysis to measure the quantum yield for CO production from 248 nm photodissociation of carbonyl sulfide (OCS) relative to the well-known quantum yield for CO production from 248 nm photolysis of phosgene (Cl2CO2). The temporal resolution of the experiments was sufficient to distinguish CO formed directly by photodissociation from that formed by subsequent S((sup 3)P(sub J)) reaction with OCS. Under the experimental conditions employed, CO formation via the fast S((sup 1)D(sub 2)) + OCS reaction was minimal. Measurements at 297K and total pressures from 4 to 100 Torr N2 + N2O show the CO yield to be greater than 0.95 and most likely unity. This result suggests that the contribution of OCS as a precursor to the lower stratospheric sulfate aerosol layer is somewhat larger than previously thought.

Ozone in the Atmosphere: I. The Upper Atmosphere.

ERIC Educational Resources Information Center

Phillips, Paul S.

1990-01-01

Research concerning the role of stratospheric ozone and the effect of chlorofluorocarbons on stratospheric ozone are discussed. The consequences of global ozone depletion are projected. The Montreal Protocol is reviewed. (CW)

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)

NASA Technical Reports Server (NTRS)

Voemel, Holger

2004-01-01

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.

Nitric oxide in the upper stratosphere - Measurements and geophysical interpretation

NASA Technical Reports Server (NTRS)

Harvath, J. J.; Frederick, J. E.; Orsini, N.; Douglass, A. R.

1983-01-01

A rocket-borne parachute-deployed chemiluminescence instrument has obtained seven new measurements of atmospheric nitric oxide for altitudes between 30 and 50 km at mid-latitudes. These results, when combined with profiles measured by an earlier version of the instrument, cover all four seasons and provide a more comprehensive picture of upper stratospheric nitric oxide than has been available previously. At the highest altitudes studied, the vertical gradient in mixing ratio displays positive and negative values during different observations, with the largest values tending to appear at the greatest heights in summer. Examination of the differences among the profiles, which exceed a factor of 3 near the stratopause, suggests that they arise from the action of transport processes which carry air into the mid-latitude upper stratosphere from regions of the atmosphere that contain widely different odd-nitrogen abundances.

Simulated forecast error and climate drift resulting from the omission of the upper stratosphere in numerical models

NASA Technical Reports Server (NTRS)

Boville, Byron A.; Baumhefner, David P.

1990-01-01

Using an NCAR community climate model, Version I, the forecast error growth and the climate drift resulting from the omission of the upper stratosphere are investigated. In the experiment, the control simulation is a seasonal integration of a medium horizontal general circulation model with 30 levels extending from the surface to the upper mesosphere, while the main experiment uses an identical model, except that only the bottom 15 levels (below 10 mb) are retained. It is shown that both random and systematic errors develop rapidly in the lower stratosphere with some local propagation into the troposphere in the 10-30-day time range. The random growth rate in the troposphere in the case of the altered upper boundary was found to be slightly faster than that for the initial-condition uncertainty alone. However, this is not likely to make a significant impact in operational forecast models, because the initial-condition uncertainty is very large.

Normal mode Rossby waves observed in the upper stratosphere

NASA Technical Reports Server (NTRS)

Hirooka, T.; Hirota, I.

1985-01-01

In recent years, observational evidence has been obtained for westward traveling planetary waves in the middle atmosphere with the aid of global data from satellites. There is no doubt that the fair portion of the observed traveling waves can be understood as the manifestation of the normal mode Rossby waves which are theoretically derived from the tidal theory. Some observational aspects of the structure and behavior of the normal model Rossby waves in the upper stratosphere are reported. The data used are the global stratospheric geopotential thickness and height analyses which are derived mainly from the Stratospheric Sounding Units (SSUs) on board TIROS-N and NOAA satellites. A clear example of the influence of the normal mode Rossby wave on the mean flow is reported. The mechanism considered is interference between the normal mode Rossby wave and the quasi-stationary wave.

An extreme anomaly in stratospheric ozone over Europe in 1940-1942

NASA Astrophysics Data System (ADS)

Brönnimann, S.; Luterbacher, J.; Staehelin, J.; Svendby, T. M.

2004-04-01

Reevaluated historical total ozone data reveal extraordinarily high values over several European sites in 1940-1942, concurrent with extreme climatic anomalies at the Earth's surface. Using historical radiosonde data, reconstructed upper-level fields, and total ozone data from Arosa (Switzerland), Dombås, and Tromsø (Norway), this unusual case of stratosphere-troposphere coupling is analyzed. At Arosa, numerous strong total ozone peaks in all seasons were due to unusually frequent upper troughs over central Europe and related ozone redistribution in the lower stratosphere. At the Norwegian sites, high winter total ozone was most likely caused by major stratospheric warmings in Jan./Feb. 1940, Feb./Mar. 1941, and Feb. 1942. Results demonstrate that the dynamically driven interannual variability of total ozone can be much larger than that estimated based on the past 25-40 years.

Observations of the upper troposphere and lower stratosphere using the urbana coherent-scatter radar

NASA Technical Reports Server (NTRS)

Goss, L. D.; Bowhill, S. A.

1983-01-01

The Urbana coherent-scatter radar was used to observe the upper troposphere and lower stratosphere, and 134 hours of data were collected. Horizontal wind measurements show good agreement with balloon-measured winds. Gravity waves were frequently observed, and were enhanced during convective activity. Updrafts and downdrafts were observed within thunderstorms. Power returns are related to hydrostatic stability, and changes in echo specularity are shown.

Why is the Great Red Spot Red? The Exogenic, Photolytic Origin of the UV/Blue-Absorbing Chromophores of Jupiter’s Great Red Spot as Determined by Spectral Analysis of Cassini/VIMS Observations using New Laboratory Optical Coefficients

NASA Astrophysics Data System (ADS)

Baines, Kevin H.; Carlson, Robert W.; Momary, Thomas W.

2014-11-01

For centuries, a major question for Jupiter has been: Why is the Great Red Spot red? In particular, two major theories have been proposed: (1) that the coloring is due to photolytic processes in the upper cloud layer, or (2) it is due to the upwellimg of red materials processed relatively deep within the troposphere. Utilizing indices of refraction for red choromophores generated by the photolysis of ammonia and acetylene in the laboratory, we present results of a spectral analysis of the core of Jupiter’s Great Red Spot (GRS) as observed by the visual channel of the Cassini/Visual Infrared Mapping Spectrometer (VIMS). Consistent with the physical origin of such laboratory-generated chromophores in Jupiter - i.e., by solar-driven UV photolysis within the upper levels of the GRS structure near ~ 0.3 bar - our spectral modeling yields satisfactory results for such Mie scattering chromophores only when they are confined to the upper ~ 100 mbar of the GRS. Beneath this reddish upper cloud layer, our models indicate that the remainder of the GRS cloud - assumed to extend down to at least the ammonia condensation level near 0.6 bar - must be relatively spectrally bright throughout the UV-red spectrum; that is, they must be predominantly a whitish or grey color at depth. Thus, our 0.35-1.0 micron spectral models of the GRS are inconsistent with an endogenic origin of the reddish coloring originating in the depths of Jupiter, but are consistent with a photolytic origin due to the photolysis of ammonia and acetylene in the upper troposphere.

Evidence for a Continuous Decline in Lower Stratospheric Ozone Offsetting Ozone Layer Recovery

NASA Technical Reports Server (NTRS)

Ball, William T.; Alsing, Justin; Mortlock, Daniel J.; Staehelin, Johannes; Haigh, Joanna D.; Peter, Thomas; Tummon, Fiona; Stuebi, Rene; Stenke, Andrea; Anderson, John;

Evidence for a continuous decline in lower stratospheric ozone offsetting ozone layer recovery

NASA Astrophysics Data System (ADS)

Ball, William T.; Alsing, Justin; Mortlock, Daniel J.; Staehelin, Johannes; Haigh, Joanna D.; Peter, Thomas; Tummon, Fiona; Stübi, Rene; Stenke, Andrea; Anderson, John; Bourassa, Adam; Davis, Sean M.; Degenstein, Doug; Frith, Stacey; Froidevaux, Lucien; Roth, Chris; Sofieva, Viktoria; Wang, Ray; Wild, Jeannette; Yu, Pengfei; Ziemke, Jerald R.; Rozanov, Eugene V.

2018-02-01

Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer-Dobson circulation (BDC), forming a protective ozone layer around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60° S and 60° N outside the polar regions (60-90°). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60° S and 60° N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60° S and 60° N. We find that total column ozone between 60° S and 60° N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.

Model sensitivity studies of the decrease in atmospheric carbon tetrachloride

DOE PAGES

Chipperfield, Martyn P.; Liang, Qing; Rigby, Matthew; ...

2016-12-20

Carbon tetrachloride (CCl 4) is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. But, the current observed rate of this decrease is known to be slower than expected based on reported CCl 4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl 4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (74 % ofmore » total), but a reported 10 % uncertainty in its combined photolysis cross section and quantum yield has only a modest impact on the modelled rate of CCl 4 decay. This is partly due to the limiting effect of the rate of transport of CCl 4 from the main tropospheric reservoir to the stratosphere, where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9 % of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (17 % of total) has the largest impact on modelled CCl 4 decay due to its sizeable contribution to CCl 4 loss and large lifetime uncertainty range (147 to 241 years). Furthermore, with an assumed CCl 4 emission rate of 39 Gg year -1, the reference simulation with the best estimate of loss processes still underestimates the observed CCl 4 (overestimates the decay) over the past 2 decades but to a smaller extent than previous studies. Changes to the rate of CCl 4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 47 Gg year -1. Further progress in constraining the CCl 4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the National Oceanic and Atmospheric Administration (NOAA) network are larger than from the Advanced Global Atmospheric Gases Experiment (AGAGE) network but have shown a steeper decreasing trend over the past 2 decades. The observed differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl 4 sinks.« less

Model sensitivity studies of the decrease in atmospheric carbon tetrachloride

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chipperfield, Martyn P.; Liang, Qing; Rigby, Matthew

Carbon tetrachloride (CCl 4) is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. But, the current observed rate of this decrease is known to be slower than expected based on reported CCl 4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl 4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (74 % ofmore » total), but a reported 10 % uncertainty in its combined photolysis cross section and quantum yield has only a modest impact on the modelled rate of CCl 4 decay. This is partly due to the limiting effect of the rate of transport of CCl 4 from the main tropospheric reservoir to the stratosphere, where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9 % of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (17 % of total) has the largest impact on modelled CCl 4 decay due to its sizeable contribution to CCl 4 loss and large lifetime uncertainty range (147 to 241 years). Furthermore, with an assumed CCl 4 emission rate of 39 Gg year -1, the reference simulation with the best estimate of loss processes still underestimates the observed CCl 4 (overestimates the decay) over the past 2 decades but to a smaller extent than previous studies. Changes to the rate of CCl 4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 47 Gg year -1. Further progress in constraining the CCl 4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the National Oceanic and Atmospheric Administration (NOAA) network are larger than from the Advanced Global Atmospheric Gases Experiment (AGAGE) network but have shown a steeper decreasing trend over the past 2 decades. The observed differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl 4 sinks.« less

Constraints on the photolysis and the equilibrium constant of ClO-dimer from airborne and balloon-borne measurements of chlorine compounds

NASA Astrophysics Data System (ADS)

Kleinboehl, A.; Canty, T. P.; Salawitch, R. J.; Khosravi, M.; Urban, J.; Toon, G. C.; Kuellmann, H.; Notholt, J.

2011-12-01

Significant differences exist between different laboratory measurements of the photolysis cross-sections of ClO-dimer, and the rate constant controlling the thermal equilibrium between ClO-dimer and ClO. This leads to uncertainties in the calculations of stratospheric ozone loss in the winter polar regions. One way to constrain the plausibility of these parameters is the measurement of ClO across the terminator in the activated polar vortex. Here we analyze measurements of ClO taken by the airborne submillimeter radiometer ASUR in the Arctic winter of 1999/2000. We use measured ClO at low solar zenith angles (SZA) to estimate the total active chlorine (ClOx). We estimate total available inorganic chlorine (Cly) using ASUR measurements of N2O in January 2000 and a N2O-Cly correlation established by a balloon measurement of the MarkIV interferometer in December 1999. We compare the ClOx estimates based on different photolysis rates of ClO-Dimer. Our results show that cross-sections leading to fast photolysis rates like the ones by Burkholder et al. [1990] or Papanastasiou et al. [2009] give ClOx mixing ratios that overlap with our estimated range of available Cly. Slower photolysis rates like the ones by von Hobe et al. [2009] and Pope et al. [2007] lead to ClOx values that are significantly higher than the available Cly. We use the calculated ClOx from low SZA to estimate the ClO in darkness with different equilibrium constants, and compare it with ASUR ClO measurements before sunrise (SZA > 95). We find that calculations with equilibrium constants published in the JPL evaluation of the last few years all give good agreement with observed ClO mixing ratios. The equilibrium constant estimated by von Hobe et al. [2005] yields ClO values that are higher than the ones observed.

Inclusion of the second Umkehr in the conventional Umkehr retrieval analysis as a means of improving ozone retrievals in the upper stratosphere

NASA Technical Reports Server (NTRS)

Gioulgkidis, Konstantinos; Lowe, Robert P.; Mcelroy, C. Tom

1994-01-01

The Umkehr method for retrieving the gross features of the vertical ozone distribution requires measurements of the ratio of zenith-sky radiances at two wavelengths in the near-UV region while the solar zenith angle (SZA) changes from 60 to 90 degrees. A Brewer spectrophotometer was used for taking such measurements extending the SZA range down to 96 degrees. Analyzed data from the Spring of 1991 imply that observations at twilight are of great significance in improving ozone retrievals in the upper stratosphere. Judged by the variance reduction for Umkehr layers 9 to 12 (25-30 percent for layer 11) and the increase in separation and amplitude of the averaging kernels for the relevant layers, the ozone retrievals in the upper stratosphere are shown to be in better agreement with climatological means.

Climatic changes in the troposphere, stratosphere and lower mesosphere in 1979-2016

NASA Astrophysics Data System (ADS)

Perevedentsev, Y. P.; Shantalinskiy, K. M.; Guryanov, V. V.

2018-01-01

Changes in thermal characteristics in the atmospheric layer from 1000 to 0,1hPa are studied based on reanalysis data. It was demonstrated that during 1979-2016 temperature increased in the troposphere in January and July, while cooling was observed in the stratosphere, and air warming in lower mesosphere in summer. Most pronounced long-period cyclic changes were registered for temperature in the upper stratosphere and the lower mesosphere, and for ozone mixing ratio in the middle stratosphere.

Theoretical Investigations of Clouds and Aerosols in the Stratosphere and Upper Troposphere

NASA Technical Reports Server (NTRS)

Toon, Owen B.

2005-01-01

support of the Atmospheric Chemistry Modeling and Data Analysis Program. We investigated a wide variety of issues involving ambient stratospheric aerosols, polar stratospheric clouds or heterogeneous chemistry, analysis of laboratory data, and particles in the upper troposphere. The papers resulting from these studies are listed below. In addition, I participated in the 1999-2000 SOLVE mission as one of the project scientists and in the 2002 CRYSTAL field mission as one of the project scientists. Several CU graduate students and research associates also participated in these mission, under support from the ACMAP program, and worked to interpret data. During the past few years my group has completed a number of projects under the

Interhemispheric comparison of atmospheric circulation features as evaluated from Nimbus satellite data. A comparison of the structure and flow characteristics of the upper troposphere and stratosphere of the Northern and Southern Hemispheres. Ph.D. Thesis. Annual Report, 1 Nov. 1973 - 31 Oct. 1974

NASA Technical Reports Server (NTRS)

Reiter, E. R.; Adler, R.; Fields, A.

1974-01-01

The general circulations of the Northern and Southern Hemispheres are compared with regard to the upper troposphere and stratosphere, using atmospheric structure obtained from multi-channel radiance data from the satellite infrared spectrometer instrument aboard the Nimbus 3 spacecraft. The inter-hemispheric comparisons are based on two months of data (one summer month and one winter month) in each hemisphere. Topics studied include: (1) mean meridional circulation in the Southern Hemisphere stratosphere; (2) magnitude and distribution of tropospheric eddy heat flux; (3) relative importance of standing and transient eddies in the two hemispheres; (4) magnitudes of energy cycle components; and (5) the relation of vortex structure to the breakdown climatology of the Antarctic stratospheric polar vortex.

STRATOSPHERIC TEMPERATURES AND WATER LOSS FROM MOIST GREENHOUSE ATMOSPHERES OF EARTH-LIKE PLANETS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kasting, James F.; Kopparapu, Ravi K.; Chen, Howard, E-mail: jfk4@psu.edu, E-mail: hwchen@bu.edu

A radiative-convective climate model is used to calculate stratospheric temperatures and water vapor concentrations for ozone-free atmospheres warmer than that of modern Earth. Cold, dry stratospheres are predicted at low surface temperatures, in agreement with recent 3D calculations. However, at surface temperatures above 350 K, the stratosphere warms and water vapor becomes a major upper atmospheric constituent, allowing water to be lost by photodissociation and hydrogen escape. Hence, a moist greenhouse explanation for loss of water from Venus, or some exoplanet receiving a comparable amount of stellar radiation, remains a viable hypothesis. Temperatures in the upper parts of such atmospheresmore » are well below those estimated for a gray atmosphere, and this factor should be taken into account when performing inverse climate calculations to determine habitable zone boundaries using 1D models.« less

Laboratory Studies of Homogeneous and Heterogeneous Chemical Processes of Importance in the Upper Atmosphere

NASA Technical Reports Server (NTRS)

Molina, Mario J.

2003-01-01

The objective of this study was to conduct measurements of chemical kinetics parameters for reactions of importance in the stratosphere and upper troposphere, and to study the interaction of trace gases with ice surfaces in order to elucidate the mechanism of heterogeneous chlorine activation processes, using both a theoretical and an experimental approach. The measurements were carried out under temperature and pressure conditions covering those applicable to the stratosphere and upper troposphere. The main experimental technique employed was turbulent flow-chemical ionization mass spectrometry, which is particularly well suited for investigations of radical-radical reactions.

Temperature Dependence of the O + HO2 Rate Coefficient

NASA Technical Reports Server (NTRS)

Nicovich, J. M.; Wine, P. H.

1997-01-01

A pulsed laser photolysis technique has been employed to investigate the kinetics of the radical-radical reaction O((sup 3)P) + HO2 OH + O2 over the temperature range 266-391 K in 80 Torr of N2 diluent gas. O((sup 3)P) was produced by 248.5-nm KrF laser photolysis of O3 followed by rapid quenching of O(1D) to O((sup 3)P) while HO2 was produced by simultaneous photolysis of H2O2 to create OH radicals which, in turn, reacted with H2O2 to yield HO2. The O((sup 3)P) temporal profile was monitored by using time-resolved resonance fluorescence spectroscopy. The HO2 concentration was calculated based on experimentally measured parameters. The following Arrhenius expression describes our experimental results: k(sub 1)(T) equals (2.91 +/- 0.70) x 10(exp -11) exp[(228 +/- 75)/T] where the errors are 2 sigma and represent precision only. The absolute uncertainty in k, at any temperature within the range 266-391 K is estimated to be +/- 22 percent. Our results are in excellent agreement with a discharge flow study of the temperature dependence of k(sub 1) in 1 Torr of He diluent reported by Keyser, and significantly reduce the uncertainty in the rate of this important stratospheric reaction at subambient temperatures.

The NASA program on upper atmospheric research

NASA Technical Reports Server (NTRS)

1976-01-01

The purpose of the NASA Upper Atmospheric Research Program is to develop a better understanding of the physical and chemical processes that occur in the earth's upper atmosphere with emphasis on the stratosphere.

21 Layer troposphere-stratosphere climate model

NASA Technical Reports Server (NTRS)

Rind, D.; Suozzo, R.; Lacis, A.; Russell, G.; Hansen, J.

1984-01-01

The global climate model is extended through the stratosphere by increasing the vertical resolution and raising the rigid model top to the 0.01 mb (75 km) level. The inclusion of a realistic stratosphere is necessary for the investigation of the climate effects of stratospheric perturbations, such as changes of ozone, aerosols or solar ultraviolet irradiance, as well as for studying the effect on the stratosphere of tropospheric climate changes. The observed temperature and wind patterns throughout the troposphere and stratosphere are simulated. In addition to the excess planetary wave amplitude in the upper stratosphere, other model deficiences include the Northern Hemisphere lower stratospheric temperatures being 5 to 10 C too cold in winter at high latitudes and the temperature at 50 to 60 km altitude near the equator are too cold. Methods of correcting these deficiencies are discussed.

Mass and Ozone Fluxes from the Lowermost Stratosphere

NASA Technical Reports Server (NTRS)

Schoeberl, Mark R.; Olsen, Mark A.

2004-01-01

Net mass flux from the stratosphere to the troposphere can be computed from the heating rate along the 380K isentropic surface and the time rate of change of the mass of the lowermost stratosphere (the region between the tropopause and the 380K isentrope). Given this net mass flux and the cross tropopause diabatic mass flux, the residual adiabatic mass flux across the tropopause can also be estimated. These fluxes have been computed using meteorological fields from a free-running general circulation model (FVGCM) and two assimilation data sets, FVDAS, and UKMO. The data sets tend to agree that the annual average net mass flux for the Northern Hemisphere is about 1P10 kg/s. There is less agreement on the southern Hemisphere flux that might be half as large. For all three data sets, the adiabatic mass flux is computed to be from the upper troposphere into the lowermost stratosphere. This flux will dilute air entering from higher stratospheric altitudes. The mass fluxes are convolved with ozone mixing ratios from the Goddard 3D CTM (which uses the FVGCM) to estimate the cross-tropopause transport of ozone. A relatively large adiabatic flux of tropospheric ozone from the tropical upper troposphere into the extratropical lowermost stratosphere dilutes the stratospheric air in the lowermost stratosphere. Thus, a significant fraction of any measured ozone STE may not be ozone produced in the higher Stratosphere. The results also illustrate that the annual cycle of ozone concentration in the lowermost stratosphere has as much of a role as the transport in the seasonal ozone flux cycle. This implies that a simplified calculation of ozone STE mass from air mass and a mean ozone mixing ratio may have a large uncertainty.

Rate constant for the fraction of atomic chlorine with formaldehyde from 200 to 500K

NASA Technical Reports Server (NTRS)

Michael, J. V.; Nava, D. F.; Payne, W. A.; Stief, L. J.

1978-01-01

A flash photolysis - resonance fluorescence technique was used to measure rate constant. The results were independent of substantial variations in H2CO, total pressure (Ar), and flash intensity (i.e., initial Cl). The rate constant was shown to be invariant with temperature, the best representation for this temperature range being K = (7.48 + or - 0.50) x 10 to the minus 11 power cu cm molecule-1 s-1 where the error is one standard deviation. The rate constant is theoretically discussed and the potential importance of the reaction in stratospheric chemistry is considered.

Long-term tropospheric and lower stratospheric ozone variations from ozonesonde observations

NASA Technical Reports Server (NTRS)

London, J.; Liu, S. C.

1992-01-01

An analysis is presented of the long-term mean pressure-latitude seasonal distribution of tropospheric and lower stratospheric ozone for the four seasons covering, in part, over 20 years of ozonesonde data. The observed patterns show minimum ozone mixing ratios in the equatorial and tropical troposphere except in regions where net photochemical production is dominant. In the middle and upper troposphere, and low stratosphere to 50 mb, ozone increases from the tropics to subpolar latitudes of both hemispheres. In mid stratosphere, the ozone mixing ratio is a maximum over the tropics. The observed vertical ozone gradient is small in the troposphere but increases rapidly above the tropopause. The amplitude of the annual variation increases from a minimum in the tropics to a maximum in polar regions. Also, the amplitude increases with height at all latitudes up to about 30 mb where the phase of the annual variation changes abruptly. The phase of the annual variation is during spring in the boundary layer, summer in mid troposphere, and spring in the upper troposhere and lower stratosphere.

Simultaneous Observations fo Polar Stratospheric Clouds and HNO3 over Scandinavia in January, 1992

NASA Technical Reports Server (NTRS)

Massie, S. T.; Santee, M. L.; Read, W. G.; Grainger, R. G.; Lambert, A.; Mergenthaler, J. L.; Dye, J. E.; Baumbardner, D.; Randel, W. J.; Tabazadeh, A.;

A laboratory study of the UV Absorption Spectrum of the ClO Dimer (Cl2O2) and the Implications for Polar Stratospheric Ozone Depletion

NASA Astrophysics Data System (ADS)

Papanastasiou, D. K.; Papadimitriou, V. C.; Fahey, D. W.; Burkholder, J. B.

2009-12-01

Chlorine containing species play an important role in catalytic ozone depleting cycles in the Antarctic and Arctic stratosphere. The ClO dimer (Cl2O2) catalytic ozone destruction cycle accounts for the majority of the observed polar ozone loss. A key step in this catalytic cycle is the UV photolysis of Cl2O2. The determination of the Cl2O2 UV absorption spectrum has been the subject of several studies since the late 1980’s. Recently, Pope et al. (J. Phys. Chem. A, 111, 4322, 2007) reported significantly lower absorption cross sections for Cl2O2 for the atmospherically relevant wavelength region, >300 nm, than currently recommended for use in atmospheric models. If correct, the Pope et al. results would alter our understanding of the chemistry of polar ozone depletion significantly. In this study, the UV absorption spectrum and absolute cross sections of gas-phase Cl2O2 are reported for the wavelength range 200 - 420 nm at ~200 K. Sequential pulsed laser photolysis of various precursors were used to produce the ClO radical and Cl2O2 via the subsequent ClO + ClO + M reaction under static conditions. UV absorption spectra of the reaction mixture were measured using a diode array spectrometer after completion of the gas-phase radical chemistry. The spectral analysis utilized the observed isosbestic points, reaction stoichiometry, and chlorine mass balance to determine the UV spectrum and absolute cross section of Cl2O2. A complementary experimental technique similar to that used by Pope et al. was also used in this study. We obtained consistent Cl2O2 UV absorption spectra using the two different techniques. The Cl2O2 absorption cross sections for wavelengths in the 300 - 420 nm range were found to be in very good agreement with the values reported previously by Burkholder et al. (J. Phys. Chem. A, 94, 687, 1990) and significantly greater than the Pope et al. values in this atmospherically important wavelength region. A possible explanation for the disagreement with the Pope et al. study will be discussed. Finally, using the Cl2O2 UV cross sections reported in this work representative atmospheric photolysis rates along with a detailed analysis of estimated uncertainties will be presented. A conclusion from this work is that the Cl2O2 absorption cross section data obtained in this work is sufficient to adequately model the observed ozone losses in the Antarctic and Arctic stratosphere.

The annual cycle of stratospheric water vapor in a general circulation model

NASA Technical Reports Server (NTRS)

Mote, Philip W.

1995-01-01

The application of general circulation models (GCM's) to stratospheric chemistry and transport both permits and requires a thorough investigation of stratospheric water vapor. The National Center for Atmospheric Research has redesigned its GCM, the Community Climate Model (CCM2), to enable studies of the chemistry and transport of tracers including water vapor; the importance of water vapor to the climate and chemistry of the stratosphere requires that it be better understood in the atmosphere and well represented in the model. In this study, methane is carried as a tracer and converted to water; this simple chemistry provides an adequate representation of the upper stratospheric water vapor source. The cold temperature bias in the winter polar stratosphere, which the CCM2 shares with other GCM's, produces excessive dehydration in the southern hemisphere, but this dry bias can be ameliorated by setting a minimum vapor pressure. The CCM2's water vapor distribution and seasonality compare favorably with observations in many respects, though seasonal variations including the upper stratospheric semiannual oscillation are generally too small. Southern polar dehydration affects midlatitude water vapor mixing ratios by a few tenths of a part per million, mostly after the demise of the vortex. The annual cycle of water vapor in the tropical and northern midlatitude lower stratosphere is dominated by drying at the tropical tropopause. Water vapor has a longer adjustment time than methane and had not reached equilibrium at the end of the 9 years simulated here.

NASA upper atmosphere research program: Research summaries, 1990 - 1991. Report to the Congress and the Environmental Protection Agency

NASA Technical Reports Server (NTRS)

1992-01-01

The objectives, status, and accomplishments of the research tasks supported under the NASA Upper Atmosphere Research Program (UARP) are presented. The topics covered include the following: balloon-borne in situ measurements; balloon-borne remote measurements; ground-based measurements; aircraft-borne measurements; rocket-borne measurements; instrument development; reaction kinetics and photochemistry; spectroscopy; stratospheric dynamics and related analysis; stratospheric chemistry, analysis, and related modeling; and global chemical modeling.

New Measurements of Methyl Ethyl Ketone (MEK) Photolysis Rates and Their Relevance to Global Oxidative Capacity

NASA Astrophysics Data System (ADS)

Brewer, J.; Ravishankara, A. R.; Mellouki, A.; Fischer, E. V.; Kukui, A.; Véronique, D.; Ait-helal, W.; Leglise, J.; Ren, Y.

2017-12-01

Methyl ethyl ketone (MEK) is one of the most abundant ketones in the atmosphere. MEK can be emitted directly into the atmosphere from both anthropogenic and natural sources, and it is also formed during the gas-phase oxidation of volatile organic compounds (VOCs). MEK is lost via reaction with OH, photolysis and deposition to the surface. Similar to the other atmospheric ketones, the photolysis of MEK may represent a source of HOx (OH + HO2) radicals in the upper troposphere. The degradation of MEK also leads to the atmospheric formation of acetaldehyde and formaldehyde. This work presents a new analysis of the temperature dependence of MEK photolysis cross-sections and a quantification of MEK photolysis rates under surface pressures using the CNRS HELIOS outdoor atmospheric chamber (Chambre de simulation atmosphérique à irradiation naturelle d'Orléans; http://www.era-orleans.org/ERA-TOOLS/helios-project.html). Additionally, we use the GEOS-Chem 3-D CTM (version 10-01, www.geos-chem.org) to investigate the impact of these newly measured rates and cross-sections on the global distribution and seasonality of MEK, as well as its importance to the tropospheric oxidative capacity.

EOS Microwave Limb Sounder Observations of the Antarctic Polar Vortex Breakup in 2004

NASA Technical Reports Server (NTRS)

Manney, G. L.; Santee, M. L.; Livesey, N. J.; Froidevaux, L.; Read, W. G.; Pumphrey, H. C.; Waters, J. W.; Pawson, S.

2005-01-01

Observations from the Microwave Limb Sounder (MLS) on NASA's new Aura satellite give an unprecedentedly detailed picture of the spring Antarctic polar vortex breakup throughout the stratosphere. HCl is a particularly valuable tracer in the lower stratosphere after chlorine deactivation. MLS HCl, N2O, H2O broke up in the upper stratosphere by early October, in the midstratosphere by early November, and in the lower stratosphere by late December. The subvortex broke up just a few days later than the lower stratospheric vortex. Vortex remnants persisted in the midstratosphere through December, but only through early January 2005 in the lower stratosphere. MLS N2O observations show diabatic descent continuing throughout November, with evidence of weak ascent after late October in the lower stratospheric vortex core.

A comparison of the momentum budget in reanalysis datasets during sudden stratospheric warming events

NASA Astrophysics Data System (ADS)

Martineau, Patrick; Son, Seok-Woo; Taguchi, Masakazu; Butler, Amy H.

2018-05-01

The agreement between reanalysis datasets, in terms of the zonal-mean momentum budget, is evaluated during sudden stratospheric warming (SSW) events. It is revealed that there is a good agreement among datasets in the lower stratosphere and troposphere concerning zonal-mean zonal wind, but less so in the upper stratosphere. Forcing terms of the momentum equation are also relatively similar in the lower atmosphere, but their uncertainties are typically larger than uncertainties of the zonal-wind tendency. Similar to zonal-wind tendency, the agreement among forcing terms is degraded in the upper stratosphere. Discrepancies among reanalyses increase during the onset of SSW events, a period characterized by unusually large fluxes of planetary-scale waves from the troposphere to the stratosphere, and decrease substantially after the onset. While the largest uncertainties in the resolved terms of the momentum budget are found in the Coriolis torque, momentum flux convergence also presents a non-negligible spread among the reanalyses. Such a spread is reduced in the latest reanalysis products, decreasing the uncertainty of the momentum budget. It is also found that the uncertainties in the Coriolis torque depend on the strength of SSW events: the SSW events that exhibit the most intense deceleration of zonal-mean zonal wind are subject to larger discrepancies among reanalyses. These uncertainties in stratospheric circulation, however, are not communicated to the troposphere.

Dependence of upper atmosphere photochemistry on the shape of the diurnal cycle of the photolysis rates

NASA Astrophysics Data System (ADS)

Montecinos, S.; Barrientos, P.

2006-03-01

A photochemical model of the atmosphere constitutes a non-linear, non-autonomous dynamical system, enforced by the Earth's rotation. Some studies have shown that the region of the mesopause tends towards non-linear responses such as period-doubling cascades and chaos. In these studies, simple go approximations for the diurnal variations of the photolysis rates are assumed. The goal of this article is to investigate what happens if the more realistic, calculated photolysis rates are introduced. It is found that, if the usual approximations-sinusoidal and step functions-are assumed, the responses of the system are similar: it converges to a 2-day periodic solution. If the more realistic, calculated diurnal cycle is introduced, a new 4-day subharmonic appear.

Linkages Between Ozone-depleting Substances, Tropospheric Oxidation and Aerosols

NASA Technical Reports Server (NTRS)

Voulgarakis, A.; Shindell, D. T.; Faluvegi, G.

2013-01-01

Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (-22.6mW/sq. m for CFCs and -6.7mW/sq. m for N2O) and sulfate aerosols (-3.0mW/sq. m for CFCs and +6.5mW/sq. m for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

CFCI3 (CFC-11): UV Absorption Spectrum Temperature Dependence Measurements and the Impact on Atmospheric Lifetime and Uncertainty

NASA Technical Reports Server (NTRS)

Mcgillen, Max R.; Fleming, Eric L.; Jackman, Charles H.; Burkholder, James B.

2014-01-01

CFCl3 (CFC-11) is both an atmospheric ozone-depleting and potent greenhouse gas that is removed primarily via stratospheric UV photolysis. Uncertainty in the temperature dependence of its UV absorption spectrum is a significant contributing factor to the overall uncertainty in its global lifetime and, thus, model calculations of stratospheric ozone recovery and climate change. In this work, the CFC-11 UV absorption spectrum was measured over a range of wavelength (184.95 - 230 nm) and temperature (216 - 296 K). We report a spectrum temperature dependence that is less than currently recommended for use in atmospheric models. The impact on its atmospheric lifetime was quantified using a 2-D model and the spectrum parameterization developed in this work. The obtained global annually averaged lifetime was 58.1 +- 0.7 years (2 sigma uncertainty due solely to the spectrum uncertainty). The lifetime is slightly reduced and the uncertainty significantly reduced from that obtained using current spectrum recommendations

DUSTER: collection of meteoric CaO and carbon smoke particles in the upper stratosphere .

NASA Astrophysics Data System (ADS)

Della Corte, V.; Rietmeijer, F. J. M.; Rotundi, A.; Ferrari, M.; Palumbo, P.

Nanometer- to micrometer-size particles present in the upper stratosphere are a mixture of terrestrial and extra-terrestrial origins. They can be extraterrestrial particles condensed after meteor ablation. Meteoric dust in bolides is occasionally deposited into the lower stratosphere around 20 km altitude. Nanometer CaO and pure carbon smoke particles were collected at 38 km altitude in the upper stratosphere in the Arctic during June 2008 using DUSTER (Dust in the Upper Stratosphere Tracking Experiment and Retrieval), a balloon-borne instrument for the non-destructive collection of solid particles between 200 nm to 40 microns. We report the collection of micron sized CaCO_3 (calcite) grains. Their morphologies show evidence of melting and condensation after vaporization suggest at temperatures of approximately 3500 K. The formation environment of the collected grains was probably a dense dust cloud formed by the disintegration of a carbonaceous meteoroid during deceleration in the Earth� atmosphere. For the first time, DUSTER collected meteor ablation products that were presumably associated with the disintegration of a bolide crossing the Earth's atmosphere. The collected mostly CaO and pure carbon nanoparticles from the debris cloud of a fireball, included: 1) intact fragments; 2) quenched melted grains; and 3) vapor phase condensation products. The DUSTER project was funded by the Italian Space Agency (ASI), PRIN2008/MIUR (Ministero dell'Istruzione dell'Universitá e della Ricerca), PNRA 2013(Piano Nazionale Ricerca Antartide). CNES graciously provided this flight opportunity. We thank E. Zona and S. Inarta at the Laboratorio di Fisica Cosmica INAF, Osservatorio Astronomico di Capodimonte-Universitá di Napoli Parthenope. F.J.M.R. was supported by grant NNX07AI39G from the NASA Cosmochemistry Program. We thank three anonymous reviewers who assisted us in introducing our new instrument.

Decomposing variations of geopotential height in the troposphere and stratosphere into stationary and travelling waves

NASA Astrophysics Data System (ADS)

Guryanov, Vladimir; Eliseev, Alexey

2016-07-01

The ERA-Interim geopotential height in the Northern Hemisphere from November to March, 1992-2015 in the layer from between pressure levels 1000 mb and 1 mb is expanded into stationary and travelling zonal waves with zonal wavenumbers, k, from 1 to 10, and with periods, T, from 2 to 156 days (the so called Hayashi spectra). Among the studied waves, the largest amplitude is attained by the stationary and travelling waves with zonal wavenumber k=1 and with periods from 3 to 4 weeks in the upper stratosphere over the latitudinal belt 60-70oN. The stationary waves with k from 1 to 3 and with T from 2 to 3 weeks are most pronounced in the stratosphere. In turn, the largest amplitudes of the travelling waves with zonal wavenumbers k ≥ 5 are found in the troposphere. The dominant periods of the latter waves are about 1 week or slightly higher, and this dominant period basically decrease with increasing wavenumber. In the upper stratosphere, the eastward travelling waves generally dominate over westward ones. The only exception is the longest zonal mode with k=1, for which the amplitude of the westward travelling wave is larger than that for the eastward one. The period of the travelling waves dominating in the upper stratosphere is close to 3 weeks. In the upper troposphere, the amplitudes of the eastward waves with k from 4 to 10 is several-fold larger than those for their westward counterparts. The latter is reflected in the larger average wavenumber of the eastward travelling wave in comparison to that of the westarward one. The period of the gravest of the dominant travelling waves in the upper troposphere is close to one week, and it decreases to 2-4 days for the dominant travelling waves with k=8-10.

Water vapor and cloud water measurements over Darwin during the STEP 1987 tropical mission

NASA Technical Reports Server (NTRS)

Kelly, K. K.; Proffitt, M. H.; Chan, K. R.; Loewenstein, M.; Podolske, J. R.; Strahan, E.; Wilson, J. C.; Kley, D.

1993-01-01

Measurements of stratospheric and upper tropospheric cloud water plus water vapor (total water) and water vapor were made with two Lyman alpha hygrometers as part of the STEP tropical experiment. The in situ measurements were made in the Darwin, Australia, area in January and February of 1987 on an ER-2 aircraft. Average stratospheric water vapor at a potential temperature of 375 K (the average value of Theta at the tropopause) was 2.4 parts per million by volume (ppmv). This water mixing ratio is below the 3.0 to 4.0 ppmv necessary to be consistent with the observed upper stratospheric dryness. Saturation with respect to ice and the potential for dehydration was observed up to Theta = 402 K.

Stratospheric Temperature Trends Observed by TIMED/SABER

NASA Astrophysics Data System (ADS)

Xian, T.; Tan, R.

2017-12-01

Trends in the stratospheric temperature are studied based on the temperature profile observation from the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER). The spatially trends are evaluated in different time scales ranging from decadal to monthly resolved. The results indicate a signature of BDC acceleration. There are strong warming trends (up to 9 K/decade) in the middle to upper stratosphere in the high latitude spring, summer, and autumn seasons, accompanied by strong cooling trends in the lower stratosphere. Besides, strong warming trends occurs through the whole stratosphere over the Southern Hemisphere, which confirms Antarctic ozone layer healing since 2000. In addition, the results demonstrate a significant warming trends in the middle of tropical stratosphere, which becomes strongest during June-July-August.

Stratospheric nitrogen dioxide in the vicinity of soufriere, st. Vincent.

PubMed

Romick, G J; Murcray, D G; Williams, W J

1982-06-04

In April 1979, measurements of nitrogen dioxide in the upper atmosphere were made near Soufriere Volcano by twilight optical-absorption techniques. The derived value of 5 x 10(15) molecules per square centimeter column implies an enhancement of 25 percent over earlier abundances measured in the same latitudinal regions. This enhancement may represent the normal stratospheric variability of nitrogen dioxide in the equatorial region but in any case may be considered an upper limit to the volcano's effect on the total nitrogen dioxide abundance.

Total Hydrogen Budget of the Equatorial Upper Stratosphere

DTIC Science & Technology

2010-02-24

series show quasi- biennial ( QBO ) variations which peak near 2.2 hPa in the equatorial upper stratosphere due to the large vertical gradients in CH4...Cordero et al., 1997] and directly relate to the observed QBO variations in H2O through CH4 oxidation. An increase in H2O mixing ratios during the early...by calculating the amplitudes of the QBO , annual, and semiannual cycles as function of pressure determined by a least squares regression fit to the

Tiny Ultraviolet Polarimeter for Earth Stratosphere from Space Investigation

NASA Astrophysics Data System (ADS)

Nevodovskyi, P. V.; Morozhenko, O. V.; Vidmachenko, A. P.; Ivakhiv, O.; Geraimchuk, M.; Zbrutskyi, O.

2015-09-01

One of the reasons for climate change (i.e., stratospheric ozone concentrations) is connected with the variations in optical thickness of aerosols in the upper sphere of the atmosphere (at altitudes over 30 km). Therefore, aerosol and gas components of the atmosphere are crucial in the study of the ultraviolet (UV) radiation passing upon the Earth. Moreover, a scrupulous study of aerosol components of the Earth atmosphere at an altitude of 30 km (i.e., stratospheric aerosol), such as the size of particles, the real part of refractive index, optical thickness and its horizontal structure, concentration of ozone or the upper border of the stratospheric ozone layer is an important task in the research of the Earth climate change. At present, the Main Astronomical Observatory of the National Academy of Sciences (NAS) of Ukraine, the National Technical University of Ukraine "KPI"and the Lviv Polytechnic National University are engaged in the development of methodologies for the study of stratospheric aerosol by means of ultraviolet polarimeter using a microsatellite. So fare, there has been created a sample of a tiny ultraviolet polarimeter (UVP) which is considered to be a basic model for carrying out space experiments regarding the impact of the changes in stratospheric aerosols on both global and local climate.

Space Shuttle Projects

NASA Image and Video Library

1992-09-12

This STS-48 onboard photo is of the Upper Atmosphere Research Satellite (UARS) in the grasp of the RMS (Remote Manipulator System) during deployment, September 1991. UARS gathers data related to the chemistry, dynamics, and energy of the ozone layer. UARS data is used to study energy input, stratospheric photo chemistry, and upper atmospheric circulation. UARS helps us understand and predict how the nitrogen and chlorine cycles, and the nitrous oxides and halo carbons which maintain them, relate to the ozone balance. It also observes diurnal variations in short-lived stratospheric chemical species important to ozone destruction. Data from UARS enables scientists to study ozone depletion in the upper atmosphere.

Space Shuttle Projects

NASA Image and Video Library

1991-09-12

This STS-48 onboard photo is of the Upper Atmosphere Research Satellite (UARS) in the grasp of the RMS (Remote Manipulator System) during deployment, September 1991. UARS gathers data related to the chemistry, dynamics, and energy of the ozone layer. UARS data is used to study energy input, stratospheric photo chemistry, and upper atmospheric circulation. UARS helps us understand and predict how the nitrogen and chlorine cycles, and the nitrous oxides and halo carbons which maintain them, relate to the ozone balance. It also observes diurnal variations in short-lived stratospheric chemical species important to ozone destruction. Data from UARS enables scientists to study ozone depletion in the upper atmosphere.

Static Stability in the Global Upper Troposphere and Lower Stratosphere: Observations of Long-term Mean Structure and Variability using GPS Radio Occultation Data

NASA Astrophysics Data System (ADS)

Grise, K. M.; Thompson, D. W.; Birner, T.

2009-12-01

Static stability is a fundamental dynamical quantity that measures the vertical temperature stratification of the atmosphere. The long-term mean static stability field is characterized by the well-known transition from low values in the troposphere to high values in the stratosphere. However, the magnitude and structure of fine-scale static stability features near the tropopause are difficult to discern in temperature data with low vertical resolution. In this study, the authors apply over six years of high vertical resolution Global Positioning System radio occultation temperature profiles to document the long-term mean structure and variability of static stability in the global upper troposphere and lower stratosphere (UTLS). The results of this study demonstrate that a shallow but pronounced maximum in static stability exists just above the tropopause at all latitudes (i.e., the “tropopause inversion layer,” or TIL). This study also uncovers two novel aspects of static stability in the global UTLS. In the tropical lower stratosphere, the results reveal a unique vertically and horizontally varying static stability structure, with maxima located at ~17 km and ~19 km. The upper feature peaks during the NH cold season and has its largest magnitude between 10 and 15 degrees latitude in both hemispheres; the lower feature exhibits a weaker seasonal cycle and is centered at the Equator. The results also demonstrate that the strength of the TIL is closely tied to stratospheric dynamic variability. The magnitude of the TIL is enhanced following sudden stratospheric warmings in the polar regions and the easterly phase of the quasi-biennial oscillation in the tropics.

Static Stability in the Global Upper Troposphere and Lower Stratosphere: Observations of Long-term Mean Structure and Variability using GPS Radio Occultation Data

NASA Astrophysics Data System (ADS)

Grise, Kevin M.; Thompson, David W. J.; Birner, Thomas

2010-05-01

Static stability is a fundamental dynamical quantity that measures the vertical temperature stratification of the atmosphere. The long-term mean static stability field is characterized by the well-known transition from low values in the troposphere to high values in the stratosphere. However, the magnitude and structure of fine-scale static stability features near the tropopause are difficult to discern in temperature data with low vertical resolution. In this study, the authors apply over six years of high vertical resolution Global Positioning System radio occultation temperature profiles to document the long-term mean structure and variability of static stability in the global upper troposphere and lower stratosphere (UTLS). The results of this study demonstrate that a shallow but pronounced maximum in static stability exists just above the tropopause at all latitudes (i.e., the "tropopause inversion layer," or TIL). This study also uncovers two novel aspects of static stability in the global UTLS. In the tropical lower stratosphere, the results reveal a unique vertically and horizontally varying static stability structure, with maxima located at ~17 km and ~19 km. The upper feature peaks during the NH cold season and has its largest magnitude between 10 and 15 degrees latitude in both hemispheres; the lower feature exhibits a weaker seasonal cycle and is centered at the Equator. The results also demonstrate that the strength of the TIL is closely tied to stratospheric dynamic variability. The magnitude of the TIL is enhanced following sudden stratospheric warmings in the polar regions and the easterly phase of the quasi-biennial oscillation in the tropics.

Space-time patterns of trends in stratospheric constituents derived from UARS measurements

NASA Astrophysics Data System (ADS)

Randel, William J.; Wu, Fei; Russell, James M.; Waters, Joe

1999-02-01

The spatial and temporal behavior of low-frequency changes (trends) in stratospheric constituents measured by instruments on the Upper Atmosphere Research Satellite (UARS) during 1991-98 is investigated. The data include CH4, H2O, HF, HCl, O3, and NO2 from the Halogen Occultation Experiment (HALOE), and O3, ClO, and HNO3 from the Microwave Limb Sounder (MLS). Time series of global anomalies are analyzed by linear regression and empirical orthogonal function analysis. Each of the constituents show significant linear trends over at least some region of the stratosphere, and the spatial patterns exhibit coupling between the different species. Several of the constituents (namely CH4, H2O, HF, HCl, O3, and NO2) exhibit a temporal change in trend rates, with strong changes prior to 1996 and weaker (or reversed) trends thereafter. Positive trends are observed in upper stratospheric ClO, with a percentage rate during 1993-97 consistent with stratospheric HCl increases and with tropospheric chlorine emission rates. Significant negative trends in ozone in the tropical middle stratosphere are found in both HALOE and MLS data during 1993-97, together with positive trends in the tropics near 25 km. These trends are very different from the decadal-scale ozone trends observed since 1979, and this demonstrates the variability of trends calculated over short time periods. Positive trends in NO2 are found in the tropical middle stratosphere, and spatial coincidence to the observed ozone decreases suggests the ozone is responding to the NO2 increase. Significant negative trends in HNO3 are found in the lower stratosphere of both hemispheres. These coupled signatures offer a fingerprint of chemical evolution in the stratosphere for the UARS time frame.

Titan. [Voyager IRIS observation of satellite atmosphere

NASA Technical Reports Server (NTRS)

Lunine, Jonathan I.

1990-01-01

Saturn's satellite Titan is the second-largest in the solar system. Its dense atmosphere is mostly molecular nitrogen with an admixture of methane, a surface pressure of 1.5 bars and a surface temperature of 94K. The fundamental driving force in the long-term evolution of Titan's atmosphere is the photolysis of methane in the stratosphere to form higher hydrocarbons and aerosols. The current rate of photolysis and undersaturation of methane in the lower troposphere suggests the presence of a massive ethane-methane-nitrogen ocean. The ocean evolves to a more ethane-rich state over geologic time, driving changes in the atmospheric thermal structure. An outstanding issue concerning Titan's earliest history is the origin of atmospheric nitrogen: was it introduced into Titan as molecular nitrogen or ammonia? Measurement of the argon-to-nitrogen ratio in the present atmosphere provides a diagnostic test of these competing hypotheses. Many of the questions raised by the Voyager encounters about Titan and its atmosphere can be adequately addressed only by an entry probe, such as that planned for the Cassini mission.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wuebbles, D.J.; Kinnison, D.E.; Lean, J.L.

Over the past decade, knowledge of the magnitude and temporal structure of the variations in the sun's ultraviolet irradiance has increased steadily. A number of theoretical modeling studies have shown that changes in the solar ultraviolet flux during the 11-year solar cycle can have a significant effect on stratospheric ozone concentrations. With the exception of Brasseur et al., who examined a very broad range of solar flux variations, all of these studies assumed much larger changes in the ultraviolet flux than measurements now indicate. These studies either calculated the steady-state effect at solar maximum and solar minimum or assumed sinusoidalmore » variations in the solar flux changes with time. It is now possible to narrow the uncertainty range of the expected effects on upper stratospheric ozone and temperature resulting from the 11-year solar cycle. A more accurate representation of the solar flux changes with time is used in this analysis, as compared to previous published studies. This study also evaluates the relative roles of solar flux variations and increasing concentrations of long-lived trace gases in determining the observed trends in upper stratospheric ozone and temperature. The LLNL two-dimensional chemical-radiative-transport model of the global atmosphere is used to evaluate the combined effects on the stratosphere from changes in solar ultraviolet irradiances and trace gas concentrations over the last several decades. Derived trends in upper stratospheric ozone concentrations and temperature are then compared with available analyses of ground-based and satellite measurements over this time period.« less

Present State of Knowledge of the Upper Atmosphere 1996: An Assessment Report to Congress and the Environmental Protection Agency

NASA Technical Reports Server (NTRS)

Kurylo, M. J.; Kaye, J. A.; Decola, P. L.; Friedl, R. R.; Peterson, D. B.

1997-01-01

This document is issued in response to the Clean Air Act Amendment of 1990, Public Law 101-549, which mandates that the National Aeronautics and Space Administration (NASA) and other key agencies submit triennial report to congress and the Environmental Protection Agency. NASA is charged with the responsibility to report on the state of our knowledge of the Earth's upper atmosphere, particularly the Stratosphere. Part 1 of this report summarizes the objectives, status, and accomplishments of the research tasks supported under NASA's Upper Atmosphere Research Program and Atmospheric Chemistry Modeling and Analysis Program for the period of 1994-1996. Part 2 (this document) presents summaries of several scientific assessments, reviews, and summaries. These include the executive summaries of two scientific assessments: (Section B) 'Scientific Assessment of Ozone Depletion: 1994'; (Section C) 'l995 Scientific Assessment of the Atmospheric Effects of Stratospheric Aircraft); end of mission/series statements for three stratospherically-focused measurement campaigns: (Section D) 'ATLAS End-of-Series Statement'; (Section E) 'ASHOE/MAESA End-of-Mission Statement'; (Section F) 'TOTE/VOTE End-of-Mission Statement'; a summary of NASA's latest biennial review of fundamental photochemical processes important to atmospheric chemistry 'Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling'; and (Section H) the section 'Atmospheric Ozone Research" from the Mission to Planet Earth Science Research Plan, which describes NASA's current and future research activities related to both tropospheric and stratospheric chemistry.

The fate of atmospheric phosgene and the stratospheric chlorine loadings of its parent compounds: CCl4, C2Cl4, C2HCL3, CH3CCl3, and CHCl3

NASA Technical Reports Server (NTRS)

Kindler, T. P.; Chameides, W. L.; Wine, P. H.; Cunnold, D. M.; Alyea, F. N.; Franklin, J. A.

1995-01-01

A study of the tropospheric and stratospheric cycles of phosgene is carried out to determine its fate and ultimate role in controlling the ozone depletion potentials of its parent compounds. Tropospheric phosgene is produced from the OH-initiated oxidation of C2Cl4, CH3CCl3, CHCl3, and C2HCl3. Simulations using a two-dimensional model indicate that these processes produce about 90 pptv/yr of tropospheric phosgene with an average concentration of about 18 pptv, in reasonable agreement with observations. We estimate a residence time of about 70 days for tropospheric phosgene, with the vast majority being removed by hydrolysis in cloudwater. Only about 0.4% of the phosgene produced in the troposphere avoids wet removal and is transported to the stratosphere, where its chlorine can be released to participate in the catalytic destruction of ozone. Stratospheric phosgene is produced from the photochemical degradation of CCl4, C2Cl4, CHCl3, and CH3CCl3 and is removed by photolysis and downward transport to the troposphere. Model calculations, in good agreement with observations, indicate that these processes produce a peak stratospheric concentration of about 25-30 pptv at an altitude of about 25 km. In contrast to tropospheric phosgene, stratospheric phosgene is found to have a lifetime against photochemical removal of the order of years. As a result, a significant portion of the phosgene that is produced in the stratosphere is ultimately returned to the troposphere, where it is rapidly removed by clouds. This phenomenon effectively decreases the amount of reactive chlorine injected into the stratosphere and available for ozone depletion from phosgene's parent compounds. A similar phenomenon due to the downward transport of stratospheric COFCl produced from CFC-11 is estimated to cause a 7% decrease in the amount of reactive chlorine injected into the stratosphere from this compound. Our results are potentially sensitive to a variety of parameters, most notably the rate of reaction of phosgene with sulfate aerosols. However, on the basis of the observed vertical distribution of COCl2, we estimate that the reaction of COCl2 with sulfate aerosol most likely has a gamma less than 5 x 10(exp -5) and, as a result, has a negligible impact on the stratospheric chlorine loadings of the phosgene parent compounds.

Photochemistry, mixing and transport in Jupiter's stratosphere constrained by Cassini

NASA Astrophysics Data System (ADS)

Hue, V.; Hersant, F.; Cavalié, T.; Dobrijevic, M.; Sinclair, J. A.

2018-06-01

In this work, we aim at constraining the diffusive and advective transport processes in Jupiter's stratosphere, using Cassini/CIRS observations published by Nixon et al. (2007,2010). The Cassini-Huygens flyby of Jupiter on December 2000 provided the highest spatially resolved IR observations of Jupiter so far, with the CIRS instrument. The IR spectrum contains the fingerprints of several atmospheric constituents and allows probing the tropospheric and stratospheric composition. In particular, the abundances of C2H2 and C2H6, the main compounds produced by methane photochemistry, can be retrieved as a function of latitude in the pressure range at which CIRS is sensitive to. CIRS observations suggest a very different meridional distribution for these two species. This is difficult to reconcile with their photochemical histories, which are thought to be tightly coupled to the methane photolysis. While the overall abundance of C2H2 decreases with latitude, C2H6 becomes more abundant at high latitudes. In this work, a new 2D (latitude-altitude) seasonal photochemical model of Jupiter is developed. The model is used to investigate whether the addition of stratospheric transport processes, such as meridional diffusion and advection, are able to explain the latitudinal behavior of C2H2 and C2H6. We find that the C2H2 observations are fairly well reproduced without meridional diffusion. Adding meridional diffusion to the model provides an improved agreement with the C2H6 observations by flattening its meridional distribution, at the cost of a degradation of the fit to the C2H2 distribution. However, meridional diffusion alone cannot produce the observed increase with latitude of the C2H6 abundance. When adding 2D advective transport between roughly 30 mbar and 0.01 mbar, with upwelling winds at the equator and downwelling winds at high latitudes, we can, for the first time, reproduce the C2H6 abundance increase with latitude. In parallel, the fit to the C2H2 distribution is degraded. The strength of the advective winds needed to reproduce the C2H6 abundances is particularly sensitive to the value of the meridional eddy diffusion coefficient. The coupled fate of these methane photolysis by-products suggests that an additional process is missing in the model. Ion-neutral chemistry was not accounted for in this work and might be a good candidate to solve this issue.

Upper-Level Waves of Synoptic Scale at Midlatitudes

NASA Astrophysics Data System (ADS)

Rivest, Chantal

1990-01-01

Upper-level waves of synoptic scale are important dynamical entities at midlatitudes. They often induce surface cyclogenesis (cf. Peterssen and Smebye, 1971), and their life duration is typically longer than time scales for disruption by the ambient shear (Sanders, 1988). The objectives of the present thesis are to explain the maintenance and genesis of upper-level synoptic-scale waves in the midlatitude flow. We develop an analytical model of waves on generalized Eady basic states that have uniform tropospheric and stratospheric potential vorticity, but allow for the decay of density with height. The Eady basic state represents the limiting case of infinite stratospheric stability and constant density. We find that the Eady normal mode characteristics hold in the presence of realistic tropopause and stratosphere. In particular, the basic states studied support at the synoptic scale upper-level normal modes. These modes provide simple models for the dynamics of upper-level synoptic-scale waves, as waves supported by the large latitudinal gradients of potential vorticity at the tropopause. In the presence of infinitesimal positive tropospheric gradients of potential vorticity, the upper-level normal mode solutions no longer exist, as was demonstrated in Green (1960). Disappearance of the normal mode solution when a parameter changes slightly represents a dilemma that we seek to understand. We examine what happens to the upper-level normal modes in the presence of tropospheric gradients of potential vorticity in a series of initial -value experiments. Our results show that the normal modes become slowly decaying quasi-modes. Mathematically the quasi-modes consist of a superposition of singular modes sharply peaked in the phase speed domain, and their decay proceeds as the modes interfere with one another. We repeat these experiments in basic states with a smooth tropopause in the presence of tropospheric and stratospheric gradients, and similar results are obtained. Basic states with positive tropospheric and stratospheric gradients of potential vorticity are found to support upper-level synoptic-scale waves for time scales consistent with observations. Following Farrell (1989), we then identify a class of near optimal initial conditions for the excitation of upper-level waves. The initial conditions consist of upper -tropospheric disturbances that lean against the shear. They strongly excite upper-level waves not only in the absence of tropospheric potential vorticity gradients, but also in their presence. This result demonstrates that quasi -modes are as likely to emerge from favorably configured initial conditions as real normal modes, although their excitation is followed by a slow decay. (Copies available exclusively from MIT Libraries, Rm. 14-0551, Cambridge, MA 02139-4307. Ph. 617-253-5668; Fax 617-253-1690.).

Stratospheric cooling and downward planetary-wave propagation in the lowermost stratosphere during the 2010-11 winter

NASA Astrophysics Data System (ADS)

Nishii, K.; Nakamura, H.; Orsolini, Y. J.

2012-04-01

Dynamical cooling in the polar stratosphere is induced by weakening of E-P flux convergence (i.e. anomalous divergence) in the stratosphere. As the E-P flux convergence is mainly contributed to by upward planetary-wave (PW) propagation from the troposphere, the intensity of its propagation is well correlated with the E-P flux convergence and the polar stratospheric temperature. Recent studies (Orsolini et al. 2009, QJRMS; Nishii et al. 2010, GRL) pointed out that a tropospheric blocking high over the western Pacific, whose anomalous circulation is projected strongly onto the Western Pacific (WP) teleconnection pattern, tends to weaken the upward PW propagation and thus lower the polar stratospheric temperature. In this study, we present a possibility that downward PW propagation in the lowermost stratosphere can also cause the E-P flux divergence in the polar stratosphere and thereby the stratospheric cooling. On the basis of prominent downward events of the 100-hPa E-P flux averaged over the mid- to high-latitudes in the northern hemisphere, we performed a lag composite analysis for each of the terms of the transformed Eulerian mean (TEM) equation. In the composite time evolution, downward E-P flux in the lowermost stratosphere and the E-P flux divergence aloft are evident around the reference date, followed by persistent cooling of the polar stratosphere for more than two weeks. About one week before the reference date, enhanced upward E-P flux and its convergence lead to the deceleration of upper-stratospheric zonal winds and thus the weakening of their vertical shear , which may result in the formation of a turning surface for upward-propagating PWs. Our results are overall consistent with Harnik (2009, JGR), who showed that a short pulse of upward-propagating PWs forms a turning surface in the upper stratosphere, where the PWs that subsequently propagate upward can be reflected back. By taking above results into consideration, we analyzed the prolonged cold 2010-11 winter. We found that while three cooling events in December and January were accompanied by tropospheric WP pattern events, cooling in February and March was led by downward-propagating PW events.

Solar-induced oscillations in the stratosphere - A myth or reality?

NASA Technical Reports Server (NTRS)

Chandra, S.

1985-01-01

Chandra (1984) has provided an assessment of the solar cycle ozone relationship based on seven years of Nimbus 4 BUV (backscattered ultraviolet) data. It was found that the globally averaged ozone in the upper stratosphere, when corrected for the changes in instrument sensitivity, decreased from 1970 to 1976 by 3-4 percent. This decrease is in accordance with the current estimates of solar UV variability over a solar cycle. The present investigation has the objective to determine if measured changes in ozone and temperature in the upper stratosphere on a time scale of a solar rotation are of solar origin, i.e., directly induced by changes in solar irradiance. The conducted study is based on the first two years (1970-1972) of ozone and temperature data obtained from the Nimbus 4 BUV and the Selective Chopper Radiometer (SCR) experiments. Attention is given to the response of the stratosphere to changes in solar activity associated with the 27-day solar rotation.

Trends in aerosol abundances and distributions

NASA Technical Reports Server (NTRS)

Turco, R. P.; Mccormick, M. P.; Clancy, R. T.; Curran, R.; Deluisi, J.; Hamill, P.; Kent, G.; Rosen, J. M.; Toon, O. B.; Yue, G.

1989-01-01

The properties of aerosols that reside in the upper atmosphere are described. Special emphasis is given to the influence these aerosols have on ozone observation systems, mainly through radiative effects, and on ambient ozone concentrations, mainly through chemical effects. It has long been appreciated that stratospheric particles can interfere with the remote sensing of ozone distribution. The mechanism and magnitude of this interference are evaluated. Separate sections deal with the optical properties of upper atmospheric aerosols, long-term trends in stratospheric aerosols, perturbations of the stratospheric aerosol layer by volcanic eruptions, and estimates of the impacts that such particles have on remotely measured ozone concentrations. Another section is devoted to a discussion of the polar stratospheric clouds (PSC's). These unique clouds, recently discovered by satellite observation, are now thought to be intimately connected with the Antarctic ozone hole. Accordingly, interest in PSC's has grown considerably in recent years. This chapter describes what we know about the morphology, physical chemistry, and microphysics of PSC's.

Evidence of localized strong enhancements in lower stratospheric CH3CN following intense forest fire activity

NASA Technical Reports Server (NTRS)

Livesey, N.

2000-01-01

On 24 August 1992, the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite observed a significant enhancement in the abundance of lower stratospheric methyl cyanide at approximately 16-19 km in altitude in a small region off the coast of Florida. Concentrations of order 1400 parts per trillion by volume were observed, compared to a typical stratospheric background level of 30 pptv.

The Polar Mesopause Sulfate Aerosol Layer

NASA Astrophysics Data System (ADS)

Mills, M. J.; Toon, O. B.; Thomas, G.; Solomon, S.

2001-05-01

Noctilucent ("night-luminous") clouds (NLC), or as seen from space, Polar Mesospheric Clouds (PMC), are typically 1 to 2 km thick and located at altitudes of 80 to 85 km, where the temperature is near 150K. NLC generally occur between 50 degrees latitude to the pole from May to August in the Northern Hemisphere, with occasional sightings at lower latitudes. An extraordinary low-latitude sighting occurred on June 21, 1999 at 41oN. Direct evidence that PMC are composed of water ice was recently reported from satellite observations made in the near infrared. The formation of ice clouds in the upper atmosphere has been studied extensively as a result of the role of Polar Stratospheric Clouds (PSC) in polar ozone depletion. There exists ample evidence that preexisting stratospheric liquid sulfate aerosol plays an important role in the formation of solid PSC particles. Until recent laboratory measurements showed otherwise, however, it was believed that photolysis of sulfuric acid in the upper stratosphere would prevent the formation of such aerosol in the mesosphere. We present here calculations from a microphysical atmospheric model which point to sulfate from volcanic and non-volcanic sources alike as the origin of nuclei on which PMC and NLC form. Current theories have relied on meteor 'smoke' particles arising from meteor ablation and recondensation to explain the nucleation of NLC/PMC ice particles. Our calculated sizes and concentrations of high latitude summer mesosphere sulfate aerosol particles are comparable to or exceed those expected of the meteor source. The model shows that large volcanic eruptions will add significantly to this particle population, several years following the injection. The record of the number of NLC sightings in response to large volcanic eruptions is contradictory. However, microphysical models show that injections of particles may result in positive, negative or neutral response in the visual brightness of NLC, depending on sulfur, water vapor, and particulate injections, which have not been observed in the past A related radar phenomenon, Polar Mesopheric Summertime Echoes (PMSE), involves attachment of free electrons to condensates near the mesopause. Theory predicts that such particles would have to be smaller than 10 nm and number in the thousands per cm3. Up to now they were believed to be composed of water-ice. However these intense radar echoes have been detected as far south as 52N, where the mesopause is normally too warm for water-ice saturation, but in the range of sulfuric-acid condensation. We calculate mesospheric sulfate aerosol concentrations of up to 12000 /cm3, the vast majority of which are smaller than 10 nm. The concentration, size, and seasonal and latitudinal distribution of sulfate aerosol corresponds well to PMSE theory and observations.

Trends of ozone total columns and vertical distribution from FTIR observations at 8 NDACC stations around the globe

NASA Astrophysics Data System (ADS)

Vigouroux, C.; Blumenstock, T.; Coffey, M.; Errera, Q.; García, O.; Jones, N. B.; Hannigan, J. W.; Hase, F.; Liley, B.; Mahieu, E.; Mellqvist, J.; Notholt, J.; Palm, M.; Persson, G.; Schneider, M.; Servais, C.; Smale, D.; Thölix, L.; De Mazière, M.

2014-09-01

Ground-based Fourier transform infrared (FTIR) measurements of solar absorption spectra can provide ozone total columns with a precision of 2%, but also independent partial column amounts in about four vertical layers, one in the troposphere and three in the stratosphere up to about 45 km, with a precision of 5-6%. We use eight of the Network for the Detection of Atmospheric Compososition Change (NDACC) stations having a long-term time series of FTIR ozone measurements to study the total and vertical ozone trends and variability, namely: Ny-Alesund (79° N), Thule (77° N), Kiruna (68° N), Harestua (60° N), Jungfraujoch (47° N), Izaña (28° N), Wollongong (34° S) and Lauder (45° S). The length of the FTIR time-series varies by station, but is typically from about 1995 to present. We applied to the monthly means of the ozone total and four partial columns a stepwise multiple regression model including the following proxies: solar cycle, Quasi-Biennial Oscillation (QBO), El Niño-Southern Oscillation (ENSO), Arctic and Antarctic Oscillation (AO/AAO), tropopause pressure (TP), equivalent latitude (EL), Eliassen-Palm flux (EPF), and volume of polar stratospheric clouds (VPSC). At the Arctic stations, the trends are found mostly negative in the troposphere and lower stratosphere, very mixed in the middle stratosphere, positive in the upper stratosphere due to a large increase in the 1995-2003 period, and non-significant when considering the total columns. The trends for mid-latitude and subtropical stations are all non-significant, except at Lauder in the troposphere and upper stratosphere, and at Wollongong for the total columns and the lower and middle stratospheric columns; at Jungfraujoch, the upper stratospheric trend is close to significance (+0.9 ± 1.0 % decade-1). Therefore, some signs of the onset of ozone mid-latitude recovery are observed only in the Southern Hemisphere, while a few more years seems to be needed to observe it at the northern mid-latitude station.

Trends of ozone total columns and vertical distribution from FTIR observations at eight NDACC stations around the globe

NASA Astrophysics Data System (ADS)

Vigouroux, C.; Blumenstock, T.; Coffey, M.; Errera, Q.; García, O.; Jones, N. B.; Hannigan, J. W.; Hase, F.; Liley, B.; Mahieu, E.; Mellqvist, J.; Notholt, J.; Palm, M.; Persson, G.; Schneider, M.; Servais, C.; Smale, D.; Thölix, L.; De Mazière, M.

2015-03-01

Ground-based Fourier transform infrared (FTIR) measurements of solar absorption spectra can provide ozone total columns with a precision of 2% but also independent partial column amounts in about four vertical layers, one in the troposphere and three in the stratosphere up to about 45km, with a precision of 5-6%. We use eight of the Network for the Detection of Atmospheric Composition Change (NDACC) stations having a long-term time series of FTIR ozone measurements to study the total and vertical ozone trends and variability, namely, Ny-Ålesund (79° N), Thule (77° N), Kiruna (68° N), Harestua (60° N), Jungfraujoch (47° N), Izaña (28° N), Wollongong (34° S) and Lauder (45° S). The length of the FTIR time series varies by station but is typically from about 1995 to present. We applied to the monthly means of the ozone total and four partial columns a stepwise multiple regression model including the following proxies: solar cycle, quasi-biennial oscillation (QBO), El Niño-Southern Oscillation (ENSO), Arctic and Antarctic Oscillation (AO/AAO), tropopause pressure (TP), equivalent latitude (EL), Eliassen-Palm flux (EPF), and volume of polar stratospheric clouds (VPSC). At the Arctic stations, the trends are found mostly negative in the troposphere and lower stratosphere, very mixed in the middle stratosphere, positive in the upper stratosphere due to a large increase in the 1995-2003 period, and non-significant when considering the total columns. The trends for mid-latitude and subtropical stations are all non-significant, except at Lauder in the troposphere and upper stratosphere and at Wollongong for the total columns and the lower and middle stratospheric columns where they are found positive. At Jungfraujoch, the upper stratospheric trend is close to significance (+0.9 ± 1.0% decade-1). Therefore, some signs of the onset of ozone mid-latitude recovery are observed only in the Southern Hemisphere, while a few more years seem to be needed to observe it at the northern mid-latitude station.

Impacts of Horizontal Propagation of Orographic Gravity Waves on the Wave Drag in the Stratosphere and Lower Mesosphere

NASA Astrophysics Data System (ADS)

Xu, Xin; Wang, Yuan; Xue, Ming; Zhu, Kefeng

2017-11-01

The impact of horizontal propagation of mountain waves on the orographic gravity wave drag (OGWD) in the stratosphere and lower mesosphere of the Northern Hemisphere is evaluated for the first time. Using a fine-resolution (1 arc min) terrain and 2.5°×2.5° European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis data during 2011-2016, two sets of OGWD are calculated offline according to a traditional parameterization scheme (without horizontal propagation) and a newly proposed scheme (with horizontal propagation). In both cases, the zonal mean OGWDs show similar spatial patterns and undergo a notable seasonal variation. In winter, the OGWD is mainly distributed in the upper stratosphere and lower mesosphere of middle to high latitudes, whereas the summertime OGWD is confined in the lower stratosphere. Comparison between the two sets of OGWD reveal that the horizontal propagation of mountain waves tends to decrease (increase) the OGWD in the lower stratosphere (middle to upper stratosphere and lower mesosphere). Consequently, including the horizontal propagation of mountain waves in the parameterization of OGWD can reduce the excessive OGWD in the lower stratosphere and strengthen the insufficient gravity wave forcing in the mesosphere, which are the known problems of traditional OGWD schemes. The impact of horizontal propagation is more prominent in winter than in summer, with the OGWD in western Tibetan Plateau, Rocky Mountains, and Greenland notably affected.

The simulation of stratospheric water vapor in the NH summer monsoon regions in a suite of WACCM models

NASA Astrophysics Data System (ADS)

Wang, X.; Wu, Y.; Huang, Y.; Tilmes, S.

2016-12-01

Water vapor maxima are found in the upper troposphere lower stratosphere (UTLS) over Asian and North America monsoon regions during Northern Hemisphere (NH) summer months. High concentrations of stratospheric water vapor are associated with the upper-level anticyclonic circulation and they play an important role in the radiative forcing for the climate system. However, discrepancies in the simulation of stratospheric water vapor are found among different models. In this study, we use both observational data: Aura Microwave Limb Sounder satellite observations (MLS), the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2) and chemistry climate model outputs: different configurations of the Whole Atmosphere Community Climate Model (WACCM), including standard configuration of WACCM, WACCM L110, specified chemistry (SC) WACCM and specified dynamics (SD) WACCM. We find that WACCM L110 with finer vertical resolution better simulates the stratospheric water vapor maxima over the summer monsoon regions. To better understand the mechanism, we examine the simulated temperature at around 100 hPa since 100 hPa is known to act as a dehydration mechanism, i.e. the warmer the temperature, the wetter the stratospheric water vapor. We find that both WACCM L110 and SD-WACCM better simulate the temperature at 100 hPa as compared to that of MERRA2. This suggests that improving model vertical resolution and dynamical processes in the UTLS is crucial in simulating the stratospheric water vapor concentrations.

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

NASA Technical Reports Server (NTRS)

Jing, P.; Cunnold, D. M.; Yang, E.-S.; Wang, H.-J.

2005-01-01

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.

Signals of El Niño Modoki in the tropical tropopause layer and stratosphere

NASA Astrophysics Data System (ADS)

Xie, F.; Li, J.; Tian, W.; Feng, J.; Huo, Y.

2012-06-01

The effects of El Niño Modoki events on the tropical tropopause layer (TTL) and on the stratosphere were investigated using European Center for Medium Range Weather Forecasting (ECMWF) reanalysis data, oceanic El Niño indices, and general climate model outputs. El Niño Modoki events tend to depress convective activities in the western and eastern Pacific but enhance convective activities in the central and northern Pacific. Consequently, during El Niño Modoki events, negative water vapor anomalies occur in the western and eastern Pacific upper troposphere, whereas there are positive anomalies in the central and northern Pacific upper troposphere. The spatial patterns of the outgoing longwave radiation (OLR) and upper tropospheric water vapor anomalies exhibit a tripolar form. The empirical orthogonal function (EOF) analysis of the OLR and upper tropospheric water vapor anomalies reveals that canonical El Niño events are associated with the leading mode of the EOF, while El Niño Modoki events correspond to the second mode. The composite analysis based on ERA-interim data indicate that El Niño Modoki events have a reverse effect on middle-high latitudes stratosphere, as compared with the effect of typical El Niño events, i.e., the northern polar vortex is stronger and colder but the southern polar vortex is weaker and warmer during El Niño Modoki events. According to the simulation' results, we found that the reverse effect on the middle-high latitudes stratosphere is resulted from a complicated interaction between quasi-biennial oscillation (QBO) signal of east phase and El Niño Modoki signal. This interaction is not a simply linear overlay of QBO signal and El Niño Modoki signal in the stratosphere, it is El Niño Modoki that leads to different tropospheric zonal wind anomalies with QBO forcing from that caused by typical El Niño, thus, the planetary wave propagation from troposphere to the stratosphere during El Niño Modoki events is different from that during canonical El Niño events. However, when QBO is in its west phase, El Niño Modoki events have the same effect on middle-high latitudes stratosphere as the typical El Niño events. Our simulations also suggest that canonical El Niño and El Niño Modoki activities actually have the same influence on the middle-high latitudes stratosphere when in the absence of QBO forcing.

The solar and equatorial QBO influences on the stratospheric circulation during the early northern-hemisphere winter. [Quasi-Biennial Oscillation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kodera, Kunihiko

1991-06-01

A case study was conducted to investigate the mechanism of how the solar cycle and the equatorial quasi-biennial oscillation (QBO) influence the stratospheric circulation during the Northern-Hemisphere winter. It was found that the solar and QBO influences on the stratospheric jet exist rather independently in the upper stratosphere during December. The mean-zonal wind anomalies produced in early winter persist by deformation until late winter through wave-mean flow interactions with planetary waves. The modulation effect of the solar influence by the QBO takes place during this process.

Origins of tropospheric ozone interannual variation over Réunion: A model investigation

NASA Astrophysics Data System (ADS)

Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Françoise

2016-01-01

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Réunion Island (21.1°S, 55.5°E) in June-August. Here we examine possible causes of the observed ozone variation at Réunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications meteorological fields. Réunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange. Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Réunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Réunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited to the lower troposphere near the surface in August-September.

Origins of Tropospheric Ozone Interannual Variation (IAV) over Reunion: A Model Investigation

NASA Technical Reports Server (NTRS)

Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Francoise

2016-01-01

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Reunion Island (21.1 degrees South Latitude, 55.5 degrees East Longitude) in June-August. Here we examine possible causes of the observed ozone variation at Reunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Reunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange. Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Reunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Reunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited tothe lower troposphere near the surface in August-September.

NO(x) Concentrations in the Upper Troposphere as a Result of Lightning

NASA Technical Reports Server (NTRS)

Penner, Joyce E.

1998-01-01

Upper tropospheric NO(x) controls, in part, the distribution of ozone in this greenhouse-sensitive region of the atmosphere. Many factors control NO(x) in this region. As a result it is difficult to assess uncertainties in anthropogenic perturbations to NO from aircraft, for example, without understanding the role of the other major NO(x) sources in the upper troposphere. These include in situ sources (lightning, aircraft), convection from the surface (biomass burning, fossil fuels, soils), stratospheric intrusions, and photochemical recycling from HNO3. This work examines the separate contribution to upper tropospheric "primary" NO(x) from each source category and uses two different chemical transport models (CTMS) to represent a range of possible atmospheric transport. Because aircraft emissions are tied to particular pressure altitudes, it is important to understand whether those emissions are placed in the model stratosphere or troposphere and to assess whether the models can adequately differentiate stratospheric air from tropospheric air. We examine these issues by defining a point-by-point "tracer tropopause" in order to differentiate stratosphere from troposphere in terms of NO(x) perturbations. Both models predict similar zonal average peak enhancements of primary NO(x) due to aircraft (approx. = 10-20 parts per trillion by volume (pptv) in both January and July); however, the placement of this peak is primarily in a region of large stratospheric influence in one model and centered near the level evaluated as the tracer tropopause in the second. Below the tracer tropopause, both models show negligible NO(x) derived directly from the stratospheric source. Also, they predict a typically low background of 1 - 20 pptv NO(x) when tropospheric HNO3 is constrained to be 100 pptv of HNO3. The two models calculate large differences in the total background NO(x) (defined as the source of NO(x) from lightning + stratosphere + surface + HNO3) when using identical loss frequencies for NO(x). This difference is primarily due to differing treatments of vertical transport. An improved diagnosis of this transport that is relevant to NO(x) requires either measurements of a surface-based tracer with a substantially shorter lifetime than Rn-222 or diagnosis and mapping of tracer correlations with different source signatures. Because of differences in transport by the two models we cannot constrain the source of NO(x) from lightning through comparison of average model concentrations with observations of NO(x).

Overview of the Stratospheric Aerosol and Gas Experiment II water vapor observations - Method, validation, and data characteristics

NASA Technical Reports Server (NTRS)

Rind, D.; Chiou, E.-W.; Chu, W.; Oltmans, S.; Lerner, J.; Larsen, J.; Mccormick, M. P.; Mcmaster, L.

1993-01-01

Results are presented of water vapor observations in the troposphere and stratosphere performed by the Stratospheric Aerosol and Gas Experiment II solar occultation instrument, and the analysis procedure, the instrument errors, and data characteristics are discussed. The results are compared with correlative in situ measurements and other satellite data. The features of the data set collected between 1985 and 1989 include an increase in middle- and upper-tropospheric water vapor during northern hemisphere summer and autumn; minimum water vapor values of 2.5-3 ppmv in the tropical lower stratosphere; slowly increasing water vapor values with altitude in the stratosphere, reaching 5-6 ppmv or greater near the stratopause; extratropical values with minimum profile amounts occurring above the conventionally defined tropopause; and higher extratropical than tropical water vapor values throughout the stratosphere except in locations of possible polar stratospheric clouds.

Influence of Tropospheric SO2 Emissions on Particle Formation and the Stratospheric Humidity

NASA Technical Reports Server (NTRS)

Notholt, J.; Luo, B. P.; Fueglistaler, S.; Weisenstein, D.; Rex, M.; Lawrence, M. G.; Bingemer, H.; Wohltmann, I.; Corti, T.; Warneke, T.;

Radiolysis and Photolysis of Icy Satellite Surfaces: Experiments and Theory

NASA Technical Reports Server (NTRS)

Cassidy, T.; Coll, P.; Raulin, F.; Carlson, R. W.; Hand, K. P.; Johnson, R. E.; Loeffler, M. J.; Baragiola, R. A.

2010-01-01

The transport and exchange of material between bodies in the outer solar system is often facilitated by their exposure to ionizing radiation. With this in mind we review the effects of energetic ions, electrons and UV photons on materials present in the outer solar system. We consider radiolysis, photolysis, and sputtering of low temperature solids. Radiolysis and photolysis are the chemistry that follows the bond breaking and ionization produced by incident radiation, producing, e.g., O2 and H2 from irradiated H2O ice. Sputtering is the ejection of molecules by incident radiation. Both processes are particularly effective on ices in the outer solar system. Materials reviewed include H2O ice, sulfur-containing compounds (such as S02 and S8), carboncontajning compounds (such as CH4), nitrogen-containing compounds (such as NH3 and N2), and mixtures of those compounds. We also review the effects of ionizing radiation on a mixture of N2 and CH4 gases, as appropriate to Titan's upper atmosphere, where radiolysis and photolysis produce complex organic compounds (tholins).

Detectability of the impacts of ozone-depleting substances and greenhouse gases upon stratospheric ozone accounting for nonlinearities in historical forcings

NASA Astrophysics Data System (ADS)

Bandoro, Justin; Solomon, Susan; Santer, Benjamin D.; Kinnison, Douglas E.; Mills, Michael J.

2018-01-01

We perform a formal attribution study of upper- and lower-stratospheric ozone changes using observations together with simulations from the Whole Atmosphere Community Climate Model. Historical model simulations were used to estimate the zonal-mean response patterns (fingerprints) to combined forcing by ozone-depleting substances (ODSs) and well-mixed greenhouse gases (GHGs), as well as to the individual forcing by each factor. Trends in the similarity between the searched-for fingerprints and homogenized observations of stratospheric ozone were compared to trends in pattern similarity between the fingerprints and the internally and naturally generated variability inferred from long control runs. This yields estimated signal-to-noise (S/N) ratios for each of the three fingerprints (ODS, GHG, and ODS + GHG). In both the upper stratosphere (defined in this paper as 1 to 10 hPa) and lower stratosphere (40 to 100 hPa), the spatial fingerprints of the ODS + GHG and ODS-only patterns were consistently detectable not only during the era of maximum ozone depletion but also throughout the observational record (1984-2016). We also develop a fingerprint attribution method to account for forcings whose time evolutions are markedly nonlinear over the observational record. When the nonlinearity of the time evolution of the ODS and ODS + GHG signals is accounted for, we find that the S/N ratios obtained with the stratospheric ODS and ODS + GHG fingerprints are enhanced relative to standard linear trend analysis. Use of the nonlinear signal detection method also reduces the detection time - the estimate of the date at which ODS and GHG impacts on ozone can be formally identified. Furthermore, by explicitly considering nonlinear signal evolution, the complete observational record can be used in the S/N analysis, without applying piecewise linear regression and introducing arbitrary break points. The GHG-driven fingerprint of ozone changes was not statistically identifiable in either the upper- or lower-stratospheric SWOOSH data, irrespective of the signal detection method used. In the WACCM simulations of future climate change, the GHG signal is statistically identifiable between 2020 and 2030. Our findings demonstrate the importance of continued stratospheric ozone monitoring to improve estimates of the contributions of ODS and GHG forcing to global changes in stratospheric ozone.

Investigation of Dynamic and Physical Processes in the Upper Troposphere and Lower Stratosphere

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.; Pfister, Leonhard (Technical Monitor)

2002-01-01

Research under this Cooperative Agreement has been funded by several NASA Earth Science programs: the Atmospheric Effects of Radiation Program (AEAP), the Upper Atmospheric Research Program (UARP), and most recently the Atmospheric Chemistry and Modeling Assessment Program (ACMAP). The purpose of the AEAP was to understand the impact of the present and future fleets of conventional jet traffic on the upper troposphere and lower stratosphere, while complementary airborne observations under UARP seek to understand the complex interactions of dynamical and chemical processes that affect the ozone layer. The ACMAP is a more general program of modeling and data analysis in the general area of atmospheric chemistry and dynamics, and the Radiation Sciences program.

Methane photochemistry and methane production on Neptune

NASA Technical Reports Server (NTRS)

Romani, P. N.; Atreya, S. K.

1988-01-01

The Neptune stratosphere's methane photochemistry is presently studied by means of a numerical model in which the observed mixing ratio of methane prompts photolysis near the CH4 homopause. Haze generation by methane photochemistry has its basis in the formation of hydrocarbon ices and polyacetylenes; the hazes can furnish the requisite aerosol haze at the appropriate pressure levels required by observations of Neptune in the visible and near-IR. Comparisons of model predictions with Uranus data indicate a lower ratio of polyacetylene production to hydrocarbon ice, as well as a lower likelihood of UV postprocessing of the acetylene ice to polymers on Neptune, compared to Uranus.

Evaluation of the Cloud Fields in the UK Met Office HadGEM3-UKCA Model Using the CCCM Satellite Data Product to Advance Our Understanding of the Influence of Clouds on Tropospheric Composition and Chemistry

NASA Technical Reports Server (NTRS)

Varma, Sunil; Voulgarakis, Apostolos; Liu, Hongyu; Crawford, James H.; White, James

2016-01-01

To determine the role of clouds in driving inter-annual and inter-seasonal variability of trace gases in the troposphere and lower stratosphere with a particular focus on the importance of cloud modification of photolysis. To evaluate the cloud fields and their vertical distribution in the HadGEM3 model utilizing CCCM, a unique 3-D cloud data product merged from multiple A-Train satellites (CERES, CloudSat, CALIPSO, and MODIS) developed at the NASA Langley Research Center.

Exponential approximation for daily average solar heating or photolysis. [of stratospheric ozone layer

NASA Technical Reports Server (NTRS)

Cogley, A. C.; Borucki, W. J.

1976-01-01

When incorporating formulations of instantaneous solar heating or photolytic rates as functions of altitude and sun angle into long range forecasting models, it may be desirable to replace the time integrals by daily average rates that are simple functions of latitude and season. This replacement is accomplished by approximating the integral over the solar day by a pure exponential. This gives a daily average rate as a multiplication factor times the instantaneous rate evaluated at an appropriate sun angle. The accuracy of the exponential approximation is investigated by a sample calculation using an instantaneous ozone heating formulation available in the literature.

The high-resolution Doppler imager on the Upper Atmosphere Research Satellite

NASA Technical Reports Server (NTRS)

Hays, Paul B.; Abreu, Vincent J.; Dobbs, Michael E.; Gell, David A.; Grassl, Heinz J.; Skinner, Wilbert R.

1993-01-01

The high-resolution Doppler imager (HRDI) on the Upper Atmosphere Research Satellite is a triple-etalon Fabry-Perot interferometer designed to measure winds in the stratosphere, mesosphere, and lower thermosphere. Winds are determined by measuring the Doppler shifts of rotational lines of the O2 atmospheric band, which are observed in emission in the mesosphere and lower thermosphere and in absorption in the stratosphere. The interferometer has high resolution (0.05/cm), good offhand rejection, aud excellent stability. This paper provides details of the design and capabilities of the HRDI instrument.

Large Scale Winter Time Disturbances in Meteor Winds over Central and Eastern Europe

NASA Technical Reports Server (NTRS)

Greisiger, K. M.; Portnyagin, Y. I.; Lysenko, I. A.

1984-01-01

Daily zonal wind data of the four pre-MAP-winters 1978/79 to 1981/82 obtained over Central Europe and Eastern Europe by the radar meteor method were studied. Available temperature and satellite radiance data of the middle and upper stratosphere were used for comparison, as well as wind data from Canada. The existence or nonexistence of coupling between the observed large scale zonal wind disturbances in the upper mesopause region (90 to 100 km) and corresponding events in the stratosphere are discussed.

Stratospheric nitrogen dioxide in the vicinity of Soufriere, St. Vincent

NASA Technical Reports Server (NTRS)

Romick, G. J.; Murcray, D. G.; Williams, W. J.

1982-01-01

In April 1979, measurements of nitrogen dioxide in the upper atmosphere were made near Soufriere Volcano by twilight optical-absorption techniques. The derived value of 5 x 10 to the 15th molecules per square centimeter column implies an enhancement of 25 percent over earlier abundances measured in the same latitudinal regions. This enhancement may represent the normal stratospheric variability of nitrogen dioxide in the equatorial region, but in any case may be considered an upper limit to the volcano's effect on the total nitrogen dioxide abundance.

Production of Nitrogen Oxides by Laboratory Simulated Transient Luminous Events

NASA Astrophysics Data System (ADS)

Peterson, H.; Bailey, M.; Hallett, J.; Beasley, W.

2007-12-01

Restoration of the polar stratospheric ozone layer has occurred at rates below those originally expected following reductions in chlorofluorocarbon (CFC) usage. Additional reactions affecting ozone depletion now must also be considered. This research examines nitrogen oxides (NOx) produced in the middle atmosphere by transient luminous events (TLEs), with NOx production in this layer contributing to the loss of stratospheric ozone. In particular, NOx produced by sprites in the mesosphere would be transported to the polar stratosphere via the global meridional circulation and downward diffusion. A pressure-controlled vacuum chamber was used to simulate middle atmosphere pressures, while a power supply and in-chamber electrodes were used to simulate TLEs in the pressure controlled environment. Chemiluminescence NOx analyzers were used to sample NOx produced by the chamber discharges- originally a Monitor Labs Model 8440E, later a Thermo Environment Model 42. Total NOx production for each discharge as well as NOx per ampere of current and NOx per Joule of discharge energy were plotted. Absolute NOx production was greatest for discharge environments with upper tropospheric pressures (100-380 torr), while NOx/J was greatest for discharge environments with stratospheric pressures (around 10 torr). The different production efficiencies in NOx/J as a function of pressure pointed to three different production regimes, each with its own reaction mechanisms: one for tropospheric pressures, one for stratospheric pressures, and one for upper stratospheric to mesospheric pressures (no greater than 1 torr).

Disentangling the Roles of Various Forcing Mechanisms on Stratospheric Temperature Changes Since 1979 with the NASA GEOSCCM

NASA Technical Reports Server (NTRS)

Aquila, Valentina; Swartz, W.; Colarco, P.; Pawson, S.; Polvani, L.; Stolarski, R.; Waugh, D.

2015-01-01

Observations show that the cooling of global stratospheric temperatures from 1979 to 2015 took place in two major steps coincident with the 1982 El Chichon and 1991 Mount Pinatubo eruptions. In order to attribute the features of the global stratospheric temperature time series to the main forcing agents, we performed a set of simulations with the NASA Goddard Earth Observing System Chemistry Climate Model. Our results show that the characteristic step-like behavior is to be attributed to the effects of the solar cycle, except for the post-1995 flattening of the lower stratospheric temperatures, where the decrease in ozone depleting substances due to the Montreal Protocol slowed ozone depletion and therefore also the cooling of the stratosphere. Volcanic eruptions also caused a significant warming of the stratosphere after 1995. The observed general cooling is mainly caused by increasing ozone depleting substances in the lower stratosphere, and greenhouse gases in the middle and upper stratosphere.

Wave Activity and Its Changes in the Troposphere and Stratosphere of the Northern Hemisphere in Winters of 1979-2016

NASA Astrophysics Data System (ADS)

Guryanov, V. V.; Eliseev, A. V.; Mokhov, I. I.; Perevedentsev, Yu. P.

2018-03-01

An analysis of spectra of wave disturbances with zonal wave numbers 1 ≤ k ≤ 10 is carried out using winter (November to March) ERA-Interim reanalysis geopotential data in the troposphere and stratosphere for 1979-2016. Contributions of eastward-traveling ( E), westward-traveling ( W), and stationary ( S) waves are estimated. The intensification of wave activity is observed in the tropical troposphere and stratosphere and in the upper stratosphere of the entire Northern Hemisphere. The intensification of wave activity in the tropics and subtropics is noted for waves of all types ( E, W, and S), while in the middle and higher latitudes it is related mainly to stationary and eastward waves. Near the subtropical tropopause, the energy of stationary waves has increased in recent decades. In addition, in the tropical and subtropical troposphere and in the subtropical lower stratosphere, the energy of the eastward-traveling waves in El Niño years may be one and a half times or twice the energy in La Niña years. The spectrally weighted zonal wave numbers for waves of all types ( E, W, and S) are the largest in the upper subtropical troposphere. The spectrally weighted zonal wave number for W and S waves is correlated with the Atlantic Multidecadal Oscillation index and varies by 15% in 1979-2016 (on an interdecadal time scale). The spectrally weighted wave period is larger in the stratosphere than in the troposphere. It is maximal in the middle extratropical stratosphere. The spectrally weighted wave periods correlate with the activity of sudden stratospheric warmings. The sign of this correlation depends on the latitude, atmospheric layer, and zonal wave number.

Understanding Differences in Chemistry Climate Model Projections of Stratospheric Ozone

NASA Technical Reports Server (NTRS)

Douglass, A. R.; Strahan, S. E.; Oman, L. D.; Stolarski, R. S.

2014-01-01

Chemistry climate models (CCMs) are used to project future evolution of stratospheric ozone as concentrations of ozone-depleting substances (ODSs) decrease and greenhouse gases increase, cooling the stratosphere. CCM projections exhibit not only many common features but also a broad range of values for quantities such as year of ozone return to 1980 and global ozone level at the end of the 21st century. Multiple linear regression is applied to each of 14 CCMs to separate ozone response to ODS concentration change from that due to climate change. We show that the sensitivity of lower stratospheric ozone to chlorine change Delta Ozone/Delta inorganic chlorine is a near-linear function of partitioning of total inorganic chlorine into its reservoirs; both inorganic chlorine and its partitioning are largely controlled by lower stratospheric transport. CCMs with best performance on transport diagnostics agree with observations for chlorine reservoirs and produce similar ozone responses to chlorine change. After 2035, differences in Delta Ozone/Delta inorganic chlorine contribute little to the spread in CCM projections as the anthropogenic contribution to inorganic chlorine becomes unimportant. Differences among upper stratospheric ozone increases due to temperature decreases are explained by differences in ozone sensitivity to temperature change Delta Ozone/Delta T due to different contributions from various ozone loss processes, each with its own temperature dependence. Ozone decrease in the tropical lower stratosphere caused by a projected speedup in the Brewer-Dobson circulation may or may not be balanced by ozone increases in the middle- and high-latitude lower stratosphere and upper troposphere. This balance, or lack thereof, contributes most to the spread in late 21st century projections.

Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

PubMed Central

Hirose, Katsumi; Povinec, Pavel P.

2015-01-01

Plutonium isotopes have primarily been injected to the stratosphere by the atmospheric nuclear weapon tests and the burn-up of the SNAP-9A satellite. Here we show by using published data that the stratospheric plutonium exponentially decreased with apparent residence time of 1.5 ± 0.5 years, and that the temporal variations of plutonium in surface air followed the stratospheric trends until the early 1980s. In the 2000s, plutonium and its isotope ratios in the atmosphere varied dynamically, and sporadic high concentrations of 239,240Pu reported for the lower stratospheric and upper tropospheric aerosols may be due to environmental events such as the global dust outbreaks and biomass burning. PMID:26508010

Evidence for slowdown in stratospheric ozone loss: First stage of ozone recovery

NASA Technical Reports Server (NTRS)

Newchurch, M. J.; Yang, Eun-Su; Cunnold, D. M.; Reinsel, C.; Zawodny, J. M.; Russell, James M., III

2003-01-01

Global ozone trends derived from the Stratospheric Aerosol and Gas Experiment I and II (SAGE I/II) combined with the more recent Halogen Occultation Experiment (HALOE) observations provide evidence of a slowdown in stratospheric ozone losses since 1997. This evidence is quantified by the cumulative sum of residual differences from the predicted linear trend. The cumulative residuals indicate that the rate of ozone loss at 35- 45 km altitudes globally has diminished. These changes in loss rates are consistent with the slowdown of total stratospheric chlorine increases characterized by HALOE HCI measurements. These changes in the ozone loss rates in the upper stratosphere are significant and constitute the first stage of a recovery of the ozone layer.

Micro-Scale Sulfur and Carbon Isotope Analysis of a Neoarchean Stromatolite: Evidence for a Profound Redox Transition in Shelf Margins prior to the Great Oxidation Event

NASA Astrophysics Data System (ADS)

Ilhardt, P.; House, C. H.; Altermann, W.

2016-12-01

Neoarchean shelf margin environments such as the Campbellrand-Malmani platform are believed to have been sites of substantial O2 accumulation and nutrient cycling prior to the Great Oxidation Event (GOE). Stromatolites in particular serve as biogeochemical "hotspots" where evidence of various metabolic pathways and bacterial lineages can be traced through geochemical fingerprints. We identified morphologically-unique, organic-rimmed pyrite grains embedded in the dolomitic lamina of a Campbellrand Subgroup stromatolite (2.6 Ga). Carbon and sulfur isotopes measured in situ revealed a multi-layered microbial community employing photoautotrophic carbon fixation, organic matter respiration, sulfate reduction, and potentially assimilation of methane. In particular, unusually high kerogen δ13Corg and pyrite δ34S compositions are consistent with a semi-aerobic ecosystem recycling photosynthetic biomass and sulfate reduction in sulfate-limited porewaters, respectively. In addition, an array of positive Δ33S values suggests incorporation of atmospherically-derived sulfur formed from volcanic SO2 photochemistry and isolated in particulate form. We argue the Δ33S-δ34S trend is best explained by mixing between a δ34S-enriched coastal marine sulfate reservoir and stratospheric Δ33S-positive sulfate or elemental sulfur aerosols. The hypothesized buildup of sulfur gases at higher altitudes agrees with prior arguments for increased subaerial felsic volcanism and intense plume activity coinciding with oxidation of the upper mantle. We suggest explosive subaerial eruptions sustained a stratospheric SO2 reservoir that underwent photochemistry via long-wavelength (250-330 nm) UV radiation to produce positive MIF-carrying aerosol particles (sulfate or sulfur) in the Neoarchean. This contrasts with Paleoarchean sulfur chemistry dominated by SO2 photolysis in the 190-220 nm excitation band and points to an evolving Archean atmosphere, culminating in a coupled biogeochemical-tectonic redox transformation that fundamentally changed the atmospheric sulfur cycle and ultimately prompted the GOE.

Measurement of HO2 and other trace gases in the stratosphere using a high resolution far-infrared spectrometer

NASA Technical Reports Server (NTRS)

Traub, Wesley A.; Chance, Kelly V.; Johnson, David G.; Jucks, Kenneth W.; Salawitch, Ross J.; Xue, Jim Changqin; Ciarpallini, Paola

1995-01-01

This report covers the time period 1 January 1994 to 31 December 1994. During this reporting period we had our fourth Upper Atmosphere Research Satellite (UARS) correlative balloon flight; the data from this flight have been reduced and submitted to the UARS CDHF. We have spent most of the past year analyzing data from this and past flights. For example, using data from our September 1989 balloon flight we have demonstrated for the first time ever that the rates of production and loss of ozone are in balance in the upper stratosphere. As part of this analysis, we have completed the most detailed study to date of radical partitioning throughout the stratosphere. We have also produced the first measurement of HBr and HOBr mixing ratio profiles over a full diurnal cycle.

A fiery birth of aluminosilica analogs of refractory dust in the upper stratosphere

NASA Astrophysics Data System (ADS)

Rietmeijer, F. J. M.; Ferrari, M.; Della Corte, V.; Rotundi, A.; Palumbo, P.; De Angelis, S.; Galluzzi, V.

2017-11-01

Following a successful dust collection flight in the upper stratosphere our DUSTER (Dust in the Upper Stratosphere Tracking Experiment and Retrieval) made a safe remote landing at its assigned location on Baffin Island during early June 2009. When the balloon payload that included DUSTER was retrieved it was found part of the payload had experienced a lithium-sparked fire while the payload was being dragged across the landing site. In this process the housing of DUSTER had developed a pin-sized hole that allowed smoke of the fire to enter the collector. Numerous smoke particles were found covering both the DUSTER collection and blank collector surfaces an indication that our experiment to collect upper stratospheric dust had failed! Both collector surfaces were covered by numerous carbon smoke and amorphous, aluminosilica nanoparticles. The compositions of vast majority of these aluminosilica nanoparticles, Al2O3 = 49 wt% and SiO2 = 51 wt%, was both surprising and unique because it was an exact match of the Deep Metastable Eutectic (DME) nanoparticles found in vapor phase condensation experiments. These vapor phase condensation experiments were conducted to explore the formation of extraterrestrial dust particles. We are not claiming an extraterrestrial origin for these particles from this DUSTER experiment. We submit that given the appropriate conditions of high temperature alumina and silica vapors and rapid quenching in a contained natural environment, DME aluminosilica nanoparticles will likely condense. This serendipitous result can be used to explore nanoparticle formation inside incandescent clouds associated with bolides and fireballs.

Simultaneous lidar observations of the water vapor and ozone signatures of a stratospheric intrusion during the MOHAVE-2009 campaign

NASA Astrophysics Data System (ADS)

Leblanc, T.; McDermid, I. S.; Pérot, K.

2010-12-01

Ozone and water vapor signatures of a stratospheric intrusion were simultaneously observed by the Jet Propulsion Laboratory lidars located at Table Mountain Facility, California (TMF, 34.4N, 117.7W) during the Measurements of Humidity in the Atmosphere and Validation Experiments (MOHAVE-2009) campaign in October 2009. These observations are placed in the context of the meridional displacement and folding of the tropopause, and resulting contrast in the properties of the air masses sampled by lidar. The lidar observations are supported by model data, specifically potential vorticity fields advected by the high-resolution transport model MIMOSA, and by 10-day backward isentropic trajectories. The ozone and water vapor anomalies measured by lidar were largely anti-correlated, and consistent with the assumption of a wet and ozone-poor subtropical upper troposphere, and a dry and ozone-rich extra-tropical lowermost stratosphere. However, it is shown that this anti-correlation relation collapsed just after the stratospheric intrusion event of October 20, suggesting mixed air embedded along the subtropical jet stream and sampled by lidar during its displacement south of TMF (tropopause fold). The ozone-PV expected positive correlation relation held strongly throughout the measurement period, including when a lower polar stratospheric filament passed over TMF just after the stratospheric intrusion. The numerous highly-correlated signatures observed during this event demonstrate the strong capability of the water vapor and ozone lidars at TMF, and provide new confidence in the future detection by lidar of long-term variability of water vapor and ozone in the Upper Troposphere-Lower Stratosphere (UTLS).

Multi-Model Assessment of the Factors Driving Stratospheric Ozone Evolution Over the 21st Century

NASA Technical Reports Server (NTRS)

Oman, L. D.; Plummer, D. A.; Waugh, D. W.; Austin, J.; Scinocca, J.; Douglass, A. R.; Salawitch, R. J.; Canty, T.; Akiyoshi, H.; Bekki, S.;

Utilization of UARS Data in Validation of Photochemical and Dynamical Mechanisms in Stratospheric Models

NASA Technical Reports Server (NTRS)

Ko, M. K. W.; Rodriquez, J. M.; Hu, W.; Danilin, M. Y.; Shia, R.-L.

1998-01-01

The proposed work utilized Upper Atmosphere Research Satellite (UARS) measurements of short-lived and long-lived species, in conjunction with existing photochemical "box" models, trajectory models, and two-dimensional global models, to elucidate outstanding questions in our understanding of photochemical and dynamical mechanisms in the stratosphere. Particular emphasis was given to arriving at the best possible understanding of the chemical and dynamical contributions to the stratospheric ozone budget. Such understanding will increase confidence in the simulations carried out by assessment models.

Utilization of UARS Data in Validation of Photochemical and Dynamical Mechanisms in Stratospheric Models

NASA Technical Reports Server (NTRS)

Ko, Malcolm K. W.; Rodriquez, Jose M.; Hu, Wenjie; Danilin, Michael Y.; Shia, Run-Li

1998-01-01

The proposed work utilized Upper Atmosphere Research Satellite (UARS) measurements of short-lived and long-lived species, in conjunction with existing photochemical "box" models, trajectory models, and two-dimensional global models, to elucidate outstanding questions in our understanding of photochemical and dynamical mechanisms in the stratosphere. Particular emphasis was given to arriving at the best possible understanding of the chemical and dynamical contribution to the stratospheric ozone budget. Such understanding will increase confidence in the simulations carried out by assessment models.

On the Observed Changes in Upper Stratospheric and Mesospheric Temperatures from UARS HALOE

NASA Technical Reports Server (NTRS)

Remsberg, Ellis E.

2006-01-01

Temperature versus pressure or T(p) time series from the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite (UARS) have been extended and re-analyzed for the period of 1991-2005 and for the upper stratosphere and mesosphere in 10-degree wide latitude zones from 60S to 60N. Even though sampling from a solar occultation experiment is somewhat limited, it is shown to be quite adequate for developing both the seasonal and longer-term variations in T(p). Multiple linear regression (MLR) techniques were used in the re-analyses for the seasonal and the significant interannual, solar cycle (SC-like or decadal-scale), and linear trend terms. A simple SC-like term of 11-yr period was fitted to the time series residuals after accounting for the seasonal and interannual terms. Highly significant SC-like responses were found for both the upper mesosphere and the upper stratosphere. The phases of these SC-like terms were checked for their continuity with latitude and pressure-altitude, and in almost all cases they are directly in-phase with that of standard proxies for the solar flux variations. The analyzed, max minus min, responses at low latitudes are of order 1 K, while at middle latitudes they are as large as 3 K in the upper mesosphere. Highly significant, linear cooling trends were found at middle latitudes of the middle to upper mesosphere (about -2 K/decade), at tropical latitudes of the middle mesosphere (about -1 K/decade), and at 2 hPa (or order -1 K/decade).

Effects of Greenhouse Gas Increase and Stratospheric Ozone Depletion on Stratospheric Mean Age of Air in 1960-2010

NASA Astrophysics Data System (ADS)

Li, F.; Newman, P. A.; Pawson, S.; Perlwitz, J.

2017-12-01

The strength of the stratospheric Brewer-Dobson circulation (BDC) in a changing climate has been extensively studied, but the relative importance of greenhouse gas (GHG) increases and stratospheric ozone depletion in driving the BDC changes remains uncertain. This study separates the impacts of GHG and stratospheric ozone forcings on stratospheric mean age of air in the 1960-2010 period using the Goddard Earth Observing System Model (GEOS) Chemistry-Climate Model (CCM). The experiment compares a set of controlled simulations using a coupled atmosphere-ocean version of the GEOS CCM, in which either GHGs, or stratospheric ozone, or both factors evolve over time. The model results show that GHGs and stratospheric ozone have about equal contributions to the simulated mean age decrease. It is also found that GHG increases account for about two thirds of the enhanced strength of the lower stratospheric residual circulation. The results show that ozone depletion causes an increase in the mean age of air in the Antarctic summer lower stratosphere through two processes: 1) a seasonal delay in the Antarctic polar vortex breakup, that inhibits young mid-latitude air from mixing with the older air inside the vortex; and 2) enhanced Antarctic downwelling, that brings older air from middle and upper stratosphere into the lower stratosphere.

Impact of Stratospheric Ozone Distribution on Features of Tropospheric Circulation

NASA Astrophysics Data System (ADS)

Barodka, Siarhei; Krasouski, Aliaksandr; Mitskevich, Yaroslav; Shalamyansky, Arkady

2016-04-01

In this work we study connections between stratospheric ozone distribution and general circulation patterns in the troposphere and aim to investigate the causal relationship between them, including the practical side of the influence of stratospheric ozone on tropospheric medium-range weather and regional climate. Analysis of several decades of observational data, which has been performed at the A.I. Voeikov Main Geophysical Observatory, suggests a clear relation between the stratospheric ozone distribution, upper stratospheric temperature field and planetary-scale air-masses boundaries in the troposphere [1]. Furthermore, it has been shown that each global air-mass, which can be attributed to the corresponding circulation cell in a conceptual model of tropospheric general circulation, has a distinct "regime" of ozone vertical distribution in the stratosphere [1-3]. Proceeding from atmospheric reanalyses combined with satellite and ground-based observations, we study time evolution of the upper-level frontal zones (stationary fronts) with the relevant jet streams, which can be treated as boundaries of global air-masses, in connection with the tropopause height and distribution of ozone in the stratosphere. For that, we develop an algorithm for automated identification of jet streams, stationary fronts and tropopause surface from gridded data (reanalyses or modelling results), and apply it for several cases associated with rapid changes in the stratospheric temperature and ozone fields, including SSW events over Eastern Siberia. Aiming to study the causal relationship between the features of tropospheric circulation and changes in the stratospheric ozone field, we estimate the time lag between these categories of processes on different time scales. Finally, we discuss the possibility to use the elementary circulation mechanisms classification (by B.L. Dzerdzeevski) in connection with analysis of the stratospheric ozone field and the relevant stratosphere-troposphere interactions. [1] Shalamyansky A.M., Proceedings of Voeikov MGO, St. Petersburg, V. 568, pp. 173-194, 2013 [2] R.D. Hudson et al, J. Atmos. Sci., V. 60, pp. 1669-1677, 2003 [3] R.D. Hudson et al, Atmos. Chem. Phys., V. 6, pp. 5183-5191, 2006

Isolating the roles of different forcing agents in global stratospheric temperature changes using model integrations with incrementally added single forcings

NASA Astrophysics Data System (ADS)

Aquila, V.; Swartz, W. H.; Waugh, D. W.; Colarco, P. R.; Pawson, S.; Polvani, L. M.; Stolarski, R. S.

2016-07-01

Satellite instruments show a cooling of global stratospheric temperatures over the whole data record (1979-2014). This cooling is not linear and includes two descending steps in the early 1980s and mid-1990s. The 1979-1995 period is characterized by increasing concentrations of ozone-depleting substances (ODSs) and by the two major volcanic eruptions of El Chichón (1982) and Mount Pinatubo (1991). The 1995-present period is characterized by decreasing ODS concentrations and by the absence of major volcanic eruptions. Greenhouse gas (GHG) concentrations increase over the whole time period. In order to isolate the roles of different forcing agents in the global stratospheric temperature changes, we performed a set of simulations using the NASA Goddard Earth Observing System Chemistry-Climate Model with prescribed sea surface temperatures. We find that in our model simulations the cooling of the stratosphere from 1979 to present is mostly driven by changes in GHG concentrations in the middle and upper stratosphere and by GHG and ODS changes in the lower stratosphere. While the cooling trend caused by increasing GHGs is roughly constant over the satellite era, changing ODS concentrations cause a significant stratospheric cooling only up to the mid-1990s, when they start to decrease because of the implementation of the Montreal Protocol. Sporadic volcanic events and the solar cycle have a distinct signature in the time series of stratospheric temperature anomalies but do not play a statistically significant role in the long-term trends from 1979 to 2014. Several factors combine to produce the step-like behavior in the stratospheric temperatures: in the lower stratosphere, the flattening starting in the mid-1990s is due to the decrease in ozone-depleting substances; Mount Pinatubo and the solar cycle cause the abrupt steps through the aerosol-associated warming and the volcanically induced ozone depletion. In the middle and upper stratosphere, changes in solar irradiance are largely responsible for the step-like behavior of global temperature anomalies, together with volcanically induced ozone depletion and water vapor increases in the post-Pinatubo years.

Isolating the Roles of Different Forcing Agents in Global Stratospheric Temperature Changes Using Model Integrations with Incrementally Added Single Forcings

NASA Technical Reports Server (NTRS)

Aquila, V.; Swartz, W. H.; Waugh, D. W.; Colarco, P. R.; Pawson, S.; Polvani, L. M.; Stolarski, R. S.

2016-01-01

Satellite instruments show a cooling of global stratospheric temperatures over the whole data record (1979-2014). This cooling is not linear and includes two descending steps in the early 1980s and mid-1990s. The 1979-1995 period is characterized by increasing concentrations of ozone depleting substances (ODS) and by the two major volcanic eruptions of El Chichon (1982) and Mount Pinatubo (1991). The 1995-present period is characterized by decreasing ODS concentrations and by the absence of major volcanic eruptions. Greenhouse gas (GHG) concentrations increase over the whole time period. In order to isolate the roles of different forcing agents in the global stratospheric temperature changes, we performed a set of AMIP-style simulations using the NASA Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). We find that in our model simulations the cooling of the stratosphere from 1979 to present is mostly driven by changes in GHG concentrations in the middle and upper stratosphere and by GHG and ODS changes in the lower stratosphere. While the cooling trend caused by increasing GHGs is roughly constant over the satellite era, changing ODS concentrations cause a significant stratospheric cooling only up to the mid-1990s, when they start to decrease because of the implementation of the Montreal Protocol. Sporadic volcanic events and the solar cycle have a distinct signature in the time series of stratospheric temperature anomalies but do not play a statistically significant role in the long-term trends from 1979 to 2014. Several factors combine to produce the step-like behavior in the stratospheric temperatures: in the lower stratosphere, the flattening starting in the mid-1990s is due to the decrease in ozone-depleting substances; Mount Pinatubo and the solar cycle cause the abrupt steps through the aerosol-associated warming and the volcanically induced ozone depletion. In the middle and upper stratosphere, changes in solar irradiance are largely responsible for the step-like behavior of global temperature anomalies, together with volcanically induced ozone depletion and water vapor increases in the post-Pinatubo years.

Isolating the roles of different forcing agents in global stratospheric temperature changes using model integrations with incrementally added single forcings.

PubMed

Aquila, V; Swartz, W H; Waugh, D W; Colarco, P R; Pawson, S; Polvani, L M; Stolarski, R S

2016-07-16

Satellite instruments show a cooling of global stratospheric temperatures over the whole data record (1979-2014). This cooling is not linear, and includes two descending steps in the early 1980s and mid-1990s. The 1979-1995 period is characterized by increasing concentrations of ozone depleting substances (ODS) and by the two major volcanic eruptions of El Chichón (1982) and Mount Pinatubo (1991). The 1995-present period is characterized by decreasing ODS concentrations and by the absence of major volcanic eruptions. Greenhouse gas (GHG) concentrations increase over the whole time period. In order to isolate the roles of different forcing agents in the global stratospheric temperature changes, we performed a set of AMIP-style simulations using the NASA Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). We find that in our model simulations the cooling of the stratosphere from 1979 to present is mostly driven by changes in GHG concentrations in the middle and upper stratosphere and by GHG and ODS changes in the lower stratosphere. While the cooling trend caused by increasing GHGs is roughly constant over the satellite era, changing ODS concentrations cause a significant stratospheric cooling only up to the mid-1990s, when they start to decrease because of the implementation of the Montreal Protocol. Sporadic volcanic events and the solar cycle have a distinct signature in the time series of stratospheric temperature anomalies but do not play a statistically significant role in the long-term trends from 1979 to 2014. Several factors combine to produce the step-like behavior in the stratospheric temperatures: in the lower stratosphere, the flattening starting in the mid 1990's is due to the decrease in ozone depleting substances; Mount Pinatubo and the solar cycle cause the abrupt steps through the aerosol-associated warming and the volcanically induced ozone depletion. In the middle and upper stratosphere, changes in solar irradiance are largely responsible for the step-like behavior of global temperatures anomalies, together with volcanically induced ozone depletion and water vapor increases in the post-Pinatubo years.

Isolating the roles of different forcing agents in global stratospheric temperature changes using model integrations with incrementally added single forcings

PubMed Central

Aquila, V.; Swartz, W. H.; Waugh, D. W.; Colarco, P. R.; Pawson, S.; Polvani, L. M.; Stolarski, R. S.

2018-01-01

Satellite instruments show a cooling of global stratospheric temperatures over the whole data record (1979–2014). This cooling is not linear, and includes two descending steps in the early 1980s and mid-1990s. The 1979–1995 period is characterized by increasing concentrations of ozone depleting substances (ODS) and by the two major volcanic eruptions of El Chichón (1982) and Mount Pinatubo (1991). The 1995-present period is characterized by decreasing ODS concentrations and by the absence of major volcanic eruptions. Greenhouse gas (GHG) concentrations increase over the whole time period. In order to isolate the roles of different forcing agents in the global stratospheric temperature changes, we performed a set of AMIP-style simulations using the NASA Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). We find that in our model simulations the cooling of the stratosphere from 1979 to present is mostly driven by changes in GHG concentrations in the middle and upper stratosphere and by GHG and ODS changes in the lower stratosphere. While the cooling trend caused by increasing GHGs is roughly constant over the satellite era, changing ODS concentrations cause a significant stratospheric cooling only up to the mid-1990s, when they start to decrease because of the implementation of the Montreal Protocol. Sporadic volcanic events and the solar cycle have a distinct signature in the time series of stratospheric temperature anomalies but do not play a statistically significant role in the long-term trends from 1979 to 2014. Several factors combine to produce the step-like behavior in the stratospheric temperatures: in the lower stratosphere, the flattening starting in the mid 1990’s is due to the decrease in ozone depleting substances; Mount Pinatubo and the solar cycle cause the abrupt steps through the aerosol-associated warming and the volcanically induced ozone depletion. In the middle and upper stratosphere, changes in solar irradiance are largely responsible for the step-like behavior of global temperatures anomalies, together with volcanically induced ozone depletion and water vapor increases in the post-Pinatubo years. PMID:29593948

Stratospheric influence on the seasonal cycle of nitrous oxide in the troposphere as deduced from aircraft observations and model simulations

NASA Astrophysics Data System (ADS)

Ishijima, Kentaro; Patra, Prabir K.; Takigawa, Masayuki; Machida, Toshinobu; Matsueda, Hidekazu; Sawa, Yosuke; Steele, L. Paul; Krummel, Paul B.; Langenfelds, Ray L.; Aoki, Shuji; Nakazawa, Takakiyo

2010-10-01

The atmospheric N2O variations between the Earth's surface and the lower stratosphere, simulated by an atmospheric general circulation model-based chemistry transport model (ACTM), are compared with aircraft and satellite observations. We validate the newly developed ACTM simulations of N2O for loss rate and transport in the stratosphere using satellite observations from the Aura Microwave Limb Sounder (Aura-MLS), with optimized surface fluxes for reproducing N2O trends observed at the surface stations. Observations in the upper troposphere/lower stratosphere (UT/LS) obtained by the Japan AirLines commercial flights commuting between Narita (36°N), Japan, and Sydney (34°S), Australia, have been used to study the role of stratosphere-troposphere exchange (STE) on N2O variability near the tropopause. Low N2O concentration events in the UT region are shown to be captured statistically significantly by the ACTM simulation. This is attributed to successful reproduction of stratospheric air intrusion events and N2O vertical/horizontal gradients in the lower stratosphere. The meteorological fields and N2O concentrations reproduced in the ACTM are used to illustrate the mechanisms of STE and subsequent downward propagation of N2O-depleted stratospheric air in the troposphere. Aircraft observations of N2O vertical profile over Surgut (West Siberia, Russia; 61°N), Sendai-Fukuoka (Japan; 34°N-38°N), and Cape Grim (Tasmania, Australia; 41°S) have been used to estimate the relative contribution of surface fluxes, transport seasonality in the troposphere, and STE to N2O seasonal cycles at different altitude levels. Stratospheric N2O tracers are incorporated in the ACTM for quantitative estimation of the stratospheric influence on tropospheric N2O. The results suggest strong latitude dependency of the stratospheric contribution to the tropospheric N2O seasonal cycle. The periods of seasonal minimum in the upper troposphere, which are spring over Japan and summer over Surgut, are in good agreement between the ACTM and observation and indicate a different propagation path of the stratospheric signal between the two sites in the Northern Hemisphere. The stratospheric tracer simulations, when utilized with the observed seasonal cycle, also provide qualitative information on the seasonal variation in surface fluxes of N2O.

Validation of UARS Microwave Limb Sounder 183 GHz H2O Measurements

NASA Technical Reports Server (NTRS)

Lahoz, W. A.; Suttie, M. R.; Froidevaux, L.; Harwood, R. S.; Lau, C. L.; Lungu, T. A.; Peckham, G. E.; Pumphrey, H. C.; Read, W. G.; Shippony, Z.;

Laboratory Studies of Homogeneous and Heterogeneous Chemical Processes of Importance in the Upper Atmosphere

NASA Technical Reports Server (NTRS)

Molina, Mario J.

2001-01-01

The objective of this study is to conduct measurements of chemical kinetics parameters for reactions of importance in the stratosphere and upper troposphere, and to study the interaction of trace gases such as HCl with ice surfaces in order to elucidate the mechanism of heterogeneous chlorine activation processes, using both a theoretical and an experimental approach. The measurements will be carried out under temperature and pressure conditions covering those applicable to the stratosphere and upper troposphere. The techniques to be employed include turbulent flow - chemical ionization mass spectrometry, and optical ellipsometry. The next section summarizes our research activities during the second year of the project, and the section that follows consists of the statement of work for the third year.

Investigation of the Physical Processes Governing Large-Scale Tracer Transport in the Stratosphere and Troposphere

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.

2001-01-01

This report summarizes work conducted from January 1996 through April 1999 on a program of research to investigate the physical mechanisms that underlie the transport of trace constituents in the stratosphere-troposphere system. The primary scientific goal of the research has been to identify the processes which transport air masses within the lower stratosphere, particularly between the tropics and middle latitudes. This research was conducted in collaboration with the Subsonic Assessment (SASS) of the NASA Atmospheric Effects of Radiation Program (AEAP) and the Upper Atmospheric Research Program (UARP). The SASS program sought to understand the impact of the present and future fleets of conventional jet traffic on the upper troposphere and lower stratosphere, while complementary airborne observations under UARP seek to understand the complex interactions of dynamical and chemical processes that affect the ozone layer. The present investigation contributed to the goals of each of these by diagnosing the history of air parcels intercepted by NASA research aircraft in UARP and AEAP campaigns. This was done by means of a blend of trajectory analyses and tracer correlation techniques.

The Origins of Air Parcels Uplifted in a Two Dimensional Gravity Wave in the Tropical Upper Troposphere During the NASA Stratosphere Troposphere Exchange Project (STEP)

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.; Pfister, Leonhard; Chan, K. Roland; Kritz, Mark; Kelly, Ken

1989-01-01

During January and February 1987, as part of the Stratosphere-Troposphere Exchange Project, the NASA ER-2 made 11 flights from Darwin, Australia to investigate dehydration mechanisms in the vicinity of the tropical tropopause. After the monsoon onset in the second week of January, steady easterly flow of 15-25 ms (exp -1) was established in the upper troposphere and lower stratosphere over northern Australia and adjacent seas. Penetrating into this regime were elements of the monsoon convection such as overshooting convective turrets and extensive anvils including cyclone cloud shields. In cases of the latter, the resulting flow obstructions tended to produce mesoscale gravity waves. In several instances the ER- 2 meteorological and trace constituent measurements provide a detailed description of the structure of these gravity waves. Among these was STEP Flight 6, 22-23 January. It is of particular interest to STEP because of the close proximity of ice-laden and dehydrated air on the same isentropic surfaces. Convective events inject large amounts of ice into the upper troposphere and lower stratosphere which may not be completely removed by local precipitation processes. In the present instance, a gravity wave for removed from the source region appears to induce relativity rapid upward motion in the ice-laden air and subsequent dessication. Potential mechanisms for such a localized removal process are under investigation.

Mesoscale Simulations of Gravity Waves During the 2008-2009 Major Stratospheric Sudden Warming

NASA Technical Reports Server (NTRS)

Limpasuvan, Varavut; Alexander, M. Joan; Orsolini, Yvan J.; Wu, Dong L.; Xue, Ming; Richter, Jadwiga H.; Yamashita, Chihoko

2011-01-01

A series of 24 h mesoscale simulations (of 10 km horizontal and 400 m vertical resolution) are performed to examine the characteristics and forcing of gravity waves (GWs) relative to planetary waves (PWs) during the 2008-2009 major stratospheric sudden wam1ing (SSW). Just prior to SSW occurrence, widespread westward propagating GWs are found along the vortex's edge and associated predominantly with major topographical features and strong near-surface winds. Momentum forcing due to GWs surpasses PW forcing in the upper stratosphere and tends to decelerate the polar westerly jet in excess of 30 m/s/d. With SSW onset, PWs dominate the momentum forcing, providing decelerative effects in excess of 50 m/s/d throughout the upper polar stratosphere. GWs related to topography become less widespread largely due to incipient wind reversal as the vortex starts to elongate. During the SSW maturation and early recovery, the polar vortex eventually splits and both wave signatures and forcing greatly subside. Nonetheless, during SSW, westward and eastward propagating GWs are found in the polar region and may be generated in situ by flow adjustment processes in the stratosphere or by secondary GW breaking. The simulated large-scale features agree well with those resolved in satellite observations and analysis products.

Inorganic Chlorine Partitioning in the Summer Lower Stratosphere: Modeled and Measured [ClONO2/HCl] During POLARIS

NASA Technical Reports Server (NTRS)

Voss, P. B.; Stimpfle, R. M.; Cohen, R. C.; Hanisco, T. F.; Bonne, G. P.; Perkins, K. K.; Lanzendorf, E. J.; Anderson, J. G.; Salawitch, R. J.

2001-01-01

We examine inorganic chlorine (Cly) partitioning in the summer lower stratosphere using in situ ER-2 aircraft observations made during the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) campaign. New steady state and numerical models estimate [ClONO2]/[HCl] using currently accepted photochemistry. These models are tightly constrained by observations with OH (parameterized as a function of solar zenith angle) substituting for modeled HO2 chemistry. We find that inorganic chlorine photochemistry alone overestimates observed [ClONO2]/[HCl] by approximately 55-60% at mid and high latitudes. On the basis of POLARIS studies of the inorganic chlorine budget, [ClO]/[ClONO2], and an intercomparison with balloon observations, the most direct explanation for the model-measurement discrepancy in Cly partitioning is an error in the reactions, rate constants, and measured species concentrations linking HCl and ClO (simulated [ClO]/[HCl] too high) in combination with a possible systematic error in the ER-2 ClONO2 measurement (too low). The high precision of our simulation (+/-15% 1-sigma for [ClONO2]/[HCl], which is compared with observations) increases confidence in the observations, photolysis calculations, and laboratory rate constants. These results, along with other findings, should lead to improvements in both the accuracy and precision of stratospheric photochemical models.

Upper atmosphere pollution measurements (GASP)

NASA Technical Reports Server (NTRS)

Rudey, R. A.; Holdeman, J. D.

1975-01-01

The environmental effects are discussed of engine effluents of future large fleets of aircraft operating in the stratosphere. Topics discussed include: atmospheric properties, aircraft engine effluents, upper atmospheric measurements, global air sampling, and data reduction and analysis

The reactions of O(ID) and OH with CH3OH, oxidation of the HCO radial, and the photochemical oxidation of formaldehyde. [photochemical reactions in stratosphere

NASA Technical Reports Server (NTRS)

Osif, T. L.

1976-01-01

An experimental, laboratory study of the various photochemical reactions that can occur in the mesosphere and stratosphere is presented. N2O was photolyzed at 2139 A in the presence of CH3OH and CO. The O(id) produced in the photolysis reacted with CH3OH to produce OH radicals, and thus the reactions of both O(id) and OH were able to be studied. Also considered was the oxidation of the HCO radical. Mixtures of Cl2, O2, H2CO, and sometimes N2 or He were irradiated at 3660 A at several temperatures to photodecompose the Cl2. The photochemical oxidation of formaldehyde was studied as follows: formaldehyde in the presence of N2 and/or O2 (usually dry air) was photolyzed with a medium pressure Hg lamp used in conjunction with various filters which transmit different relative amounts of Hg lines from 2894 A to 3660 A. Results are presented and discussed, along with a description of experimental procedures and apparatus, and chemical reaction kinetics.

The Ozone Budget in the Upper Troposphere from Global Modeling Initiative (GMI)Simulations

NASA Technical Reports Server (NTRS)

Rodriquez, J.; Duncan, Bryan N.; Logan, Jennifer A.

2006-01-01

Ozone concentrations in the upper troposphere are influenced by in-situ production, long-range tropospheric transport, and influx of stratospheric ozone, as well as by photochemical removal. Since ozone is an important greenhouse gas in this region, it is particularly important to understand how it will respond to changes in anthropogenic emissions and changes in stratospheric ozone fluxes.. This response will be determined by the relative balance of the different production, loss and transport processes. Ozone concentrations calculated by models will differ depending on the adopted meteorological fields, their chemical scheme, anthropogenic emissions, and treatment of the stratospheric influx. We performed simulations using the chemical-transport model from the Global Modeling Initiative (GMI) with meteorological fields from (It)h e NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM), (2) the atmospheric GCM from NASA's Global Modeling and Assimilation Office(GMAO), and (3) assimilated winds from GMAO . These simulations adopt the same chemical mechanism and emissions, and adopt the Synthetic Ozone (SYNOZ) approach for treating the influx of stratospheric ozone -. In addition, we also performed simulations for a coupled troposphere-stratosphere model with a subset of the same winds. Simulations were done for both 4degx5deg and 2degx2.5deg resolution. Model results are being tested through comparison with a suite of atmospheric observations. In this presentation, we diagnose the ozone budget in the upper troposphere utilizing the suite of GMI simulations, to address the sensitivity of this budget to: a) the different meteorological fields used; b) the adoption of the SYNOZ boundary condition versus inclusion of a full stratosphere; c) model horizontal resolution. Model results are compared to observations to determine biases in particular simulations; by examining these comparisons in conjunction with the derived budgets, we may pinpoint deficiencies in the representation of chemical/dynamical processes.

Stratospheric Tracers of Atmospheric Transport (STRAT) Campaign: ER-2 Participation

NASA Technical Reports Server (NTRS)

Anderson, James G.

1999-01-01

The NASA Stratospheric Tracers of Atmospheric Transport (STRAT) mission was initiated to advance knowledge of the major transport mechanisms of the upper troposphere-lower stratosphere. This is the region of the atmosphere within which exchange processes take place that critically determine the response of the climate system and ozone distribution to changing conditions triggered by the release of chemicals at the surface. The mission series that extended from October 1995 to November 1997 was extremely successful. The scientific advances that emerged from that mission include analyses of- troposphere-to-stratosphere transport in the lowermost stratosphere from measurements of H2O, CO2, N2O, and O3; the effects of tropical cirrus clouds on the abundance of lower stratospheric ozone; the role of HO, in super- and subsonic aircraft exhaust plumes; and dehydration and denitrification in the arctic polar vortex during the 1995-96 winter.

Stratospheric Tracers of Atmospheric Transport (STRAT) Campaign: ER-2 Participation

NASA Technical Reports Server (NTRS)

Anderson, James G.

1995-01-01

The NASA Stratospheric Tracers of Atmospheric Transport (STRAT) mission was initiated to advance knowledge of the major transport mechanisms of the upper troposphere-lower stratosphere. This is the region of the atmosphere within which exchange processes take place that critically determine the response of the climate system and ozone distribution to changing conditions triggered by the release of chemicals at the surface. The mission series that extended from October 1995 to November 1997 was extremely successful. The scientific advances that emerged from that mission include analyses of: (1)troposphere-to-stratosphere transport in the lowermost stratosphere from measurements of H2O, CO2, N2O, and O3; (2) the effects of tropical cirrus clouds on the abundance of lower stratospheric ozone; and (3) the role of HO(x) in super- and subsonic aircraft exhaust plumes; and dehydration and denitrification in the arctic polar vortex during the 1995-96 winter.

Origins of tropospheric ozone interannual variation (IAV) over Réunion: A model investigation.

PubMed

Liu, Junhua; Rodriguez, Jose M; Thompson, Anne M; Logan, Jennifer A; Douglass, Anne R; Olsen, Mark A; Steenrod, Stephen D; Posny, Francoise

2016-01-16

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Réunion Island (21.1°S, 55.5°E) in June-August. Here we examine possible causes of the observed ozone variation at Réunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model (GMI-CTM) for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Réunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange (STE). Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Réunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Réunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited to the lower troposphere near the surface in August - September.

Origins of tropospheric ozone interannual variation (IAV) over Réunion: A model investigation

PubMed Central

Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Francoise

2018-01-01

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Réunion Island (21.1°S, 55.5°E) in June-August. Here we examine possible causes of the observed ozone variation at Réunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model (GMI-CTM) for 1992–2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Réunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange (STE). Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Réunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Réunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited to the lower troposphere near the surface in August – September. PMID:29657911

A latitudinal survey of mesospheric and upper stratospheric water vapor

NASA Technical Reports Server (NTRS)

Croskey, C. L.; Martone, J. P.; Olivero, J. J.; Puliafito, S. E.

1994-01-01

As part of the LAtitudinal DIstribution of Middle Atmosphere Structure (LADIMAS) campaign, measurements of mesospheric and upper stratospheric water vapor concentration were made over a latitudinal range from 53 N to 63 S. The 22-GHz emission line of water vapor was observed by a new, portable, cryogenically cooled microwave radiometer that was carried on board the German research vessel Polarstern as it sailed from Bremerhaven, Germany, to the Antarctic during November and December, 1991. Water vapor profiles were obtained at approximately 5 deg latitude intervals for an altitude range of 40 to 80 km.

Stratospheric Influence on Summer Monsoon and Associated Planetary Wave Breaking and Mixing in the Subtropical Tropopause Region

NASA Astrophysics Data System (ADS)

Lubis, S. W.; Nakamura, N.

2017-12-01

Previous studies have shown that the monsoonal circulation plays an important role in planetary wave breaking (PWB). The highest frequency of breaking events occurs just downstream (east) of the monsoon region in summer. PWB induces mixing of potential vorticity (PV) and hence, alter the horizontal mixing in the atmosphere. Here, the authors hypothesize that the stratospheric easterlies in the boreal summer also play a significant role in the PWB and mixing associated with the summer monsoon. If the stratospheric winds were westerly in boreal summer, the frequency of PWB would be decreased due to more waves penetrating in the stratosphere, resulting in less horizontal PWB and thus reduced mixing in the subtropical tropopause region. The hypothesis is examined by using a set of idealized moist GFDL simulations. The monsoon circulation is produced by adding a land-sea contrast with a Gaussian-shaped mountains positioned in the midlatitudes. Other key ingredients for the monsoon, including albedo, oceanic warm pool, and Q-flux, were also ideally imposed in all simulations. Our control simulation produces a summer monsoon-like circulation similar to the observation. In particular, the thermally forced monsoonal circulation forms a prominent closed upper-level anticyclone that dominates the summertime upper-level flow. Associated with this circulation is an upward-bulging tropopause that forms a large reservoir of anomalously low PV. Consistent with previous studies, the well-defined tropospheric jet lies just poleward of the upper-level anticyclone, and acts as a dynamical barrier between the low-PV reservoir over the monsoonal region and the high-PV reservoir in the extratropics. This barrier disappears just northeast of the monsoon area in the jet exit region, allowing more quasi-planetary waves to break in this region. Repetitive wave breaking further weakens the PV gradient, leading to the formation of the surf zone and stronger mixing in this region. To quantify the role of the stratospheric circulation in the PWB and mixing associated with the summer monsoon, we add an artificial local cooling in the stratosphere and thereby preserve the stratospheric westerlies in summer. The extent to which PWB and mixing are modified by the presence of stratospheric westerlies will be discussed.

Global features of the semiannual oscillation in stratospheric temperatures and comparison between seasons and hemispheres

NASA Technical Reports Server (NTRS)

Gao, Xin-Hai; Yu, Wen-Bi; Stanford, John L.

1987-01-01

Four years of satellite-derived microwave and infrared radiances are analyzed for the three-dimensional and seasonal variation of semiannual oscillations (SAO) in stratospheric temperatures, with particular focus on high latitudes, to investigate the effect of stratospheric warmings on SAO. Separate analyses of individual seasons in each hemisphere reveal that the strongest SAO in temperature occur in the Northern Hemisphere (NH) winter polar upper stratosphere. These results, together with the latitudinal structure of the temperature SAO and the fact that the NH polar SAO is nearly out of phase with the lower latitude SAO, are consistent with the existence of a global-scale, meridional circulation on the SAO time scale. The results suggest that polar stratospheric warmings are an important source of SAO in both high and low latitude stratospheric temperature fields. Interannual variations, three-dimensional phase structure, and zonal asymmetry of SAO are also detailed. The SH stratospheric SAO is dominated by a localized feature in the high-latitude, eastern hemisphere which tilts westward with height.

Is there any chlorine monoxide in the stratosphere?

NASA Technical Reports Server (NTRS)

Mumma, M. J.; Rogers, J. D.; Kostiuk, T.; Deming, D.; Hillman, J. J.; Zipoy, D.

1983-01-01

A ground-based search for stratospheric 35-ClO was carried out using an infrared heterodyne spectrometer in the solar absorption mode. Lines due to stratospheric HNO3 and tropospheric OCS were detected at about 0.2% absorptance levels, but the expected 0.1% lines of ClO in this same region were not seen. We find that stratospheric ClO is at least a factor of seven less abundant than is indicated by in situ measurements, and we set an upper limit of 2.3x10 to the 13th molecules/sq cm at the 95% confidence level for the integrated vertical column density of ClO. Our results imply that the release of chlorofluorocarbons may be significantly less important for the destruction of stratospheric ozone (O3) than is currently thought.

Modeling the Chemical Effect of Tropopause-penetrating Convection using NEXRAD Observations

NASA Astrophysics Data System (ADS)

Clapp, C.; Anderson, J. G.

2017-12-01

Water vapor in the upper troposphere and lower stratosphere (UTLS) from the tropics to the poles is important both radiatively and chemically. Chemically, water vapor is the dominant source of OH in the lower stratosphere, and increases in water vapor concentrations promote stratospheric ozone loss by raising the reactivity of several key heterogeneous reactions as well as by promoting the growth of reactive surface area. We examine the chemical impact of the convective contribution of boundary layer air to stratospheric chemistry over the mid-latitude United States. Using NEXRAD observations of tropopause penetrating events during the summers of 2004 through 2013 (with approximately 3300 events reaching 390K in potential temperature per year), we calculate the loss of stratospheric ozone due to an average event and the seasonal impact.

NOy production, ozone loss and changes in net radiative heating due to energetic particle precipitation in 2002-2010

NASA Astrophysics Data System (ADS)

Sinnhuber, Miriam; Berger, Uwe; Funke, Bernd; Nieder, Holger; Reddmann, Thomas; Stiller, Gabriele; Versick, Stefan; von Clarmann, Thomas; Maik Wissing, Jan

2018-01-01

We analyze the impact of energetic particle precipitation on the stratospheric nitrogen budget, ozone abundances and net radiative heating using results from three global chemistry-climate models considering solar protons and geomagnetic forcing due to auroral or radiation belt electrons. Two of the models cover the atmosphere up to the lower thermosphere, the source region of auroral NO production. Geomagnetic forcing in these models is included by prescribed ionization rates. One model reaches up to about 80 km, and geomagnetic forcing is included by applying an upper boundary condition of auroral NO mixing ratios parameterized as a function of geomagnetic activity. Despite the differences in the implementation of the particle effect, the resulting modeled NOy in the upper mesosphere agrees well between all three models, demonstrating that geomagnetic forcing is represented in a consistent way either by prescribing ionization rates or by prescribing NOy at the model top.Compared with observations of stratospheric and mesospheric NOy from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument for the years 2002-2010, the model simulations reproduce the spatial pattern and temporal evolution well. However, after strong sudden stratospheric warmings, particle-induced NOy is underestimated by both high-top models, and after the solar proton event in October 2003, NOy is overestimated by all three models. Model results indicate that the large solar proton event in October 2003 contributed about 1-2 Gmol (109 mol) NOy per hemisphere to the stratospheric NOy budget, while downwelling of auroral NOx from the upper mesosphere and lower thermosphere contributes up to 4 Gmol NOy. Accumulation over time leads to a constant particle-induced background of about 0.5-1 Gmol per hemisphere during solar minimum, and up to 2 Gmol per hemisphere during solar maximum. Related negative anomalies of ozone are predicted by the models in nearly every polar winter, ranging from 10-50 % during solar maximum to 2-10 % during solar minimum. Ozone loss continues throughout polar summer after strong solar proton events in the Southern Hemisphere and after large sudden stratospheric warmings in the Northern Hemisphere. During mid-winter, the ozone loss causes a reduction of the infrared radiative cooling, i.e., a positive change of the net radiative heating (effective warming), in agreement with analyses of geomagnetic forcing in stratospheric temperatures which show a warming in the late winter upper stratosphere. In late winter and spring, the sign of the net radiative heating change turns to negative (effective cooling). This spring-time cooling lasts well into summer and continues until the following autumn after large solar proton events in the Southern Hemisphere, and after sudden stratospheric warmings in the Northern Hemisphere.

Electronic excitation of carbonyl sulphide (COS) by high-resolution vacuum ultraviolet photoabsorption and electron-impact spectroscopy in the energy region from 4 to 11 eV

DOE Office of Scientific and Technical Information (OSTI.GOV)

Limão-Vieira, P., E-mail: plimaovieira@fct.unl.pt; Department of Physics, Sophia University, Tokyo 102-8554; Department of Physical Sciences, The Open University, Walton Hall, Milton Keynes MK7 6AA

2015-02-14

The electronic state spectroscopy of carbonyl sulphide, COS, has been investigated using high resolution vacuum ultraviolet photoabsorption spectroscopy and electron energy loss spectroscopy in the energy range of 4.0–10.8 eV. The spectrum reveals several new features not previously reported in the literature. Vibronic structure has been observed, notably in the low energy absorption dipole forbidden band assigned to the (4π←3π) ({sup 1}Δ←{sup 1}Σ{sup +}) transition, with a new weak transition assigned to ({sup 1}Σ{sup −}←{sup 1}Σ{sup +}) reported here for the first time. The absolute optical oscillator strengths are determined for ground state to {sup 1}Σ{sup +} and {sup 1}Πmore » transitions. Based on our recent measurements of differential cross sections for the optically allowed ({sup 1}Σ{sup +} and {sup 1}Π) transitions of COS by electron impact, the optical oscillator strength f{sub 0} value and integral cross sections (ICSs) are derived by applying a generalized oscillator strength analysis. Subsequently, ICSs predicted by the scaling are confirmed down to 60 eV in the intermediate energy region. The measured absolute photoabsorption cross sections have been used to calculate the photolysis lifetime of carbonyl sulphide in the upper stratosphere (20–50 km)« less

A climatology of stratospheric aerosol

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hitchman, M.H.; Mckay, M.; Trepte, C.R.

1994-10-01

A global climatology of stratospheric aerosol is created by combining nearly a decade (1979-1981 and 1984-1990) of contemporaneous observations from the Stratospheric Aerosol and Gas Experiment (SAGE I and II) and Stratospheric Aerosol Measurement (SAM II) instruments. One goal of this work is to provide a representative distribution of the aerosol layer for use in radiative and chemical modeling. A table of decadal average 1 micron extinction values is included, extending from the tropopause to 35 km and 80 deg S to 85 deg N, which allows estimation of surface area density. We find that the aerosol layer is distinctlymore » volcanic in nature and suggest that the decadal average is a more useful estimate of future aerosol loading than a `background` loading, which is never clearly achieved during the data record. This climatology lends insight into the general circulation of the stratosphere. Latitude - altitude sections of extinction radio at 1 micron are shown, average by decade, season, and phase of the quasi-biennial oscillation (QBO). A tropical reservoir region is diagnosed, with an `upper` and a `lower` transport regime. In the tropics above 22 km (upper regime), enhanced lofting occurs in the summer, with suppressed lofting or eddy dilution in the winter. In the extratropics within two scale heights of the tropopause (lower regime), poleward and downward transport is most robust during winter, especially in the northern hemisphere. The transport patterns persist into the subsequent equinoctial season. Ascent associated with QBO easterly shear favors detrainment in the upper regime, while relative descent and poleward spreading during QBO westerly shear favors detrainment in the lower regime. Extinction radio differences between the winter-spring and summer-fall hemispheres, and differences between the two phases of the QBO, are typically 20-50%.« less

Reanalysis of the Stratosphere in GEOS-5: Lessons Learned from MERRA and Future Prospects

NASA Technical Reports Server (NTRS)

Pawson, Steven

2011-01-01

The MERRA configuration of GEOS-5 includes about 30 layers in the middle atmosphere, with an upper boundary near 80km. Stratospheric Sounding Unit (SSU) and Advanced microwave sounding unit ( AMSU) radiance data are assimilated, which yield good constraints on the analyses up to the upper stratosphere. This paper examines the performance of MERRA, with foci on: the somewhat erratic system behavior in the 1980s, as numerous SSU instruments were available for short periods; the transition from SSU to AMSU radiances; conflicts between equivalent instruments on different platforms, given in the context of bias correction and the diurnal cycle; and, the relative stability of the analyses in the 21st Century. The results from MERRA provide guidance for how to use the operational polar-orbiting datasets in future reanalyses. Additional discussion will be directed at the possible use of research data sets, from limb-sounding instruments, in future multi-decadal products.

An "island" in the stratosphere - on the enhanced annual variation of water vapour in the middle and upper stratosphere in the southern tropics and subtropics

NASA Astrophysics Data System (ADS)

Lossow, Stefan; Garny, Hella; Jöckel, Patrick

2017-09-01

The amplitude of the annual variation in water vapour exhibits a distinct isolated maximum in the middle and upper stratosphere in the southern tropics and subtropics, peaking typically around 15° S in latitude and close to 3 hPa (˜ 40.5 km) in altitude. This enhanced annual variation is primarily related to the Brewer-Dobson circulation and hence also visible in other trace gases. So far this feature has not gained much attention in the literature and the present work aims to add more prominence. Using Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) observations and ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg/Modular Earth Submodel System) Atmospheric Chemistry (EMAC) simulations we provide a dedicated illustration and a full account of the reasons for this enhanced annual variation.

Concentrations of ethane (C2H6) in the lower stratosphere and upper troposphere and acetylene (C2H2) in the upper troposphere deduced from Atmospheric Trace Molecule Spectroscopy/Spacelab 3 spectra

NASA Technical Reports Server (NTRS)

Rinsland, C. P.; Russell, J. M., III; Zander, R.; Farmer, C. B.; Norton, R. H.

1987-01-01

This paper reports the results of the spectroscopic analysis of C2H6 and C2H2 absorption spectra obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument flown on the Shuttle as part of the Spacelab 3 mission. The spectra were recorded during sunset occultations occurring between 25 deg N and 31 deg N latitudes, yielding volume-mixing ratio profiles of C2H6 in the lower stratosphere and the upper troposphere, and an upper tropospheric profile of C2H2. These results compare well with previous in situ and remote sounding data obtained at similar latitudes and with model calculations. The results demonstrate the feasibility of the ATMOS instrument to sound the lower atmosphere from space.

The photochemistry and kinetics of chlorine compounds important to stratospheric mid-latitude ozone destruction

NASA Astrophysics Data System (ADS)

Goldfarb, Leah

1997-09-01

The catalytic destruction of stratospheric ozone via chlorinated species was first proposed in the 1970's. Since that time a decline in column ozone abundance in the polar regions as well as at mid-latitudes has been observed. Much of this reduction has been attributed to the increases in anthropogenic chlorine compounds such as CFCs. This study summarizes experimental results obtained using pulsed-photolysis resonance fluorescence and pulsed- photolysis long-path absorption methods to study processes important to chlorine-catalyzed ozone destruction: the quantum yields of the products in the dissociation of ClONO2 and the reactions of free radicals with ClONO2 and ClO. The quantum yields for the production of O, Cl and ClO from ClONO2 were studied at specific laser wavelengths (193, 222, 248, and 308 nm). Cl and ClO yields were comparable at nearly all the wavelengths, expect for 193 nm, where the O atom yield was appreciable. The yields at 308 nm (a wavelength available in the stratosphere) were 0.64 ± 0.17 for Cl, 0.37 ± 0.18 for ClO and <0.05 for O. The rate coefficients of O and Cl atoms with ClONO2 were measured over a wide range of temperatures, and the NO3 product yield for the former reaction, previously unreported, was determined to be ~1. The kinetics of the reaction of O atoms with ClO were measured using a new experimental system built specifically to investigate such radical-radical reactions. A slight negative temperature dependence (E/B = -90 ± 30) was observed over the temperature range (227-363 K). From the measured Arrhenius equation the rate constant at 240 K is 4.1 × 10-11 cm3molecule-1s-1 which is in excellent agreement (l.4% greater) with the currently recommended value. This observation is significant, since this reaction is the rate limiting the dominate chlorine catalytic cycle that destroys O3 near 40 km. To analyze the implications of the kinetic and photochemical information from this work, a box model was constructed. The vertical profile of ozone concentrations and loss rates calculated by this simple model compare well with atmospheric measurements and calculations.

Evaluation of the tropospheric flows to a major Southern Hemisphere stratospheric warming event using NCEP/NCAR Reanalysis data with a PSU/NCAR nudging MM5V3 model

NASA Astrophysics Data System (ADS)

Wang, K.

2008-04-01

Previous studies of the exceptional 2002 Southern Hemisphere (SH) stratospheric warming event lead to some uncertainty, namely the question of whether excessive heat fluxes in the upper troposphere and lower stratosphere are a symptom or cause of the 2002 SH warming event. In this work, we use a hemispheric version of the MM5 model with nudging capability and we devised a novel approach to separately test the significance of the stratosphere and troposphere for this year. We paired the flow conditions from 2002 in the stratosphere and troposphere, respectively, against the conditions in 1998 (a year with displaced polar vortex) and in 1948 (a year with strong polar vortex that coincided with the geographical South Pole). Our experiments show that the flow conditions from below determine the stratospheric flow features over the polar region. Regardless of the initial stratospheric conditions in 1998 or 1948, when we simulated these past stratospheres with the troposphere/lower stratosphere conditions constrained to 2002 levels, the simulated middle stratospheres resemble those observed in 2002 stratosphere over the polar region. On the other hand, when the 2002 stratosphere was integrated with the troposphere/lower stratosphere conductions constrained to 1948 and 1998, respectively, the simulated middle stratospheric conditions over the polar region shift toward those of 1948 and 1998. Thus, our experiments further support the wave-forcing theory as the cause of the 2002 SH warming event.

In-situ measurements of chlorine activation, nitric acid redistribution and ozone depletion in the Antarctic lower vortex aboard the German research aircraft HALO during TACTS/ESMVal

NASA Astrophysics Data System (ADS)

Jurkat, Tina; Voigt, Christiane; Kaufmann, Stefan; Schlage, Romy; Gottschaldt, Klaus-Dirk; Ziereis, Helmut; Hoor, Peter; Bozem, Heiko; Müller, Stefan; Zahn, Andreas; Schlager, Hans; Oelhaf, Hermann; Sinnhuber, Björn-Martin; Dörnbrack, Andreas

2016-04-01

In-situ measurements of stratospheric chlorine compounds are rare and exhibit the potential to gain insight into small scale mixing processes where stratospheric air masses of different origin and history interact. In addition, the relationship with chemically stable trace gases helps to identify regions that have been modified by chemical processing on polar stratospheric clouds. To this end, in-situ measurements of ClONO2, HCl, HNO3, NOy, N2O and O3 have been performed in the Antarctic Polar Vortex in September 2012 aboard the German research aircraft HALO (High Altitude and Long Rang research aircraft) during the TACTS/ESMVal (Transport and Composition in the UTLS/Earth System Model Validation) mission. With take-off and landing in Capetown, HALO sampled vortex air with latitudes down to 65°S, at altitudes between 8 and 14.3 km and potential temperatures between 340 and 390 K. Before intering the vortex at 350 K potential temperature, HALO additionally sampled mid-latitude stratospheric air. The trace gas distributions at the edge of the Antarctic polar vortex show distinct signatures of processed upper stratospheric vortex air and chemically different lower stratospheric / upper tropospheric air. Diabatic descend of the vortex transports processed air into the lower stratosphere. Here small scale filaments of only a few kilometers extension form at the lower vortex boundary due to shear stress, ultimately leading to transport and irreversible mixing. Comparison of trace gas relationships with those at the beginning of the polar winter reveals substantial chlorine activation, ozone depletion de- and renitrification with high resolution. Furthermore, the measurements are compared to the chemistry climate models EMAC and supported by ECMWF analysis. Finally, we compare the Antarctic measurements with new measurements of ClONO2, HCl and HNO3 aboard HALO obtained during the Arctic mission POLSTRACC (POLar STratosphere in a Changing Climate) based in Kiruna (Sveden) and Oberpfaffenhofen (Germany) in winter 2015/16. Our measurements give new insights on the lower Arctic and Antarctic stratospheric composition impacted by polar stratospheric clouds and ozone depletion as well as mixing of mid- and high-latitude air.

Analysis of the origins and implications of the O-18 content of stratospheric water vapor

NASA Technical Reports Server (NTRS)

Kaye, Jack A.

1990-01-01

Factors influencing the O-18 content of stratospheric H2O are reviewed in order to provide a theoretical framework for the interpretation of measurements of this quantity, which are now becoming available. Depletions in O-18 of 5-10 percent in stratospheric H2O are expected based on the known correlation between that of D and O-18 in tropospheric H2O and observed measurements of large (typically 50 percent) depletions of D in stratosphere H2O. H2O formed in the stratosphere as a result of oxidation of CH4 can be expected to reflect primarily the O-18 content of stratospheric O2, which is the same as that of tropospheric O2 (slightly enhanced with respect to standard mean ocean water). Thus, a reduction in the O-18 depletion is expected with increasing altitude, but not a large enhancement in O-18 in upper stratospheric H2O as found in recent far infrared measurements. The observed large enhancement of O-18 in stratospheric O3 is not expected to be reflected in stratospheric H2O. Necessary laboratory data for the improved quantification of these effects are reviewed.

Photochemistry, mixing and transport in Jupiter’s stratosphere constrained by Cassini

NASA Astrophysics Data System (ADS)

Hue, Vincent; Hersant, Franck; Cavalié, Thibault; Dobrijevic, Michel

2015-11-01

Jupiter’s obliquity and eccentricity drive the seasonal forcing on its atmosphere. The seasonal variations on its stratospheric temperature through radiative heating and composition through photochemistry are smaller than for Saturn, due to a lower obliquity and eccentricity. Although the physical conditions in these two planets are different, the stratospheric photochemistry is initiated and controlled by the methane photolysis [1]. We adapted a 2D (altitude-latitude) seasonal photochemical model of Saturn [2] to Jupiter. We compare the seasonal effects on the atmospheric composition between these two planets. We use previous 1D photochemical models for the vertical mixing efficiency [1,3] and recent Cassini observations to constrain the meridional mixing efficiency and transport processes [4,5,6].Cassini’s flyby of Jupiter has allowed mapping its stratospheric temperature as a function of latitude [7]. It has also revealed the meridional distribution of hydrocarbons [8,9], which were suggested by earlier studies [10,4]. Previous models suggest that vertical mixing alone is not sufficient to reproduce the observations of C2H2 and C2H6 [5,6], and that meridional mixing is needed. We show that, in addition to meridional mixing, advective circulation is required to reproduce Cassini observations of C2H6. Preliminary results from our model suggest an equator-to-pole circulation cell in Jupiter’s stratosphere, around 30-0.01 mbar.References[1] Moses et al., 2005. JGR 110, 8001.[2] Hue et al., 2015. Icarus 257, 163-184.[3] Gladstone et al., 1996. Icarus 119, 1-52.[4] Kunde et al., 2004. Science 305, 1582-1587.[5] Liang et al., 2005. ApJ Lett. 635, L177-L180.[6] Lellouch et al., 2006. Icarus 184 (2), 478-497.[7] Simon-Miller et al., 2006. Icarus 180 (1), 98-112.[8] Nixon et al., 2007. Icarus 188, 47-71.[9] Nixon et al., 2010. PSS 58, 1667-1680.[10] Maguire et al., 1984. Bulletin of the AAS 16, 647-647.

Oxygen in the stratospheres of the giant planets and Titan

NASA Astrophysics Data System (ADS)

Feuchtgruber, H.; Lellouch, E.; Encrenaz, Th.; Bezard, B.; Coustenis, A.; Drossart, P.; Salama, A.; de Graauw, Th.; Davis, G. R.

1999-03-01

Infrared spectra of the Short-Wavelength Spectrometer (SWS) of ISO at wavelengths between 25 - 45 μm have provided the first detection of stratospheric H2O on all four giant planets and Titan. Together with SWS observations of CO2 at 14.98 μm, leading to first detections on Neptune, Saturn and Jupiter an external source of oxygen is required to explain the derived upper stratospheric mixing ratios of up to several ppb at mbar-μbar levels. We provide an overview on the required amounts of external oxygen fluxes and a detailed discussion on the various scenarios for the origin of CO2 in the stratospheres of the giant planets.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Penner, J.E.; Chang, J.S.

Changes in ozone, temperature, and other minor constituents resulting from eleven year variations in the solar flux between 180 and 340 nm are presented. Results were computed using a one-dimensional time dependent model that allows for all major feedbacks and time delays which may result from changing photolysis rates in the O/sub x/--NO/sub x/--HO/sub x/--ClO/sub x/ system. Since the 1950's the chlorine content of the stratosphere has been increasing. The effect of this increase on ozone variability during the last two solar cycles is analyzed. Expected variations in O/sub 3/ and temperature resulting from changes in the uv flux aremore » compared to available measurements.« less

Stratospheric ClO and ozone from the Microwave Limb Sounder on the Upper Atmosphere Research Satellite

NASA Technical Reports Server (NTRS)

Waters, J. W.; Froidevaux, L.; Read, W. G.; Manney, G. L.; Elson, L. S.; Flower, D. A.; Jarnot, R. F.; Harwood, R. S.

1993-01-01

Concentrations of atmospheric ozone and of ClO (the predominant form of reactive chlorine responsible for stratospheric ozone depletion) are reported for both the Arctic and Antarctic winters of the past 18 months. Chlorine in the lower stratosphere was almost completely converted to chemically reactive forms in both the northern and southern polar winter vortices. This occurred in the south long before the development of the Antarctic ozone hole, suggesting that ozone loss can be masked by influx of ozone-rich air.

Horizontal mixing coefficients for two-dimensional chemical models calculated from National Meteorological Center Data

NASA Technical Reports Server (NTRS)

Newman, P. A.; Schoeberl, M. R.; Plumb, R. A.

1986-01-01

Calculations of the two-dimensional, species-independent mixing coefficients for two-dimensional chemical models for the troposphere and stratosphere are performed using quasi-geostrophic potential vorticity fluxes and gradients from 4 years of National Meteorological Center data for the four seasons in both hemispheres. Results show that the horizontal mixing coefficient values for the winter lower stratosphere are broadly consistent with those currently employed in two-dimensional models, but the horizontal mixing coefficient values in the northern winter upper stratosphere are much larger than those usually used.

Balloon stratospheric research flights, April 1976 to December 1976

NASA Technical Reports Server (NTRS)

Allen, N. C.

1977-01-01

These flights were designed to measure the vertical concentration profile of trace stratospheric species which form major links in the chlorine photochemical system of the upper atmosphere, to measure the vertical concentration profiles of atomic oxygen, the hydroxyl radical and ozone in the stratosphere. An overview of the scientific goals of the program, a statement of program management and support functions, a brief description of the instrumentation flown, pertinent engineering and payload operations data, and a summary of the scientific data obtained for four flights are presented.

Seasonal variations of water vapor in the tropical lower statosphere

NASA Technical Reports Server (NTRS)

Mote, Philip W.; Rosenlof, Karen H.; Holton, James R.; Harwood, Robert S.; Waters, Joe W.

1995-01-01

Measurments of stratospheric water vapor by the Microwave Limb Sounder (MLS) aboard the Upper Atmosphere Research Satellite (UARS) show that in the tropical lower statosphere, low-frequency variations are closely related to the annual cycle in tropical tropopause temperatures. Tropical stratospheric air appears to retain information about the tropopause conditions it enconters for over a year as it rises through the stratosphere. A two-dimensional Lagrangian model is used to relate MLS measurements to the temperature that tropical air parcels encounter when crossing the 100 hPa surface.

Scale Invariance of High Altitude Aircraft Observations in the Upper Troposphere and Lower Stratosphere at Tropical and Subtropical Latitudes

NASA Technical Reports Server (NTRS)

Mahoney, M.; Hovde, S.; Kelly, K.; Proffitt, M.; Richard, E.; Thompson, T.; Tuck, A.

2000-01-01

Exchange between the upper tropical troposphere and the lower troposphere is considered by examining high altitude aircraft observations of water, ozone, methane, wind and temperature for scale invariance.

Is Ozone Going Up Now?

NASA Astrophysics Data System (ADS)

Steinbrecht, W.; Froidevaux, L.; Davis, S. M.; Degenstein, D. A.; Wild, J.; Roth, C.; Kaempfer, N.; Leblanc, T.; Godin-Beekmann, S.; Vigouroux, C.; Swart, D. P. J.; Querel, R.; Harris, N.; Nedoluha, G. E.

2016-12-01

The last WMO ozone assessment (WMO, 2014) concluded that observations show significant ozone increase, 3% per decade (±2% per decade, 2σ), in the upper stratosphere since 2000. At other levels, or for total ozone, increases were not found or not significant. Overall, this is consistent with expectations from model simulations, (e.g. CCMVal2, Eyring et al., 2010). These simulations indicate that declining chlorine levels and stratospheric cooling due to CO2 increase should contribute roughly equal parts to ozone increase in the upper stratosphere. Shortly after the assessment, results from the SI2N initiative (Harris et al., 2015) confirmed increasing ozone in the upper stratosphere. However, the SI2N results indicated smaller increases (+1.5% per decade) than the WMO assessment, and substantially larger uncertainties (±5% per decade, 2σ). Differences can be attributed to time period, 1998 to 2012, compared to 2000 to 2013/14 for the assessment, and to larger assumed instrumental drift uncertainties, 6% per decade, (only 1 to 2% per decade in WMO 2014, see also Hubert et al., 2016). Here, we explore how additional ground-based and satellite data since 2013, as well as new and improved records, affect ozone trends and uncertainties. The focus will be on ozone in the upper stratosphere, because this is the region where the earliest signs of beginning ozone recovery are expected. ReferencesEyring, V., et al.: Multi-model assessment of stratospheric ozone return dates and ozone recovery in CCMVal-2 models, Atmos. Chem. Phys., 10, 9451-9472, doi:10.5194/acp-10-9451-2010, 2010. Harris, N. R. P., et al.: Past changes in the vertical distribution of ozone - Part 3: Analysis and interpretation of trends, Atmos. Chem. Phys., 15, 9965-9982, doi:10.5194/acp-15-9965-2015, 2015. Hubert, D., et al.: Ground-based assessment of the bias and long-term stability of fourteen limb and occultation ozone profile data records, Atmos. Meas. Tech., 9, 2497-2534, doi:10.5194/amt-9-2497-2016, 2016. WMO 2014: Pawson, S., Steinbrecht, W. et al.: Update on global ozone: Past, present, and future, Chapter 2 in: Scientific Assessment of Ozone Depletion: 2014, Global Ozone Research and Monitoring Project - Report No. 55, World Meteorological Organization, Geneva, Switzerland, 2014.

The NO(x)-HNO3 System in the Lower Stratosphere: Insights from In Situ Measurements and Implications of the J(HNO3)-[OH] Relationship

NASA Technical Reports Server (NTRS)

Perkins, K. K.; Hanisco, T. F.; Cohen, R. C.; Koch, L. C.; Stimpfle, R. M.; Voss, P. B.; Bonne, G. P.; Lanzendorf, E. J.; Anderson, J. G.; Wennberg, P. O.

2001-01-01

During the 1997 Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) mission, simultaneous in situ observations of NOx and HOx radicals, their precursors, and the radiation field were obtained in the lower stratosphere. We use these observations to evaluate the primary mechanisms that control NOx-HNO3 exchange and to understand their control over the partitioning between NO2 and HNO3 in regions of continuous sunlight. We calculate NOx production (PNOx) and loss (LNOx) in a manner directly constrained by the in situ measurements and current rate constant recommendations, using approaches for representing albedo, overhead O3 and [OH] that reduce model uncertainty. We find a consistent discrepancy of 18% between modeled rates of NOx production and loss (LNOx = 1.18P(sub NOx)), which is within the measurement uncertainty of +/- 27%. The partitioning between NOx production processes is [HNO3 + OH (41 +/- 2)%; HNO3 + hv (59 +/- 2)%] and between NOx loss processes is [NO2 + OH, 90% to >97%; BrONO2 + H2O, 10% to <3%]. The steady-state description of NOx-HNO3 exchange reveals the significant influence of the tight correlation between the photolysis rate of HNO3 and [OH] established by in situ measurements throughout the lower stratosphere. Parametrizing this relationship, we find: (1) the steady-state value of [NO2](sub 24h-avg)/[HNO3] in the continuously sunlit, lower stratosphere is a function only of temperature and number density; and (2) the partitioning of NOx production between HNO3 + OH and HNO3 + hv is nearly constant throughout most of the lower stratosphere. We describe a methodology (functions of latitude, day, temperature, and pressure) for accurately predicting the steady-state value of [NO2](sub 24h-avg)/[HNO3] and the partitioning of NOx production within these regions. The results establish a metric to compare observations of [NO2](sub 24h-avg)/[HNO3] within the continuously sunlit region and provide a simple diagnostic for evaluating the accuracy of models that attempt to describe the coupled NOx-HOx photochemistry in the lower stratosphere.

Assessing the Impact of Aircraft Emissions on the Stratosphere

NASA Technical Reports Server (NTRS)

Kawa, S. R.; Anderson, D. E.

1999-01-01

For the past decade, the NASA Atmospheric Effects of Aviation Project (AEAP) has been the U.S. focal point for research on aircraft effects. In conjunction with U.S. basic research programs, AEAP and concurrent European research programs have driven remarkable progress reports released in 1999 [IPCC, 1999; Kawa et al., 1999]. The former report primarily focuses on aircraft effects in the upper troposphere, with some discussion on stratospheric impacts. The latter report focuses entirely on the stratosphere. The current status of research regarding aviation effects on stratospheric ozone and climate, as embodied by the findings of these reports, is reviewed. The following topics are addressed: Aircraft Emissions, Pollution Transport, Atmospheric Chemistry, Polar Processes, Climate Impacts of Supersonic Aircraft, Subsonic Aircraft Effect on the Stratosphere, Calculations of the Supersonic Impact on Ozone and Sensitivity to Input Conditions.

Stratospheric ion and aerosol chemistry and possible links with cirrus cloud microphysics - A critical assessment

NASA Technical Reports Server (NTRS)

Mohnen, Volker A.

1990-01-01

Aspects of stratospheric ion chemistry and physics are assessed as they relate to aerosol formation and the transport of aerosols to upper tropospheric regions to create conditions favorable for cirrus cloud formation. It is found that ion-induced nucleation and other known phase transitions involving ions and sulfuric acid vapor are probably not efficient processes for stratospheric aerosol formation, and cannot compete with condensation of sulfuric acid on preexisting particles of volcanic or meteoritic origin which are larger than about 0.15 micron in radius. Thus, galactic cosmic rays cannot have a significant impact on stratospheric aerosol population. Changes in the stratospheric aerosol burden due to volcanos are up to two orders of magnitude larger than changes in ion densities. Thus, volcanic activity may modulate the radiative properties of cirrus clouds.

Mesoscale disturbances in the tropical stratosphere excited by convection - Observations and effects on the stratospheric momentum budget

NASA Technical Reports Server (NTRS)

Pfister, Leonhard; Scott, Stanley; Loewenstein, Max; Bowen, Stuart; Legg, Marion

1993-01-01

Aircraft temperature and pressure measurements as well as satellite imagery are used to establish the amplitudes and the space and time scale of potential temperature disturbances over convective systems. A conceptual model is proposed for the generation of mesoscale gravity waves by convection. The momentum forcing that a reasonable distribution of convection might exert on the tropical stratosphere through convectively excited mesoscale gravity waves of the observed amplitudes is estimated. Aircraft measurements show that presence of mesoscale disturbances in the lower stratospheric temperature, disturbances that appear to be associated with underlying convection. If the disturbances are convectively excited mesoscale gravity waves, their amplitude is sufficient that their breakdown in the upper stratosphere will exert a zonal force comparable to but probably smaller than the planetary-scale Kelvin waves.

Photolysis of 4-Phenyl-1,3-dioxolan-2-one: An Undergraduate Experiment in Free Radical Chemistry.

ERIC Educational Resources Information Center

White, Rick C.; Ma, Sha

1988-01-01

Describes a photochemistry experiment designed to introduce photochemical techniques and experience free radical chemistry. Selects Nuclear Magnetic Resonance spectroscopy for the analysis. This activity is suggested for use in an upper level undergraduate organic course. (MVL)

Analysis and Hindcast Experiments of the 2009 Sudden Stratospheric Warming in WACCMX+DART

NASA Astrophysics Data System (ADS)

Pedatella, N. M.; Liu, H.-L.; Marsh, D. R.; Raeder, K.; Anderson, J. L.; Chau, J. L.; Goncharenko, L. P.; Siddiqui, T. A.

2018-04-01

The ability to perform data assimilation in the Whole Atmosphere Community Climate Model eXtended version (WACCMX) is implemented using the Data Assimilation Research Testbed (DART) ensemble adjustment Kalman filter. Results are presented demonstrating that WACCMX+DART analysis fields reproduce the middle and upper atmosphere variability during the 2009 major sudden stratospheric warming (SSW) event. Compared to specified dynamics WACCMX, which constrains the meteorology by nudging toward an external reanalysis, the large-scale dynamical variability of the stratosphere, mesosphere, and lower thermosphere is improved in WACCMX+DART. This leads to WACCMX+DART better representing the downward transport of chemical species from the mesosphere into the stratosphere following the SSW. WACCMX+DART also reproduces most aspects of the observed variability in ionosphere total electron content and equatorial vertical plasma drift during the SSW. Hindcast experiments initialized on 5, 10, 15, 20, and 25 January are used to assess the middle and upper atmosphere predictability in WACCMX+DART. A SSW, along with the associated middle and upper atmosphere variability, is initially predicted in the hindcast initialized on 15 January, which is ˜10 days prior to the warming. However, it is not until the hindcast initialized on 20 January that a major SSW is forecast to occur. The hindcast experiments reveal that dominant features of the total electron content can be forecasted ˜10-20 days in advance. This demonstrates that whole atmosphere models that properly account for variability in lower atmosphere forcing can potentially extend the ionosphere-thermosphere forecast range.

Lower stratospheric observations from aircraft and satellite during the 2015/2016 El Nino

NASA Astrophysics Data System (ADS)

Rosenlof, K. H.; Avery, M. A.; Davis, S. M.; Gao, R. S.; Thornberry, T. D.

2016-12-01

Winter 2015/2016 experienced a strong El Nino that was heavily observed by aircraft, radiosonde and satellite platforms. During the National Oceanographic and Atmospheric Administration's (NOAA) Sensing Hazards with Operational Unmanned Technology (SHOUT)/El Nino Rapid Response (ENRR) flights of the NASA Global Hawk, in situ ozone measurements were made in the lower stratosphere over the Pacific. These will be contrasted with ozone measurements taken during La Nina and ENSO neutral conditions during past Global Hawk aircraft campaigns. Additionally, lower stratospheric water vapor and ozone measurements from the Microwave Limb Sounder satellite instrument and stratospheric ice measurements above the tropopause from the Cloud-Aerosol Aerosol Lidar with Orthogonal Polarization (CALIOP) will be presented. Our aircraft ozone measurements are higher for the El Nino flights than during other missions previously sampled, while zonally averaged lower stratospheric water vapor and central Pacific ice path above the tropopause reached record highs. Implications and possible reasons for these anomalous observations will be discussed. Winter 2015/2016 experienced a strong El Nino that was heavily observed by aircraft, radiosonde and satellite platforms. During the National Oceanographic and Atmospheric Administration's (NOAA) Sensing Hazards with Operational Unmanned Technology (SHOUT)/El Nino Rapid Response (ENRR) flights of the NASA Global Hawk, in situ ozone measurements were made in the upper troposphere and lower stratosphere (UTLS) over the Pacific. These will be contrasted with ozone measurements made during La Nina and ENSO neutral conditions during past Global Hawk aircraft campaigns. Additionally, UTLS water vapor and ozone measurements from the Microwave Limb Sounder (MLS) satellite instrument and stratospheric ice measurements above the tropopause from the Cloud-Aerosol Aerosol Lidar with Orthogonal Polarization (CALIOP) will be presented. Our aircraft ozone measurements are higher in the upper troposphere for the El Nino flights than during other missions previously sampled, while zonally averaged lower stratospheric water vapor and ice water paths above the tropopause over the central Pacific reached record highs. Implications and possible reasons for these anomalous observations will be discussed.

Temporal Variations of Titan's Middle-Atmospheric Temperatures From 2004-2009 Observed by Cassini/CIRS

NASA Technical Reports Server (NTRS)

Achterberg, Richard K.; Gierasch, Peter J.; Flasar, F. Michael; Nixon, Conor A.

2010-01-01

We use five and one-half years of limb- and nadir-viewing temperature mapping observations by the Composite Infrared Radiometer-Spectrometer (CIRS) on the Cassini Saturn orbiter, taken between July 2004 and December 2009 (Ls from 293deg to 4deg; northern mid-winter to just after northern spring equinox), to monitor temperature changes in the upper stratosphere and lower mesosphere of Titan. The largest changes are in the northern (winter) polar stratopause, which has declined in temperature by over 20 K between 2005 and 2009. Throughout the rest of the mid to upper stratosphere and lower mesosphere, temperature changes are less than 5 K. In the southern hemisphere, temperatures in the middle stratosphere near 1 mbar increased by 1 to 2K from 2004 through early 2007, then declined by 2 to 4K throughout 2008 and 2009, with the changes, being larger at more, polar latitudes. Middle stratospheric temperatures at mid-northern latitudes show a small 1 to 2K increase, from 2005 through 2009. At north polar latitudes within the polar vortex, temperatures in the middle stratosphe=re show a approx. 4 K increase during 2007, followed by a comparable decrease in temperatures in 2008 and into early 2009. The observed temperature. changes in the north polar region are consistent with a weakening of the subsidence within the descending branch of the middle atmosphere meridional circulation.

Temporal Variations of Titan's Middle-Atmospheric Temperatures from 2004 to 2009 Observed by Cassini/CIRS

NASA Technical Reports Server (NTRS)

Achterberg, Richard K.; Gierasch, Peter J.; Conrath, Barney J.; Flasar, F. Michael; Nixon, Conor A.

2011-01-01

We use five and one-half years of limb- and nadir-viewing temperature mapping observations by the Composite Infrared Radiometer-Spectrometer (CIRS) on the Cassini Saturn orbiter, taken between July 2004 and December 2009 (Ls from 293 deg. to 48 deg.; northern mid-winter to just after northern spring equinox), to monitor temperature changes in the upper stratosphere and lower mesosphere of Titan. The largest changes are in the northern (winter) polar stratopause, which has declined in temperature by over 20 K between 2005 and 2009. Throughout the rest of the mid to upper stratosphere and lower mesosphere, temperature changes are less than 5 K. In the southern hemisphere, temperatures in the middle stratosphere near 1 mbar increased by 1-2 K from 2004 through early 2007, then declined by 2-4 K throughout 2008 and 2009, with the changes being larger at more polar latitudes. Middle stratospheric temperatures at mid-northern latitudes show a small 1-2 K increase from 2005 through 2009, at north polar latitudes within the polar vortex, temperatures in the middle stratosphere show an approximately 4 K increase during 2007, followed by a comparable decrease in temperatures in 2008 and into early 2009. The observed temperature changes in the north polar region are consistent with a weakening of the subsidence within the descending branch of the middle atmosphere meridional circulation.

The Influence of Extremely Large Solar Proton Events in a Changing Stratosphere. Stratospheric Influence of Solar Proton Events

NASA Technical Reports Server (NTRS)

Jackman, Charles H.; Fleming, Eric L.; Vitt, Francis M.

1999-01-01

Two periods of extremely large solar proton events (SPEs) occurred in the past thirty years, which forced significant long-term polar stratospheric changes. The August 2-10, 1972 and October 19-27, 1989 SPEs happened in stratospheres that were quite different chemically. The stratospheric chlorine levels were relatively small in 1972 (approximately 1.2 ppbv) and were fairly substantial in 1989 at about (approximately 3 ppbv). Although these SPEs produced both HO(x) and NO(y) constituents in the mesosphere and stratosphere, only the NO(y) constituents had lifetimes long enough to affect ozone for several months to years past the events. Our recently improved two-dimensional chemistry and transport atmospheric model was used to compute the effects of these gigantic SPEs in a changing stratosphere. Significant upper stratospheric ozone depletions > 10% are computed to last for a few months past these SPEs. The long-lived SPE-produced NO(y) constituents were transported to lower levels during winter after these huge SPEs and caused impacts in the middle and lower stratosphere. During periods of high halogen loading these impacts resulted in interference with the chlorine and bromine loss cycles for ozone destruction. The chemical state of the atmosphere, including the stratospheric sulfate aerosol density, substantially affected the predicted stratospheric influence of these extremely large SPEs.

Trends in ozone profile measurements

NASA Technical Reports Server (NTRS)

Johnston, H.; Aikin, A.; Barnes, R.; Chandra, S.; Cunnold, D.; Deluisi, J.; Gille, J. C.; Hudson, R.; Mccormick, M. P.; Mcmaster, L.

1989-01-01

From an examination of the agreements and differences between different satellite instruments, it is difficult to believe that existing satellite instruments determine upper stratospheric ozone much better than 4 pct.; by extension, it probably would require at least a 4 pct. change to be reliably detected as a change. The best estimates of the vertical profiles of ozone change in the upper stratosphere between 1979 and 1986 are judged to be those given by the two SAGE satellite instruments. SAGE-2 minus SAGE-1 gives a much lower ozone reduction than that given by the archived Solar Backscatter UV data. The average SAGE profiles of ozone changes between 20 and 50 degs north and between 20 and 50 degs south are given. The SAGE-1 and SAGE-2 comparison gives an ozone reduction of about 4 pct. at 25 km over temperate latitudes. Five ground based Umkehr stations between 36 and 52 degs north, corrected for the effects of volcanic aerosols, report an ozone reduction between 1979 and 1987 at Umkehr layer 8 of 9 + or - 5 pct. The central estimate of upper stratospheric ozone reduction given by SAGE at 40 km is less than the central value estimated by the Umkehr method at layer 8.

Trends and Solar Cycle Effects in Temperature Versus Altitude From the Halogen Occultation Experiment for the Mesosphere and Upper Stratosphere

NASA Technical Reports Server (NTRS)

Remsberg, Ellis E.

2009-01-01

Fourteen-year time series of mesospheric and upper stratospheric temperatures from the Halogen Occultation Experiment (HALOE) are analyzed and reported. The data have been binned according to ten-degree wide latitude zones from 40S to 40N and at 10 altitudes from 43 to 80 km-a total of 90 separate time series. Multiple linear regression (MLR) analysis techniques have been applied to those time series. This study focuses on resolving their 11-yr solar cycle (or SC-like) responses and their linear trend terms. Findings for T(z) from HALOE are compared directly with published results from ground-based Rayleigh lidar and rocketsonde measurements. SC-like responses from HALOE compare well with those from lidar station data at low latitudes. The cooling trends from HALOE also agree reasonably well with those from the lidar data for the concurrent decade. Cooling trends of the lower mesosphere from HALOE are not as large as those from rocketsondes and from lidar station time series of the previous two decades, presumably because the changes in the upper stratospheric ozone were near zero during the HALOE time period and did not affect those trends.

Assessment of upper tropospheric and stratospheric water vapor and ozone in reanalyses as part of S-RIP

NASA Astrophysics Data System (ADS)

Davis, Sean M.; Hegglin, Michaela I.; Fujiwara, Masatomo; Dragani, Rossana; Harada, Yayoi; Kobayashi, Chiaki; Long, Craig; Manney, Gloria L.; Nash, Eric R.; Potter, Gerald L.; Tegtmeier, Susann; Wang, Tao; Wargan, Krzysztof; Wright, Jonathon S.

2017-10-01

Reanalysis data sets are widely used to understand atmospheric processes and past variability, and are often used to stand in as "observations" for comparisons with climate model output. Because of the central role of water vapor (WV) and ozone (O3) in climate change, it is important to understand how accurately and consistently these species are represented in existing global reanalyses. In this paper, we present the results of WV and O3 intercomparisons that have been performed as part of the SPARC (Stratosphere-troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The comparisons cover a range of timescales and evaluate both inter-reanalysis and observation-reanalysis differences. We also provide a systematic documentation of the treatment of WV and O3 in current reanalyses to aid future research and guide the interpretation of differences amongst reanalysis fields.The assimilation of total column ozone (TCO) observations in newer reanalyses results in realistic representations of TCO in reanalyses except when data coverage is lacking, such as during polar night. The vertical distribution of ozone is also relatively well represented in the stratosphere in reanalyses, particularly given the relatively weak constraints on ozone vertical structure provided by most assimilated observations and the simplistic representations of ozone photochemical processes in most of the reanalysis forecast models. However, significant biases in the vertical distribution of ozone are found in the upper troposphere and lower stratosphere in all reanalyses.In contrast to O3, reanalysis estimates of stratospheric WV are not directly constrained by assimilated data. Observations of atmospheric humidity are typically used only in the troposphere, below a specified vertical level at or near the tropopause. The fidelity of reanalysis stratospheric WV products is therefore mainly dependent on the reanalyses' representation of the physical drivers that influence stratospheric WV, such as temperatures in the tropical tropopause layer, methane oxidation, and the stratospheric overturning circulation. The lack of assimilated observations and known deficiencies in the representation of stratospheric transport in reanalyses result in much poorer agreement amongst observational and reanalysis estimates of stratospheric WV. Hence, stratospheric WV products from the current generation of reanalyses should generally not be used in scientific studies.

Thermal structure and dynamics of the Jovian Atmosphere. 1: The Great Red Spot

NASA Technical Reports Server (NTRS)

Flasar, F. M.; Cunrath, B. J.; Pirraglia, J. A.; Clark, P. C.; French, R. G.; Gierasch, P. J.

1980-01-01

Temperatures and thermal winds, derived from Voyager infrared spectroscopy (IRIS) data over the Great Red Spot (GRS) and its environs, are presented. The atmosphere over the GRS is characterized by a tropopause which is cold relative to its environment and an upper stratosphere which is relatively warm. The cold tropopause implies a decrease in anticyclonic vorticity with height above 500 mb through the lower stratosphere. IRIS observations at 5 microns indicate little emission from the GRS itself, but enhanced emission in a ring about it, in agreement with recent ground based results. The behavior of the tropopause and 5 micron temperatures can be consistently interpreted as resulting from a circulation which rises within the GRS and subsides in the area around it. The explanation of the upper stratospheric temperatures is not so straightforward. A previous suggestion that they may be a manifestation of the linear vertical propagation of Rossby waves appears inconsistent with the gross east-west symmetry in the stratospheric temperatures over the GRS. The implications of the present results for various theoretical models of the GRS are examined, and the possibility that latent heat release drives the GRS is discussed.

Present state of knowledge of the upper atmosphere1993: An assessment report, part 2

NASA Technical Reports Server (NTRS)

Kurylo, Michael J.; Kaye, Jack A.; Hampson, Robert F.; Schmoltner, Anne-Marie

1994-01-01

This document is issued in response to the Clean Air Act Amendment of 1990, Public Law 101-549, which mandates that the National Aeronautics and Space Administration (NASA) and other key agencies submit triennial reports to Congress and the Environmental Protection Agency. NASA is charged with the responsibility to report on the state of our knowledge of the earth's upper atmosphere, particularly the stratosphere. Part 2 (this document) presents summaries of several scientific assessments of our current understanding of the chemical composition and physical structure of the stratosphere, in particular how the abundance and distribution of ozone is predicted to change in the future. These reviews include: (Section B) 'Scientific Assessment of Ozone Depletion: 1991'; (Section C) 'Methyl bromide and the Ozone Layer: A Summary of Current Understanding', published in 1992; (Section D) 'Concentrations, Lifetimes, and Trends of Chlorofluorocarbons (CFC's), Halons, and Related Molecules in the Atmosphere'; (Section E) 'The Atmospheric Effects of Stratospheric Aircraft: Interim Assessment Report of the NASA High-Speed Research Program'; (Section F) 'Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling'; and (Section G) a list of the contributors to this report.

Chemical Data Assimilation Estimates of Continental US Ozone and Nitrogen Budgets during INTEX-A

NASA Technical Reports Server (NTRS)

Pierce, Robert B.; Schaack, Todd K.; Al-Saadi, Jassim A.; Fairlie, T. Duncan; Kittaka, Chieko; Lingenfelser, Gretchen; Natarajan, Murali; Olson, Jennifer; Soja, Amber; Zapotocny, Tom;

Observations and theories related to Antarctic ozone changes

NASA Technical Reports Server (NTRS)

Hartmann, D.; Watson, R. T.; Cox, Richard A.; Kolb, C.; Mahlman, J.; Mcelroy, M.; Plumb, A.; Ramanathan, V.; Schoeberl, M.; Solomon, S.

1989-01-01

In 1985, there was a report of a large, sudden, and unanticipated decrease in the abundance of springtime Antarctic ozone over the last decade. By 1987, ozone decreases of more than 50 percent in the total column, and 95 percent locally between 15 and 20 km, had been observed. The scientific community quickly rose to the challenge of explaining this remarkable discovery; theoreticians soon developed a series of chemical and dynamical hypotheses to explain the ozone loss. Three basic theories were proposed to explain the springtime ozone hole. (1) The ozone hole is caused by the increasing atmospheric loadings of manmade chemicals containing chlorine (chlorofluorocarbons (CFC's) and bromine (halons)). These chemicals efficiently destroy ozone in the lower stratosphere in the Antarctic because of the special geophysical conditions, of an isolated air mass (polar vortex) with very cold temperatures, that exist there. (2) The circulation of the atmosphere in spring has changed from being predominantly downward over Antarctica to upward. This would mean that ozone poor air from the troposphere, instead of ozone rich air from the upper stratosphere, would be transported into the lower Antarctic stratosphere. (3) The abundance of the oxides of nitrogen in the lower Antarctic stratosphere is periodically enhanced by solar activity. Nitrogen oxides are produced in the upper mesosphere and thermosphere and then transported downward into the lower stratosphere in Antarctica, resulting in the chemical destruction of ozone. The climatology and trends of ozone, temperature, and polar stratospheric clouds are discussed. Also, the transport and chemical theories for the Antarctic ozone hole are presented.

Five blind men and the elephant: what can the NASA Aura ozone measurements tell us about stratosphere-troposphere exchange?

NASA Astrophysics Data System (ADS)

Tang, Q.; Prather, M. J.

2012-03-01

We examine whether the individual ozone (O3) measurements from the four Aura instruments can quantify the stratosphere-troposphere exchange (STE) flux of O3, an important term of the tropospheric O3 budget. The level 2 (L2) Aura swath data and the nearly coincident ozone sondes for the years 2005-2006 are compared with the 4-D, high-resolution (1° × 1° × 40-layer × 0.5 h) model simulation of atmospheric ozone for the same period from the University of California, Irvine chemistry transport model (CTM). The CTM becomes a transfer standard for comparing individual profiles from these five, not-quite-coincident measurements of atmospheric ozone. Even with obvious model discrepancies identified here, the CTM can readily quantify instrument-instrument biases in the tropical upper troposphere and mid-latitude lower stratosphere. In terms of STE processes, all four Aura datasets have some skill in identifying stratosphere-troposphere folds, and we find several cases where both model and measurements see evidence of high-O3 stratospheric air entering the troposphere. In many cases identified in the model, however, the individual Aura profile retrievals in the upper troposphere and lower stratosphere show too much noise, as expected from their low sensitivity and coarse vertical resolution at and below the tropopause. These model-measurement comparisons of individual profiles do provide some level of confidence in the model-derived STE O3 flux, but it will be difficult to integrate this flux from the satellite data alone.

Efficient transport of tropospheric aerosol into the stratosphere via the Asian summer monsoon anticyclone

NASA Astrophysics Data System (ADS)

Yu, Pengfei; Rosenlof, Karen H.; Liu, Shang; Telg, Hagen; Thornberry, Troy D.; Rollins, Andrew W.; Portmann, Robert W.; Bai, Zhixuan; Ray, Eric A.; Duan, Yunjun; Pan, Laura L.; Toon, Owen B.; Bian, Jianchun; Gao, Ru-Shan

2017-07-01

An enhanced aerosol layer near the tropopause over Asia during the June-September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (˜15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (˜35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.

Equatorial Oscillation and Planetary Wave Activity in Saturn's Stratosphere Through the Cassini Epoch

NASA Astrophysics Data System (ADS)

Guerlet, S.; Fouchet, T.; Spiga, A.; Flasar, F. M.; Fletcher, L. N.; Hesman, B. E.; Gorius, N.

2018-01-01

Thermal infrared spectra acquired by Cassini/Composite InfraRed Spectrometer (CIRS) in limb-viewing geometry in 2015 are used to derive 2-D latitude-pressure temperature and thermal wind maps. These maps are used to study the vertical structure and evolution of Saturn's equatorial oscillation (SEO), a dynamical phenomenon presenting similarities with the Earth's quasi-biennal oscillation (QBO) and semi-annual oscillation (SAO). We report that a new local wind maximum has appeared in 2015 in the upper stratosphere and derive the descent rates of other wind extrema through time. The phase of the oscillation observed in 2015, as compared to 2005 and 2010, remains consistent with a ˜15 year period. The SEO does not propagate downward at a regular rate but exhibits faster descent rate in the upper stratosphere, combined with a greater vertical wind shear, compared to the lower stratosphere. Within the framework of a QBO-type oscillation, we estimate the absorbed wave momentum flux in the stratosphere to be on the order of ˜7 × 10-6 N m-2. On Earth, interactions between vertically propagating waves (both planetary and mesoscale) and the mean zonal flow drive the QBO and SAO. To broaden our knowledge on waves potentially driving Saturn's equatorial oscillation, we searched for thermal signatures of planetary waves in the tropical stratosphere using CIRS nadir spectra. Temperature anomalies of amplitude 1-4 K and zonal wave numbers 1 to 9 are frequently observed, and an equatorial Rossby (n = 1) wave of zonal wave number 3 is tentatively identified in November 2009.

Photosynthesis of organic compounds in the atmosphere of Jupiter

NASA Technical Reports Server (NTRS)

Ferris, J. P.; Chen, C. T.

1975-01-01

An efficient conversion of CH4 to hydrocarbons and HCN takes place when NH3 is photolysed in the presence of CH4, H2, and He using a 184.9 nm light source. The extent of NH3 decomposition after a 1 hr exposure was determined spectrophotometrically; CH4, N2, and C2 and C3 hydrocarbons were detected and analyzed by mass spectrometry. Photolysis of one molar equivalent of NH3 results in the loss of 0.84 molar equivalent of CH4, which apparently reacts with hot hydrogen atoms produced by photolysis. The 8% of the NH3 which is not converted to N2 probably is converted to organic amines and nitrile derivatives. The results indicate that NH3 photolysis is a highly probable mechanism for the conversion of methane to more complex hydrocarbons in the upper atmosphere of Jupiter, and predict the occurrence of HCN, NH2NH2, and higher hydrocarbons in the Jovian atmosphere above the NH3 clouds.

Injection of iodine to the stratosphere

NASA Astrophysics Data System (ADS)

Saiz-Lopez, Alfonso; Baidar, Sunil; Cuevas, Carlos A.; Koening, Theodore; Fernandez, Rafael P.; Dix, Barbara; Kinnison, Douglas E.; Lamarque, Jean-Francois; Rodriguez-Lloveras, Xavier; Campos, Teresa L.; Volkamer, Rainer

2016-04-01

There are still many uncertainties about the influence of iodine chemistry in the stratosphere, as the real amount of reactive iodine injected to this layer the troposphere and the partitioning of iodine species are still unknown. In this work we report a new estimation of the injection of iodine into the stratosphere based on novel daytime (SZA < 45°) aircraft observations in the tropical tropopause layer (TORERO campaign) and a 3D global chemistry-climate model (CAM-Chem) with the most recent knowledge about iodine photochemistry. The results indicate that significant levels of total reactive iodine (0.25-0.7 pptv), between 2 and 5 times larger than the accepted upper limits, could be injected into the stratosphere via tropical convective outflow. At these iodine levels, modelled iodine catalytic cycles account for up to 30% of the contemporary ozone loss in the tropical lower stratosphere and can exert a stratospheric ozone depletion potential equivalent or even larger than that of very short-lived bromocarbons. Therefore, we suggest that iodine sources and chemistry need to be considered in assessments of the historical and future evolution of the stratospheric ozone layer.

Stratospheric Tracers of Atmospheric Transport (STRAT) Campaign: ER-2 Participation

NASA Technical Reports Server (NTRS)

Anderson, James G.

1999-01-01

The NASA Stratospheric Tracers of Atmospheric Transport (STRAT) mission was initiated to advance knowledge of the major transport mechanisms of the upper troposphere-lower stratosphere. This is the region of the atmosphere within which exchange processes take place that critically determine the response of the climate system and ozone distribution to changing conditions triggered by the release of chemicals at the surface. The mission series that extended from October 1995 to November 1997 was extremely successful. The scientific advances that emerged from that mission include analyses of: (1) troposphere-to-stratosphere transport in the lowermost stratosphere from measurements of H2O, CO2, N2O, and O3; (2) the effects of tropical cirrus clouds on the abundance of lower stratospheric ozone; (3) the role of HO(sub x) in super- and subsonic aircraft exhaust plumes; and (4) dehydration and denitrification in the arctic polar vortex during the 1995-96 winter. The abstracts from published papers are included.

Bismuth Oxide Nanoparticles in the Stratosphere

NASA Technical Reports Server (NTRS)

Rietmeijer, Frans J. M.; Mackinnon, Ian D. R.

1997-01-01

Platey grains of cubic Bi2O3, alpha-Bi2O3, and Bi2O(2.75), nanograins were associated with chondritic porous interplanetary dust particles W7029C1, W7029E5, and 2011C2 that were collected in the stratosphere at 17-19 km altitude. Similar Bi oxide nanograins were present in the upper stratosphere during May 1985. These grains are linked to the plumes of several major volcanic eruptions during the early 1980s that injected material into the stratosphere. The mass of sulfur from these eruptions is a proxy for the mass of stratospheric Bi from which we derive the particle number densities (p/cu m) for "average Bi2O3 nanograins" due to this volcanic activity and those necessary to contaminate the extraterrestrial chondritic porous interplanetary dust particles via collisional sticking. The match between both values supports the idea that Bi2O3 nanograins of volcanic origin could contaminate interplanetary dust particles in the Earth's stratosphere.

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

NASA Technical Reports Server (NTRS)

Hintsa, E. J.; Boering, K. A.; Weinstock, E. M.; Anderson, J. G.; Gary, B. L.; Pfister, L.; Daube, B. C.; Wofsy, S. C.; Loewenstein, M.; Podolske, J.R.;

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

NASA Technical Reports Server (NTRS)

Hintsa, E. J.; Boering, K. A.; Weinstock, E. M.; Anderson, J. G.; Gary, B. L.; Pfister, L.; Daube, B. C.; Wofsy, S. C.; Loewenstein, M.; Podolske, J. R.

1998-01-01

The origin of air in the lowermost stratosphere is investigated with measurements from the NASA ER-2 aircraft. Air with high water vapor mixing ratios was observed in the stratosphere at theta = 330-380 K near 40 N in May 1995, indicating the influence of intrusions of tropospheric air. Assuming that observed tracer-tracer relationships reflect mixing lines between tropospheric and stratospheric air masses, we calculate mixing ratios of H2O (12-24 ppmv) and CO2 for the admixed tropospheric air at theta = 352-364 K. Temperatures on the 355 K surface at 20-40 N were low enough to dehydrate air to these values. While most ER-2 CO2 data in both hemispheres are consistent with tropical or subtropical air entering the lowermost stratosphere, measurements from May 1995 for theta < 362 K suggest that entry of air from the midlatitude upper troposphere can occur in conjunction with mixing processes near the tropopause.

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O, and O3

NASA Technical Reports Server (NTRS)

Hintsa, E. J.; Boering, K. A.; Weinstock, E. M.; Anderson, J. G.; Gary, B. L.; Pfister, L.; Daube, B. C.; Wofsy, S. C.; Loewenstein, M.; Podolske, J. R.;

Troposphere-to-Stratosphere Transport in the Lowermost Stratosphere from Measurements of H2O, CO2, N2O and O3

NASA Technical Reports Server (NTRS)

Hintsa, E. J.; Boering, K. A.; Weinstock, E. M.; Anderson, J. G.; Gary, B. L.; Pfister, L.; Daube, B. C.; Wofsy, S. C.; Loewenstein, M.; Podolske, J. R.;

Northern Winter Climate Change: Assessment of Uncertainty in CMIP5 Projections Related to Stratosphere-Troposphere Coupling

NASA Technical Reports Server (NTRS)

Manzini, E.; Karpechko, A.Yu.; Anstey, J.; Shindell, Drew Todd; Baldwin, M.P.; Black, R.X.; Cagnazzo, C.; Calvo, N.; Charlton-Perez, A.; Christiansen, B.;

As polar ozone mends, UV shield closer to equator thins

NASA Astrophysics Data System (ADS)

Reese, April

2018-02-01

Thirty years after nations banded together to phase out chemicals that destroy stratospheric ozone, the gaping hole in Earth's ultraviolet radiation shield above Antarctica is shrinking. But new findings suggest that at midlatitudes, where most people live, the ozone layer in the lower stratosphere is growing more tenuous—for reasons that scientists are struggling to fathom. In an analysis published this week, researchers found that from 1998 to 2016, ozone in the lower stratosphere ebbed by 2.2 Dobson units—a measure of ozone thickness—even as concentrations in the upper stratosphere rose by about 0.8 Dobson units. The culprit may be ozone-eating chemicals such as dichloromethane that break down within 6 months after escaping into the air.

Anthropogenic and Volcanic Contributions to the Decadal Variations of Aerosols in the Upper Troposphere and Lower Stratosphere

NASA Technical Reports Server (NTRS)

Chin, Mian; Diehl, Thomas; Bian, Huisheng; Aquila, Valentina; Colarco, Peter R.; Tan, Qian; Burrows, John P.; Krotov, Nickolay A.; Vernier, Jean P.; Lu, Zifeng;

Effects of Subsonic Aircraft on Aerosols and Cloudiness in the Upper Troposphere and Lower Stratosphere

NASA Technical Reports Server (NTRS)

Detwiler, Andrew G.

1997-01-01

This work was accomplished primarily by Allison G. Wozniak, a graduate research assistant who has completed the Master of Science in Meteorology program at the South Dakota School of Mines and Technology. Ms. Wozniak was guided and assisted in her work by L. R. Johnson and the principal investigator. Invaluable guidance was supplied by Dr. James Holdeman, NASA Lewis, the manager of the Global Atmospheric Sampling Program (GASP). Dr. Gregory Nastrom, St. Cloud (Minnesota) State University, who has used the GASP data set to provide unique views of the distribution of ozone, clouds, and atmospheric waves and turbulence, in the upper troposphere/lower stratosphere region, was also extremely helpful. Finally, Dr. Terry Deshler, University of Wyoming, supplied observations from the university's upper atmospheric monitoring program for comparison to GASP data.

Relative Contribution of Greenhouse Gases and Ozone Change to Temperature Trends in the Stratosphere: A Chemistry/Climate Model Study

NASA Technical Reports Server (NTRS)

Stolarski, Richard S.; Douglass, A. R.; Newman, P. A.; Pawson, S.; Schoeberl, M. R.

2006-01-01

Long-term changes in greenhouse gases, primarily carbon dioxide, are expected to lead to a warming of the troposphere and a cooling of the stratosphere. We examine the cooling of the stratosphere and compare the contributions greenhouse gases and ozone change for the decades between 1980 and 2000. We use 150 years of simulation done with our coupled chemistry/climate model (GEOS 4 GCM with GSFC CTM chemistry) to calculate temperatures and constituents fiom,1950 through 2100. The contributions of greenhouse gases and ozone to temperature change are separated by a time-series analysis using a linear trend term throughout the period to represent the effects of greenhouse gases and an equivalent effective stratospheric chlorine (EESC) term to represent the effects of ozone change. The temperature changes over the 150 years of the simulation are dominated by the changes in greenhouse gases. Over the relatively short period (approx. 20 years) of ozone decline between 1980 and 2000 changes in ozone are competitive with changes in greenhouse gases. The changes in temperature induced by the ozone change are comparable to, but smaller than, those of greenhouse gases in the upper stratosphere (1-3 hPa) at mid latitudes. The ozone term dominates the temperature change near both poles with a negative temperature change below about 3-5 hPa and a positive change above. At mid latitudes in the upper stratosphere and mesosphere (above about 1 hPa) and in the middle stratosphere (3 to 70 ma), the greenhouse has term dominates. From about 70 hPa down to the tropopause at mid latitudes, cooling due to ozone changes is the largest influence on temperature. Over the 150 years of the simulation, the change in greenhouse gases is the most important contributor to temperature change. Ozone caused a perturbation that is expected to reverse over the coming decades. We show a model simulation of the expected temperature change over the next two decades (2006-2026). The simulation shows a crossover between lower atmospheric heating and upper atmospheric cooling that is located at about 90 hPa in the tropics and 30-40 hPa in the polar regions. This results from the combination of continuing increases in greehouse gases and recovery from ozone depletion.

Is there any chlorine monoxide in the stratosphere?

NASA Technical Reports Server (NTRS)

Mumma, M. J.; Rogers, J. D.; Kostiuk, T.; Deming, D.; Hillman, J. J.; Zipoy, D.

1983-01-01

A ground-based search for stratospheric 35-ClO was carried out using an infrared heterodyne spectrometer in the solar absorption mode. Lines due to stratospheric HNO3 and tropospheric OCS were detected at about 0.2 percent absorptance levels, but the expected 0.1 percent lines of ClO in this same region were not seen. We find that stratospheric ClO is at least a factor of seven less abundant than is indicated by in situ measurements, and we set an upper limit of 2.3 x 10 to the 13th molecules/sq cm at the 95 percent confidence level for the integrated vertical column density of ClO. Our results imply that the release of chlorofluorocarbons may be significantly less important for the destruction of stratospheric ozone (O3) than is currently thought. Previously announced in STAR as N83-27518

Tropospheric and lower stratospheric vertical profiles of ethane and acetylene

NASA Technical Reports Server (NTRS)

Cronn, D.; Robinson, E.

1979-01-01

The first known vertical distributions of ethane and acetylene which extend into the lower stratosphere are reported. The average upper tropospheric concentrations, between 20,000 ft and 35,000 ft, near 37 deg N-123 deg W were 1.2 micrograms/cu m (1.0 ppb) for ethane and 0.24 micrograms /cu m (0.23 ppb) for acetylene while the values near 9 N-80 W were 0.95 micrograms/cu m (0.77 ppb) and 0.09 micrograms/cu m (0.09 ppb), respectively. Detectable quantities of both ethane and acetylene are present in the lower stratosphere. There is a sharp decrease in the levels of these two compounds as one crosses the tropopause and ascends into the lower stratosphere. The observed levels of ethane and acetylene may allow some impact on the background chemistry of the troposphere and stratosphere.

Air mass origins and troposphere-to-stratosphere exchange associated with mid-latitude cyclogenesis and tropopause folding inferred from Be-7 measurements

NASA Technical Reports Server (NTRS)

Kritz, Mark A.; Rosner, Stefan W.; Danielsen, Edwin F.; Selkirk, Henry B.

1991-01-01

The 1984 extratropical mission of NASA's Stratosphere-Troposphere Exchange Project (STEP) studied cross-jet transport in regions of cyclogenesis and tropopause folding. Correlations of Be-7, ozone, water vapor, and potential vorticity measured on a NASA U-2 research aircraft flying in high shear regions above the jet core are indicative of mixing between the cyclonic and the anticyclonic sides of the jet and are consistent with the hypothesis that small-scale entrainments of upper tropospheric air into the lower stratosphere during cyclogenesis are important in maintaining the vertical gradients of Be-7, ozone, water vapor and other trace constituents in the lower few kilometers of the midlatitude stratosphere. Correlations between Be-7, and ozone suggest a lower tropical stratospheric origin for the ozone-poor lamina observed above the jet core.

On the Stratospheric Chemistry of Hydrogen Cyanide

NASA Technical Reports Server (NTRS)

Kleinbohl, Armin; Toon, Geoffrey C.; Sen, Bhaswar; Blavier, Jean-Francois L.; Weisenstein, Debra K.; Strekowski, Rafal S.; Nicovich, J. Michael; Wine, Paul H.; Wennberg, Paul O.

2006-01-01

HCN profiles measured by solar occultation spectrometry during 10 balloon flights of the JPL MkIV instrument are presented. The HCN profiles reveal a compact correlation with stratospheric tracers. Calculations with a 2D-model using established rate coefficients for the reactions of HCN with OH and O(1D) severely underestimate the measured HCN in the middle and upper stratosphere. The use of newly available rate coefficients for these reactions gives reasonable agreement of measured and modeled HCN. An HCN yield of approx.30% from the reaction of CH3CN with OH is consistent with the measurements.

The dynamics of the HSCT environment. [air pollution from High Speed Civil Transport Aircraft

NASA Technical Reports Server (NTRS)

Douglass, Anne R.; Rood, Richard B.

1991-01-01

Assessments of the impact of aircraft engine exhausts on stratospheric ozone levels are currently limited to 2D zonally-averaged models which, while completely representing chemistry, involve high parameterization of transport processes. Prospective 3D models under development by NASA-Goddard will use winds from a data-assimilation procedure; the upper troposphere/lower stratosphere behavior of one such model has been verified by direct comparison of model simulations with satellite, balloon, and sonde measurements. Attention is presently given to the stratosphere/troposphere exchange and nonzonal distribution of aircraft engine exhaust.

Dynamical Meteorology of the Equatorial and Extratropical Stratosphere

NASA Technical Reports Server (NTRS)

Dunkerton, Tomothy

1999-01-01

Observational studies were performed of westward propagating synoptic scale waves in the tropical troposphere, the structure of monsoon circulations in the upper troposphere and lower stratosphere, and zonally propagating features in deep tropical convection. The effect of the quasi-biennial oscillation (QBO) were investigated, and a numerical study of the QBO was performed using a two-dimensional model, highlighting the role of gravity waves in the momentum balance of the QBO. Vertical coupling of the troposphere and stratosphere was examined in polar regions on intraseasonal and interannual timescales. A deep circumpolar mode was discovered, now known as the Arctic Oscillation.

ISAMS observations of stratospheric aerosol

NASA Technical Reports Server (NTRS)

Lambert, Alyn; Remedios, John J.; Dudhia, Anu; Corney, Marie; Kerridge, Brian J.; Rodgers, Clive D.; Taylor, Fredric W.

1994-01-01

The Improved Stratospheric and Mesospheric (ISAMS) on board the Upper Atmosphere Research Satellite (UARS) incorporates a 12.1 micron window channel for the measurement of aerosol opacity. The retrieval scheme is discussed briefly and preliminary observations of the Mt. Pinatubo aerosol cloud are presented and compared with SAGE 2 observations at 1.02 microns. The effect of aerosol on other ISAMS channels and its spectral dependence is discussed.

High Altitude Emissions of Black Carbon Aerosols: Potential Climate Implications

NASA Astrophysics Data System (ADS)

Satheesh, S. K.

2017-12-01

Synthesizing a series of ground-based and airborne measurements of aerosols over the Indian region during summer and pre-monsoon seasons have revealed the persistence of elevated absorbing aerosol layers over most of the Indian region; more than 50% of which located above clouds. Subsequent, in situ measurements of black carbon (BC) using high-altitude balloons, showed surprising layers with high concentrations in the middle and upper troposphere even at an altitude of 8 to 10 kms. Simultaneous measurements of the vertical thermal structure have shown localized warming due to BC absorption leading to large reduction in lapse rate and sharp temperature inversion, which in turn increases the atmospheric stability. This aerosol-induced stable layer is conducive for maintaining the black carbon layer longer at that level, leading thereby to further solar absorption and subsequently triggering dry convection. These observations support the `solar escalator' concept through which absorption-warming-convection cycles lead to self-lifting of BC to upper troposphere or even to lower stratosphere under favorable conditions in a matter of a few days. Employing an on-line regional chemistry transport model (WRF-Chem), incorporating aircraft emissions, it is shown that emissions from high-flying aircrafts as the most likely source of these elevated black carbon layers. These in-situ injected particles, produce significant warming of the thin air in those heights and lift these layers to even upper tropospheric/lower stratospheric heights, aided by the strong monsoonal convection occurring over the region, which are known to overshoot the tropical tropopause leading to injection of tropospheric air mass (along with its constituent aerosols) into the stratosphere, especially during monsoon season when the tropical tropopause layer is known to be thinnest. These simulations are further supported by the CALIPSO space-borne LIDAR derived extinction coefficient profiles. Based on these, it is hypothesized that such intrusions of black carbon to lower stratosphere and its consequent longer residence time in the stratosphere, would have significant implications for stratospheric chemistry, considering the known ozone depleting potential of black carbon aerosols.

Present State of Knowledge of the Upper Atmosphere 1999: An Assessment Report. Part 2

NASA Technical Reports Server (NTRS)

Kurylo, M. J.; DeCola, P. L.; Kaye, J. A.

2000-01-01

This document is issued in response to the Clean Air Act Amendment of 1990, Public Law 101-549, which mandates that the National Aeronautics and Space Administration (NASA) and other key agencies submit triennial reports to the Congress and the Environmental Protection Agency. NASA specifically is charged with the responsibility of reporting on the state of our knowledge of the Earth's upper atmosphere, particularly the stratosphere. Part l of this report summarizes the objectives, status, and accomplishments of the research tasks supported under NASA's Upper Atmosphere Research Program and Atmospheric Chemistry Modeling and Analysis Program for the period of 1997-1999. Part 2 (this document) is a compilation of several scientific assessments, reviews, and summaries. Section B (Scientific Assessment of Ozone Depletion: 1998), Section C (a summary of the 1998 Stratospheric Processes and their Role in Climate, SPARC, ozone trends report), Section D (the policymakers summary of the Intergovernmental Panel on Climate Change, IPCC, report on Aviation and the Global Atmosphere), and Section E (the executive summary of the NASA Assessment of the Effects of High-Speed Aircraft in the Stratosphere: 1998) are summaries of the most recent assessments of our current understanding of the chemical composition and the physical structure of the stratosphere, with particular emphasis on how the abundance and distribution of ozone is predicted to change in the future. Section F (the executive summary of NASA's Second Workshop on Stratospheric Models and Measurements, M&M 11) and Section G (the end-of-mission statement for the Photochemistry of ozone Loss in the Arctic Region in Summer, POLARIS, campaign) describe the scientific results for a comprehensive modeling intercomparison exercise and an aircraft and balloon measurement campaign, respectively. Section H (Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling: Update to Evaluation Number 12 of the NASA Panel for Data Evaluation) highlights the latest of NASA's reviews of this important aspect of the atmospheric sciences. A list of contributors to each of the included documents appears in Section I of this report.

Modeling the effects of UV variability and the QBO on the troposphere-stratosphere system. Part I: The middle atmosphere

DOE Office of Scientific and Technical Information (OSTI.GOV)

Balachandran, N.K.; Rind, D.

1995-08-01

Results of experiments with a GCM involving changes in UV input ({plus_minus}25%, {plus_minus}10%, {plus_minus}5% at wavelengths below 0.3 {mu}m) and simulated equatorial QBO are presented, with emphasis on the middle atmosphere response. The UV forcing employed is larger than observed during the last solar cycle and does not vary with wavelength, hence the relationship of these results to those from actual solar UV forcing should be treated with caution. The QBO alters the location of the zero wind line and the horizontal shear of the zonal wind in the low to middle stratosphere, while the UV change alters the magnitudemore » of the polar jet and the vertical shear of the zonal wind. Both mechanisms thus affect planetary wave propagation. The east phase of the QBO leads to tropical cooling and high-latitude warming in the lower stratosphere, with opposite effects in the upper stratosphere. This quadrupole pattern is also seen in the observations. The high-latitude responses are due to altered planetary wave effects, while the model`s tropical response in the upper stratosphere is due to gravity wave drag. Increased UV forcing warms tropical latitudes in the middle atmosphere, resulting in stronger extratropical west winds, an effect which peaks in the upper stratosphere/lower mesosphere with the more extreme UV forcing but at lower altitudes and smaller wind variations with the more realistic forcing. The increased vertical gradient of the zonal wind leads to increased vertical propagation of planetary waves, altering energy convergences and temperatures. The exact altitudes affected depend upon the UV forcing applied. Results with combined QBO and UV forcing show that in the Northern Hemisphere, polar warming for the east QBO is stronger when the UV input is reduced by 25% and 5% as increased wave propagation to high latitudes (east QBO effect) is prevented from then propagating vertically (reduced UV effect). 30 refs., 14 figs., 6 tabs.« less

The Tropospheric cooling and the Stratospheric warming at Tirunelveli during the Annular Solar Eclipse of 15 January, 2010

NASA Astrophysics Data System (ADS)

Nelli, Narendra Reddy; Choudhary, Raj Kumar; Rao, Kusuma

The UTLS region, a transition region between the troposphere and the stratosphere is of concern to climate scientists as its temperature variations are crucial in determining the water vapour and the other trace gases transport between the two regions, which inturn determine the radiative warming and cooling of the troposphere and the stratosphere. To examine, the temperature variations from surface to lower stratosphere,a major experiment facility was set up for upper air and surface measurements during the Annular Solar Eclipse (ASE) of January 15, 2010 at Tirunelveli (8.72 N, 77.81 E) located in 94% eclipse path in the southern peninsular India. The instruments,namely, 1. high resolution GPS radiosonde system, 2. an instrumented 15 m high Mini Boundary Layer Mast, 3. an instrumented 1 m high Near Surface Mast (NSM), radiation and other ground sensors were operated during the period 14-19 Jan, 2010. The ASE of January 15, 2010 was unique being the longest in duration (9 min, 15.3 sec) among the similar ones that occurred in the past. The major inference from an analysis of surface and upper air measurements is the occurrence of troposphere cooling during the eclipse with the peak cooling of 5 K at 15 km height with respect to no-eclispe conditions. Also, intense warming in the stratosphere is observed with the peak warming of 7 K at 19 km height.Cooling of the Troposphere as the eclipse advanced and the revival to its normal temperature is clearly captured in upper air measurements. The downward vertical velocities observed at 100 hPa in NCEP Re-analyses, consistent with the tropospheric cooling during the ASE window, may be causing the stratospheric warming. Partly, these vertical velocities could be induced by the mesoscale circulation associated with the mesoscale convective system that prevailed parallel to the eclipse path as described in METEOSAT imageries of brightness temperatures from IR channel. Further analysis is being carried out to quantify the variations in turbulent parameters during ASE window using the high resolution GPS Radiosonde data.

Stratospheric Aerosol and Gas Experiment (SAGE 3)

NASA Technical Reports Server (NTRS)

Mccormick, M. P.

1993-01-01

The proposed SAGE III instrument would be the principal source of data for global changes of stratospheric aerosols, stratospheric water vapor, and ozone profiles, and a contributing source of data for upper tropospheric water vapor, aerosols, and clouds. The ability to obtain such data has been demonstrated by the predecessor instrument, SAGE II, but SAGE III will be substantially more capable, as discussed below. The capabilities for monitoring the profiles of atmospheric constituents have been verified in detail, including ground-based validations, for aerosol, ozone, and water vapor. Indeed, because of its self-calibrating characteristics, SAGE II was an essential component of the international ozone trend assessments, and SAGE II is now proving to be invaluable in tracking the aerosols from Mt. Pinatubo. Although SAGE profiles generally terminate at the height of the first tropospheric cloud layer, it has been found that the measurements extend down to 3 km altitude more than 40 percent of the time at most latitudes. Thus, useful information can also be obtained on upper tropospheric aerosols, water vapor, and ozone.

Ground-based microwave observations of ozone in the upper stratosphere and mesosphere

NASA Technical Reports Server (NTRS)

Connor, Brian J.; Siskind, David E.; Tsou, J. J.; Parrish, Alan; Remsberg, Ellis E.

1994-01-01

A 9-month-long series of mesurements of ozone in the upper stratosphere and mesosphere is reported. The measurements are presented as monthly averages of profiles in blocks of roughly 20 min local time and as night-to-day ratios. An error analysis predicts accuracies of 5-26% for the monthly profiles and 2.5-9% for the ratios. The data are compared to historical data from Solar Mesosphere Explorer (SME) and limb infrared monitor of the stratosphere (LIMS), and it is shown how to remove the effect of different vertical resolution from the comparisons. The microwave data typically agree to better than 10% with SMF and nighttime LIMS ozone at all altitudes below the 0.1-mbar surface. Comparison of the microwave night-to-day ratio with the corresponding ratio from LIMS suggests that nonlocal thermodynamic equilibrium effects in the LIMS daytime data exceed 10% at all pressures less than or equal to 1 mbar.

Seasonal gravity wave drags on the upper stratosphere due to the northwestern pacific typhoons

NASA Astrophysics Data System (ADS)

Chen, Zeyu; Lu, Daren

In a recent study of the first author and his co-authors (Zeyu Chen, Peter Preusse, Michael Jarisch, Manfred Ern, and Dirk Offermann, 2003), it has been revealed that a northwestern Pacific typhoon can generate stratospheric gravity waves with the horizontal scales ranging from 500 km ˜ 1000 km, and carrying a magnitude of ˜ 0.001 Pascal of momentum flux into the upper stratosphere Statistics indicates that the annual mean number of typhoon in the northwestern Pacific is about 32, most of them happen in summer. In this presentation, we show that a parameterization scheme is developed to derive the magnitude of the momentum flux of the waves from operational satellite observations that can scale the intensity of a typhoon (e.g. the brightness temperature observations from the GMS-5 satellite), and operational meteorological data analysis. The seasonal effect of the Gravity Wave Drags due to the typhoons in the area is derived.

Rate of reaction of OH with HNO3

NASA Technical Reports Server (NTRS)

Wine, P. H.; Ravishankara, A. R.; Kreutter, N. M.; Shah, R. C.; Nicovich, J. M.; Thompson, R. L.; Wuebbles, D. J.

1981-01-01

Measurements of the kinetics of the reaction of OH with HNO3, and mechanisms of HNO3 removal from the stratosphere, are reported. Bimolecular rate constants were determined at temperatures between 224 and 366 K by monitoring the concentrations of OH radicals produced by HNO3 photolysis and HNO3 according to their resonance fluorescence and 184.9-nm absorption, respectively. The rate constant measured at 298 K is found to be somewhat faster than previously accepted values, with a negative temperature dependence. Calculations of a one-dimensional transport-kinetic atmospheric model on the basis of the new rate constant indicate reductions in O3 depletion due to chlorofluoromethane release and NOx injection, of magnitudes dependent on the nature of the reaction products.

Effect of nitric oxide on photochemical ozone formation in mixtures of air with molecular chlorine and with trichlorofluoromethane

NASA Technical Reports Server (NTRS)

Bittker, D. A.; Wong, E. L.

1978-01-01

Ozone formation in a reaction chamber at room temperature and atmospheric pressure were studied for the photolysis of mixtures of NO with either Cl2 or CFCl3 in air. Both Cl2 + NO and CFCl3 + NO in air strongly inhibited O3 formation during the entire 3 to 4 hour reaction. A chemical mechanism that explains the results was presented. An important part of this mechanism was the formation and destruction of chlorine nitrate. Computations were performed with this same mechanism for CFCl3-NO-air mixtures at stratospheric temperatures, pressures, and concentrations. Results showed large reductions in steady-state O3 concentrations in these mixtures as compared with pure air.

Concentrations of carbonyl sulfide and hydrogen cyanide in the free upper troposphere and lower stratosphere deduced from ATMOS/Spacelab 3 infrared solar occultation spectra

NASA Technical Reports Server (NTRS)

Zander, R.; Rinsland, C. P.; Russell, J. M., III; Farmer, C. B.; Norton, R. H.

1988-01-01

This paper presents the results on the volume mixing ratio profiles of carbonyl sulfide and hydrogen cyanide, deduced from the spectroscopic analysis of IR solar absorption spectra obtained in the occultation mode with the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during its mission aboard Spacelab 3. A comparison of the ATMOS measurements for both northern and southern latitudes with previous field investigations at low midlatitudes shows a relatively good agreement. Southern Hemisphere volume mixing ratio profiles for both molecules were obtained for the first time, as were the profiles for the Northern Hemisphere covering the upper troposphere and the lower stratosphere simultaneously.

Model/data comparisons of ozone in the upper stratosphere and mesosphere

NASA Technical Reports Server (NTRS)

Siskind, David E.; Remsberg, Ellis E.; Eckman, Richard S.; Connor, Brian J.; Tsou, J. J.; Parrish, Alan

1994-01-01

We compare ground-based microwave observations of ozone in the upper stratosphere and mesosphere with daytime observations made from the SME (Solar Mesosphere Explorer) satellite, with nighttime data from the LIMS instrument, and with a diurnal photochemical model. The results suggest that the data are all in reasonable agreement and that the model-data discrepancy is much less than previously thought, particularly in the mesosphere. This appears to be due to the fact that the latest data are lower than earlier reports and the updated model predicts more ozone than older versions. The model and the data agree to within a factor of 1.5 at all altitudes and typically are within 20 percent.

Using the C3M Satellite Data Product to Evaluate and Constrain the Cloud Fields in the HadGEM3-UKCA Model with an Aim to Enhance Understanding of the Effects of Clouds on Atmospheric Composition via Photolysis

NASA Astrophysics Data System (ADS)

Varma, S.; Voulgarakis, A.; Liu, H.; Crawford, J. H.; Zhang, B.

2017-12-01

What drives the variability of trace gases in the troposphere is not well understood, as is the role of clouds in modulating this variability via radiative, transport, deposition, heterogeneous chemistry, and lightning effects that are associated with them. Accurately simulating tropospheric composition and its variability is of utmost importance as both could have a significant effect on the region's temperature and circulation, as well as on surface climate and the amount of UV radiation in the troposphere. In this presentation, we will examine how clouds can influence tropospheric and lower stratospheric composition through modifying solar radiation leading to changes in the local actinic flux and subsequently to photolysis, a key driver of chemistry. We will utilize C3M (a unique 3-D cloud data product merged from multiple A-Train satellites (CERES, CloudSat, CALIPSO, and MODIS) developed at the NASA Langley Research Center to evaluate the cloud fields and their vertical distribution in the HadGEM3-UKCA model developed by the Natural Environment Research Council (NERC, UK) and the Met Office. This evaluation will involve 1) comparing the effective cloud optical depth (ECOD) as calculated from C3M and the model using the approximate random overlap method, 2) applying 3-D scaling factors from C3M to the model's ECOD and analyzing the changes this makes to the model's cloud fields, and 3) running the scaled model and analyzing the impacts of this cloud field adjustment on the model's estimates of photolysis rates and key tropospheric oxidants such as ozone and OH.

The distribution of hydrogen, nitrogen, and chlorine radicals in the lower stratosphere: Implications for changes in O3 due to emission of NO(y) from supersonic aircraft

NASA Technical Reports Server (NTRS)

Salawitch, R. J.; Wofsy, S. C.; We-Nnberg, P. O.; Cohen, R. C.; Anderson, J. G.; Fahey, D. W.; Gao, R. S.; Keim, E. R.; Woodbridge, E. L.; Stimpfle, R. M.

1994-01-01

In situ measurements of hydrogen, nitrogen, and chlorine radicals obtained in the lower statosphere during SPADE are compared to results from a photochemical model that assimilates measurements of radical precursors and environmental conditions. Models allowing for heterogeneous hydrolysis of N2O5 agree well with measured concentrations of NO and ClO, but concentrations of HO2 and OH are underestimated by 10 to 25%, concentrations of NO2 are overestimated by 10 to 30%, and concentrations of HCl are overestimated by a factor of 2. Discrepancies for (OH) and (HO2) are reduced if we allow for higher yields of O((1)D) from O2 photolysis and for heterogeneous production of HNO2. The data suggest more efficent catalytic removal of O3 by hydrogen and halogen radicals relative to nitrogen oxide radicals than predicted by models using recommendend rates and cross sections. Increased in (O3) in the lower stratosphere may be larger in response to inputs of NO(y) from supersonic aircraft than estimated by current assessment models.

Evolution of chemically processed air parcels in the lower stratosphere

NASA Technical Reports Server (NTRS)

Stolarski, Richard S.; Douglass, Anne R.; Schoeberl, Mark R.

1994-01-01

Aircraft, ground-based, and satellite measurements indicate large concentrations of ClO in the lower stratosphere in and near the polar vortex. The amount of local ozone depletion caused by these large ClO concentrations will depend on the relative rates of ozone loss and ClO recovery. ClO recovery occurs when NO(x), from HNO3 photolysis, reacts with ClO to form ClONO2. We show that air parcels with large amounts of ClO will experience a subsequent ozone depletion that depends on the solar zenith angle. When the solar zenith angle is large in the middle of winter, the recovery of the ClO concentration in the parcel is slow relative to ozone depletion. In the spring, when the solar zenith angle is smaller, the ClO recovery is much faster. After ClO recovery, the chlorine chemistry has not returned to normal. The ClO has been converted to ClONO2. ClO production from further encounters with PSCs will be limited by the heterogeneous reaction of ClONO2 with water. Large ozone depletions, of the type seen in the Antarctic, occur only if there is significant irreversible denitrification in the air parcel.

Temperature dependence of the HNO3 UV absorption cross sections

NASA Technical Reports Server (NTRS)

Burkholder, James B.; Talukdar, Ranajit K.; Ravishankara, A. R.; Solomon, Susan

1993-01-01

The temperature dependence of the HNO3 absorption cross sections between 240 and 360 K over the wavelength range 195 to 350 nm has been measured using a diode array spectrometer. Absorption cross sections were determined using both (1) absolute pressure measurements at 298 K and (2) a dual absorption cell arrangement in which the absorption spectrum at various temperatures is measured relative to the room temperature absorption spectrum. The HNO3 absorption spectrum showed a temperature dependence which is weak at short wavelengths but stronger at longer wavelengths which are important for photolysis in the lower stratosphere. The 298 K absorption cross sections were found to be larger than the values currently recommended for atmospheric modeling (DeMore et al., 1992). Our absorption cross section data are critically compared with the previous measurements of both room temperature and temperature-dependent absorption cross sections. Temperature-dependent absorption cross sections of HNO3 are recommended for use in atmospheric modeling. These temperature dependent HNO3 absorption cross sections were used in a two-dimensional dynamical-photochemical model to demonstrate the effects of the revised absorption cross sections on loss rate of HNO3 and the abundance of NO2 in the stratosphere.

The source of stratospheric NO and N2O

NASA Technical Reports Server (NTRS)

Slanger, T. G.

1984-01-01

The photodissociation of O3 was investigated as a possible sources of N2O production in the stratosphere. Photolysis was conducted at 1576 A to generate the excited O2 states that react with N2 to form N2O. At this wavelength, there is a quantum yield of two for prompt production of oygen atoms, which is a consequence of the existence of two photodissociative channels giving comparable yields. One of these channels gives O(D1) and O2(b1sigma(+)subg), with a quantum yield of 0.6, whereas the other results in fragmentation of the O3, with production of three ground state oxygen atoms. The O2(b) is generated with vibrational excitation, and there are comparable populations in levels O to 3. These observations are the first to show O2(b) production from any photodissociative process, and were made under conditions in which the kinetics of vibrationally excited O2(b) can be studied. It appears that O3 photodissociation at 1576 A is not a good system for generating the higher electronic states of O2; it is likely that better results will be obtained at 1930 A.

Balloon-Borne Measurements of Stratospheric Radicals and their Precursors: Implications for the Production and Loss of Ozone

NASA Technical Reports Server (NTRS)

Osterman, G. B.; Salawitch, R. J.; Sen, B.; Toon, G. C.; Stachnik, R. A.; Pickett, H. M.; Margitan, J. J.; Blavier, J.-F.; Peterson, D. B.

1997-01-01

Measurements of hydrogen, nitrogen and chlorine radicals from a balloon flight on 25 September 1993 from Ft. Sumner, NM provide an opportunity to quantify photochemical production and loss of stratospheric ozone. Ozone loss rates determined using measured radical concentrations agree fairly well with loss rates calculated using a photochemical model. Catalytic cycles involving OH and HO2 are shown to dominate photochemical loss of ozone for altitudes between 44 and 50 km. Reactions involving NO and NO2 are the dominant sink for ozone between 25 and 38 km. The total ozone loss rate determined from the measurements balances calculated production rates for altitudes between 30 and 40 km. However, loss of ozone exceeds production by -35% between 42 and 50 km. The imbalance between production and loss of ozone above 42 km is larger than the uncertainty of any one of the critical kinetic parameters or species concentrations. No single adjustment to any of these parameters can simultaneously resolve the imbalance and satisfy constraints imposed by measured OH, HO2, NO2 and ClO. Our results are consistent with an additional mechanism for ozone production above 40 km other than photolysis of ground state O2.

Performance of the GEOS-3/Terra Data Assimilation System in the Northern Stratospheric Winter 1999/2000

NASA Technical Reports Server (NTRS)

Pawson, S.; Lamich, David; Ledvina, Andrea; Conaty, Austin; Newman, Paul A.; Lait, Leslie R.; Waugh, Darryn

2000-01-01

As part of NASA's support for the Terra satellite, which became operational in January 2000, the Data Assimilation Office introduced a new version of the GEOS data assimilation system (DAS) in November 1999. This system, GEOS-3/Terra, differs from its predecessor in several ways, notably through an increase in horizontal resolution (from 2-by-2.5 degrees to 1-by-1 degree), a slightly lower upper boundary (0.1 instead of 0.01hPa) with fewer levels (48 as opposed to 70), and substantial changes to the tropospheric physics package. This paper will address the performance of the GEOS-3/Terra DAS in the stratosphere. it focusses on the analyses (produced four times daily) and the five-day forecasts (produced twice daily). These were important for the meteorological support of the SAGE-3 Ozone Loss and Validation Experiment, based in Kiruna, Northern Sweden, in the winter of 1999/2000. It is shown that the analyses of basic meteorological fields (temperature, geopotential height, and horizontal wind) are in good agreement with those from other centers. The analyses captured the cold polar vortex which persisted through most of the winter. It is shown that forecasts (up to five days) tend to have a warm bias, which is important for the prediction of polar stratospheric clouds, which are triggered by temperatures of 195K (or lower). The importance of accurate upper tropospheric forecasts in predicting the stratospheric flow is highlighted in the context of the evolution of the shape of the stratospheric polar vortex. A prominent blocking high in the Atlantic region in January was an important factor determining the shape of the distorted lower stratospheric vortex; the predictive skill of these features was strongly coupled in the GEOS-3/Terra system.

The Effect of Cirrus Clouds on Water Vapor Transport in the Upper Troposphere and Lower Stratosphere

NASA Astrophysics Data System (ADS)

Lei, L.; McCormick, M. P.; Anderson, J.

2017-12-01

Water vapor plays an important role in the Earth's radiation budget and stratospheric chemistry. It is widely accepted that a large percentage of water vapor entering the stratosphere travels through the tropical tropopause and is dehydrated by the cold tropopause temperature. The vertical transport of water vapor is also affected by the radiative effects of cirrus clouds in the tropical tropopause layer. This latter effect of cirrus clouds was investigated in this research. The work focuses on the tropical and mid-latitude region (50N-50S). Water vapor data from the Microwave Limb Sounder (MLS) and cirrus cloud data from the Cloud-Aerosol Lidar and Infrared pathfinder Satellite Observation (CALIPSO) instruments were used to investigate the relationship between the water vapor and the occurrence of cirrus cloud. A 10-degree in longitude by 10-degree in latitude resolution was chosen to bin the MLS and CALIPSO data. The result shows that the maximum water vapor in the upper troposphere (below 146 hPa) is matched very well with the highest frequency of cirrus cloud occurrences. Maximum water vapor in the lower stratosphere (100 hPa) is partly matched with the maximum cirrus cloud occurrence in the summer time. The National Oceanic and Atmospheric Administration Interpolated Outgoing Longwave Radiation data and NCEP-DOE Reanalysis 2 wind data were used also to investigate the relationship between the water vapor entering the stratosphere, deep convection, and wind. Results show that maximum water vapor at 100 hPa coincides with the northern hemisphere summer-time anticyclone. The effects from both single-layer cirrus clouds and cirrus clouds above the anvil top on the water vapor entering the stratosphere were also studied and will be presented.

A 4 U Laser Heterodyne Radiometer for Methane (CH4) and Carbon Dioxide (CO2) Measurements from an Occultation-Viewing CubSat

NASA Technical Reports Server (NTRS)

Wilson, Emily L.; DiGregorio, A. J.; Riot, Vincent J.; Ammons, Mark S.; Bruner, WIlliam W.; Carter, Darrell; Mao, Jianping; Ramanathan, Anand; Strahan, Susan E.; Oman, Luke D.;

High resolution modeling of the upper troposphere and lower stratosphere region over the Arctic - GEM-AC simulations for the future climate with and without aviation emissions.

NASA Astrophysics Data System (ADS)

Porebska, Magdalena; Struzewska, Joanna; Kaminski, Jacek W.

2016-04-01

Upper troposphere and lower stratosphere (UTLS) region is a layer around the tropopause. Perturbation of the chemical composition in the UTLS region can impact physical and dynamical processes that can lead to changes in cloudiness, precipitation, radiative forcing, stratosphere-troposphere exchange and zonal flow. The objective of this study is to investigate the potential impacts of aviation emissions on the upper troposphere and lower stratosphere. In order to assess the impact of the aviation emissions we will focus on changes in atmospheric dynamic due to changes in chemical composition in the UTLS over the Arctic. Specifically, we will assess perturbations in the distribution of the wind, temperature and pressure fields in the UTLS region. Our study will be based on simulations using a high resolution chemical weather model for four scenarios of current (2006) and future (2050) climate: with and without aircraft emissions. The tool that we use is the GEM-AC (Global Environmental Multiscale with Atmospheric Chemistry) chemical weather model where air quality, free tropospheric and stratospheric chemistry processes are on-line and interactive in an operational weather forecast model of Environment Canada. In vertical, the model domain is defined on 70 hybrid levels with model top at 0.1 mb. The gas-phase chemistry includes detailed reactions of Ox, NOx, HOx, CO, CH4, ClOx and BrO. Also, the model can address aerosol microphysics and gas-aerosol partitioning. Aircraft emissions are from the AEDT 2006 database developed by the Federal Aviation Administration (USA) and the future climate simulations are based on RCP8.5 projection presented by the IPCC in the fifth Assessment Report AR5. Results from model simulations on a global variable grid with 0.5o x 0.5o uniform resolution over the Arctic will be presented.

Physical and Chemical Characterization of Particles in the Upper Troposphere and Lower Stratosphere: Microanalysis of Aerosol Impactor Samples

NASA Technical Reports Server (NTRS)

Sheridan, Patrick J.

1999-01-01

Herein is reported activities to support the characterization of the aerosol in the upper troposphere (UT) and lower stratosphere (LS) collected during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) missions in 1994. Through a companion proposal, another group was to measure the size distribution of aerosols in the 0.008 to 2 micrometer diameter range and to collect for us impactor samples of particles larger than about 0.02 gm. In the first year, we conducted laboratory studies related to particulate deposition patterns on our collection substrates, and have performed the analysis of many ASHOE/MAESA aerosol samples from 1994 using analytical electron microscopy (AEM). We have been building an "aerosol climatology" with these data that documents the types and relative abundances of particles observed at different latitudes and altitudes. The second year (and non-funded extension periods) saw continued analyses of impactor aerosol samples, including more ASHOE/MAESA samples, some northern hemisphere samples from the NASA Stratospheric Photochemistry Aerosols and Dynamics Expedition (SPADE) program for comparison, and a few aerosol samples from the NASA Stratospheric TRacers of Atmospheric Transport (STRAT) program. A high-resolution field emission microscope was used for the analysis and re-analysis of a number of samples to determine if this instrument was superior in performance to our conventional electron microscope. In addition, some basic laboratory studies were conducted to determine the minimum detectable and analyzable particle size for different types of aerosols. In all, 61 aerosol samples were analyzed, with a total of over 30,000 individual particle analyses. In all analyzed samples, sulfate particles comprised the major aerosol number fraction. It must be stressed that particles composed of more than one species, for example sulfate and organic carbon, were classified according to the major fraction. Thus, many of the particles classified as sulfate may have contained significant mass fractions of carbonaceous or other material. These particles for the most part did not show two physical phases, however. Nonsulfate particles were classified according to the physical and chemical characteristics of each particle, and were grouped into the major nonsulfate particle classes, including C-rich, crustal, metallic, and salts. Our UT and LS sample analyses indicate a maximum for crustal and C-rich particle abundance in the Northern Hemisphere upper troposphere, and a salt particle maximum in the Southern Hemisphere upper troposphere. Metallic particles are clearly more prevalent in the troposphere than in the stratosphere, but interhemispheric differences appear small.

Particulate sulfur in the upper troposphere and lowermost stratosphere - sources and climate forcing

NASA Astrophysics Data System (ADS)

Martinsson, Bengt G.; Friberg, Johan; Sandvik, Oscar S.; Hermann, Markus; van Velthoven, Peter F. J.; Zahn, Andreas

2017-09-01

This study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8-12 km altitude of the IAGOS-CARIBIC platform in the time period 1999-2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.

Solubility of methanol in low-temperature aqueous sulfuric acid and implications for atmospheric particle composition

NASA Technical Reports Server (NTRS)

Iraci, Laura T.; Essin, Andrew M.; Golden, David M.; Hipskind, R. Stephen (Technical Monitor)

2001-01-01

Using traditional Knudsen cell techniques, we find well-behaved Henry's law uptake of methanol in aqueous 45 - 70 wt% H2SO4 solutions at temperatures between 197 and 231 K. Solubility of methanol increases with decreasing temperature and increasing acidity, with an effective Henry's law coefficient ranging from 10(exp 5) - 10(exp 8) M/atm. Equilibrium uptake of methanol into sulfuric acid aerosol particles in the upper troposphere and lower stratosphere will not appreciably alter gas-phase concentrations of methanol. The observed room temperature reaction between methanol and sulfuric acid is too slow to provide a sink for gaseous methanol at the temperatures of the upper troposphere and lower stratosphere. It is also too slow to produce sufficient quantities of soluble reaction products to explain the large amount of unidentified organic material seen in particles of the upper troposphere.

Stratospheric sulfuric acid fraction and mass estimate for the 1982 volcanic eruption of El Chichon

NASA Technical Reports Server (NTRS)

Hofmann, D. J.; Rosen, J. M.

1983-01-01

The stratospheric sulfuric acid fraction and mass for the 1982 volcanic eruptions of El Chichon are investigated using data from balloon soundings at Laramie (41 deg N) and in southern Texas (27-29 deg N). The total stratospheric mass of these eruptions is estimated to be approximately 8 Tg about 6.5 months after the eruption with possibly as much as 20 Tg in the stratosphere about 45 days after the eruption. Observations of the aerosol in Texas revealed two primary layers, both highly volatile at 150 C. Aerosol in the upper layer at about 25 km was composed of an approximately 80 percent H2SO4 solution while the lower layer at approximately 18 km was composed of a 60-65 percent H2SO4 solution aerosol. It is calculated that an H2SO4 vapor concentration of at least 3 x 10 to the 7th molecules/cu cm is needed to sustain the large droplets in the upper layer. An early bi-modal nature in the size distribution indicates droplet nucleation from the gas phase during the first 3 months, while the similarity of the large particle profiles 2 months apart shows continued particle growth 6.5 months after the explosion.

Observations of vertical velocities in the tropical upper troposphere and lower stratosphere using the Arecibo 430-MHz radar

NASA Technical Reports Server (NTRS)

Cornish, C. R.

1988-01-01

The first clear-air observations of vertical velocities in the tropical upper troposphere and lower stratosphere (8-22 km) using the Arecibo 430-MHz radar are presented. Oscillations in the vertical velocity near the Brunt-Vaisala period are observed in the lower stratosphere during the 12-hour observation period. Frequency power spectra from the vertical velocity time series show a slope between -0.5 and -1.0. Vertical wave number spectra computed from the height profiles of vertical velocities have slopes between -1.0 and -1.5. These observed slopes do not agree well with the slopes of +1/3 and -2.5 for frequency and vertical wave number spectra, respectively, predicted by a universal gravity-wave spectrum model. The spectral power of wave number spectra of a radial beam directed 15 deg off-zenith is enhanced by an order of magnitude over the spectral power levels of the vertical beam. This enhancement suggests that other geophysical processes besides gravity waves are present in the horizontal flow. The steepening of the wave number spectrum of the off-vertical beam in the lower stratosphere to near -2.0 is attributed to a quasi-inertial period wave, which was present in the horizontal flow during the observation period.

Subtropical Potential Vorticity Intrusion Drives Increasing Tropospheric Ozone over the Tropical Central Pacific.

PubMed

Nath, Debashis; Chen, Wen; Graf, Hans-F; Lan, Xiaoqing; Gong, Hainan; Nath, Reshmita; Hu, Kaiming; Wang, Lin

2016-02-12

Drawn from multiple reanalysis datasets, an increasing trend and westward shift in the number of Potential Vorticity intrusion events over the Pacific are evident. The increased frequency can be linked to a long-term trend in upper tropospheric equatorial westerly wind and subtropical jets during boreal winter to spring. These may be resulting from anomalous warming and cooling over the western Pacific warm pool and the tropical eastern Pacific, respectively. The intrusions brought dry and ozone rich air of stratospheric origin deep into the tropics. In the tropical upper troposphere, interannual ozone variability is mainly related to convection associated with El Niño/Southern Oscillation. Zonal mean stratospheric overturning circulation organizes the transport of ozone rich air poleward and downward to the high and midlatitudes leading there to higher ozone concentration. In addition to these well described mechanisms, we observe a long-term increasing trend in ozone flux over the northern hemispheric outer tropical (10-25°N) central Pacific that results from equatorward transport and downward mixing from the midlatitude upper troposphere and lower stratosphere during PV intrusions. This increase in tropospheric ozone flux over the Pacific Ocean may affect the radiative processes and changes the budget of atmospheric hydroxyl radicals.

Effects of Greenhouse Gas Increase and Stratospheric Ozone Depletion on Stratospheric Mean Age of Air in 1960-2010

NASA Technical Reports Server (NTRS)

Li, Feng; Newman, Paul; Pawson, Steven; Perlwitz, Judith

2018-01-01

The relative impacts of greenhouse gas (GHG) increase and stratospheric ozone depletion on stratospheric mean age of air in the 1960-2010 period are quantified using the Goddard Earth Observing System Chemistry-�Climate Model. The experiment compares controlled simulations using a coupled atmosphere-�ocean version of the Goddard Earth Observing System Chemistry-�Climate Model, in which either GHGs or ozone depleting substances, or both factors evolve over time. The model results show that GHGs and ozone-depleting substances have about equal contributions to the simulated mean age decrease, but GHG increases account for about two thirds of the enhanced strength of the lower stratospheric residual circulation. It is also found that both the acceleration of the diabatic circulation and the decrease of the mean age difference between downwelling and upwelling regions are mainly caused by GHG forcing. The results show that ozone depletion causes an increase in the mean age of air in the Antarctic summer lower stratosphere through two processes: (1) a seasonal delay in the Antarctic polar vortex breakup that inhibits young midlatitude air from mixing with the older air inside the vortex, and (2) enhanced Antarctic downwelling that brings older air from middle and upper stratosphere into the lower stratosphere.

Understanding Differences in Upper Stratospheric Ozone Response to Changes in Chlorine and Temperature as Computed Using CCMVal Models

NASA Technical Reports Server (NTRS)

Douglass, A. R.; Stolarski, R. S.; Strahan, S. E.; Oman, L. D.

2012-01-01

Projections of future ozone levels are made using models that couple a general circulation model with a representation of atmospheric photochemical processes, allowing interactions among photochemical processes, radiation, and dynamics. Such models are known as chemistry and climate models (CCMs). Although developed from common principles and subject to the same boundary conditions, simulated ozone time series vary for projections of changes in ozone depleting substances (ODSs) and greenhouse gases. In the upper stratosphere photochemical processes control ozone level, and ozone increases as ODSs decrease and temperature decreases due to greenhouse gas increase. Simulations agree broadly but there are quantitative differences in the sensitivity of ozone to chlorine and to temperature. We obtain insight into these differences in sensitivity by examining the relationship between the upper stratosphere annual cycle of ozone and temperature as produced by a suite of models. All simulations conform to expectation in that ozone is less sensitive to temperature when chlorine levels are highest because chlorine catalyzed loss is nearly independent of temperature. Differences in sensitivity are traced to differences in simulated temperature, ozone and reactive nitrogen when chlorine levels are close to background. This work shows that differences in the importance of specific processes underlie differences in simulated sensitivity of ozone to composition change. This suggests a) the multi-model mean is not a best estimate of the sensitivity of upper ozone to changes in ODSs and temperature; b) the spread of values is not an appropriate measure of uncertainty.

Contributions to Future Stratospheric Climate Change: An Idealized Chemistry-Climate Model Sensitivity Study

NASA Technical Reports Server (NTRS)

Hurwitz, M. M.; Braesicke, P.; Pyle, J. A.

2010-01-01

Within the framework of an idealized model sensitivity study, three of the main contributors to future stratospheric climate change are evaluated: increases in greenhouse gas concentrations, ozone recovery, and changing sea surface temperatures (SSTs). These three contributors are explored in combination and separately, to test the interactions between ozone and climate; the linearity of their contributions to stratospheric climate change is also assessed. In a simplified chemistry-climate model, stratospheric global mean temperature is most sensitive to CO2 doubling, followed by ozone depletion, then by increased SSTs. At polar latitudes, the Northern Hemisphere (NH) stratosphere is more sensitive to changes in CO2, SSTs and O3 than is the Southern Hemisphere (SH); the opposing responses to ozone depletion under low or high background CO2 concentrations, as seen with present-day SSTs, are much weaker and are not statistically significant under enhanced SSTs. Consistent with previous studies, the strength of the Brewer-Dobson circulation is found to increase in an idealized future climate; SSTs contribute most to this increase in the upper troposphere/lower stratosphere (UT/LS) region, while CO2 and ozone changes contribute most in the stratosphere and mesosphere.

An emission module for ICON-ART 2.0: implementation and simulations of acetone

NASA Astrophysics Data System (ADS)

Weimer, Michael; Schröter, Jennifer; Eckstein, Johannes; Deetz, Konrad; Neumaier, Marco; Fischbeck, Garlich; Hu, Lu; Millet, Dylan B.; Rieger, Daniel; Vogel, Heike; Vogel, Bernhard; Reddmann, Thomas; Kirner, Oliver; Ruhnke, Roland; Braesicke, Peter

2017-06-01

We present a recently developed emission module for the ICON (ICOsahedral Non-hydrostatic)-ART (Aerosols and Reactive Trace gases) modelling framework. The emission module processes external flux data sets and increments the tracer volume mixing ratios in the boundary layer accordingly. The performance of the emission module is illustrated with simulations of acetone, using a simplified chemical depletion mechanism based on a reaction with OH and photolysis only. In our model setup, we calculate a tropospheric acetone lifetime of 33 days, which is in good agreement with the literature. We compare our results with ground-based as well as with airborne IAGOS-CARIBIC measurements in the upper troposphere and lowermost stratosphere (UTLS) in terms of phase and amplitude of the annual cycle. In all our ICON-ART simulations the general seasonal variability is well represented but uncertainties remain concerning the magnitude of the acetone mixing ratio in the UTLS region. In addition, the module for online calculations of biogenic emissions (MEGAN2.1) is implemented in ICON-ART and can replace the offline biogenic emission data sets. In a sensitivity study we show how different parametrisations of the leaf area index (LAI) change the emission fluxes calculated by MEGAN2.1 and demonstrate the importance of an adequate treatment of the LAI within MEGAN2.1. We conclude that the emission module performs well with offline and online emission fluxes and allows the simulation of the annual cycles of emissions-dominated substances.

NASA's Upper Atmosphere Research Program (UARP) and Atmospheric Chemistry Modeling and Analysis Program (ACMAP): Research Summaries 1997-1999

NASA Technical Reports Server (NTRS)

Kurylo, M. J.; DeCola, P. L.; Kaye, J. A.

2000-01-01

Under the mandate contained in the FY 1976 NASA Authorization Act, the National Aeronautics and Space Administration (NASA) has developed and is implementing a comprehensive program of research, technology development, and monitoring of the Earth's upper atmosphere, with emphasis on the upper troposphere and stratosphere. This program aims at expanding our chemical and physical understanding to permit both the quantitative analysis of current perturbations as well as the assessment of possible future changes in this important region of our environment. It is carried out jointly by the Upper Atmosphere Research Program (UARP) and the Atmospheric Chemistry Modeling and Analysis Program (ACMAP), both managed within the Research Division in the Office of Earth Science at NASA. Significant contributions to this effort have also been provided by the Atmospheric Effects of Aviation Project (AEAP) of NASA's Office of Aero-Space Technology. The long-term objectives of the present program are to perform research to: understand the physics, chemistry, and transport processes of the upper troposphere and the stratosphere and their control on the distribution of atmospheric chemical species such as ozone; assess possible perturbations to the composition of the atmosphere caused by human activities and natural phenomena (with a specific emphasis on trace gas geographical distributions, sources, and sinks and the role of trace gases in defining the chemical composition of the upper atmosphere); understand the processes affecting the distributions of radiatively active species in the atmosphere, and the importance of chemical-radiative-dynamical feedbacks on the meteorology and climatology of the stratosphere and troposphere; and understand ozone production, loss, and recovery in an atmosphere with increasing abundances of greenhouse gases. The current report is composed of two parts. Part 1 summarizes the objectives, status, and accomplishments of the research tasks supported under NASA UARP and ACMAP in a document entitled, Research Summaries 1997- 1999. Part 2 is entitled Present State of Knowledge of the Upper Atmosphere 1999 An Assessment Report.

Modeled Full-Flight Aircraft Emissions Impacts on Air Quality and Their Sensitivity to Grid Resolution

EPA Science Inventory

Aviation is a unique anthropogenic source with four-dimensional varying emissions, peaking at cruise altitudes (9–12 km). Aircraft emission budgets in the upper troposphere lower stratosphere region and their potential impacts on upper troposphere and surface air quality ar...

Quantifying stratospheric ozone trends: Complications due to stratospheric cooling

NASA Astrophysics Data System (ADS)

McLinden, C. A.; Fioletov, V.

2011-02-01

Recent studies suggest that ozone turnaround (the second stage of ozone recovery) is near. Determining precisely when this occurs, however, will be complicated by greenhouse gas-induced stratospheric cooling as ozone trends derived from profile data in different units and/or vertical co-ordinates will not agree. Stratospheric cooling leads to simultaneous trends in air density and layer thicknesses, confounding the interpretation of ozone trends. A simple model suggests that instruments measuring ozone in different units may differ as to the onset of turnaround by a decade, with some indicting a continued decline while others an increase. This concept was illustrated by examining the long-term (1979-2005) ozone trends in the SAGE (Stratospheric Aerosol and Gas Experiment) and SBUV (Solar Backscatter Ultraviolet) time series. Trends from SAGE, which measures number density as a function of altitude, and SBUV, which measures partial column as a function of pressure, are known to differ by 4-6%/decade in the upper stratosphere. It is shown that this long-standing difference can be reconciled to within 2%/decade when the trend in temperature is properly accounted for.

Development of algorithms for using satellite meteorological data sets to study global transport of stratospheric aerosols and ozone

NASA Technical Reports Server (NTRS)

Want, P. H.; Deepak, A.

1985-01-01

The utilization of stratospheric aerosol and ozone measurements obtained from the NASA developed SAM II and SAGE satellite instruments were investigated for their global scale transports. The stratospheric aerosols showed that during the stratospheric warming of the winter 1978 to 1979, the distribution of the zonal mean aerosol extinction ratio in the northern high latitude exhibited distinct changes. Dynamic processes might have played an important role in maintenance role in maintenance of this zonal mean distribution. As to the stratospheric ozone, large poleward ozone transports are shown to occur in the altitude region from 24 km to 38 km near 55N during this warming. This altitude region is shown to be a transition region of the phase relationship between ozone and temperature waves from an in-phase one above 38 km. It is shown that the ozone solar heating in the upper stratosphere might lead to enhancement of the damping rate of the planetary waves due to infrared radiation alone in agreement with theoretical analyses and an earlier observational study.

Drift-corrected Odin-OSIRIS ozone product: algorithm and updated stratospheric ozone trends

NASA Astrophysics Data System (ADS)

Bourassa, Adam E.; Roth, Chris Z.; Zawada, Daniel J.; Rieger, Landon A.; McLinden, Chris A.; Degenstein, Douglas A.

2018-01-01

A small long-term drift in the Optical Spectrograph and Infrared Imager System (OSIRIS) stratospheric ozone product, manifested mostly since 2012, is quantified and attributed to a changing bias in the limb pointing knowledge of the instrument. A correction to this pointing drift using a predictable shape in the measured limb radiance profile is implemented and applied within the OSIRIS retrieval algorithm. This new data product, version 5.10, displays substantially better both long- and short-term agreement with Microwave Limb Sounder (MLS) ozone throughout the stratosphere due to the pointing correction. Previously reported stratospheric ozone trends over the time period 1984-2013, which were derived by merging the altitude-number density ozone profile measurements from the Stratospheric Aerosol and Gas Experiment (SAGE) II satellite instrument (1984-2005) and from OSIRIS (2002-2013), are recalculated using the new OSIRIS version 5.10 product and extended to 2017. These results still show statistically significant positive trends throughout the upper stratosphere since 1997, but at weaker levels that are more closely in line with estimates from other data records.

Historical Tropospheric and Stratospheric Ozone Radiative Forcing Using the CMIP6 Database

NASA Astrophysics Data System (ADS)

Checa-Garcia, Ramiro; Hegglin, Michaela I.; Kinnison, Douglas; Plummer, David A.; Shine, Keith P.

2018-04-01

We calculate ozone radiative forcing (RF) and stratospheric temperature adjustments for the period 1850-2014 using the newly available Coupled Model Intercomparison Project phase 6 (CMIP6) ozone data set. The CMIP6 total ozone RF (1850s to 2000s) is 0.28 ± 0.17 W m-2 (which is 80% higher than our CMIP5 estimation), and 0.30 ± 0.17 W m-2 out to the present day (2014). The total ozone RF grows rapidly until the 1970s, slows toward the 2000s, and shows a renewed growth thereafter. Since the 1990s the shortwave RF exceeds the longwave RF. Global stratospheric ozone RF is positive between 1930 and 1970 and then turns negative but remains positive in the Northern Hemisphere throughout. Derived stratospheric temperature changes show a localized cooling in the subtropical lower stratosphere due to tropospheric ozone increases and cooling in the upper stratosphere due to ozone depletion by more than 1 K already prior to the satellite era (1980) and by more than 2 K out to the present day (2014).

Implications of the stratospheric water vapor distribution as determined from the Nimbus 7 LIMS experiment. [Limb Infrared Monitor of Stratosphere

NASA Technical Reports Server (NTRS)

Remsberg, E. E.; Russell, J. M., III; Gordley, L. L.; Gille, J. C.; Bailey, P. L.

1984-01-01

The LIMS experiment on Nimbus 7 has provided new results on the stratospheric water vapor distribution. The data show (1) a latitudinal gradient with mixing ratios that increase by a factor of 2 from equator to + or - 60 degrees at 50 mb, (2) most of the time there is a fairly uniform mixing ratio of 5 ppmv at high latitudes, but more variation exists during winter, (3) a well-developed hygropause at low to midlatitudes of the lower stratosphere, (4) a source region of water vapor in the upper stratospehere to lower mesosphere that is consistent with methane oxidation chemistry, at least within the uncertainties of the data, (5) an apparent zonal mean H2O distribution that is consistent with the circulation proposed by Brewer in 1949, and (6) a zonal mean distribution in the lower stratosphere that is consistent with the idea of quasi-isentropic transport by eddies in the meridional direction. Limits to the use of the data in the refinement of our understanding of the stratospheric water vapor budget are noted.

UARS MLS observations of lower stratospheric ClO in the 1992-93 and 1993-94 Arctic winter vortices

NASA Technical Reports Server (NTRS)

Waters, J. W.; Manney, G. L.; Read, W. G.; Froidevaux, L.; Flower, D. A.; Jarnot, R. F.

1995-01-01

Upper Atmosphere Research Satellite (UARS) Microwave Limb Sounder (MLS) measurements of lower stratospheric ClO during 1992-93 and 1993-94 Arctic winters are presented. Enhanced ClO in the 1992-93 winter was first observed in early December, and extensively during February when temperatures were continually low enough for polar stratospheric cloud (PSCs). Sporadic episodes of enhanced ClO were observed for most of the 1993-94 winter as minimum temperatures hovered near the PSC threshold, with largest ClO amounts occurring in early March after a sudden deep cooling in late February.

Extratropical Stratosphere-Troposphere Mass Exchange

NASA Technical Reports Server (NTRS)

Schoeberl, Mark R.

2004-01-01

Understanding the exchange of gases between the stratosphere and the troposphere is important for determining how pollutants enter the stratosphere and how they leave. This study does a global analysis of that the exchange of mass between the stratosphere and the troposphere. While the exchange of mass is not the same as the exchange of constituents, you can t get the constituent exchange right if you have the mass exchange wrong. Thus this kind of calculation is an important test for models which also compute trace gas transport. In this study I computed the mass exchange for two assimilated data sets and a GCM. The models all agree that amount of mass descending from the stratosphere to the troposphere in the Northern Hemisphere extra tropics is approx. 10(exp 10) kg/s averaged over a year. The value for the Southern Hemisphere by about a factor of two. ( 10(exp 10) kg of air is the amount of air in 100 km x 100 km area with a depth of 100 m - roughly the size of the D.C. metro area to a depth of 300 feet.) Most people have the idea that most of the mass enters the stratosphere through the tropics. But this study shows that almost 5 times more mass enters the stratosphere through the extra-tropics. This mass, however, is quickly recycled out again. Thus the lower most stratosphere is a mixture of upper stratospheric air and tropospheric air. This is an important result for understanding the chemistry of the lower stratosphere.

Synoptic-scale variability of arctic gravity wave activity during summer and potential impacts on the high latitude middle atmosphere

NASA Astrophysics Data System (ADS)

Gerrard, Andrew John

Although the role of gravity waves in the global atmospheric circulation is generally understood, discussion of synoptic gravity wave activity, especially pertaining to high latitude summer environments, is lacking in the literature. Tropospherically generated gravity waves greatly contribute to the zonal drag necessary to induce meridional outflow and subsequent upwelling observed in the adiabatically cooled summer mesosphere, ultimately resulting in an environment conducive to mesospheric cloud formation. However, the very gravity wave activity responsible for this induced cooling is also believed to be a major source of variability on mesospheric clouds over shorter time scales, and this topic should be of considerable interest if such clouds are to be used as tracers of the global climate. It is therefore the purpose of this thesis to explore high latitude synoptic gravity wave activity and ultimately seek an understanding of the associated influence on overlaying summer mesospheric clouds. Another goal is to better understand and account for potential variability in high latitude middle and upper atmospheric measurements that can be directly associated with "weather conditions" at lower altitudes. These endeavors are addressed through Rayleigh/aerosol lidar data obtained from the ARCtic LIdar TEchnology (ARCLITE) facility located at Sondrestrom, Greenland (67°N, 310°E), global tropospheric and stratospheric analyses and forecasts, and the Gravity-wave Regional Or Global RAy Tracer (GROGRAT) model. In this study we are able to show that (a) the upper stratospheric gravity wave strength and the brightness of overlaying mesospheric clouds, as measured by representative field proxies, are negatively correlated over time scales of less than a day, (b) such upper stratospheric gravity wave variability is inversely related to mesospheric cloud variability on time scales of ˜1 to 4 hours, (c) gravity wave hindcasts faithfully reproduce experimental lidar observations taken over the month of August 1996, (d) the observed upper stratospheric gravity wave activity is shown to originate from regionalized, non-orographic sources in the troposphere, (e) such gravity wave activity can propagate through the middle atmosphere, potentially impacting overlaying mesospheric clouds, and (f) the forecasting of such upper stratospheric gravity wave activity, and therefore the corresponding mesospheric cloud activity, is feasible. In conclusion, the results herein provide additional evidence of gravity wave influence on mesospheric clouds, a step towards the forecasting of regional gravity wave activity, and ultimately a better understanding of synoptic gravity wave activity at high latitudes.

Homogeneous processes of atmospheric interest

NASA Technical Reports Server (NTRS)

Rossi, M. J.; Barker, J. R.; Golden, D. M.

1983-01-01

Upper atmospheric research programs in the department of chemical kinetics are reported. Topics discussed include: (1) third-order rate constants of atmospheric importance; (2) a computational study of the HO2 + HO2 and DO2 + DO2 reactions; (3) measurement and estimation of rate constants for modeling reactive systems; (4) kinetics and thermodynamics of ion-molecule association reactions; (5) entropy barriers in ion-molecule reactions; (6) reaction rate constant for OH + HOONO2 yields products over the temperature range 246 to 324 K; (7) very low-pressure photolysis of tert-bytyl nitrite at 248 nm; (8) summary of preliminary data for the photolysis of C1ONO2 and N2O5 at 285 nm; and (9) heterogeneous reaction of N2O5 and H2O.

NASA's Upper Atmosphere Research Program UARP and Atmospheric Chemistry Modeling and Analysis Program (ACMAP): Research Summaries 1994 - 1996. Report to Congress and the Environmental Protection Agency

NASA Technical Reports Server (NTRS)

Kendall, Rose (Compiler); Wolfe, Kathy (Compiler)

1997-01-01

Under the mandate contained in the FY 1976 NASA Authorization Act, the National Aeronautics and Space Administration (NASA) has developed and is implementing a comprehensive program of research, technology, and monitoring of the Earth's upper atmosphere, with emphasis on the stratosphere. This program aims at expanding our understanding to permit both the quantitative analysis of current perturbations as well as the assessment of possible future changes in this important region of our environment. It is carried out jointly by the Upper Atmosphere Research Program (UARP) and the Atmospheric Chemistry Modeling and Analysis Program (ACMAP), both managed within the Science Division in the Office of Mission to Planet Earth at NASA. Significant contributions to this effort are also provided by the Atmospheric Effects of Aviation Project (AEAP) of NASA's Office of Aeronautics. The long-term objectives of the present program are to perform research to: understand the physics, chemistry, and transport processes of the upper atmosphere and their effect on the distribution of chemical species in the stratosphere, such as ozone; understand the relationship of the trace constituent composition of the lower stratosphere and the lower troposphere to the radiative balance and temperature distribution of the Earth's atmosphere; and accurately assess possible perturbations of the upper atmosphere caused by human activities as well as by natural phenomena. In compliance with the Clean Air Act Amendments of 1990, Public Law 101-549, NASA has prepared a report on the state of our knowledge of the Earth's upper atmosphere, particularly the stratosphere, and on the progress of UARP and ACMAP. The report for the year 1996 is composed of two parts. Part 1 summarizes the objectives, status, and accomplishments of the research tasks supported under NASA UARP and ACMAP in a document entitled, Research Summary 1994-1996. Part 2 is entitled Present State of Knowledge of the Upper Atmosphere 1996.- An Assessment Report. It consists primarily of the Executive Summary and Chapter Summaries of the World Meteorological Organization Global Ozone Research and Monitoring Project Report No. 37, Scientific Assessment of Ozone Depletion: 1994, sponsored by NASA, the National Oceanic and Atmospheric Administration (NOAA), the UK Department of the Environment, the United Nations Environment Program, and the World Meteorological Organization. Other sections of Part 11 include summaries of the following: an Atmospheric Ozone Research Plan from NASA's Office of Mission to Planet Earth; summaries from a series of Space Shuttle-based missions and two recent airborne measurement campaigns; the Executive Summary of the 1995 Scientific Assessment of the Atmospheric Effects of Stratospheric Aircraft, and the most recent evaluation of photochemical and chemical kinetics data (Evaluation No. 12 of the NASA Panel for Data Evaluation) used as input parameters for atmospheric models.

Changes in tropospheric composition and air quality due to stratospheric ozone depletion.

PubMed

Solomon, Keith R; Tang, Xiaoyan; Wilson, Stephen R; Zanis, Prodromos; Bais, Alkiviadis F

2003-01-01

Increased UV-B through stratospheric ozone depletion leads to an increased chemical activity in the lower atmosphere (the troposphere). The effect of stratospheric ozone depletion on tropospheric ozone is small (though significant) compared to the ozone generated anthropogenically in areas already experiencing air pollution. Modeling and experimental studies suggest that the impacts of stratospheric ozone depletion on tropospheric ozone are different at different altitudes and for different chemical regimes. As a result the increase in ozone due to stratospheric ozone depletion may be greater in polluted regions. Attributable effects on concentrations are expected only in regions where local emissions make minor contributions. The vertical distribution of NOx (NO + NO2), the emission of volatile organic compounds and the abundance of water vapor, are important influencing factors. The long-term nature of stratospheric ozone depletion means that even a small increase in tropospheric ozone concentration can have a significant impact on human health and the environment. Trifluoroacetic acid (TFA) and chlorodifluoroacetic acid (CDFA) are produced by the atmospheric degradation of hydrochlorofluorocarbons (HCFCs) and hydrofluorocarbons (HFCs). TFA has been measured in rain, rivers, lakes, and oceans, the ultimate sink for these and related compounds. Significant anthropogenic sources of TFA other than degradation HCFCs and HFCs have been identified. Toxicity tests under field conditions indicate that the concentrations of TFA and CDFA currently produced by the atmospheric degradation of HFCs and HCFCs do not present a risk to human health and the environment. The impact of the interaction between ozone depletion and future climate change is complex and a significant area of current research. For air quality and tropospheric composition, a range of physical parameters such as temperature, cloudiness and atmospheric transport will modify the impact of UV-B. Changes in the chemical composition of the atmosphere including aerosols will also have an impact. For example, tropospheric OH is the 'cleaning' agent of the troposphere. While increased UV-B increases the OH concentration, increases in concentration of gases like methane, carbon monoxide and volatile organic compounds will act as sinks for OH in troposphere and hence change air quality and chemical composition in the troposphere. Also, changes in the aerosol content of the atmosphere resulting from global climate change may affect ozone photolysis rate coefficients and hence reduce or increase tropospheric ozone concentrations.

MIPAS ESA v7 carbon tetrachloride data: distribution, trend and atmospheric lifetime estimation

NASA Astrophysics Data System (ADS)

Valeri, M.; Barbara, F.; Boone, C. D.; Ceccherini, S.; Gai, M.; Maucher, G.; Raspollini, P.; Ridolfi, M.; Sgheri, L.; Wetzel, G.; Zoppetti, N.

2017-12-01

Carbon tetrachloride (CCl4) is a strong ozone-depleting atmospheric gas regulated by the Montreal protocol. Recently it received increasing interest due to the so called "mystery of CCl4": it was found that its atmospheric concentration at the surface declines with a rate significantly smaller than its lifetime-limited rate. Indeed there is a discrepancy between atmospheric observations and the estimated distribution based on the reported production and consumption. Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) measurements are used to estimate CCl4 distributions, its trend, and atmospheric lifetime in the upper troposphere / lower stratosphere (UTLS) region. In particular, here we use MIPAS product generated with Version 7 of the Level 2 algorithm operated by the European Space Agency. The CCl4 distribution shows features typical of long-lived species of anthropogenic origin: higher concentrations in the troposphere, decreasing with altitude due to the photolysis. We compare MIPAS CCl4 data with independent observations from Atmospheric Chemistry Experiment - Fourier Transform Spectrometer (ACE - FTS) and stratospheric balloon version of MIPAS (MIPAS-B). The comparison shows a general good agreement between the different datasets. CCl4 trends are evaluated as a function of both latitude and altitude: negative trends (-10/ -15 pptv/decade, -10/ -30 %/decade) are found at all latitudes in the UTLS, apart from a region in the Southern mid-latitudes between 50 and 10 hPa where the trend is slightly positive (5/10 pptv/decade, 15/20 %/decade). At the lowest altitudes sounded by the MIPAS scan we find trend values consistent with those determined on the basis of the Advanced Global Atmospheric Gases Experiment (AGAGE) and the National Oceanic and Atmospheric Administration / Earth System Research Laboratory / Halocarbons and other Atmospheric Trace Species (NOAA / ESRL / HATS) networks. CCl4 global average lifetime of 47(39 - 61) years has been estimated using the tracer-tracer linear correlations approach and the CFC-11 as the reference tracer. This estimation is consistent with the most recent literature result of 44(36 - 58) years.

Stratospheric aerosols from the Sarychev volcano eruption in the 2009 Arctic summer

NASA Astrophysics Data System (ADS)

Jégou, F.; Berthet, G.; Brogniez, C.; Renard, J.-B.; François, P.; Haywood, J. M.; Jones, A.; Bourgeois, Q.; Lurton, T.; Auriol, F.; Godin-Beekmann, S.; Guimbaud, C.; Krysztofiak, G.; Gaubicher, B.; Chartier, M.; Clarisse, L.; Clerbaux, C.; Balois, J. Y.; Verwaerde, C.

2013-02-01

Aerosols from the Sarychev volcano eruption (Kuril Islands, northeast of Japan) were observed in the Arctic lower stratosphere a few days after the strongest SO2 injection which occurred on 15 and 16 June 2009. From the observations provided by the Infrared Atmospheric Sounding Interferometer (IASI) an estimated 0.9 Tg of sulphur dioxide was injected into the Upper Troposphere and Lower Stratosphere (UTLS). The resultant stratospheric sulphate aerosols were detected by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instruments. By the first week of July the aerosol plume had spread out over the entire Arctic region. The Sarychev-induced stratospheric aerosol over the Kiruna region (north of Sweden) was measured by the Stratospheric and Tropospheric Aerosol Counter (STAC) during eight balloon flights planned in August and September 2009. During this balloon campaign the Micro RADIomètre BALlon (MicroRADIBAL) and the Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) remote-sensing instruments also observed these aerosols. Aerosol concentrations returned to near-background levels by spring 2010. The effective radius, the Surface Area Density (SAD), the aerosol extinction, and the total sulphur mass from STAC in situ measurements are enhanced with mean values in the range 0.15-0.21 μm, 5.5-14.7 μm2 cm-3, 5.5-29.5×10-4 km-1, and 4.9-12.6×10-10 kg [S] kg-1 [air], respectively, between 14 km and 18 km. The observed and modelled e-folding time of sulphate aerosols from the Sarychev eruption is around 70-80 days, a value much shorter than the 12-14 months calculated for aerosols from the 1991 eruption of Mt. Pinatubo. The OSIRIS stratospheric Aerosol Optical Depth (AOD) at 750 nm is enhanced by a factor of 6 with a value of 0.02 in late July compared to 0.0035 before the eruption. The HadGEM2 and MIMOSA model outputs indicate that aerosol layers in polar region up to 14-15 km are largely modulated by stratosphere-troposphere exchange processes. The spatial extension of the Sarychev plume is well represented in the HadGEM2 model with lower altitudes of the plume being controlled by upper tropospheric troughs which displace the plume downward and upper altitudes around 18-20 km in agreement with lidar observations. A good consistency is found between the HadGEM2 sulphur mass density and the value inferred from the STAC observations with a maximum located about 1 km above the tropopause ranging from 1 to 2×10-9 kg [S] kg-1 [air], which is one order of magnitude higher than the background level.

Observed temporal evolution of global mean age of stratospheric air for the 2002 to 2010 period

NASA Astrophysics Data System (ADS)

Stiller, G. P.; von Clarmann, T.; Haenel, F.; Funke, B.; Glatthor, N.; Grabowski, U.; Kellmann, S.; Kiefer, M.; Linden, A.; Lossow, S.; López-Puertas, M.

2012-04-01

An extensive observational data set from MIPAS measurements, consisting of more than one million SF6 vertical profiles distributed globally has been condensed into monthly zonal means of mean age of air for the period September 2002 to January 2010, binned at 10° latitude and 1-2 km altitude. The data were analysed with respect to their temporal variation by fitting a regression model consisting of: a constant and a linear increase term, 2 proxies for the QBO variation, sinusoidal terms for the seasonal and semi-annual variation and overtones for the correction of the shapes to the observed data set. The impact of subsidence of mesospheric SF6-depleted air and in-mixing into non-polar latitudes on mid-latitudinal age of air and its linear increase was assessed and found to be small. The linear increase of mean age of stratospheric air was found to be positive and partly larger than the trend derived by Engel et al. (2009) for most of the Northern mid-latitudes, the middle stratosphere in the tropics, and parts of the Southern mid-latitudes, as well as for the Southern polar upper stratosphere. Multi-year decrease of age of air was found for the lowermost and the upper stratospheric tropics, for parts of Southern mid-latitudes, and for the Northern polar regions. Analyses of the amplitudes and phases of the seasonal variation shed light on the coupling between different stratospheric regions. In particular, the Northern mid-latitude stratosphere is well coupled to the tropics, while the Northern lowermost mid-latitudinal stratosphere is decoupled, confirming the separation of the shallow branch of the Brewer-Dobson circulation from the deep branch. We suggest an overall increased tropical upwelling, together with a weakening of mixing barriers, especially in the Northern hemisphere, as possible explanations for the observed patterns. Reference: Engel, A., Möbius, T., Bönisch, H., Schmidt, U., Heinz, R., Levin, I., Atlas, E., Aoki, S., Nakazawa, T., Sugawara, S., Moore, F., Hurst, D., Elkins, J., Schauffler, S., Andrews, A., and Boering, K.: Age of stratospheric air unchanged within uncertainties over the past 30 years, Nature Geosci., 2, 28-31, doi:10.1038/ngeo388, 2009.

Modelled thermal and dynamical responses of the middle atmosphere to EPP-induced ozone changes

NASA Astrophysics Data System (ADS)

Karami, K.; Braesicke, P.; Kunze, M.; Langematz, U.; Sinnhuber, M.; Versick, S.

2015-11-01

Energetic particles including protons, electrons and heavier ions, enter the Earth's atmosphere over the polar regions of both hemispheres, where they can greatly disturb the chemical composition of the upper and middle atmosphere and contribute to ozone depletion in the stratosphere and mesosphere. The chemistry-climate general circulation model EMAC is used to investigate the impact of changed ozone concentration due to Energetic Particle Precipitation (EPP) on temperature and wind fields. The results of our simulations show that ozone perturbation is a starting point for a chain of processes resulting in temperature and circulation changes over a wide range of latitudes and altitudes. In both hemispheres, as winter progresses the temperature and wind anomalies move downward with time from the mesosphere/upper stratosphere to the lower stratosphere. In the Northern Hemisphere (NH), once anomalies of temperature and zonal wind reach the lower stratosphere, another signal develops in mesospheric heights and moves downward. Analyses of Eliassen and Palm (EP) flux divergence show that accelerating or decelerating of the stratospheric zonal flow is in harmony with positive and negative anomalies of the EP flux divergences, respectively. This results suggest that the oscillatory mode in the downwelling signal of temperature and zonal wind in our simulations are the consequence of interaction between the resolved waves in the model and the mean stratospheric flow. Therefore, any changes in the EP flux divergence lead to anomalies in the zonal mean zonal wind which in turn feed back on the propagation of Rossby waves from the troposphere to higher altitudes. The analyses of Rossby waves refractive index show that the EPP-induced ozone anomalies are capable of altering the propagation condition of the planetary-scale Rossby waves in both hemispheres. It is also found that while ozone depletion was confined to mesospheric and stratospheric heights, but it is capable to alter Rossby wave propagation down to tropospheric heights. In response to an accelerated polar vortex in the Southern Hemisphere (SH) late wintertime, we found almost two weeks delay in the occurrence of mean dates of Stratospheric Final Warming (SFW). These results suggest that the stratosphere is not merely a passive sink of wave activity from below, but it plays an active role in determining its own budget of wave activity.

Constraining Upper Troposphere/Lower Stratosphere Aerosol Physical Processes with High-Altitude Aircraft Measurements

NASA Technical Reports Server (NTRS)

Jensen, Eric; Rosenlof, Karen H.; Thornberry, Troy

2018-01-01

Interest in a more complete understanding of the sources, composition and microphysics of stratospheric aerosol particles has intensified during recent years for several reasons: (1) small volcanic eruptions have been recognized as a driver of short-term changes in climate forcing; (2) emissions of sulfur dioxide (SO2) and other aerosol precursors have shifted to south Asia and other low latitude regions with intense vertical transport; (3) organic material has been recognized as a key contributor to lower stratospheric aerosol mass; and (4) interest in possible solar radiation management (geoengineering) through significant enhancements in stratospheric aerosols has intensified. To address stratospheric aerosol science issues, we are proposing a NASA Earth Ventures mission to NASA to provide extensive high-altitude aircraft measurements of critical gas-phase and aerosol properties at multiple locations across the planet. In this presentation, we will discuss the objectives of the proposed campaign, the measurements provided, the sampling strategy, and the modeling and analysis approaches that would be used to address specific science questions.

Measurements of IO in the Tropical Marine Boundary Layer using Laser-Induced Fluorescence Spectroscopy

NASA Astrophysics Data System (ADS)

Walker, H.; Ingham, T.; Heard, D. E.

2012-12-01

Halogenated short-lived substances (VSLS) are emitted from the oceans by marine species such as macroalgae and phytoplankton and contribute to halogen loading in the troposphere and lower stratosphere. Transport of halogenated VSLS into the stratosphere occurs mainly in the tropics, where ascending warm air carries them aloft, and leads to catalytic depletion of stratospheric ozone on a global scale and formation of the Antarctic ozone hole. The tropical marine environment is therefore an important region in which to study the effects of these short-lived halogen species on ozone depletion. The SHIVA (Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere) project combines ship-borne, aircraft-based and ground-based measurements in and over the South China Sea and the Sulu Sea, and around the coast of Malaysian Borneo, to reduce uncertainties in the amount of halogenated VSLS reaching the stratosphere, the associated ozone depletion, and the effects of a changing climate on these processes. In this work we present measurements of IO radicals made onboard the German research vessel Sonne during SHIVA, between Singapore and Manila. IO is formed via photolysis of iodine-containing source gases (e.g. I2, CH3I) to produce I atoms, which react with ozone. It is therefore an important species to consider when assessing the impacts of halogen chemistry on ozone depletion. Measurements of IO were made over a two-week period by the University of Leeds Laser-Induced Fluorescence (LIF) instrument, which excites IO radicals at λ ~ 445 nm and detects the resultant fluorescence at λ ~ 512 nm. A suite of supporting gas- and aqueous-phase measurements were also made, including concentrations of halocarbons (e.g. CHBr3, CH3I), trace pollutant gases (e.g. CO, O3, NOx), and biological parameters (e.g. abundance and speciation of phytoplankton). Preliminary data analysis indicates that IO was detected above the instrumental limit of detection (0.3 pptv for a 30 minute averaging period) on 9 days during the cruise, with a maximum mixing ratio of ~ 2.5 pptv. The results are analysed with a photochemical box model using concurrent measurements of source gases (I2, CH3I).

Dispersion and photochemical evolution of reactive pollutants in street canyons

NASA Astrophysics Data System (ADS)

Kwak, Kyung-Hwan; Baik, Jong-Jin; Lee, Kwang-Yeon

2013-05-01

Dispersion and photochemical evolution of reactive pollutants in street canyons with canyon aspect ratios of 1 and 2 are investigated using a computational fluid dynamics (CFD) model coupled with the carbon bond mechanism IV (CBM-IV). Photochemical ages of NOx and VOC are expressed as a function of the NO2-to-NOx and toluene-to-xylene ratios, respectively. These are found to be useful for analyzing the O3 and OH oxidation processes in the street canyons. The OH oxidation process (O3 oxidation process) is more pronounced in the upper (lower) region of the street canyon with a canyon aspect ratio of 2, which is characterized by more (less) aged air. In the upper region of the street canyon, O3 is chemically produced as well as transported downward across the roof level, whereas O3 is chemically reduced in the lower region of the street canyon. The O3 chemical production is generally favorable when the normalized photochemical ages of NOx and VOC are larger than 0.55 and 0.28, respectively. The sensitivities of O3 chemical characteristics to NOx and VOC emission rates, photolysis rate, and ambient wind speed are examined for the lower and upper regions of the street canyon with a canyon aspect ratio of 2. The O3 concentration and the O3 chemical production rate divided by the O3 concentration increase as the NOx emission rate decreases and the VOC emission rate and photolysis rate increase. The O3 concentration is less sensitive to the ambient wind speed than to other factors considered. The relative importance of the OH oxidation process compared to the O3 oxidation process increases with increasing NOx emission rate and photolysis rate and decreasing VOC emission rate. In this study, both O3 and OH oxidation processes are found to be important in street-canyon scale chemistry. The methodology of estimating the photochemical ages can potentially be adopted to neighborhood scale chemistry.

Investigation of the Physical Processes Governing Large-scale Tracer Transport in the Stratosphere and Troposphere

NASA Technical Reports Server (NTRS)

Selkirk, Henry B.

1996-01-01

This report reviews the second year of a three-year research program to investigate the physical mechanisms which underlie the transport of trace constituents in the stratosphere- troposphere system. The primary scientific goal of the research is to identify the processes which transport air masses within the lower stratosphere, particularly between the tropics and middle latitudes. The SASS program seeks to understand the impact of the present and future fleets of conventional jet traffic on the upper troposphere and lower stratosphere, while complementary airborne observations under UARP seek to understand the complex interactions of dynamical and chemical processes that affect the ozone layer. The present investigation contributes to the goals of each of these by diagnosing the history of air parcels intercepted by NASA research aircraft in UARP and AEAP campaigns.

Improvement of the basic knowledge of the climatology of the vertical ozone layer by enhanced balloon sounding

NASA Technical Reports Server (NTRS)

Attmannspacher, W.; Hartmannsgrubber, R.; Lang, P.

1984-01-01

Balloon sounding of the ozone in the Earth atmosphere was performed in order to determine the natural behavior of ozone and its recognizable deviations. The importance of ozone in the Earth atmosphere and the orographic situation of observatories and ozone sounding statistics since 1966 are explained. The physical processes governing the total amount of ozone, and the behavior of stratospheric ozone are described. Measurements in the upper stratosphere show a decrease of the ozone partial pressure above 26 km altitude since 1977. The behavior of tropospheric ozone is discussed. Data since 1977 show increasing ozone values in the troposphere, up to 50% to 70%. This increase is independent of the solar radiation intensity and the reinforced transport of stratospheric ozone into the troposphere. The increase in the troposphere cannot compensate the stratospheric decrease.

Stratospheric Sudden Warming Effects on the Upper Thermosphere

NASA Astrophysics Data System (ADS)

Yamazaki, Y.; Kosch, M. J.; Emmert, J. T.

2015-12-01

It has been controversial whether a stratospheric sudden warming (SSW) event has any measurable impact on the upper thermosphere. In this study, we use long-term records of the global average thermospheric total mass density derived from satellite orbital decay data during 1967-2013. This enables, for the first time, a statistical investigation of the thermospheric density response to SSW events. A superposed epoch analysis of 37 SSW events reveals a density reduction of 3-7% at 250-575 km around the time of polar vortex weakening. The temperature perturbation is estimated to be -7.0 K at 400 km. We suggest enhanced wave forcing from the lower atmosphere as a possible cause for the density reduction observed during SSWs.

Decadal-Scale Responses in Middle and Upper Stratospheric Ozone From SAGE II Version 7 Data

NASA Technical Reports Server (NTRS)

Remsberg, E. E.

2014-01-01

Stratospheric Aerosol and Gas Experiment (SAGE II) version 7 (v7) ozone profiles are analyzed for their decadal-scale responses in the middle and upper stratosphere for 1991 and 1992-2005 and compared with those from its previous version 6.2 (v6.2). Multiple linear regression (MLR) analysis is applied to time series of its ozone number density vs. altitude data for a range of latitudes and altitudes. The MLR models that are fit to the time series data include a periodic 11 yr term, and it is in-phase with that of the 11 yr, solar UV (Ultraviolet)-flux throughout most of the latitude/ altitude domain of the middle and upper stratosphere. Several regions that have a response that is not quite in-phase are interpreted as being affected by decadal-scale, dynamical forcings. The maximum minus minimum, solar cycle (SClike) responses for the ozone at the low latitudes are similar from the two SAGE II data versions and vary from about 5 to 2.5% from 35 to 50 km, although they are resolved better with v7. SAGE II v7 ozone is also analyzed for 1984-1998, in order to mitigate effects of end-point anomalies that bias its ozone in 1991 and the analyzed results for 1991-2005 or following the Pinatubo eruption. Its SC-like ozone response in the upper stratosphere is of the order of 4%for 1984-1998 vs. 2.5 to 3%for 1991-2005. The SAGE II v7 results are also recompared with the responses in ozone from the Halogen Occultation Experiment (HALOE) that are in terms of mixing ratio vs. pressure for 1991-2005 and then for late 1992- 2005 to avoid any effects following Pinatubo. Shapes of their respective response profiles agree very well for 1992-2005. The associated linear trends of the ozone are not as negative in 1992-2005 as in 1984-1998, in accord with a leveling off of the effects of reactive chlorine on ozone. It is concluded that the SAGE II v7 ozone yields SC-like ozone responses and trends that are of better quality than those from v6.2.

Effects of oil dispersants on photodegradation of parent and alkylated anthracene in seawater.

PubMed

Cai, Zhengqing; Liu, Wen; Fu, Jie; O'Reilly, S E; Zhao, Dongye

2017-10-01

This study investigated effects of three model oil dispersants on photodegradation of two model PAHs (anthracene and 9,10-dimethyanthracene (9,10-DMA)) under simulated sunlight. All three dispersants, i.e. Corexit EC9500A, Corexit EC9527A and SPC 1000, promoted the photolysis rate of 9,10-DMA, following the order of Corexit EC9500A > Corexit EC9527A > SPC 1000. The photodegradation rate was well interpreted by a two-stage, first-order kinetic law with a faster initial photolysis rate in the presence of the dispersants. Span 80, Tween 85 and kerosene were found as the key dispersant components, of which Span 80 and Tween 85 promoted the photodegradation by boosting absorbance of solar irradiation while kerosene by dispersing more PAHs in the upper layer of the water column. Dissolved oxygen (DO) inhibited photolysis of anthracene regardless of dispersant resulting from quenching the excited states of the PAH, while DO facilitated photolysis of 9,10-DMA due to the formation singlet oxygen ( 1 O 2 ) radicals in the presence of oil dispersants. The other ROS, i.e. •O 2 - and •OH, played a negligible role on the photodegradation of anthracene and 9,10-DMA. Fluorescence analysis showed that more anthracene was associated with dispersant than 9,10-DMA, which favored the direct transfer of energy to anthracene, while energy is more likely transferred to oxygen to form 1 O 2 in the case of 9,10-DMA. Direct photolysis dominated the photodegradation of anthracene and 9,10-DMA. Both direct ionization of anthracene and the electron transfer from excited 9,10-DMA to oxygen can lead to formation of the corresponding PAH radical cations. Overall, the oil dispersants accelerated the photolysis rates of the PAHs without altering the degradation pathway. The findings are useful for understanding photochemical weathering of dispersed oil components in the environment. Copyright © 2017 Elsevier Ltd. All rights reserved.

SAGE III solar ozone measurements: Initial results

NASA Technical Reports Server (NTRS)

Wang, Hsiang-Jui; Cunnold, Derek M.; Trepte, Chip; Thomason, Larry W.; Zawodny, Joseph M.

2006-01-01

Results from two retrieval algorithms, o3-aer and o3-mlr , used for SAGE III solar occultation ozone measurements in the stratosphere and upper troposphere are compared. The main differences between these two retrieved (version 3.0) ozone are found at altitudes above 40 km and below 15 km. Compared to correlative measurements, the SAGE II type ozone retrievals (o3-aer) provide better precisions above 40 km and do not induce artificial hemispheric differences in upper stratospheric ozone. The multiple linear regression technique (o3_mlr), however, can yield slightly more accurate ozone (by a few percent) in the lower stratosphere and upper troposphere. By using SAGE III (version 3.0) ozone from both algorithms and in their preferred regions, the agreement between SAGE III and correlative measurements is shown to be approx.5% down to 17 km. Below 17 km SAGE III ozone values are systematically higher, by 10% at 13 km, and a small hemispheric difference (a few percent) appears. Compared to SAGE III and HALOE, SAGE II ozone has the best accuracy in the lowest few kilometers of the stratosphere. Estimated precision in SAGE III ozone is about 5% or better between 20 and 40 km and approx.10% at 50 km. The precision below 20 km is difficult to evaluate because of limited coincidences between SAGE III and sondes. SAGE III ozone values are systematically slightly larger (2-3%) than those from SAGE II but the profile shapes are remarkably similar for altitudes above 15 km. There is no evidence of any relative drift or time dependent differences between these two instruments for altitudes above 15-20 km.

Level 2 processing for the imaging Fourier transform spectrometer GLORIA: derivation and validation of temperature and trace gas volume mixing ratios from calibrated dynamics mode spectra

NASA Astrophysics Data System (ADS)

Ungermann, J.; Blank, J.; Dick, M.; Ebersoldt, A.; Friedl-Vallon, F.; Giez, A.; Guggenmoser, T.; Höpfner, M.; Jurkat, T.; Kaufmann, M.; Kaufmann, S.; Kleinert, A.; Krämer, M.; Latzko, T.; Oelhaf, H.; Olchewski, F.; Preusse, P.; Rolf, C.; Schillings, J.; Suminska-Ebersoldt, O.; Tan, V.; Thomas, N.; Voigt, C.; Zahn, A.; Zöger, M.; Riese, M.

2015-06-01

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an airborne infrared limb imager combining a two-dimensional infrared detector with a Fourier transform spectrometer. It was operated aboard the new German Gulfstream G550 High Altitude LOng Range (HALO) research aircraft during the Transport And Composition in the upper Troposphere/lowermost Stratosphere (TACTS) and Earth System Model Validation (ESMVAL) campaigns in summer 2012. This paper describes the retrieval of temperature and trace gas (H2O, O3, HNO3) volume mixing ratios from GLORIA dynamics mode spectra that are spectrally sampled every 0.625 cm-1. A total of 26 integrated spectral windows are employed in a joint fit to retrieve seven targets using consecutively a fast and an accurate tabulated radiative transfer model. Typical diagnostic quantities are provided including effects of uncertainties in the calibration and horizontal resolution along the line of sight. Simultaneous in situ observations by the Basic Halo Measurement and Sensor System (BAHAMAS), the Fast In-situ Stratospheric Hygrometer (FISH), an ozone detector named Fairo, and the Atmospheric chemical Ionization Mass Spectrometer (AIMS) allow a validation of retrieved values for three flights in the upper troposphere/lowermost stratosphere region spanning polar and sub-tropical latitudes. A high correlation is achieved between the remote sensing and the in situ trace gas data, and discrepancies can to a large extent be attributed to differences in the probed air masses caused by different sampling characteristics of the instruments. This 1-D processing of GLORIA dynamics mode spectra provides the basis for future tomographic inversions from circular and linear flight paths to better understand selected dynamical processes of the upper troposphere and lowermost stratosphere.

Level 2 processing for the imaging Fourier transform spectrometer GLORIA: derivation and validation of temperature and trace gas volume mixing ratios from calibrated dynamics mode spectra

NASA Astrophysics Data System (ADS)

Ungermann, J.; Blank, J.; Dick, M.; Ebersoldt, A.; Friedl-Vallon, F.; Giez, A.; Guggenmoser, T.; Höpfner, M.; Jurkat, T.; Kaufmann, M.; Kaufmann, S.; Kleinert, A.; Krämer, M.; Latzko, T.; Oelhaf, H.; Olchewski, F.; Preusse, P.; Rolf, C.; Schillings, J.; Suminska-Ebersoldt, O.; Tan, V.; Thomas, N.; Voigt, C.; Zahn, A.; Zöger, M.; Riese, M.

2014-12-01

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an airborne infrared limb-imager combining a two-dimensional infrared detector with a Fourier transform spectrometer. It was operated aboard the new German Gulfstream G550 research aircraft HALO during the Transport And Composition in the upper Troposphere/lowermost Stratosphere (TACTS) and Earth System Model Validation (ESMVAL) campaigns in summer 2012. This paper describes the retrieval of temperature and trace gas (H2O, O3, HNO3) volume mixing ratios from GLORIA dynamics mode spectra. 26 integrated spectral windows are employed in a joint fit to retrieve seven targets using consecutively a fast and an accurate tabulated radiative transfer model. Typical diagnostic quantities are provided including effects of uncertainties in the calibration and horizontal resolution along the line-of-sight. Simultaneous in-situ observations by the BAsic HALO Measurement And Sensor System (BAHAMAS), the Fast In-Situ Stratospheric Hygrometer (FISH), FAIRO, and the Atmospheric chemical Ionization Mass Spectrometer (AIMS) allow a validation of retrieved values for three flights in the upper troposphere/lowermost stratosphere region spanning polar and sub-tropical latitudes. A high correlation is achieved between the remote sensing and the in-situ trace gas data, and discrepancies can to a large fraction be attributed to differences in the probed air masses caused by different sampling characteristics of the instruments. This 1-D processing of GLORIA dynamics mode spectra provides the basis for future tomographic inversions from circular and linear flight paths to better understand selected dynamical processes of the upper troposphere and lowermost stratosphere.

Observations and Modeling of Composition of Upper Troposphere/Lower Stratosphere (UTILS): Isentropic Mixing Events and Morphology of HNO3 as Observed by HIRDLS and Comparison with Results from Global Modeling Initiative

NASA Technical Reports Server (NTRS)

Rodriquez, J. M.; Douglass, A.R.; Yoshida, Y.; Strahan, S.; Duncan, B.; Olsen, M.; Gille, J.; Yudin, V.; Nardi, B.

2008-01-01

isentropic exchange of air masses between the tropical upper troposphere and mid-latitude lowermost stratosphere (the so-called "middle world") is an important pathway for stratospheric-tropospheric exchange. A seasonal, global view of this process has been difficult to obtain, in part due to the lack of the vertical resolution in satellite observations needed to capture the laminar character of these events. Ozone observations at a resolution of about 1 km from the High Resolution Dynamic Limb Sounder (HIRDLS) on NASA's Aura satellite show instances of these intrusions. Such intrusions should also be observable in HN03 observations; however, the abundances of nitric acid could be additionally controlled by chemical processes or incorporation and removal into ice clouds. We present a systematic examination of the HIRDLS data on O3 and HNO3 to determine the seasonal and spatial characteristics of the distribution of isentropic intrusions. At the same time, we compare the observed distributions with those calculated by the Global Modeling Initiative combined tropospheric-stratospheric model, which has a vertical resolution of about I km. This Chemical Transport Model (CTM) is driven by meteorological fields obtained from the GEOS-4 system of NASA/Goddard Global Modeling and Assimilation Office (GMAO), for the Aura time period, at a vertical resolution of about 1 km. Such comparison brings out the successes and limitations of the model in representing isentropic stratospheric-tropospheric exchange, and the different processes controlling HNO3 in the UTAS.

Interactions between meteoric smoke particles and the stratospheric aerosol layer

NASA Astrophysics Data System (ADS)

Mann, G. W.; Marshall, L.; Brooke, J. S. A.; Dhomse, S.; Plane, J. M. C.; Feng, W.; Neely, R.; Bardeen, C.; Bellouin, N.; Dalvi, M.; Johnson, C.; Abraham, N. L.; Schmidt, A.; Carslaw, K. S.; Chipperfield, M.; Deshler, T.; Thomason, L. W.

2017-12-01

In-situ measurements in the Arctic, Antarctic and at mid-latitudes suggest a widespread presence of meteoric smoke particles (MSPs), as an inclusion within a distinct class of stratospheric aerosol particles. We apply the UM-UKCA stratosphere-troposphere composition-climate model, with interactive aerosol microphysics, to map the global distribution of these "meteoric-sulphuric particles" and explore the implications of their presence. Comparing to balloon-borne stratospheric aerosol measurements, we indirectly constrain the uncertain MSP flux into the upper mesosphere, and assess whether meteoric inclusion can explain observed refractory/non-volatile particle concentrations. Our experiments suggest meteoric-sulphuric particles are present at all latitudes, the Junge layer transitioning from mostly homogeneously nucleated particles at the bottom, to mostly meteoric-sulphuric particles at the top. We find MSPs exert a major influence on the quiescent Junge layer, with meteoric-sulphuric particles generally bigger than homogeneously nucleated particles, and therefore more rapidly removed into the upper troposphere. Resolving the smoke interactions weakens homogeneous nucleation in polar spring, reduces the quiescent sulphur burden, and improves comparisons to a range of different stratospheric aerosol measurements. The refractory nature of meteoric-sulphuric particles also means they "survive" ascent through the uppermost Junge layer, whereas homogeneously nucleated particles evaporate completely. Simulations through the Pinatubo-perturbed period are more realistic, with greater volcanic enhancement of effective radius, causing faster decay towards quiescent conditions, both effects matching better with observations. Overall, our experiments suggest meteoric-sulphuric particles are an important component of the Junge layer, strongly influential in both quiescent and volcanically perturbed conditions.

Constraining the Stratosphere-Troposphere Exchange of Radiocarbon using AirCore 14CO2 Measurements

NASA Astrophysics Data System (ADS)

Chen, H.

2016-12-01

Radiocarbon (14C) plays an important role in the carbon cycle studies to understand both natural and anthropogenic carbon fluxes, but also in atmospheric chemistry to constrain hydroxyl radical (OH) concentrations in the atmosphere. Apart from the enormous 14C emissions from nuclear bomb testing in the 1950s and 1960s, radiocarbon is primarily produced in the upper atmosphere due to reactions of nitrogen nuclei with thermal neutrons that are induced by cosmic rays. 14C is quickly oxidized to 14CO, which is then further oxidized to 14CO2 by OH. To this end, better understanding the radiocarbon source is very useful to advance the use of radiocarbon for these applications. However, upper atmospheric 14C observations have been very sparse to constrain the magnitude and the location of the 14C production as well as the transport of radiocarbon from the stratosphere to the troposphere. Recently we have successfully made stratospheric 14CO2 measurements using AirCore samples from Sodankylä, Northern Finland, along with regular AirCore profiles of CO2, CH4, and CO since 2013. In this study, we calculate the stratosphere-troposphere exchange of 14C using the correlation between 14CO2 and N2O, and the estimated N2O loss rate. Besides this, we assess the impact of the mean age of air on 14CO2 profiles. Furthermore, we will evaluate the influence of different cosmogenic 14C production scenarios and the uncertainties in the OH field on the seasonal cycles of radiocarbon and on the stratosphere-troposphere exchange.

Multimodel Estimates of Atmospheric Lifetimes of Long-lived Ozone-Depleting Substances: Present and Future

NASA Technical Reports Server (NTRS)

Chipperfield, M. P.; Liang, Q.; Strahan, S. E.; Morgenstern, O.; Dhomse, S. S.; Abraham, N. L.; Archibald, A. T.; Bekki, S.; Braesicke, P.; Di Genova, G.;

Multimodel Estimates of Atmospheric Lifetimes of Long-Lived Ozone-Depleting Substances: Present and Future

NASA Technical Reports Server (NTRS)

Chipperfield, M. P.; Liang, Q.; Strahan, S. E.; Morgenstern, O.; Dhomse, S. S.; Abraham, N. L.; Archibald, A. T.; Bekki, S.; Braesicke, P.; Di Genova, G.;

On the HCN and CO 2 abundance and distribution in Jupiter's stratosphere

NASA Astrophysics Data System (ADS)

Lellouch, E.; Bézard, B.; Strobel, D. F.; Bjoraker, G. L.; Flasar, F. M.; Romani, P. N.

2006-10-01

Observations of Jupiter by Cassini/CIRS, acquired during the December 2000 flyby, provide the latitudinal distribution of HCN and CO 2 in Jupiter's stratosphere with unprecedented spatial resolution and coverage. Following up on a preliminary study by Kunde et al. [Kunde, V.G., and 41 colleagues, 2004. Science 305, 1582-1587], the analysis of these observations leads to two unexpected results (i) the total HCN mass in Jupiter's stratosphere in 2000 was (6.0±1.5)×10 g, i.e., at least three times larger than measured immediately after the Shoemaker-Levy 9 (SL9) impacts in July 1994 and (ii) the latitudinal distributions of HCN and CO 2 are strikingly different: while HCN exhibits a maximum at 45° S and a sharp decrease towards high Southern latitudes, the CO 2 column densities peak over the South Pole. The total CO 2 mass is (2.9±1.2)×10 g. A possible cause for the HCN mass increase is its production from the photolysis of NH 3, although a problem remains because, while millimeter-wave observations clearly indicate that HCN is currently restricted to submillibar ( ˜0.3 mbar) levels, immediate post-impact infrared observations have suggested that most of the ammonia was present in the lower stratosphere near 20 mbar. HCN appears to be a good atmospheric tracer, with negligible chemical losses. Based on 1-dimensional (latitude) transport models, the HCN distribution is best interpreted as resulting from the combination of a sharp decrease (over an order of magnitude in K) of wave-induced eddy mixing poleward of 40° and an equatorward transport with ˜7 cms velocity. The CO 2 distribution was investigated by coupling the transport model with an elementary chemical model, in which CO 2 is produced from the conversion of water originating either from SL9 or from auroral input. The auroral source does not appear adequate to reproduce the CO 2 peak over the South Pole, as required fluxes are unrealistically high and the shape of the CO 2 bulge is not properly matched. In contrast, the CO 2 distribution can be fit by invoking poleward transport with a ˜30 cms velocity and vigorous eddy mixing ( K=2×10 cms). While the vertical distribution of CO 2 is not measured, the combined HCN and CO 2 results imply that the two species reside at different stratospheric levels. Comparing with the circulation regimes predicted by earlier radiative-dynamical models of Jupiter's stratosphere, and with inferences from the ethane and acetylene stratospheric latitudinal distribution, we suggest that CO 2 lies in the middle stratosphere near or below the 5-mbar level.

Effect of the 1997 El Niño on the distribution of upper tropospheric cirrus

NASA Astrophysics Data System (ADS)

Massie, Steven; Lowe, Paul; Tie, Xuexi; Hervig, Mark; Thomas, Gary; Russell, James

2000-09-01

Geographical distributions of Halogen Occultation Experiment (HALOE) aerosol extinction data for 1993-1998 are analyzed in the troposphere and stratosphere at pressures between 121 and 46 hPa. The El Niño conditions of 1997 increased upper tropospheric cirrus over the mid-Pacific and decreased cirrus over Indonesia. Longitudinal centroids of cirrus in the Pacific and over Indonesia shifted eastward by 25° in the troposphere in 1997. Longitudinal centroids of aerosol in the lower stratosphere do not exhibit longitudinal shifts in 1997, indicating that the effects of El Niño upon equatorial particle distributions are confined to the troposphere. The correlation of the longitudinal centroids of outgoing longwave radiation and HALOE extinction confirms the spatial relationship between deep convective clouds and upper tropospheric cirrus. The number of cirrus events observed each year in 1993-1998 in the upper troposphere are quite similar for the region from the Indian Ocean to the mid-Pacific (30°S to 30°N, 50° to 240°E).

Temperature Responses to Spectral Solar Variability on Decadal Time Scales

NASA Technical Reports Server (NTRS)

Cahalan, Robert F.; Wen, Guoyong; Harder, Jerald W.; Pilewskie, Peter

2010-01-01

Two scenarios of spectral solar forcing, namely Spectral Irradiance Monitor (SIM)-based out-of-phase variations and conventional in-phase variations, are input to a time-dependent radiative-convective model (RCM), and to the GISS modelE. Both scenarios and models give maximum temperature responses in the upper stratosphere, decreasing to the surface. Upper stratospheric peak-to-peak responses to out-of-phase forcing are approx.0.6 K and approx.0.9 K in RCM and modelE, approx.5 times larger than responses to in-phase forcing. Stratospheric responses are in-phase with TSI and UV variations, and resemble HALOE observed 11-year temperature variations. For in-phase forcing, ocean mixed layer response lags surface air response by approx.2 years, and is approx.0.06 K compared to approx.0.14 K for atmosphere. For out-of-phase forcing, lags are similar, but surface responses are significantly smaller. For both scenarios, modelE surface responses are less than 0.1 K in the tropics, and display similar patterns over oceanic regions, but complex responses over land.

Airborne gas chromatograph for in situ measurements of long-lived species in the upper troposphere and lower stratosphere

NASA Astrophysics Data System (ADS)

Elkins, J. W.; Fahey, D. W.; Gilligan, J. M.; Dutton, G. S.; Baring, T. J.; Volk, C. M.; Dunn, R. E.; Myers, R. C.; Montzka, S. A.; Wamsley, P. R.; Hayden, A. H.; Butler, J. H.; Thompson, T. M.; Swanson, T. H.; Dlugokencky, E. J.; Novelli, P. C.; Hurst, D. F.; Lobert, J. M.; Ciciora, S. J.; McLaughlin, R. J.; Thompson, T. L.; Winkler, R. H.; Fraser, P. J.; Steele, L. P.; Lucarelli, M. P.

A new instrument, the Airborne Chromatograph for Atmospheric Trace Species IV (ACATS-IV), for measuring long-lived species in the upper troposphere and lower stratosphere is described. Using an advanced approach to gas chromatography and electron capture detection, the instrument can detect low levels of CFC-11 (CCl3F), CFC-12 (CCl2F2), CFC-113 (CCl2F-CClF2), methyl chloroform (CH3CCl3), carbon tetrachloride (CCl4), nitrous oxide (N2O), sulfur hexafluoride (SF6), Halon-1211 (CBrClF2), hydrogen (H2), and methane (CH4) acquired in ambient samples every 180 or 360 s. The instrument operates fully-automated onboard the NASA ER-2 high-altitude aircraft on flights lasting up to 8 hours or more in duration. Recent measurements include 24 successful flights covering a broad latitude range (70°S-61°N) during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) campaign in 1994.

Driving Roles of Tropospheric and Stratospheric Thermal Anomalies in Intensification and Persistence of the Arctic Superstorm in 2012

NASA Astrophysics Data System (ADS)

Tao, Wei; Zhang, Jing; Fu, Yunfei; Zhang, Xiangdong

2017-10-01

Intense synoptic-scale storms have been more frequently observed over the Arctic during recent years. Specifically, a superstorm hit the Arctic Ocean in August 2012 and preceded a new record low Arctic sea ice extent. In this study, the major physical processes responsible for the storm's intensification and persistence are explored through a series of numerical modeling experiments with the Weather Research and Forecasting model. It is found that thermal anomalies in troposphere as well as lower stratosphere jointly lead to the development of this superstorm. Thermal contrast between the unusually warm Siberia and the relatively cold Arctic Ocean results in strong troposphere baroclinicity and upper level jet, which contribute to the storm intensification initially. On the other hand, Tropopause Polar Vortex (TPV) associated with the thermal anomaly in lower stratosphere further intensifies the upper level jet and accordingly contributes to a drastic intensification of the storm. Stacking with the enhanced surface low, TPV intensifies further, which sustains the storm to linger over the Arctic Ocean for an extended period.

Seasonal Variations of Stratospheric Age Spectra in GEOSCCM

NASA Technical Reports Server (NTRS)

Li, Feng; Waugh, Darryn; Douglass, Anne R.; Newman, Paul A.; Pawson, Steven; Stolarski, Richard S.; Strahan, Susan E.; Nielsen, J. Eric

2011-01-01

There are many pathways for an air parcel to travel from the troposphere to the stratosphere, each of which takes different time. The distribution of all the possible transient times, i.e. the stratospheric age spectrum, contains important information on transport characteristics. However, it is computationally very expensive to compute seasonally varying age spectra, and previous studies have focused mainly on the annual mean properties of the age spectra. To date our knowledge of the seasonality of the stratospheric age spectra is very limited. In this study we investigate the seasonal variations of the stratospheric age spectra in the Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). We introduce a method to significantly reduce the computational cost for calculating seasonally dependent age spectra. Our simulations show that stratospheric age spectra in GEOSCCM have strong seasonal cycles and the seasonal cycles change with latitude and height. In the lower stratosphere extratropics, the average transit times and the most probable transit times in the winter/early spring spectra are more than twice as old as those in the summer/early fall spectra. But the seasonal cycle in the subtropical lower stratosphere is nearly out of phase with that in the extratropics. In the middle and upper stratosphere, significant seasonal variations occur in the sUbtropics. The spectral shapes also show dramatic seasonal change, especially at high latitudes. These seasonal variations reflect the seasonal evolution of the slow Brewer-Dobson circulation (with timescale of years) and the fast isentropic mixing (with timescale of days to months).

Kinetics of the BrO + NO2 Association Reaction. Temperature and Pressure Dependence in the Falloff Regime

NASA Technical Reports Server (NTRS)

Thron, R. P.; Daykin, E. P.; Wine, P.H.

1997-01-01

A laser flash photolysis-long path absorption technique has been employed to study the kinetics of the reaction BrO + NO2 + M yields (k1) products as a function of temperature (248-346 K), pressure (16-800 torr), and buffer gas identity (N2,CF4) The reaction is found to be in the falloff regime between third and second-order over the entire range of conditions investigated This is the first study where temperature-dependent measurements of k1(P,T) have been reported at pressures greater than 12 torr; hence, our results help constrain choices of k1(P,T) for use in models of lower stratospheric BrO(x) chemistry. Approximate falloff parameters in a convenient form for atmospheric modeling are derived.

Hydrogen chemistry - Perspective on experiment and theory. [atmospheric chemistry

NASA Technical Reports Server (NTRS)

Kaufman, F.

1975-01-01

A review is presented of the advantages and limitations of various experimental methods for the investigation of the kinetics of hydrogen chemistry, including classic thermal and photochemical methods and the crossed molecular beam method. Special attention is given to the flash photolysis-resonance fluorescence apparatus developed by Braun et al, in which repetitive vacuum UV flashes result in the photolytic generation of the desired species, and to the discharge-flow technique. The use of various theoretical methods for the selection or elimination of kinetic data is considered in a brief discussion of the rate theory of two-body encounters and recombination-dissociation processes in neutral reactions. Recent kinetic studies of a series of OH reactions and of a major loss process for odd H in the stratosphere are summarized.

Assessing cloud radiative effects on tropospheric photolysis rates and key oxidants during aircraft campaigns using satellite cloud observations and a global chemical transport model

NASA Astrophysics Data System (ADS)

Zhang, B.; Liu, H.; Crawford, J. H.; Chen, G.; Voulgarakis, A.; Fairlie, T. D.; Duncan, B. N.; Ham, S. H.; Kato, S.; Payer Sulprizio, M.; Yantosca, R.

2017-12-01

Clouds affect tropospheric photochemistry through modifying solar radiation that determines photolysis rates. Observational and modeling studies have indicated that photolysis rates are enhanced above and in the upper portion of cloud layers and are reduced below optically thick clouds due to their dominant backscattering effect. However, large uncertainties exist in the representation of cloud spatiotemporal (especially vertical) distributions in global models, which makes understanding of cloud radiative effects on tropospheric chemistry challenging. Our previous study using a global 3-D chemical transport model (GEOS-Chem) driven by various meteorological data sets showed that the radiative effects of clouds on photochemistry are more sensitive to the differences in the vertical distribution of clouds than to those in the magnitude of column cloud optical depths. In this work, we evaluate monthly mean cloud optical properties and distributions in the MERRA-2 reanalysis with those in C3M, a 3-D cloud data product developed at NASA Langley Research Center and merged from multiple A-Train satellite (CERES, CloudSat, CALIPSO, and MODIS) observations. We conduct tropospheric chemistry simulations for the periods of several aircraft campaigns, including ARCTAS (April, June-July, 2008), DC3 (May-June, 2012), and SEAC4RS (August-September, 2013) with GEOS-Chem driven by MERRA-2. We compare model simulations with and without constraints of cloud optical properties and distributions from C3M, and evaluate model photolysis rates (J[O1D] and J[NO2]) and key oxidants (e.g., OH and ozone) with aircraft profile measurements. We will assess whether the constraints provided by C3M improve model simulations of photolysis rates and oxidants as well as their variabilities.

Increase in the Stratospheric NO2 Content Derived from Results of Ground-Based Observations after the October 2003 Solar Proton Event

NASA Astrophysics Data System (ADS)

Ageyeva, V. Yu.; Gruzdev, A. N.; Elokhov, A. S.

2018-04-01

This paper reports on the first experimental evidence of the impact of a solar proton event on the stratospheric NO2 content derived from ground-based spectrometric measurements at middle and high latitudes of the Northern Hemisphere. In October 2003, a solar proton event caused an increase in the NO2 content in the upper stratosphere by 0.6 × 1015 cm-2, which accounted for about one-third of the increase in the column NO2 content. Solar proton events may be an essential factor for variability of the column NO2 content in the atmosphere of the high and middle latitudes.

Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) Observations of Polar Winter Conditions in 2009; Comparisons with Years 2002-2008

DTIC Science & Technology

2011-02-03

focused upon the tropospheric forcing, for example the role of blocking systems (large-scale, quasi-stationary, high-pressure systems that may steer...disruptions of the stratosphere may in turn perturb the troposphere and even affect surface weather. In early February 2009, London received heavy snowfall...global measurements from twelve SSW periods, found cooling in the equatorial lower stratosphere and upper troposphere that is associated with increased

Balloon stratospheric research flights, November 1974 to January 1976

NASA Technical Reports Server (NTRS)

Allen, N. C.

1976-01-01

These flights were designed to measure the vertical concentration profile of trace stratospheric species which form major links in the photochemical system of the upper atmosphere. An overview of the specific goals of the program, a statement of program management and support functions, a brief description of the instrumentation flown, pertinent engineering and payload operations data, and a summary of the scientific data obtained for each of the last five flights during this period are presented.

Temporal Decrease in Upper Atmospheric Chlorine

NASA Technical Reports Server (NTRS)

Froidevaux, L.; Livesey, N. J.; Read, W. G.; Salawitch, R. J.; Waters, J. W.; Drouin, B.; MacKenzie, I. A.; Pumphrey, H. C.; Bernath, P.; Boone, C.;

Vertical structure of the upper troposphere-low stratosphere in the tropics, at mid-latitude and in polar region based on recent N2O and CH4 measured by SPIRALE in situ balloon borne instrument.

NASA Astrophysics Data System (ADS)

Huret, N.; Catoire, V.; Pirre, M.; Hauchecornes, A.; Robert, C.

2006-12-01

In the framework of ENVISAT validation campaign, three flights of the SPIRALE balloon borne instrument took place in the tropics on 22 June 2005, at mid-latitude on 02 October 2002 and in the polar region on 21 January 2003. SPIRALE utilises a direct absorption technique using tunable diodes laser operating in the mid-infrared. For the three flights N2O and CH4 profiles allow us to highlight detailed vertical structures of the atmosphere from the upper troposphere to the stratosphere with small vertical extents layers of less than 1 km. In addition to the previous study of Huret et al. (JGR 2006), we present and discuss the recent tropical measurements of N2O and CH4 from the upper troposphere to the TTL and to the stratosphere. N2O-CH4 correlation points measured by SPIRALE are compared with correlation curves derived from ATMOS space shuttle measurements. The high vertical resolution (5m) and high precision of the measurements allow us to discuss in detail the origin of the air masses sampled and the occurrence of mixing processes. To help with the interpretation the potential vorticity maps calculated using the contour advection model MIMOSA have been used.

The Sources and Significance of Stratospheric Water Vapor: Mechanistic Studies from Equator to Pole

NASA Astrophysics Data System (ADS)

Smith, Jessica Birte

It is the future of the stratospheric ozone layer, which protects life at Earth's surface from harmful ultraviolet (UV) radiation, that is the focus of the present work. Fundamental changes in the composition and structure of the stratosphere in response to anthropogenic climate forcing may lead to catastrophic ozone loss under current, and even reduced, stratospheric halogen loading. In particular, the evolution toward a colder, wetter stratosphere, threatens to enhance the heterogeneous conversion of inorganic halogen from its reservoir species to its catalytically active forms, and thus promote in situ ozone loss. Water vapor concentrations control the availability of reactive surface area, which facilitates heterogeneous chemistry. Furthermore, the rates of the key heterogeneous processes are tightly controlled by the ambient humidity. Thus, credible predictions of UV dosage require a quantitative understanding of both the sensitivity of these chemical mechanisms to water vapor concentrations, and an elucidation of the processes controlling stratospheric water vapor concentrations. Toward this end, we present a set of four case studies utilizing high resolution in situ data acquired aboard NASA aircraft during upper atmospheric research missions over the past two decades. 1) We examine the broad scale humidity structure of the upper troposphere and lower stratosphere from the midlatitudes to the tropics, focusing on cirrus formation and dehydration at the cold-point tropical tropopause. The data show evidence for frequent supersaturation in clear air, and sustained supersaturation in the presence of cirrus. These results challenge the strict thermal control of the tropical tropopause. 2) We investigate the likelihood of cirrus-initiated activation of chlorine in the midlatitude lower stratosphere. At midlatitudes the transition from conditions near saturation below the local tropopause to undersaturated air above greatly reduces the probability of heterogeneous activation and in situ ozone loss in this region. 3) We probe the details of heterogeneous processing in the wintertime Arctic vortex, and find that in situ measurements of OH provide incontrovertible evidence for the heterogeneous reaction of HOCl with HCl. This reaction is critical to sustaining catalytically active chlorine and prolonging ozone loss in the springtime vortex. 4) We revisit the topic of midlatitude ozone loss with an emphasis upon the response of ozone in this region to changes in the chemical composition and thermal structure of the lower stratosphere induced by anthropogenic climate change. Specifically, we show evidence for episodic moisture plumes in the overworld stratosphere generated by the rapid evaporation of ice injected into this region by deep convection, and find that these high water vapor plumes have the potential to alter the humidity of the lower stratosphere, and drastically increase the rate of heterogeneous chemistry and in situ ozone loss, given sufficient reactive surface.

A 4 U laser heterodyne radiometer for methane (CH4) and carbon dioxide (CO2) measurements from an occultation-viewing CubeSat

NASA Astrophysics Data System (ADS)

Wilson, Emily L.; DiGregorio, A. J.; Riot, Vincent J.; Ammons, Mark S.; Bruner, William W.; Carter, Darrell; Mao, Jianping; Ramanathan, Anand; Strahan, Susan E.; Oman, Luke D.; Hoffman, Christine; Garner, Richard M.

2017-03-01

We present a design for a 4 U (20 cm  ×  20 cm  ×  10 cm) occultation-viewing laser heterodyne radiometer (LHR) that measures methane (CH4), carbon dioxide (CO2) and water vapor (H2O) in the limb that is designed for deployment on a 6 U CubeSat. The LHR design collects sunlight that has undergone absorption by the trace gas and mixes it with a distributive feedback (DFB) laser centered at 1640 nm that scans across CO2, CH4, and H2O absorption features. Upper troposphere/lower stratosphere measurements of these gases provide key inputs to stratospheric circulation models: measuring stratospheric circulation and its variability is essential for projecting how climate change will affect stratospheric ozone.

Comparison of NOAA/NMC stratospheric wind analyses with UARS high resolution Doppler Imager wind measurements

NASA Technical Reports Server (NTRS)

Miller, A. J.; Hays, P. B.; Abreu, V.; Long, C.; Kann, D.

1994-01-01

The NOAA National Weather Service currently derives global stratospheric wind analyses via several procedures. The first is the operational data assimilation system that extends from the surface up to about 50 mb and is in process of being tested to about 10 mb. In addition, a balanced wind is determined from the available Climate Analysis Center stratospheric height analyses that encompass the 70-0.4 mb region. The High Resolution Doppler Imager (HRDI) recently launched as a member of the Upper Atmosphere Research Satellite (UARS) is the first satellite instrument designed to measure winds in this stratospheric region and, thus, provide a basic evaluation of the NMC derived products. The HRDI accomplishes this by utilizing a triple-etalon Fabry-Perot interferometer that allows one to measure the Doppler shift of O2 absorption and emission features of the atmosphere, from which the wind field can be determined.

Microphysical processes affecting stratospheric aerosol particles

NASA Technical Reports Server (NTRS)

Hamill, P.; Toon, O. B.; Kiang, C. S.

1977-01-01

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

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

NASA Technical Reports Server (NTRS)

Boering, Kristie A.; Connell, Peter; Rotman, Douglas

2005-01-01

Until recently, the stable isotopic composition of chemically and datively important stratospheric species, such as ozone (O3), carbon dioxide (CO2), nitrous oxide (N2O), and methane (CH4), was largely unexplored, despite indications from the few measurements available and theoretical studies that global-scale isotopic variations will provide a unique tool for quantifying rates of global-scale mass transport into, within, and out of the stratosphere and for understanding the mechanisms of chemical reactions involved in ozone production. The number and geographical extent of observations are beginning to increase rapidly, however, as access to the stratosphere, both directly and by remote-sensing, has increased over the last 10 years and as new analytical techniques have been developed that make global-scale isotope measurements by whole-air sampling more feasible. The objective of this study, begun in April 1999, is to incorporate into the Livermore 2D model the likely photochemical fractionation processes that determine the isotopic compositions of stratospheric CO2, N2O, CH4, and O3, and to use the model results and new observations from NASA field campaigns in 1996 and 1997 to investigate stratospheric chemistry and mass transport. Additionally, since isotopic signatures from the stratosphere are transferred to the troposphere by downward transport at middle and high latitudes, the isotopic compositions may also serve as sensitive tracers of stratosphere-totroposphere transport. Comparisons of model results with stratospheric and upper tropospheric observations from these campaigns, as well as with ground-based observations from new NOAA and NSF-sponsored studies, will help determine whether the magnitudes of the stratospheric fractionation processes are large enough to use as global-scale tracers of transport into the troposphere and, if so, will be used to help constrain the degree of coupling between the troposphere and the stratosphere.

The global warming potential of methane reassessed with combined stratosphere and troposphere chemistry

NASA Astrophysics Data System (ADS)

Holmes, C. D.; Archibald, A. T.; Eastham, S. D.; Søvde, O. A.

2017-12-01

Methane is a direct and indirect greenhouse gas. The direct greenhouse effect comes from the radiation absorbed and emitted by methane itself. The indirect greenhouse effect comes from radiatively active gases that are produced during methane oxidation: principally O3, H2O, and CO2. Methane also suppresses tropospheric OH, which indirectly affects numerous greenhouses gases and aerosols. Traditionally, the methane global warming potential (GWP) has included the indirect effects on tropospheric O3 and OH and stratospheric H2O, with these effects estimated independently from unrelated tropospheric and stratospheric chemistry models and observations. Using this approach the CH4 is about 28 over 100 yr (without carbon cycle feedbacks, IPCC, 2013). Here we present a comprehensive analysis of the CH4 GWP in several 3-D global atmospheric models capable of simulating both tropospheric and stratospheric chemistry (GEOS-Chem, Oslo CTM3, UKCA). This enables us to include, for the first time, the indirect effects of CH4 on stratospheric O3 and stratosphere-troposphere coupling. We diagnose the GWP from paired simulations with and without a 5% perturbation to tropospheric CH4 concentrations. Including stratospheric chemistry nearly doubles the O3 contribution to CH4 GWP because of O3 production in the lower stratosphere and because CH4 inhibits Cl-catalyzed O3 loss in the upper stratosphere. In addition, stratosphere-troposphere coupling strengthens the chemical feedback on its own lifetime. In the stratosphere, this feedback operates by a CH4 perturbation thickening the stratospheric O3 layer, which impedes UV-driven OH production in the troposphere and prolongs the CH4 lifetime. We also quantify the impact of CH4-derived H2O on the stratospheric HOx cycles but these effects are small. Combining all of the above, these models suggest that the 100-yr GWP of CH4 is over 33.5, a 20% increase over the latest IPCC assessment.

High-resolution optical measurements of atmospheric winds from space. I - Lower atmosphere molecular absorption

NASA Technical Reports Server (NTRS)

Hays, P. B.

1982-01-01

A high-resolution spectroscopic technique, analogous to that used in the thermosphere to measure the vector wind fields in the upper troposphere and stratosphere, is described which uses narrow features in the spectrum of light scattered from the earth's lower atmosphere to provide Doppler information on atmospheric scattering and absorption. It is demonstrated that vector winds can be measured from a satellite throughout the lower atmosphere, using a multiple-etalon Fabry-Perot interferometer of modest aperture. It is found that molecular oxygen and water vapor absorption lines in the spectrum of sunlight scattered by the atmosphere are Doppler-shifted by the line of sight wind, so that they may be used to monitor the global wind systems in the upper troposphere and stratosphere.

ISAMS and MLS for NASA's Upper Atmosphere Research Satellite

NASA Astrophysics Data System (ADS)

Llewellyn-Jones, D.; Dickinson, P. H. G.

1990-04-01

The primary goal of NASA's Upper Atmosphere Research Satellite (UARS), planned to be launched in 1991, is to compile data about the structure and behavior of the stratospheric ozone layer, and especially about the threat of the chlorine-based pollutants to its stablility. Two of the payload instruments, manufactured in the UK, are described: the Improved Stratospheric and Mesospheric Sounder (ISAMS), a radiometer designed to measure thermal emission from selected atmospheric constituents at the earth's limb, then making it possible to obtain nearly global coverage of the vertical distribution of temperature and composition from 80 deg S to 80 deg N latitude; and the Microwave Limb Sounder (MLS), a limb sounding radiometer, measuring atmospheric thermal emission from selected molecular spectral lines at mm wavelength, in the frequency regions of 63, 183, and 205 GHz.

An analysis of Solar Mesospheric Explorer temperatures for the upper stratosphere and mesosphere

NASA Technical Reports Server (NTRS)

Clancy, R. Todd; Rusch, David W.

1993-01-01

We proposed to analyze Solar Mesosphere Explorer (SME) limb profiles of Rayleigh scattered solar flux at wavelengths of 304, 313, and 443 nm to retrieve atmospheric temperature profiles over the 40-65 km altitude region. These temperatures can be combined with the previous analysis of SME 296 nm limb radiances to construct a monthly average climatology of atmospheric temperatures over the 40-90 km, upper stratosphere-mesosphere region, with approximately 4 km vertical resolution. We proposed to investigate the detailed nature of the global temperature structure of this poorly measured region, based on these 1982-1986 SME temperatures. The average vertical structure of temperatures between the stratopause and mesopause has never been determined globally with vertical resolution sufficient to retrieve even scale-height structures. Hence, the SME temperatures provided a unique opportunity to study the detailed thermal structure of the mesosphere, in advance of Upper Atmosphere Research Satellite (UARS) measurements and the Thermosphere Ionosphere Mesosphere Energy and Dynamics (TIMED) mission.

Vertical Propagation and Temporal Growth of Perturbations in the Winter Atmosphere

NASA Astrophysics Data System (ADS)

Christiansen, B.

2001-12-01

We present a general circulation model study of the temporal growth and vertically propagation of perturbations following vertical confined forcings. Both transient and sustained forcings are considered. The motivation for the study is the recent recognition of downward propagation of anomalies from the stratosphere to the troposphere and its implications both for medium range forecasts and for a possible physical mechanism for stratospheric impacts on weather and climate. The dynamical link might also offer a mechanism for changes in the upper atmosphere to affect the tropospheric climate. Here we are thinking of changes in trace gases such as ozone, but also of modulations of the upper atmospheric structure related to the 11-year solar cycle. The model atmosphere is chaotic and shows growth of perturbations no matter which level is forced. The perturbations grow to a size comparable to the variability of the unperturbed atmosphere on a time-scale of 20 - 25 days in the troposphere and 30 - 40 days in the stratosphere. After the initial period of growth the perturbations have the same structure as the unperturbed atmosphere. Although the forcing is restricted to the northern hemisphere the perturbations encompass the whole atmosphere and develop on the same time scale on both hemispheres. Perturbations grow with time squared both when zonal mean and single cell values are considered. Such a power law growth suggest the existence of a finite predictability time which is independent of the initial perturbation as long as it is small. In the unperturbed atmosphere the stratospheric variability has the form of downward propagating stratospheric vacillations. However, in the initial period of growth the perturbations do not propagate downward and seem in general uncoupled to the background vacillations. This suggests that the downward propagation is a robust feature determined more by the processes in the troposphere than the state of the stratosphere. We note that downward propagation may still be a source for enhanced predictability of near-surface weather.

Sulfate geoengineering impact on methane transport and lifetime: results from the Geoengineering Model Intercomparison Project (GeoMIP)

NASA Astrophysics Data System (ADS)

Visioni, Daniele; Pitari, Giovanni; Aquila, Valentina; Tilmes, Simone; Cionni, Irene; Di Genova, Glauco; Mancini, Eva

2017-09-01

Sulfate geoengineering (SG), made by sustained injection of SO2 in the tropical lower stratosphere, may impact the CH4 abundance through several photochemical mechanisms affecting tropospheric OH and hence the methane lifetime. (a) The reflection of incoming solar radiation increases the planetary albedo and cools the surface, with a tropospheric H2O decrease. (b) The tropospheric UV budget is upset by the additional aerosol scattering and stratospheric ozone changes: the net effect is meridionally not uniform, with a net decrease in the tropics, thus producing less tropospheric O(1D). (c) The extratropical downwelling motion from the lower stratosphere tends to increase the sulfate aerosol surface area density available for heterogeneous chemical reactions in the mid-to-upper troposphere, thus reducing the amount of NOx and O3 production. (d) The tropical lower stratosphere is warmed by solar and planetary radiation absorption by the aerosols. The heating rate perturbation is highly latitude dependent, producing a stronger meridional component of the Brewer-Dobson circulation. The net effect on tropospheric OH due to the enhanced stratosphere-troposphere exchange may be positive or negative depending on the net result of different superimposed species perturbations (CH4, NOy, O3, SO4) in the extratropical upper troposphere and lower stratosphere (UTLS). In addition, the atmospheric stabilization resulting from the tropospheric cooling and lower stratospheric warming favors an additional decrease of the UTLS extratropical CH4 by lowering the horizontal eddy mixing. Two climate-chemistry coupled models are used to explore the above radiative, chemical and dynamical mechanisms affecting CH4 transport and lifetime (ULAQ-CCM and GEOSCCM). The CH4 lifetime may become significantly longer (by approximately 16 %) with a sustained injection of 8 Tg-SO2 yr-1 starting in the year 2020, which implies an increase of tropospheric CH4 (200 ppbv) and a positive indirect radiative forcing of sulfate geoengineering due to CH4 changes (+0.10 W m-2 in the 2040-2049 decade and +0.15 W m-2 in the 2060-2069 decade).

Evaluation of Near-Tropopause Ozone Distributions in the Global Modeling Initiative Combined Stratosphere/Troposphere Model with Ozonesonde Data

NASA Technical Reports Server (NTRS)

Considine, David B.; Logan, Jennifer A.; Olsen, Mark A.

2008-01-01

The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. Model ozone is high biased at the SH tropical and NH midlatitude tropopause by approx. 45% in a 4 deg. latitude x 5 deg. longitude model simulation. Increasing the resolution to 2 deg. x 2.5 deg. increases the NH tropopause high bias to approx. 60%, but decreases the tropical tropopause bias to approx. 30%, an effect of a better-resolved residual circulation. The tropopause ozone biases appear not to be due to an overly vigorous residual circulation or excessive stratosphere/troposphere exchange, but are more likely due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. NH and tropical mean model lower stratospheric biases are less than 20%. In the upper troposphere, the 2 deg. x 2.5 deg. simulation exhibits mean high biases of approx. 20% and approx. 35% during April in the tropics and NH midlatitudes, respectively, compared to the pressure averaged climatology. However, relative-to-tropopause averaging produces upper troposphere high biases of approx. 30% and 70% in the tropics and NH midlatitudes. This is because relative-to-tropopause averaging better preserves large cross-tropopause O3 gradients, which are seen in the daily sonde data, but not in daily model profiles. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is approx. 30% weaker than in the real atmosphere.

Ozone and aerosol distributions measured by airborne lidar during the 1988 Arctic Boundary Layer Experiment

NASA Technical Reports Server (NTRS)

Browell, Edward V.; Butler, Carolyn F.; Kooi, Susan A.

1991-01-01

Consideration is given to O3 and aerosol distributions measured from an aircraft using a DIAL system in order to study the sources and sinks of gases and aerosols over the tundra regions of Alaska during summer 1988. The tropospheric O3 budget over the Arctic was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were usually correlated with descending air from the upper troposphere or lower stratosphere.

Aerosol elemental concentrations in the tropopause region from intercontinental flights with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform

NASA Astrophysics Data System (ADS)

Papaspiropoulos, Giorgos; Martinsson, Bengt G.; Zahn, Andreas; Brenninkmeijer, Carl A. M.; Hermann, Markus; Heintzenberg, Jost; Fischer, Herbert; van Velthoven, Peter F. J.

2002-12-01

This study with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform investigates the aerosol elemental concentrations at 9-11 km altitude in the northern hemisphere. Measurements from 31 intercontinental flights over a 2-year period between Germany and Sri Lanka/Maldives in the Indian Ocean are presented. Aerosol samples were collected with an impaction technique and were analyzed for the concentration of 18 elements using particle-induced X-ray emission (PIXE). Additional measurements of particle number concentrations, ozone and carbon monoxide concentrations, and meteorological modeling were included in the interpretation of the aerosol elemental concentrations. Particulate sulphur was found to be by far the most abundant element. Its upper tropospheric concentration increased, on average, by a factor of 2 from the tropics to midlatitudes, with another factor 2 higher concentrations in the lowermost stratosphere over midlatitudes. Correlation patterns and source profiles suggest contributions from crustal sources and biomass burning, but not from meteor ablation. Coinciding latitudinal gradients in particulate sulphur concentrations and emissions suggest that fossil fuel combustion is an important source of the aerosol in the upper troposphere and lowermost stratosphere. The measurements indicate aerosol transport along isentropic surfaces across the tropopause into the lowermost stratosphere. As a result of the prolonged residence time, ageing via oxidation of sulphur dioxide in the lowermost stratosphere was found to be a likely high-altitude, strong source that, along with downward transport of stratospheric air, could explain the vertical gradient of particulate sulphur mass concentration around the extratropical tropopause.

Stratospheric aerosols from the Sarychev volcano eruption in the 2009 Arctic summer

NASA Astrophysics Data System (ADS)

Jégou, F.; Berthet, G.; Brogniez, C.; Renard, J.-B.; François, P.; Haywood, J. M.; Jones, A.; Bourgeois, Q.; Lurton, T.; Auriol, F.; Godin-Beekmann, S.; Guimbaud, C.; Krysztofiak, G.; Gaubicher, B.; Chartier, M.; Clarisse, L.; Clerbaux, C.; Balois, J. Y.; Verwaerde, C.; Daugeron, D.

2013-07-01

Aerosols from the Sarychev volcano eruption (Kuril Islands, northeast of Japan) were observed in the Arctic lower stratosphere a few days after the strongest SO2 injection which occurred on 15 and 16 June 2009. From the observations provided by the Infrared Atmospheric Sounding Interferometer (IASI) an estimated 0.9 Tg of sulphur dioxide was injected into the upper troposphere and lower stratosphere (UTLS). The resultant stratospheric sulphate aerosols were detected from satellites by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and from the surface by the Network for the Detection of Atmospheric Composition Changes (NDACC) lidar deployed at OHP (Observatoire de Haute-Provence, France). By the first week of July the aerosol plume had spread out over the entire Arctic region. The Sarychev-induced stratospheric aerosol over the Kiruna region (north of Sweden) was measured by the Stratospheric and Tropospheric Aerosol Counter (STAC) during eight balloon flights planned in August and September 2009. During this balloon campaign the Micro Radiomètre Ballon (MicroRADIBAL) and the Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) remote-sensing instruments also observed these aerosols. Aerosol concentrations returned to near-background levels by spring 2010. The effective radius, the surface area density (SAD), the aerosol extinction, and the total sulphur mass from STAC in situ measurements are enhanced with mean values in the range 0.15-0.21 μm, 5.5-14.7 μm2 cm-3, 5.5-29.5 × 10-4 km-1, and 4.9-12.6 × 10-10 kg[S] kg-1[air], respectively, between 14 km and 18 km. The observed and modelled e-folding time of sulphate aerosols from the Sarychev eruption is around 70-80 days, a value much shorter than the 12-14 months calculated for aerosols from the 1991 eruption of Mt Pinatubo. The OSIRIS stratospheric aerosol optical depth (AOD) at 750 nm is enhanced by a factor of 6, with a value of 0.02 in late July compared to 0.0035 before the eruption. The HadGEM2 and MIMOSA model outputs indicate that aerosol layers in polar region up to 14-15 km are largely modulated by stratosphere-troposphere exchange processes. The spatial extent of the Sarychev plume is well represented in the HadGEM2 model with lower altitudes of the plume being controlled by upper tropospheric troughs which displace the plume downward and upper altitudes around 18-20 km, in agreement with lidar observations. Good consistency is found between the HadGEM2 sulphur mass density and the value inferred from the STAC observations, with a maximum located about 1 km above the tropopause ranging from 1 to 2 × 10-9 kg[S] kg-1[air], which is one order of magnitude higher than the background level.

Reanalysis comparisons of upper tropospheric-lower stratospheric jets and multiple tropopauses

NASA Astrophysics Data System (ADS)

Manney, Gloria L.; Hegglin, Michaela I.; Lawrence, Zachary D.; Wargan, Krzysztof; Millán, Luis F.; Schwartz, Michael J.; Santee, Michelle L.; Lambert, Alyn; Pawson, Steven; Knosp, Brian W.; Fuller, Ryan A.; Daffer, William H.

2017-09-01

The representation of upper tropospheric-lower stratospheric (UTLS) jet and tropopause characteristics is compared in five modern high-resolution reanalyses for 1980 through 2014. Climatologies of upper tropospheric jet, subvortex jet (the lowermost part of the stratospheric vortex), and multiple tropopause frequency distributions in MERRA (Modern-Era Retrospective analysis for Research and Applications), ERA-I (ERA-Interim; the European Centre for Medium-Range Weather Forecasts, ECMWF, interim reanalysis), JRA-55 (the Japanese 55-year Reanalysis), and CFSR (the Climate Forecast System Reanalysis) are compared with those in MERRA-2. Differences between alternate products from individual reanalysis systems are assessed; in particular, a comparison of CFSR data on model and pressure levels highlights the importance of vertical grid spacing. Most of the differences in distributions of UTLS jets and multiple tropopauses are consistent with the differences in assimilation model grids and resolution - for example, ERA-I (with coarsest native horizontal resolution) typically shows a significant low bias in upper tropospheric jets with respect to MERRA-2, and JRA-55 (the Japanese 55-year Reanalysis) a more modest one, while CFSR (with finest native horizontal resolution) shows a high bias with respect to MERRA-2 in both upper tropospheric jets and multiple tropopauses. Vertical temperature structure and grid spacing are especially important for multiple tropopause characterizations. Substantial differences between MERRA and MERRA-2 are seen in mid- to high-latitude Southern Hemisphere (SH) winter upper tropospheric jets and multiple tropopauses as well as in the upper tropospheric jets associated with tropical circulations during the solstice seasons; some of the largest differences from the other reanalyses are seen in the same times and places. Very good qualitative agreement among the reanalyses is seen between the large-scale climatological features in UTLS jet and multiple tropopause distributions. Quantitative differences may, however, have important consequences for transport and variability studies. Our results highlight the importance of considering reanalyses differences in UTLS studies, especially in relation to resolution and model grids; this is particularly critical when using high-resolution reanalyses as an observational reference for evaluating global chemistry-climate models.

Is there any chlorine monoxide in the stratosphere?

NASA Technical Reports Server (NTRS)

Rogers, J. D.; Mumma, M. J.; Kostiuk, T.; Deming, D.; Hillman, J. J.; Faris, J.; Zipoy, D.

1982-01-01

A ground based search for the 856.50137/cm R(9.5) and for the 859.76765 R(12.5) transitions of stratospheric (Cl-35)O was made in the solar absorption mode using an infrared heterodyne spectrometer. Lines due to stratospheric HNO3 and tropospheric OCS were detected, at about 0.3% absorption levels. The expected lines of ClO in this same region were not detected, even though the optical depth of the ClO lines should be on the order of 0.2% using currently accepted ClO abundances. These infrared measurements suggest that stratospheric ClO is at least a factor of 7 less abundant than is indicated by indirect in situ fluorescence measurements, and the upper limit of 2.4x10 to the 13th power molecules/sq cm to the integrated column density of ClO is a factor of over 4 less than is indicted by microwave measurements. Results imply that the release of fluorocarbon precursors of ClO may be significantly less important for the destruction of stratospheric ozone than was previously thought.

Estimate of the effect of the 11-year solar activity cycle on the ozone content in the stratosphere

NASA Astrophysics Data System (ADS)

Gruzdev, A. N.

2014-09-01

Using spectral, cross-spectral, and regression methods, we analyzed the effect of the 11-year cycle of solar activity on the ozone content in the stratosphere and lower mesosphere via satellite measurement data obtained with the help of SBUV/SBUV2 instruments in 1978-2003. We revealed a high coherence between the ozone content and solar activity level on the solar cycle scale. In much of this area, the ozone content varies approximately in phase with the solar cycle; however, in areas of significant gradients of ozone mixing ratio in the middle stratosphere, the phase shift between ozone and solar oscillations can be considerable, up to π/2. This can be caused by dynamical processes. The altitude maxima of ozone sensitivity to the 11-year solar cycle were found in the upper vicinity of the stratopause (50-55 km), in the middle stratosphere (35-40 km), and the lower stratosphere (below 25 km). Maximal changes in ozone content in the solar cycle (up to 10% and more) were found in winter and spring in polar regions.

An ultrahot gas-giant exoplanet with a stratosphere.

PubMed

Evans, Thomas M; Sing, David K; Kataria, Tiffany; Goyal, Jayesh; Nikolov, Nikolay; Wakeford, Hannah R; Deming, Drake; Marley, Mark S; Amundsen, David S; Ballester, Gilda E; Barstow, Joanna K; Ben-Jaffel, Lotfi; Bourrier, Vincent; Buchhave, Lars A; Cohen, Ofer; Ehrenreich, David; García Muñoz, Antonio; Henry, Gregory W; Knutson, Heather; Lavvas, Panayotis; Etangs, Alain Lecavelier des; Lewis, Nikole K; López-Morales, Mercedes; Mandell, Avi M; Sanz-Forcada, Jorge; Tremblin, Pascal; Lupu, Roxana

2017-08-02

Infrared radiation emitted from a planet contains information about the chemical composition and vertical temperature profile of its atmosphere. If upper layers are cooler than lower layers, molecular gases will produce absorption features in the planetary thermal spectrum. Conversely, if there is a stratosphere-where temperature increases with altitude-these molecular features will be observed in emission. It has been suggested that stratospheres could form in highly irradiated exoplanets, but the extent to which this occurs is unresolved both theoretically and observationally. A previous claim for the presence of a stratosphere remains open to question, owing to the challenges posed by the highly variable host star and the low spectral resolution of the measurements. Here we report a near-infrared thermal spectrum for the ultrahot gas giant WASP-121b, which has an equilibrium temperature of approximately 2,500 kelvin. Water is resolved in emission, providing a detection of an exoplanet stratosphere at 5σ confidence. These observations imply that a substantial fraction of incident stellar radiation is retained at high altitudes in the atmosphere, possibly by absorbing chemical species such as gaseous vanadium oxide and titanium oxide.

Massive global ozone loss predicted following regional nuclear conflict

PubMed Central

Mills, Michael J.; Toon, Owen B.; Turco, Richard P.; Kinnison, Douglas E.; Garcia, Rolando R.

2008-01-01

We use a chemistry-climate model and new estimates of smoke produced by fires in contemporary cities to calculate the impact on stratospheric ozone of a regional nuclear war between developing nuclear states involving 100 Hiroshima-size bombs exploded in cities in the northern subtropics. We find column ozone losses in excess of 20% globally, 25–45% at midlatitudes, and 50–70% at northern high latitudes persisting for 5 years, with substantial losses continuing for 5 additional years. Column ozone amounts remain near or <220 Dobson units at all latitudes even after three years, constituting an extratropical “ozone hole.” The resulting increases in UV radiation could impact the biota significantly, including serious consequences for human health. The primary cause for the dramatic and persistent ozone depletion is heating of the stratosphere by smoke, which strongly absorbs solar radiation. The smoke-laden air rises to the upper stratosphere, where removal mechanisms are slow, so that much of the stratosphere is ultimately heated by the localized smoke injections. Higher stratospheric temperatures accelerate catalytic reaction cycles, particularly those of odd-nitrogen, which destroy ozone. In addition, the strong convection created by rising smoke plumes alters the stratospheric circulation, redistributing ozone and the sources of ozone-depleting gases, including N2O and chlorofluorocarbons. The ozone losses predicted here are significantly greater than previous “nuclear winter/UV spring” calculations, which did not adequately represent stratospheric plume rise. Our results point to previously unrecognized mechanisms for stratospheric ozone depletion. PMID:18391218

Solar Effects on Climate and the Maunder Minimum: Minimum Certainty

NASA Technical Reports Server (NTRS)

Rind, David

2003-01-01

The current state of our understanding of solar effects on climate is reviewed. As an example of the relevant issues, the climate during the Maunder Minimum is compared with current conditions in GCM simulations that include a full stratosphere and parameterized ozone response to solar spectral irradiance variability and trace gas changes. The GISS Global Climate/Middle Atmosphere Model coupled to a q-flux/mixed layer model is used for the simulations, which begin in 1500 and extend to the present. Experiments were made to investigate the effect of total versus spectrally-varying solar irradiance changes; spectrally-varying solar irradiance changes on the stratospheric ozone/climate response with both pre-industrial and present trace gases; and the impact on climate and stratospheric ozone of the preindustrial trace gases and aerosols by themselves. The results showed that: (1) the Maunder Minimum cooling relative to today was primarily associated with reduced anthropogenic radiative forcing, although the solar reduction added 40% to the overall cooling. There is no obvious distinguishing surface climate pattern between the two forcings. (2)The global and tropical response was greater than 1 C, in a model with a sensitivity of 1.2 C per W m-2. To reproduce recent low-end estimates would require a sensitivity 1/4 as large. (3) The global surface temperature change was similar when using the total and spectral irradiance prescriptions, although the tropical response was somewhat greater with the former, and the stratospheric response greater with the latter. (4) Most experiments produce a relative negative phase of the NAO/AO during the Maunder Minimum, with both solar and anthropogenic forcing equally capable, associated with the tropical cooling and relative poleward EP flux refraction. (5) A full stratosphere appeared to be necessary for the negative AO/NAO phase, as was the case with this model for global warming experiments, unless the cooling was very large, while the ozone response played a minor role and did not influence surface temperature significantly. (6) Stratospheric ozone was most affected by the difference between present day and preindustrial atmospheric composition and chemistry, with increases in the upper and lower stratosphere during the Maunder Minimum. While the estimated UV reduction led to ozone decreases, this was generally less important than the anthropogenic effect except in the upper middle stratosphere, as judged by two different ozone photochemistry schemes. (7) The effect of the reduced solar irradiance on stratospheric ozone and on climate was similar in Maunder Minimum and current atmospheric conditions.

Influence of Transport on Two-Dimensional Model Simulation. Tracer Sensitivity to 2-D Model Transport. 1; Long Lived Tracers

NASA Technical Reports Server (NTRS)

Fleming, Eric L.; Jackman, Charles H.; Considine, David B.; Stolarski, Richard S.

1999-01-01

In this study, we examine the sensitivity of long lived tracers to changes in the base transport components in our 2-D model. Changes to the strength of the residual circulation in the upper troposphere and stratosphere and changes to the lower stratospheric K(sub zz) had similar effects in that increasing the transport rates decreased the overall stratospheric mean age, and increased the rate of removal of material from the stratosphere. Increasing the stratospheric K(sub yy) increased the mean age due to the greater recycling of air parcels through the middle atmosphere, via the residual circulation, before returning to the troposphere. However, increasing K(sub yy) along with self-consistent increases in the corresponding planetary wave drive, which leads to a stronger residual circulation, more than compensates for the K(sub yy)-effect, and produces significantly younger ages throughout the stratosphere. Simulations with very small tropical stratospheric K(sub yy) decreased the globally averaged age of air by as much as 25% in the middle and upper stratosphere, and resulted in substantially weaker vertical age gradients above 20 km in the extratropics. We found only very small stratospheric tracer sensitivity to the magnitude of the horizontal mixing across the tropopause, and to the strength of the mesospheric gravity wave drag and diffusion used in the model. We also investigated the transport influence on chemically active tracers and found a strong age-tracer correlation, both in concentration and calculated lifetimes. The base model transport gives the most favorable overall comparison with a variety of inert tracer observations, and provides a significant improvement over our previous 1995 model transport. Moderate changes to the base transport were found to provide modest agreement with some of the measurements. Transport scenarios with residence times ranging from moderately shorter to slightly longer relative to the base case simulated N2O lifetimes that were within the observational estimates of Volk et al. [1997]. However, only scenarios with rather fast transport rates were comparable with the Volk et al. estimates of CFCl3 lifetimes. This is inconsistent with model-measurement comparisons of mean age in which the base model or slightly slower transport rates compared the most favorably with balloon SF6 data. For all comparisons shown, large transport changes away from the base case resulted in simulations that were outside the range of measurements, and in many cases, far outside this range.

Transient-Absorption Spectroscopy of Cis-Trans Isomerization of N,N-dimethyl-4,4'-Azodianiline with 3D-Printed Temperature-Controlled Sample Holder

ERIC Educational Resources Information Center

Kosenkov, Dmytro; Shaw, James; Zuczek, Jennifer; Kholod, Yana

2016-01-01

The laboratory unit demonstrates a project based approach to teaching physical chemistry laboratory where upper-division undergraduates carry out a transient-absorption experiment investigating the kinetics of cis-trans isomerization of N,N-dimethyl-4,4'-azodianiline. Students participate in modification of a standard flash-photolysis spectrometer…

Observations of low-frequency inertia-gravity waves in the lower stratosphere over Arecibo

NASA Technical Reports Server (NTRS)

Cornish, C. R.; Larsen, M. F.

1989-01-01

Results are presented of a detailed analysis of the horizontal wind data in the subtropical upper troposphere and lower stratosphere, obtained with the 430-MHz radar at Arecibo (Puerto Rico) in May 1982 and April 1983. Both sets of observations displayed a slowly varying anticyclonically rotating persistent structure in the wind field just above the tropopause, of the type that would be expected if the oscillations were associated with quasi-inertial period waves. The quasi-inertial period structure in the Arecibo observations appears to be typical of the results of a number of other studies, indicating that quasi-inertial period waves are a ubiquitous feature in the lower stratosphere, similar to what is observed in the oceans.

Investigation of N2O Production from 266 and 532 nm Laser Flash Photolysis of O3/N2/O2 Mixtures

NASA Technical Reports Server (NTRS)

Estupinan, E. G.; Nicovich, J. M.; Li, J.; Cunnold, D. M.; Wine, P. H.

2002-01-01

Tunable diode laser absorption spectroscopy has been employed to measure the amount of N2O produced from laser flash photolysis of O3/N2/O2 mixtures at 266 and 532 nm. In the 532 nm photolysis experiments very little N2O is observed, thus allowing an upper limit yield of 7 x 10(exp -8) to be established for the process O3 + N2 yield N2O + O2, where O3 is nascent O3 that is newly formed via O(3P(sub J)) + O2 recombination (with vibrational excitation near the dissociation energy of O3). The measured upper limit yield is a factor of approx. 600 smaller than a previous literature value and is approximately a factor of 10 below the threshold for atmospheric importance. In the 266 nm photolysis experiments, significant N2O production is observed and the N2O quantum yield is found to increase linearly with pressure over the range 100 - 900 Torr in air bath gas. The source of N2O in the 266 nm photolysis experiments is believed to be the addition reaction O(1D(sub 2)) + N2 + M yields (k(sub sigma)) N2O + M, although reaction of (very short-lived) electronically excited O3 with N2 cannot be ruled out by the available data. Assuming that all observed N2O comes from the O(1D(sub 2)) + N2 + M reaction, the following expression describes the temperature dependence of k(sub sigma) (in its third-order low-pressure limit) that is consistent with the N2O yield data: k(sub sigma) = (2.8 +/- 0.1) x 10(exp -36)(T/300)(sup -(0-88+0.36)) cm(sup 6) molecule(sup -2)/s, where the uncertainties are 2(sigma) and represent precision only. The accuracy of the reported rate coefficients at the 95% confidence level is estimated to be 30 - 40% depending on the temperature. Model calculations suggest that gas phase processes initiated by ozone absorption of a UV photon represent about 1.4% of the currently estimated global source strength of atmospheric N2O. However, these processes could account for a significant fraction of the oxygen mass-independent enrichment observed in atmospheric N2O, and they appear to be the first suggested photochemical mechanism that is capable of explaining the altitude dependence of the observed mass -independent isotopic signature.

Upper Atmosphere Research Satellite (UARS): A program to study global ozone change

NASA Technical Reports Server (NTRS)

1991-01-01

A general overview of NASA's Upper Atmosphere Research Satellite (UARS) program is presented in a broad based informational publication. The UARS will be responsible for carrying out the first systematic, comprehensive study of the stratosphere and will furnish important new data on the mesosphere and thermosphere. The UARS mission objectives are to provide an increased understanding of energy input into the upper atmosphere; global photochemistry of the upper atmosphere; dynamics of the upper atmosphere; coupling among these processes; and coupling between the upper and lower atmosphere. These mission objectives are briefly described along with the UARS on-board instrumentation and related data management systems.

The strength of the meridional overturning circulation of the stratosphere

PubMed Central

Linz, Marianna; Plumb, R. Alan; Gerber, Edwin P.; Haenel, Florian J.; Stiller, Gabriele; Kinnison, Douglas E.; Ming, Alison; Neu, Jessica L.

2017-01-01

The distribution of gases such as ozone and water vapour in the stratosphere — which affect surface climate — is influenced by the meridional overturning of mass in the stratosphere, the Brewer–Dobson circulation. However, observation-based estimates of its global strength are difficult to obtain. Here we present two calculations of the mean strength of the meridional overturning of the stratosphere. We analyze satellite data that document the global diabatic circulation between 2007– 2011, and compare these to three re-analysis data sets and to simulations with a state-of-the-art chemistry-climate model. Using measurements of sulfur hexafluoride (SF6) and nitrous oxide, we calculate the global mean diabatic overturning mass flux throughout the stratosphere. In the lower stratosphere, these two estimates agree, and at a potential temperature level of 460 K (about 20 km or 60 hPa in tropics), the global circulation strength is 6.3–7.6 × 109 kg/s. Higher in the atmosphere, only the SF6-based estimate is available, and it diverges from the re-analysis data and simulations. Interpretation of the SF6 data-based estimate is limited because of a mesospheric sink of SF6; however, the reanalyses also differ substantially from each other. We conclude that the uncertainty in the mean meridional overturning circulation strength at upper levels of the stratosphere amounts to at least 100 %. PMID:28966661

AO/NAO Response to Climate Change. 1; Respective Influences of Stratospheric and Tropospheric Climate Changes

NASA Technical Reports Server (NTRS)

Rind, D.; Perlwitz, J.; Lonergan, P.

2005-01-01

We utilize the GISS Global Climate Middle Atmosphere Model and 8 different climate change experiments, many of them focused on stratospheric climate forcings, to assess the relative influence of tropospheric and stratospheric climate change on the extratropical circulation indices (Arctic Oscillation, AO; North Atlantic Oscillation, NAO). The experiments are run in two different ways: with variable sea surface temperatures (SSTs) to allow for a full tropospheric climate response, and with specified SSTs to minimize the tropospheric change. The results show that tropospheric warming (cooling) experiments and stratospheric cooling (warming) experiments produce more positive (negative) AO/NAO indices. For the typical magnitudes of tropospheric and stratospheric climate changes, the tropospheric response dominates; results are strongest when the tropospheric and stratospheric influences are producing similar phase changes. Both regions produce their effect primarily by altering wave propagation and angular momentum transports, but planetary wave energy changes accompanying tropospheric climate change are also important. Stratospheric forcing has a larger impact on the NAO than on the AO, and the angular momentum transport changes associated with it peak in the upper troposphere, affecting all wavenumbers. Tropospheric climate changes influence both the A0 and NAO with effects that extend throughout the troposphere. For both forcings there is often vertical consistency in the sign of the momentum transport changes, obscuring the difference between direct and indirect mechanisms for influencing the surface circulation.

Comparisons of planetary wave propagation to the upper atmosphere during stratospheric warming events at different QBO phases

NASA Astrophysics Data System (ADS)

Koval, Andrey V.; Gavrilov, Nikolai M.; Pogoreltsev, Alexander I.; Savenkova, Elena N.

2018-06-01

The dynamical coupling of the lower and upper atmosphere by planetary waves (PWs) is studied. Numerical simulations of planetary wave (PW) amplitudes during composite sudden stratospheric warming (SSW) events in January-February are made using a model of general circulation of the middle and upper atmosphere with initial and boundary conditions typical for the westerly and easterly phases of quasi-biennial oscillation (QBO). The changes in PW amplitudes in the middle atmosphere before, during and after SSW event for the different QBO phases are considered. Near the North Pole, the increase in the mean temperature during SSW reaches 10-30 K at altitudes 30-50 km for four pairs of the model runs with the eQBO and wQBO, which is characteristic for the sudden stratospheric warming event. Amplitudes of stationary PWs in the middle atmosphere of the Northern hemisphere may differ up to 30% during wQBO and eQBO before and during the SSW. After the SSW event SPW amplitudes are substantially larger during wQBO phase. PW refractivity indices and Eliassen-Palm flux vectors are calculated. The largest EP-fluxes in the middle atmosphere correspond to PWs with zonal wavenumber m=1. Simulated changes in PW amplitudes correspond to inhomogeneities of the global circulation, refractivity index and EP-flux produced by the changes in QBO phases. Comparisons of differences in PW characteristics and circulation between the wQBO and eQBO show that PWs could provide effective coupling mechanism and transport dynamical changes from local regions of the lower atmosphere to distant regions of the upper atmosphere of both hemispheres.

Increase in upper tropospheric and lower stratospheric aerosol levels and its potential connection with Asian pollution.

PubMed

Vernier, J-P; Fairlie, T D; Natarajan, M; Wienhold, F G; Bian, J; Martinsson, B G; Crumeyrolle, S; Thomason, L W; Bedka, K M

2015-02-27

Satellite observations have shown that the Asian Summer Monsoon strongly influences the upper troposphere and lower stratosphere (UTLS) aerosol morphology through its role in the formation of the Asian Tropopause Aerosol Layer (ATAL). Stratospheric Aerosol and Gas Experiment II solar occultation and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations show that summertime UTLS Aerosol Optical Depth (AOD) between 13 and 18 km over Asia has increased by three times since the late 1990s. Here we present the first in situ balloon measurements of aerosol backscatter in the UTLS from Western China, which confirm high aerosol levels observed by CALIPSO since 2006. Aircraft in situ measurements suggest that aerosols at lower altitudes of the ATAL are largely composed of carbonaceous and sulfate materials (carbon/sulfur elemental ratio ranging from 2 to 10). Back trajectory analysis from Cloud-Aerosol Lidar with Orthogonal Polarization observations indicates that deep convection over the Indian subcontinent supplies the ATAL through the transport of pollution into the UTLS. Time series of deep convection occurrence, carbon monoxide, aerosol, temperature, and relative humidity suggest that secondary aerosol formation and growth in a cold, moist convective environment could play an important role in the formation of ATAL. Finally, radiative calculations show that the ATAL layer has exerted a short-term regional forcing at the top of the atmosphere of -0.1 W/m 2 in the past 18 years. Increase of summertime upper tropospheric aerosol levels over Asia since the 1990s Upper tropospheric enhancement also observed by in situ backscatter measurements Significant regional radiative forcing of -0.1 W/m 2 .

Microwave limb sounding of the UT/LS: Stratosphere-Troposphere Exchange And Climate Monitor (STEAM) and related projects

NASA Astrophysics Data System (ADS)

Urban, Joachim

The Stratosphere-Troposphere Exchange And climate Monitor (STEAM) radiometer is designed to provide vertically and horizontally well resolved profiles of key species in the climate relevant upper troposphere and lower stratosphere (UT/LS) altitude region such as H2O, O3, CO, HCN, CH3CN, CH3Cl, N2O, HNO3, and temperature. The instrument is a multi-beam limb sounder employing 12GHz wide sub-harmonically pumped double sideband mixers targeting the 324-336GHz (lower sideband) and 343.25-355.25GHz (upper sideband) spectral bands with a local oscillator set at 339.625GHz. Whilst the instrument configuration had been optimized during the recent years to fit the ESA Earth Explorer 7 candidate mission PREMIER, the instrument payload is now being studied in a smaller configuration for a different satellite mission in collaboration with international partners. The presentation provides an overview of the STEAM project and its science objectives and focuses on a description of the measurement capabilities of the newly configured STEAM radiometer, in comparison to related projects and existing sensors such as Odin/SMR and Aura/MLS.

The Impact of ENSO on Trace Gas Composition in the Upper Troposphere to Lower Stratosphere

NASA Technical Reports Server (NTRS)

Oman, Luke; Douglass, Anne; Ziemke, Jerry; Waugh, Darryn Warwick

2016-01-01

The El Nino-Southern Oscillation (ENSO) is the dominant mode of interannual variability in the tropical troposphere and its effects extend well into the stratosphere. Its impact on atmospheric dynamics and chemistry cause important changes to trace gas constituent distributions. A comprehensive suite of satellite observations, reanalyses, and chemistry climate model simulations are illuminating our understanding of processes like ENSO. Analyses of more than a decade of observations from NASAs Aura and Aqua satellites, combined with simulations from the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM) and other Chemistry Climate Modeling Initiative (CCMI) models, and the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) reanalysis have provided key insights into the response of atmospheric composition to ENSO. While we will primarily focus on ozone and water vapor responses in the upper troposphere to lower stratosphere, the effects of ENSO ripple through many important trace gas species throughout the atmosphere. The very large 2015-2016 El Nino event provides an opportunity to closely examine these impacts with unprecedented observational breadth. An improved quantification of natural climate variations, like those from ENSO, is needed to detect and quantify anthropogenic climate changes.

The effect of the solar rotational irradiance variation on the middle and upper atmosphere calculated by a three-dimensional chemistry-climate model

NASA Astrophysics Data System (ADS)

Gruzdev, A. N.; Schmidt, H.; Brasseur, G. P.

2009-01-01

This paper analyzes the effects of the solar rotational (27-day) irradiance variations on the chemical composition and temperature of the stratosphere, mesosphere and lower thermosphere as simulated by the three-dimensional chemistry-climate model HAMMONIA. Different methods are used to analyze the model results, including high resolution spectral and cross-spectral techniques. To force the simulations, an idealized irradiance variation with a constant period of 27 days (apparent solar rotation period) and with constant amplitude is used. While the calculated thermal and chemical responses are very distinct and permanent in the upper atmosphere, the responses in the stratosphere and mesosphere vary considerably in time despite the constant forcing. The responses produced by the model exhibit a non-linear behavior: in general, the response sensitivities (not amplitudes) decrease with increasing amplitude of the forcing. In the extratropics the responses are, in general, seasonally dependent with frequently stronger sensitivities in winter than in summer. Amplitude and phase lag of the ozone response in the tropical stratosphere and lower mesosphere are in satisfactory agreement with available observations. The agreement between the calculated and observed temperature response is generally worse than in the case of ozone.

Forty-eight-inch lidar aerosol measurements taken at the Langley Research Center, May 1974 to December 1987

NASA Technical Reports Server (NTRS)

Fuller, W. H., Jr.; Osborn, M. T.; Hunt, W. H.

1988-01-01

A ground based lidar system located at NASA Langley Research Center in Hampton, Va., was used to obtain high resolution vertical profiles of the stratospheric and upper tropospheric aerosol since 1974. More than 200 measurements obtained at a wavelength of 0.6943 microns during 1974 to 1987 are summarized. Plots of peak backscatter mixing ratio and integrated backscatter vs time are presented for the entire measurement sequence. The plots highlight the influence of several major volcanic eruptions on the long term stratospheric aerosol layer. In particular, the eruptions of El Chichon in late Mar. to early Apr. 1982, produced a massive aerosol layer. Aerosol enhancement from El Chichon reached Hampton, Va. by May 1982, with a scattering ratio of approx. 50 detected on Jul. 1, 1982. In addition, scattering ratio profiles for June 1982 to December 1987, along with tables containing numerical values of the backscatter ratio and backscattering function versus altitude, are included to further describe the upper tropospheric and stratospheric aerosol layer. A 14 year summary is presented, in a ready to use format, of lidar observations at a fixed midlatitude location to be used for further study.

Seasonal variation of the stratospheric circulation

NASA Technical Reports Server (NTRS)

Hirota, I.; Shiotani, M.

1985-01-01

An extensive analysis is made of the extratropical stratospheric circulation in terms of the seasonal variation of large-scale motion fields, with the aid of height and temperature data obtained from the TIROS satellite. Special attention is paid to a comparison of climatological aspects between the Northern Hemisphere (NH) and the Southern Hemisphere (SH). In order to see the general picture of the annual mach of the upper stratosphere, the zonal mean values of geopotential height of the 1 mb level at 70 deg N and 70 deg S were plotted on the daily basis throughout a year. It is observed that, during the winter, the zonal mean 1 mb height in the NH is much more variable than that in the SH. It is also notable that the SH height is rather oscillatory throughout the longer period from midwinter to early summer. Since the zonal mean height in the polar latitude is a rough measure of the mean zonal flow in extratropical latitudes, the difference of the seasonal variation between the two hemispheres mentioned above is considered to be due mainly to the planetary wave-mean flow interaction in the middle atmosphere. The wave activity in the middle atmosphere is represented more rigorously by the Eliassen-Palm flux associated with vertically propagating planetary waves forced from below. The day-to-day variation of the EP flux in the upper stratosphere shows that the wave activity varies intermittently with a characteristic time scale of about two weeks.

A study of the middle atmospheric thermal structure over western India: Satellite data and comparisons with models

NASA Astrophysics Data System (ADS)

Sharma, Som; Kumar, Prashant; Vaishnav, Rajesh; Jethva, Chintan; Beig, G.

2017-12-01

Long term variations of the middle atmospheric thermal structure in the upper stratosphere and lower mesosphere (20-90 km) have been studied over Ahmedabad (23.1°N, 72.3°E, 55 m amsl), India using SABER (Sounding of the Atmosphere using Broadband Emission Radiometry) onboard TIMED (Thermosphere, Ionosphere, Mesosphere, Energetics and Dynamics) observations during year 2002 to year 2014. For the same period, three different atmospheric models show over-estimation of temperature (∼10 K) near the stratopause and in the upper mesosphere, and a signature of under-estimation is seen above mesopause when compared against SABER measured temperature profiles. Estimation of monthly temperature anomalies reveals a semiannual and ter-annual oscillation moving downward from the mesosphere to the stratosphere during January to December. Moreover, Lomb Scargle periodogram (LSP) and Wavelet transform techniques are employed to characterize the semi-annual, annual and quasi-biennial oscillations to diagnose the wave dynamics in the stratosphere-mesosphere system. Results suggested that semi-annual, annual and quasi-biennial oscillations are exist in stratosphere, whereas, semi-annual and annual oscillations are observed in mesosphere. In lower mesosphere, LSP analyses revealed conspicuous absence of annual oscillations in altitude range of ∼55-65 km, and semi-annual oscillations are not existing in 35-45 km. Four monthly oscillations are also reported in the altitude range of about 45-65 km. The temporal localization of oscillations using wavelet analysis shows strong annual oscillation during year 2004-2006 and 2009-2011.

Regional Differences in Stratospheric Intrusions over the USA Investigated using the NASA MERRA-2 Reanalysis

NASA Astrophysics Data System (ADS)

Knowland, K. E.; Ott, L.; Hodges, K.; Wargan, K.; Duncan, B. N.

2016-12-01

Stratospheric intrusions (SI) - the introduction of ozone-rich stratospheric air into the troposphere - have been linked with surface ozone air quality exceedences, especially at the high elevations in the western USA in springtime. However, the impact of SIs in the remaining seasons and over the rest of the USA is less clear. This study investigates the atmospheric dynamics that generate SIs over the western USA and the different mechanisms through which SIs may influence atmospheric chemistry and surface air quality over the eastern USA. An analysis of the spatiotemporal variability of SIs over the continental US is performed using NASA's Modern-Era Retrospective Analysis for Research and Applications Version-2 (MERRA-2) reanalysis dataset and other Goddard Earth Observing System Model, Version 5 (GEOS-5) model products. Both upper-level and lower-level dynamical features are examined on seasonal timescales using the tracking algorithm of Hodges (1995, 1999). We show how upper-level relative vorticity maxima - representing troughs and cut-off lows - can be tracked and related to the lower-level storm tracks. The influence of both sets of tracks on the assimilated MERRA-2 ozone and meteorological parameters throughout the troposphere and lower stratosphere is quantified. By focusing on the major modes of variability that influence the weather patterns in the USA, namely the Pacific North American (PNA) pattern, Arctic Oscillation (AO) and the North Atlantic Oscillation (NAO), predicative patterns in the meteorological fields that are associated with SIs are identified for their regional effects.

Ultraviolet spectrum and chemical reactivity of the ClO dimer

NASA Technical Reports Server (NTRS)

Demore, W. B.; Tschuikow-Roux, E.

1990-01-01

The ClO dimer was prepared by photolysis (wavelength greater than 300 nm) of Cl2/Cl2O or Cl2/O3 mixtures or by photolysis of Cl2O alone. Temperatures were in the range 195-217 K, and experiments were carried out both in the gas phase and in the cryogenic solvents CF4, CO2, and N2O. Dimer cross sections in the range 190-400 nm are reported both in the gas phase and in the solvents. Results indicate that ClOOCl is the only dimer structure formed as a stable product. Upper limits of 1 x 10 to the -19th and 1 x 10 to the -20th cu cm/s are placed on the reactions of ClOOCl with O3 and with itself, respectively.

Observations of planetary mixed Rossby-gravity waves in the upper stratosphere

NASA Technical Reports Server (NTRS)

Randel, William J.; Boville, Byron A.; Gille, John C.

1990-01-01

Observational evidence is presented for planetary scale (zonal wave number 1-2) mixed Rossby-gravity (MRG) waves in the equatorial upper stratosphere (35-50 km). These waves are detected in LIMS measurements as coherently propagating temperature maxima of amplitude 0.1-0.3 K, which are antisymmetric (out of phase) about the equator, centered near 10-15 deg north and south latitude. These features have vertical wavelengths of order 10-15 km, periods near 2-3 days, and zonal phase velocities close to 200 m/s. Both eastward and westward propagating waves are found, and the observed vertical wavelengths and meridional structures are in good agreement with the MRG dispersion relation. Theoretical estimates of the zonal accelerations attributable to these waves suggest they do not contribute substantially to the zonal momentum balance in the middle atmosphere.

Latitudinal distribution of black carbon soot in the upper troposphere and lower stratosphere

NASA Technical Reports Server (NTRS)

Blake, David F.; Kato, Katharine

1995-01-01

Black carbon soot from the upper troposphere and lower stratosphere has been systematically collected at latitudes from 90 deg N to 45 deg S. The measured latitudinal distribution of this soot at 10 to 11 km altitude is found to covary with commercial air traffic fuel use, suggesting that aircraft fuel combustion at altitude is the principal source. In addition, at latitudes where the commercial air traffic is high, measured black carbon soot values are high even at 20 km altitude, suggesting that aircraft-generated soot injected just above the tropopause may be transported to higher altitudes. During the volcanically influenced period in which these samples were collected, the number abundances, total mass, and calculated total surface area of black carbon soot are 2-3 orders of magnitude lower than similar measures of sulfuric acid aerosol. During volcanically quiescent periods, the calculated total surface area of black carbon soot aerosol is of the same order of magnitude as that of the background sulfuric acid aerosol. It appears from this comparison that black carbon soot is only capable of influencing lower stratosphere or upper troposphere chemistry during periods when the aerosol budget is not dominated by volcanic activity. It remains to determine the extent to which black carbon soot particles act as nuclei for sulfuric acid aerosol formation. However, mass balance calculations suggest that aircraft soot injected at altitude does not represent a significant source of condensation nuclei for sulfuric acid aerosols.

The Influence of the Several Very Large Solar Proton Events in Years 2000-2003 on the Neutral Middle Atmosphere

NASA Technical Reports Server (NTRS)

Jackman, Charles H.; Sinnhuber, Miriam; Anderson, John; McPeters, Richard D.; FLeming, Eric L.; Russell, James M.

2004-01-01

Solar proton events (SPEs) are known to have caused changes in constituents in the Earth's neutral middle atmosphere. The highly energetic protons produce ionizations, excitations, dissociations, and dissociative ionizations of the background constituents, which lead to the production of HOx (H, OH, HO2) and NOy (N, NO, NO2, NO3, N2O5, HNO3, HO2NO2, ClONO2, BrONO2). The HOx increases lead to short-lived ozone decreases in the mesosphere and upper stratosphere due to the short lifetimes of the HOx constituents. The NOy increases lead to long-lived stratospheric ozone changes because of the long lifetime of the NOy family in this region. The past four years, 2000-2003, have been replete with SPEs and huge fluxes of high energy protons occurred in July and November 2000, September and November 2001, April 2002, and October 2003. Smaller, but still substantial, proton fluxes impacted the Earth during other months from year 2000 to 2003. The Goddard Space Flight Center (GSFC) Two-dimensional (2D) Model was used in computing the influence of the SPEs. The impact of these extremely large SPEs was calculated to be especially large in the upper stratosphere and mesosphere. The results of the GSFC 2D Model will be shown along with comparisons to the Upper Atmosphere Research Satellite (UARS) Halogen Occultation Experiment (HALOE) and Solar Backscatter Ultraviolet 2 (SBUV/2) instruments.

The Origin of Titan’s External Oxygen: Further Constraints from ALMA Upper Limits on CS and CH2NH

NASA Astrophysics Data System (ADS)

Teanby, N. A.; Cordiner, M. A.; Nixon, C. A.; Irwin, P. G. J.; Hörst, S. M.; Sylvestre, M.; Serigano, J.; Thelen, A. E.; Richards, A. M. S.; Charnley, S. B.

2018-06-01

Titan’s atmospheric inventory of oxygen compounds (H2O, CO2, CO) are thought to result from photochemistry acting on externally supplied oxygen species (O+, OH, H2O). These species potentially originate from two main sources: (1) cryogenic plumes from the active moon Enceladus and (2) micrometeoroid ablation. Enceladus is already suspected to be the major O+ source, which is required for CO creation. However, photochemical models also require H2O and OH influx to reproduce observed quantities of CO2 and H2O. Here, we exploit sulphur as a tracer to investigate the oxygen source because it has very different relative abundances in micrometeorites (S/O ∼ 10‑2) and Enceladus’ plumes (S/O ∼ 10‑5). Photochemical models predict most sulphur is converted to CS in the upper atmosphere, so we use Atacama Large Millimeter/submillimeter Array (ALMA) observations at ∼340 GHz to search for CS emission. We determined stringent CS 3σ stratospheric upper limits of 0.0074 ppb (uniform above 100 km) and 0.0256 ppb (uniform above 200 km). These upper limits are not quite stringent enough to distinguish between Enceladus and micrometeorite sources at the 3σ level and a contribution from micrometeorites cannot be ruled out, especially if external flux is toward the lower end of current estimates. Only the high-flux micrometeorite source model of Hickson et al. can be rejected at 3σ. We determined a 3σ stratospheric upper limit for CH2NH of 0.35 ppb, which suggests cosmic rays may have a smaller influence in the lower stratosphere than predicted by some photochemical models. Disk-averaged C3H4 and C2H5CN profiles were determined and are consistent with previous ALMA and Cassini/CIRS measurements.

1,2-Dichlorohexafluoro-Cyclobutane (1,2-c-C4F6Cl2, R-316c) a Potent Ozone Depleting Substance and Greenhouse Gas: Atmospheric Loss Processes, Lifetimes, and Ozone Depletion and Global Warming Potentials for the (E) and (Z) stereoisomers

NASA Technical Reports Server (NTRS)

Papadimitriou, Vassileios C.; McGillen, Max R.; Smith, Shona C.; Jubb, Aaron M.; Portmann, Robert W.; Hall, Bradley D.; Fleming, Eric L.; Jackman, Charles H.; Burkholder, James B.

2013-01-01

The atmospheric processing of (E)- and (Z)-1,2-dichlorohexafluorocyclobutane (1,2-c-C4F6Cl2, R-316c) was examined in this work as the ozone depleting (ODP) and global warming (GWP) potentials of this proposed replacement compound are presently unknown. The predominant atmospheric loss processes and infrared absorption spectra of the R-316c isomers were measured to provide a basis to evaluate their atmospheric lifetimes and, thus, ODPs and GWPs. UV absorption spectra were measured between 184.95 to 230 nm at temperatures between 214 and 296 K and a parametrization for use in atmospheric modeling is presented. The Cl atom quantum yield in the 193 nm photolysis of R- 316c was measured to be 1.90 +/- 0.27. Hexafluorocyclobutene (c-C4F6) was determined to be a photolysis co-product with molar yields of 0.7 and 1.0 (+/-10%) for (E)- and (Z)-R-316c, respectively. The 296 K total rate coefficient for the O(1D) + R-316c reaction, i.e., O(1D) loss, was measured to be (1.56 +/- 0.11) × 10(exp -10)cu cm/ molecule/s and the reactive rate coefficient, i.e., R-316c loss, was measured to be (1.36 +/- 0.20) × 10(exp -10)cu cm/molecule/s corresponding to a approx. 88% reactive yield. Rate coefficient upper-limits for the OH and O3 reaction with R-316c were determined to be <2.3 × 10(exp -17) and <2.0 × 10(exp -22)cu cm/molecule/s, respectively, at 296 K. The quoted uncertainty limits are 2(sigma) and include estimated systematic errors. Local and global annually averaged lifetimes for the (E)- and (Z)-R-316c isomers were calculated using a 2-D atmospheric model to be 74.6 +/- 3 and 114.1 +/-10 years, respectively, where the estimated uncertainties are due solely to the uncertainty in the UV absorption spectra. Stratospheric photolysis is the predominant atmospheric loss process for both isomers with the O(1D) reaction making a minor, approx. 2% for the (E) isomer and 7% for the (Z) isomer, contribution to the total atmospheric loss. Ozone depletion potentials for (E)- and (Z)-R-316c were calculated using the 2-D model to be 0.46 and 0.54, respectively. Infrared absorption spectra for (E)- and (Z)-R-316c were measured at 296 K and used to estimate their radiative efficiencies (REs) and GWPs; 100-year time-horizon GWPs of 4160 and 5400 were obtained for (E)- and (Z)-R-316c, respectively. Both isomers of R-316c are shown in this work to be long-lived ozone depleting substances and potent greenhouse gases.

Microbial survival in the stratosphere and implications for global dispersal

USGS Publications Warehouse

Smith, David J.; Griffin, Dale W.; McPeters, Richard D.; Ward, Peter D.; Schuerger, Andrew C.

2011-01-01

Spores of Bacillus subtilis were exposed to a series of stratosphere simulations. In total, five distinct treatments measured the effect of reduced pressure, low temperature, high desiccation, and intense ultraviolet (UV) irradiation on stratosphereisolated and ground-isolated B. subtilis strains. Environmental conditions were based on springtime data from a mid-latitude region of the lower stratosphere (20 km). Experimentally, each treatment consisted of the following independent or combined conditions: -70 °C, 56 mb, 10-12%relative humidity and 0.00421, 5.11, and 54.64 W/m2 of UVC (200-280 nm), UVB (280-315 nm), UVA (315-400 nm), respectively. Bacteria were deposited on metal coupon surfaces in monolayers of ~1 x 106 spores and prepared with palagonite (particle size< 20 μm). After 6 h of exposure to the stratosphere environment, 99.9% of B. subtilis spores were killed due to UV irradiation. In contrast, temperature, desiccation, and pressure simulations without UV had no effect on spore viability up through 96 h. There were no differences in survival between the stratosphere-isolated versus ground-isolated B. subtilis strains. Inactivation of most bacteria in our simulation indicates that the stratosphere can be a critical barrier to long-distance microbial dispersal and that survival in the upper atmosphere may be constrained by UV irradiation.

Measurements of 32SO2, 33SO2, 34SO2 and 36SO2 high-resolution cross-sections and isotope effects by SO2 self-shielding

NASA Astrophysics Data System (ADS)

Endo, Y.; Ogawa, M.; Danielache, S. O.; Ueno, Y.

2017-12-01

Archean sulfur mass-independent fractionation (S-MIF) is a unique proxy within the geological and geochemical records for studying the composition of the Archean atmosphere. S-MIF signatures are defined as Δ33S = δ33S - 0.515×δ34S and Δ36S = δ36S - 1.90×δ34S. Archean S-MIF is characterized as Δ36S/Δ33S = -1. Recent SO2 photochemical experiments under specific reducing conditions reproduced the Archean trend for the first time [1]. Self-shielding of SO2 photolysis and intersystem crossing in excited SO2 are probably key mechanisms for explaining Archean S-MIF. Self-shielding is originated from UV spectra changed by upper SO2 own absorption. Because 32S accounts for about 95% of all sulfur isotopes, the photolysis rate constant of only 32SO2 is lower than other isotopologue. Thus, SO2 photolysis in the bottom of the atmosphere undergoes mass-independent fractionation. Fractionation factors by SO2 photolysis reaction can be calculated by absorption cross-sections of 32SO2, 33SO2, 34SO2 and 36SO2 and respective quantum yields. Quantitative estimations self-shielding fractionation factors requires high-spectral resolution cross-sections, but they have not been reported yet. Here we report measurements of high-resolution cross-sections (1cm-1) and fractionation factors by SO2 photolysis including self-shielding. Moreover, because the absorption wavelength varies with each isotopologue, photolysis rate constants of all isotopologues (32S16O2, 32S16O18O, etc) should be different. Then self-shielding may affect the ratio of isotopologues such as clumped-isotopes. We calculated preliminary calculation clumped isotope enrichment in residual species by self-shielding. Reference: [1] Endo, Y., Ueno, Y., Aoyama, S., & Danielache, S. O. (2016). Sulfur isotope fractionation by broadband UV radiation to optically thin SO2 under reducing atmosphere. EPSL, 453, 9-22.

Dynamical variability in the modelling of chemistry-climate interactions.

PubMed

Pyle, J A; Braesicke, P; Zeng, G

2005-01-01

We have used a version of the Met Office's climate model, into which we have introduced schemes for atmospheric chemistry, to study chemistry-dynamics-climate interactions. We have considered the variability of the stratospheric polar vortex, whose behaviour influences stratospheric ozone loss and will affect ozone recovery. In particular, we analyse the dynamical control of high latitude ozone in a model version which includes an assimilation of the equatorial quasi-biennial oscillation (QBO), demonstrating the stability of the linear relation between vortex strength and high latitude ozone. We discuss the effect of interactive model ozone on polar stratospheric cloud (PSC) area/volume and winter-spring stratospheric ozone loss in the northern hemisphere. In general we find larger polar ozone losses calculated in those model integrations in which modelled ozone is used interactively in the radiation scheme, even though we underestimate the slope of the ozone loss per PSC volume relation derived from observations. We have also looked at the influence of changing stratosphere-to-troposphere exchange on the tropospheric oxidizing capacity and, in particular, have considered the variability of tropospheric composition under different climate regimes (El Niño/La Niña, etc.). Focusing on the UT/LS, we show the response of ozone to El Niño in two different model set-ups (tropospheric/ stratospheric). In the stratospheric model set-up we find a distinct signal in the lower tropical stratosphere, which shows an anti-correlation between the Niño 3 index and the ozone column amount. In contrast ozone generally increases in the upper troposphere of the tropospheric model set-up after an El Niño. Understanding future trends in stratospheric ozone and tropospheric oxidizing capacity requires an understanding of natural variability, which we explore here.

An Update on Ozone Profile Trends for the Period 2000 to 2016

NASA Technical Reports Server (NTRS)

Steinbrecht, Wolfgang; Froidevaux, Lucien; Fuller, Ryan; Wang, Ray; Anderson, John; Roth, Chris; Bourassa, Adam; Degenstein, Doug; Damadeo, Robert; Zawodny, Joe;

Long Term δ17O, δ18O measurements of tropospheric carbon dioxide and potential application to the global carbon cycle. (Invited)

NASA Astrophysics Data System (ADS)

Thiemens, M. H.

2009-12-01

Stable isotope ratio measurements have played an important role in defining the global carbon cycle for the past half century. In the past decades, mass independent isotopic measurements of stratospheric carbon dioxide have been shown to be an important indice for understanding stratospheric ozone chemistry and the interaction with carbon dioxide. In this specific role, it is the O(1D) produced from ozone photolysis that interacts with CO2 and inscribes a mass independent isotopic composition (see review by (1)). This photochemical process simultaneously provides an isotopic record in carbon dioxide of the integrated exposure to ozone/atomic oxygen and stratosphere troposphere mixing. As a consequence of these processes, it has been observed that tropospheric oxygen possesses a mass independent composition that may be used as a tracer of bioproductivity (2) and as a potential measure of carbon dioxide levels during and following the snowball earth event (3). In addition, the magnitude of the stratospheric anomaly in the troposphere may directly reflect the atmospheric turnover rates of carbon dioxide, which is an important component of the carbon cycle (4, 5). To further develop this new methodology, the rates and magnitude of the relevant processes must be identified and quantified. Samples of tropospheric carbon dioxide were obtained in La Jolla, Ca. over a 10 year plus time period. All samples were taken under identical conditions and analyzed immediately for all three oxygen isotopes. There was no sample storage and samples were thoroughly isolated from water. All conditions, including standardization and mass spectrometry were constant throughout that time period. The data are consistent with an identifiable steady state component of stratospheric carbon dioxide. In addition, other features of the data suggest other processes operative that are presently unaccounted for, and, are only observable in the mass independent composition. References 1. Thiemens, M.H. (2006). Annual Rev. earth Planet Sci. 34, 217 (2006). 2.Luz, B., Bender, M.L., Thiemens, M.H., Boering, K. Nature 400, 547 (2002). 3.Bao, H., Lyons, J.R., Zhou, Chuanming. Nature 453, 504 (2008). 4.Hoag, K.J., Still, C.J., Fung, I.Y., Boering, K.A. Geophys. Res. Lett 32, L02802 (2005). 5.Liang, M-C., Blake, G.A., Yung, Y.L. J. Geophys. Res 113, D12305 (2008).

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reiter, R.; Kanter, H. J.; Sladkovic, R.

The balance of the tropospheric ozone is studied with regard to sources and sinks. The influx of stratospheric ozone through stratospheric intrusions and photochemical production under pure air conditions is discussed. The 4-year measuring series (1977-1980) of the ozone concentration measured at 3 different levels are evaluated, the influence of meteorological parameters is examined. The time variation of the ozone layer between 1000 and 3000 m ASL is investigated as a function of different ozone sources. First results show that stratospheric ozone arriving at the troposphere penetrates only in a few rare cases to the ground layer below 1500 mmore » ASL. Most of the time, the variation of ozone concentration in this layer is determined by photochemical processes which are, in turn, controlled by meteorological parameters. The upper boundary of the photochemically active layer is found at about 500 m above ground. Variability of the concentration of stratospheric aerosol and its optical properties after the volcanic eruptions in the year 1980 are discussed on the basis on lidar backscattering measurements.« less

Sources of enhanced SO2 in the tropical Western Pacific UT/LS

NASA Astrophysics Data System (ADS)

Rollins, A. W.; Thornberry, T. D.; Liu, S.; Ray, E. A.; Atlas, E. L.; Navarro, M. A.; Schauffler, S.; Bui, T. V.; Gao, R. S.

2017-12-01

Sulfur dioxide is an important precursor to aerosols in the stratosphere. Typical mixing ratios of SO2 in the tropical upper troposphere and lower stratosphere (UT/LS) are on the order of a few pptv. Convective transport of SO2 from source regions near the surface can produce local enhancements in the UT/LS of more than one order of magnitude compared to typical values. These local enhancements if sufficient in number and/or magnitude might be important for the stratospheric aerosol budget. Here we analyze three such local enhancements observed during the NASA POSIDON mission. We use back-trajectories and tracer species to demonstrate that significant SO2 in the UT/LS on different occasions originated from 1) a volcano in Papua New Guinea, 2) convection over Asia, and 3) transport of air by a typhoon. These examples that were observed on three out of ten flights indicate that significant SO2 over the Western Pacific is not uncommon, and may be an important fraction of the stratospheric aerosol budget.

A Lagrangian Simulation of Subsonic Aircraft Exhaust Emissions

NASA Technical Reports Server (NTRS)

Schoeberl, M. R.; Morris, G. A.

1999-01-01

To estimate the effect of subsonic and supersonic aircraft exhaust on the stratospheric concentration of NO(y), we employ a trajectory model initialized with air parcels based on the standard release scenarios. The supersonic exhaust simulations are in good agreement with 2D and 3D model results and show a perturbation of about 1-2 ppbv of NO(y) in the stratosphere. The subsonic simulations show that subsonic emissions are almost entirely trapped below the 380 K potential temperature surface. Our subsonic results contradict results from most other models, which show exhaust products penetrating above 380 K, as summarized. The disagreement can likely be attributed to an excessive vertical diffusion in most models of the strong vertical gradient in NO(y) that forms at the boundary between the emission zone and the stratosphere above 380 K. Our results suggest that previous assessments of the impact of subsonic exhaust emission on the stratospheric region above 380 K should be considered to be an upper bound.

Identification of Stratospheric Waves in Ozone in the Tropics from OMI High Spectral Resolution Measurements

NASA Technical Reports Server (NTRS)

Ziemke, J. R.; Liu, X.; Bhartia, P. K.

2007-01-01

Previous studies using Total Ozone Mapping Spectrometer (TOMS) measurements have identified several types of tropical waves in the stratosphere. These waves include Kelvin waves, mixed Rossby-gravity waves, equatorial Rossby waves, and global normal modes. All of these detected waves occur when their zonal phase speeds are opposite the zonal winds in the low-mid stratosphere associated with the Quasi-biennial Oscillation (QBO). Peak-to-peak amplitudes in all cases are typically 5 DU. While total ozone data from TOMS is sensitive in detecting these tropical waves, they provide each day only a single horizontal cross-sectional map. The high spatial and spectral resolution of the Aura Ozone Monitoring Instrument (OMI) provides a unique means to evaluate 3D structure in these waves including their propagation characteristics. Ozone profiles retrieved from OMI radiances for wavelengths 270-310 nm are utilized to examine the nature of these wave disturbances extending from the lower to upper stratosphere.

The Variability of the Horizontal Circulation in the Troposphere and Stratosphere: A Comparison

NASA Technical Reports Server (NTRS)

Perlwitz, Judith; Graf, Hans-F.; Hansem, James E. (Technical Monitor)

2001-01-01

The variability of the horizontal circulation in the stratosphere and troposphere of the Northern Hemisphere (NH) is compared by using various approaches. Spatial degrees of freedom (dof) on different time scales were derived. Modes of variability were computed in geopotential height fields at the tropospheric and stratospheric pressure levels by applying multivariate statistical approaches. Features of the spatial and temporal variability of the winterly zonal wind were studied with the help of recurrence and persistence analyses. The geopotential height and zonally-averaged zonal wind at the 50-, 500- and 1000-hPa level are used to investigate the behavior of the horizontal circulation in the lower stratosphere, mid-troposphere and at the near surface level, respectively. It is illustrated that the features of the variability of the horizontal circulation are very similar in the mid-troposphere and at the near surface level. Due to the filtering of tropospheric disturbances by the stratospheric and upper tropospheric zonal mean flow, the variability of the stratospheric circulation exhibits less spatial complexity than the circulation at tropospheric pressure levels. There exist enormous differences in the number of degrees of freedom (or free variability modes) between both atmospheric layers. Results of the analyses clearly show that the concept of a zonally symmetric AO with a simple structure in the troposphere similar to the one in the stratosphere is not valid. It is concluded that the spatially filtered climate change signal can be detected earlier in the stratosphere than in the mid-troposphere or at the near surface level.

Characterization of the Nimbus-7 SBUV radiometer for the long-term monitoring of stratospheric ozone

NASA Technical Reports Server (NTRS)

Cebula, Richard P.; Park, H.; Heath, D. F.

1988-01-01

Precise knowledge of in-orbit sensitivity change is critical for the successful monitoring of stratospheric ozone by satellite-based remote sensors. This paper evaluates those aspects of the in-flight operation that influence the long-term stability of the upper stratospheric ozone measurements made by the Nimbus-7 SBUV spectroradiometer and chronicles methods used to maintain the long-term albedo calibration of this UV sensor. It is shown that the instrument's calibration for the ozone measurement, the albedo calibration, has been maintained over the first 6 yr of operation to an accuracy of approximately + or - 2 percent. The instrument's wavelength calibration is shown to drift linearly with time. The knowledge of the SBUV wavelength assignment is maintained to a 0.02-nm precision.

Measurements of stratospheric NO, NO2, and N2O5 by ISAMS: Preliminary observations and data validation

NASA Technical Reports Server (NTRS)

Kerridge, Brian J.; Ballard, J.; Knight, R. J.; Stevens, A. D.; Reburn, J.; Morris, P.; Remedios, John J.; Taylor, Fredric W.

1994-01-01

The Improved Stratospheric and Mesospheric Sounder (ISAMS) is a multichannel radiometer and forms part of the science payload of the Upper Atmosphere Research Satellite (UARS). ISAMS measures infrared emissions from the Earth's atmosphere in several wavelength bands. Three such bands include emission from nitric oxide, nitrogen dioxide, and dinitrogen pentoxide. In this paper, we briefly discuss how the ISAMS instrument measures NO, NO2, and N2O5. We also present preliminary data from these channels and describe preliminary validation work.

The mean observed meteorological structure and circulation of the stratosphere and mesosphere

NASA Technical Reports Server (NTRS)

Theon, J. S.; Smith, W. S.; Casey, J. F.; Kirkwood, B. R.

1972-01-01

Meteorological soundings of the upper stratosphere and mesosphere, conducted with in situ rocket techniques during all seasons of the year from several sites, ranging in latitude from 8 deg S to 71 deg N, are analyzed. The resulting data are compiled into mean monthly and seasonal profiles of temperature, pressure, density, and wind for each site and are presented in graphical and tabular form. Analyses of these mean values produced time cross sections, quasi-meridional cross sections, and constant level maps which are included.

Stratospheric Aerosol and Gas Experiment (SAGE) II and III Aerosol Extinction Measurements in the Arctic Middle and Upper Troposphere

NASA Technical Reports Server (NTRS)

Treffeisen, R. E.; Thomason, L. W.; Strom, J.; Herber, A. B.; Burton, S. P.; Yamanouchi, T.

2006-01-01

In recent years, substantial effort has been expended toward understanding the impact of tropospheric aerosols on Arctic climate and chemistry. A significant part of this effort has been the collection and documentation of extensive aerosol physical and optical property data sets. However, the data sets present significant interpretive challenges because of the diverse nature of these measurements. Among the longest continuous records is that by the spaceborne Stratospheric Aerosol and Gas Experiment (SAGE) II. Although SAGE tropospheric measurements are restricted to the middle and upper troposphere, they may be able to provide significant insight into the nature and variability of tropospheric aerosol, particularly when combined with ground and airborne observations. This paper demonstrates the capacity of aerosol products from SAGE II and its follow-on experiment SAGE III to describe the temporal and vertical variations of Arctic aerosol characteristics. We find that the measurements from both instruments are consistent enough to be combined. Using this combined data set, we detect a clear annual cycle in the aerosol extinction for the middle and upper Arctic troposphere.

Ionospheric disturbances in Asian region of Russia during sudden stratospheric warmings

NASA Astrophysics Data System (ADS)

Kurkin, Vladimir; Chernigovskaya, Marina; Medvedeva, Irina; Orlov, Igor

This paper presents an investigation of the subauroral and mid-latitude ionosphere variations in the Asian region of Russia during stratospheric warmings in 2008, 2009 and 2010. We used the data from network of vertical and oblique-incidence sounding ionosounders of ISTP SB RAS. Irkutsk chirp-sounder (vertical incidence sounding) run every 1 minute on 24-hour basis for 30 days in winter of 2008, 2009 and 2010 to study small-scale and medium-scale distur-bances. The experiments on the radio paths Magadan-Irkutsk, Khabarovsk-Irkutsk and Norilsk -Irkutsk were conducted in order to study large-scale ionospheric disturbances. The frequency range was from 4 to 30 MHz, the sweep rate used 500 kHz/sec. To identify the stratospheric warming events the Berlin Meteorological University data (http://strat-www.met.fu-berlin.de) on stratospheric warming at standard isobaric levels and the atmospheric temperature height profiles measured by the Microwave Limb Sounder (MLS) aboard the EOS Aura spacecraft were used. The increase of wave activity in upper ionosphere over Asian region of Russia has recorded during stratospheric warmings. Spectrums of multi-scale variations were derived from the data obtained during the prolonged experiments. The analysis of experimental data has revealed the amplitudes of planetary waves in ionosphere during stratospheric warmings in 2008 and 2010 larger than ones in winter 2009 as opposed to amplitude variations of temperature in stratosphere. This work was supported by Russian Foundation for Basic Research (grant 08-05-00658).

Mesosphere-Stratosphere Coupling: Implications for Climate Variability and Trends

NASA Technical Reports Server (NTRS)

Baldwin, Mark P.

2004-01-01

A key aspect of this project is the establishment of a causal link from circulation anomalies in the lower mesosphere and stratopause region downward through the stratosphere to the troposphere. The observational link for stratospheric sudden warmings and surface climate is fairly clear. However, our understanding of the dynamics is incomplete. We have been making significant progress in the area of dynamical mechanisms by which circulation anomalies in the stratosphere affect the troposphere. We are trying to understand the details and sequence of events that occur when a middle atmosphere (wind) anomaly propagates downward to near the tropopause. The wind anomaly could be caused by a warming or solar variations in the low-latitude stratopause region, or could have other causes. The observations show a picture that is consistent with a circulation anomaly that descends to the tropopause region, and can be detected as low as the mid-troposphere. Processes near the stratopause in the tropics appear to be important precursors to the wintertime development of the northern polar vortex. This may affect significantly our understanding of the process by which low-latitude wind anomalies in the low mesosphere and upper stratosphere evolve through the winter and affect the polar vortex.

Analysis of a rapid increase of stratospheric ozone during late austral summer 2008 over Kerguelen (49.4° S, 70.3° E)

NASA Astrophysics Data System (ADS)

Bencherif, H.; El Amraoui, L.; Kirgis, G.; Leclair de Bellevue, J.; Hauchecorne, A.; Mzé, N.; Portafaix, T.

2010-07-01

This paper reports on an increase of ozone event observed over Kerguelen (49.4° S, 70.3° E) in relationship with large-scale isentropic transport. It is evidenced from ground-based observations, together with satellite global observations and assimilated fields. The study is based on the analyses of the first ozonesonde experiment never recorded at the Kerguelen site in the framework of a French campaign called ROCK that took place from April to August 2008. Comparisons and interpretations of the observed event are supported by co-localised SAOZ observations, by global mapping of tracers (O3, N2O and columns of O3) from Aura/MLS and Aura/OMI experiments, and by model simulations of Ertel Potential Vorticity initialised by ECMWF (European Centre for Medium-Range Weather Forecasts) data reanalyses. Satellite and ground-based observational data revealed a consistent increase of ozone in the local stratosphere by mid-April 2008. Additionally, Ozone (O3) and nitrous oxide (N2O) profiles obtained during January-May 2008 by the Microwave Lamb Sounder (MLS) aboard the Aura satellite are assimilated into MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle), a global three-dimensional chemistry transport model of Météo-France. The assimilated total O3 values are consistent with SAOZ ground observations (within ±5%), and isentropic distributions of O3 are matching well with maps of advected potential vorticity (APV) derived from the MIMOSA model, a high-resolution advection transport model, and from ECMWF reanalysis. The studied event seems to be related to isentropic transport of air masses that took place simultaneously in the lower- and middle-stratosphere, respectively from the polar region and from tropics to the mid-latitudes. In fact, the studied ozone increase by mid April 2008 results simultaneously: (1) from an equator-ward departure of polar air masses characterised with a high-ozone layer in the lower stratosphere (nearby the 475 K isentropic level), and (2) from a reverse isentropic transport from tropics to mid- and high-latitudes in the upper stratosphere (nearby the 700 K level). The increase of ozone observed over Kerguelen from the 16-April ozonesonde profile is then attributed to a concomitant isentropic transport of ozone in two stratospheric layers: the tropical air moving southward and reaches over Kerguelen in the upper stratosphere, and the polar air passing over the same area but in the lower stratosphere.

Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange

NASA Astrophysics Data System (ADS)

Liang, Q.; Rodriguez, J. M.; Douglass, A. R.; Crawford, J. H.; Olson, J. R.; Apel, E.; Bian, H.; Blake, D. R.; Brune, W.; Chin, M.; Colarco, P. R.; da Silva, A.; Diskin, G. S.; Duncan, B. N.; Huey, L. G.; Knapp, D. J.; Montzka, D. D.; Nielsen, J. E.; Pawson, S.; Riemer, D. D.; Weinheimer, A. J.; Wisthaler, A.

2011-12-01

We use aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission to examine the distributions and source attributions of O3 and NOy in the Arctic and sub-Arctic region. Using a number of marker tracers, we distinguish various air masses from the background troposphere and examine their contributions to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has a mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreasing from ~145 ppbv in spring to ~100 ppbv in summer. These observed mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in emissions and stratospheric ozone layer in the past two decades that influence Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses, with mean O3 concentrations of 140-160 ppbv, are significant direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin displays net O3 formation in the Arctic due to its sustainable, high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer). The air masses influenced by the stratosphere sampled during ARCTAS-B also show conversion of HNO3 to PAN. This active production of PAN is the result of increased degradation of ethane in the stratosphere-troposphere mixed air mass to form CH3CHO, followed by subsequent formation of PAN under high NOx conditions. These findings imply that an adequate representation of stratospheric NOy input, in addition to stratospheric O3 influx, is essential to accurately simulate tropospheric Arctic O3, NOx and PAN in chemistry transport models. Plumes influenced by recent anthropogenic and biomass burning emissions observed during ARCTAS show highly elevated levels of hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contain O3 higher than that in the Arctic tropospheric background except some aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

The Global Climate Anomaly in 1940-1942

NASA Astrophysics Data System (ADS)

Brönnimann, S.; Luterbacher, J.; Staehelin, J.; Svendby, T. M.

2003-12-01

An unprecedented climatic anomaly occurred in the tropics and in the Northern Hemisphere in 1940-1942. During a strong and prolonged El Niño [Bigg & Inoué, QJRMS 118 (1992), 125], extremely cold winters were observed in Europe, accompanied by very warm temperatures in Alaska and large parts of the Arctic and a cold North Pacific. The anomalies were strong (comprising the two coldest European winters of the 20th century) and extraordinarily persistent. In addition, exceptionally high values of total ozone are reported [Langlo, Geofys. Publ. 18/6 (1952)], pointing to an anomalous stratospheric circulation. Events of this magnitude have a strong economical and environmental impact; the 1940s anomaly even affected World War II. Studying this anomaly in detail contributes to (1) document the extent of 20th century climate variability, (2) understand large-scale coupling processes between the tropics and the extratropics and between the troposphere and the stratosphere and (3) develop tools to analyze past upper-level climate variability prior to 1948, i.e., the reanalysis period. For this study we have compiled, digitized, and re-evaluated several tens of thousands of temperature and pressure profiles from aircraft and radiosonde ascents up to 50 hPa [Brönnimann, Int. J. Clim. 23 (2003), 769]. The upper-air data were supplemented with data from the Earth's surface and used to statistically reconstruct monthly upper-level fields for the extratropical Northern Hemisphere up to 100 hPa [Brönnimann & Luterbacher, Clim. Dyn., submitted]. Although the quality of the reconstructed stratospheric fields is not comparable to more recent data, it is sufficient to allow a broad characterization of the circulation at 100 hPa during the early 1940s. In addition to upper-air data, several total ozone series from the 1940s were re-evaluated [Brönnimann et al., QJRMS 129 (2003), 2819], providing further information on the stratosphere. In this paper we present an analysis of these new data sets and compare the results to climate model data. It is demonstrated that the climate anomaly at the ground was accompanied in the lower stratosphere by a weak polar vortex and warm temperatures over the polar region, Eurasia, and the North Pacific. The total ozone data show a peak in 1940-1942 in all available records, at sites as far apart as China, North America, central Europe, and the Arctic. The co-occurrence of warm tropical SSTs (due to El Niño), a weak polar vortex and warm lower stratosphere over polar regions, and a total ozone increase is in agreement with findings by van Loon and Labitzke [Mon. Wea. Rev. 115 (1987), 357]. Using the 290-yr control run of the Community Climate System Model CCSM-2.0 provided by UCAR we show that such large-scale coupling events are related to an exceptionally large difference between tropical and northern-extratropical SSTs such as during strong El Niños. The coupling most likely proceeds through a change in planetary wave activity in the northern extratropics that manifests itself in a strong Aleutian low and a weak Icelandic low and in a disturbance of the polar vortex in the stratosphere. The 1940-1942 climate anomaly is not well known among scientists, but it is unprecedented in strength, yet exemplary in character, providing a unique opportunity to study large-scale climate variability.

The GCOS Reference Upper-Air Network (GRUAN)

NASA Astrophysics Data System (ADS)

Vömel, H.; Berger, F. H.; Immler, F. J.; Seidel, D.; Thorne, P.

2009-04-01

While the global upper-air observing network has provided useful observations for operational weather forecasting for decades, its measurements lack the accuracy and long-term continuity needed for understanding climate change. Consequently, the scientific community faces uncertainty on such key issues as the trends of temperature in the upper troposphere and stratosphere or the variability and trends of stratospheric water vapour. To address these shortcomings, and to ensure that future climate records will be more useful than the records to date, the Global Climate Observing System (GCOS) program initiated the GCOS Reference Upper Air Network (GRUAN). GRUAN will be a network of about 30-40 observatories with a representative sampling of geographic regions and surface types. These stations will provide upper-air reference observations of the essential climate variables, i.e. temperature, geopotential, humidity, wind, radiation and cloud properties using specialized radiosondes and complementary remote sensing profiling instrumentation. Long-term stability, quality assurance / quality control, and a detailed assessment of measurement uncertainties will be the key aspects of GRUAN observations. The network will not be globally complete but will serve to constrain and adjust data from more spatially comprehensive global observing systems including satellites and the current radiosonde networks. This paper outlines the scientific rationale for GRUAN, its role in the Global Earth Observation System of Systems, network requirements and likely instrumentation, management structure, current status and future plans.

ARB 48-inch LIDAR Data and Information

Atmospheric Science Data Center

2015-11-19

... vertical measurements have resulted in a valuable long-term record of the mid-latitude upper tropospheric and stratospheric aerosol. These data have been used in scientific studies such as in studies of volcanic eruptions and in comparisons ...

Antarctic Polar Descent and Planetary Wave Activity Observed in ISAMS CO from April to July 1992

NASA Technical Reports Server (NTRS)

Allen, D. R.; Stanford, J. L.; Nakamura, N.; Lopez-Valverde, M. A.; Lopez-Puertas, M.; Taylor, F. W.; Remedios, J. J.

2000-01-01

Antarctic polar descent and planetary wave activity in the upper stratosphere and lower mesosphere are observed in ISAMS CO data from April to July 1992. CO-derived mean April-to-May upper stratosphere descent rates of 15 K/day (0.25 km/day) at 60 S and 20 K/day (0.33 km/day) at 80 S are compared with descent rates from diabatic trajectory analyses. At 60 S there is excellent agreement, while at 80 S the trajectory-derived descent is significantly larger in early April. Zonal wavenumber 1 enhancement of CO is observed on 9 and 28 May, coincident with enhanced wave 1 in UKMO geopotential height. The 9 May event extends from 40 to 70 km and shows westward phase tilt with height, while the 28 May event extends from 40 to 50 km and shows virtually no phase tilt with height.

In-situ measurements of nitric oxide in the high latitude upper stratosphere

NASA Technical Reports Server (NTRS)

Horvath, J. J.; Frederick, J. E.

1985-01-01

The vertical profiles of nitric acid were measured over Poker Flat, Alaska, in August 1984 and January and February 1985 using a rocket-launched parachute-deployed chemiluminescence sensor. Results for the altitude range 35-45 km indicate a large seasonal variation, with wintertime mixing ratios being a factor of two above summer values. The winter profiles contain sharp positive vertical gradients persisting through the highest altitudes observed. Above the stratopause, the mixing ratio observed in February increases rapidly and between 52 and 53 km reaches 148.9 ppbv, an order of magnitude greater than typical mid-latitude values measured with this instrument. Such behavior is consistent with the idea that nitric oxide produced at greater altitudes reaches the high-latitude upper stratosphere or lower mesosphere in winter. The results support the existence of a vertical coupling between diverse regions of the atmosphere in the high-latitude winter.

Structure of the Upper Troposphere-Lower Stratosphere (UTLS) in GEOS-5

NASA Technical Reports Server (NTRS)

Pawson, Steven

2011-01-01

This study examines the structure of the upper troposphere and lower stratosphere in the GEOS-5 data assimilation system. Near-real time analyses, with a horizontal resolution of one-half or one quarter degree and a vertical resolution of about 1km in the tropopause region are examined with an emphasis on spatial structures at and around the tropopause. The contributions of in-situ observations of temperature and microwave and infrared radiances to the analyses are discussed, with some focus on the interplay between these types of observations. For a historical analysis (Merra) performed with GEOS-5, the impacts of changing observations on the assimilation system are examined in some detail - this documents some aspects of the time dependence of analysis that must be taken into account in the isolation of true geophysical trends. Finally, some sensitivities of the ozone analyses to input data and correlated errors between temperature and ozone are discussed.

Western Pacific Tropospheric Ozone and Potential Vorticity: Implications for Asian Pollution

NASA Technical Reports Server (NTRS)

Browell, Edward V.; Newell, Reginald E.; Davis, Douglas D.; Liu, Shaw C.

1997-01-01

Tropospheric ozone (03) cross sections measured with lidar from a DC-8 aircraft over the western Pacific correspond closely with potential vorticity (PV). Both are transported from the middle latitude stratosphere, although this is not the only source of 03, and both have sinks in the tropical boundary layer. 03 and PV are good indicators of photochemical and transport process interactions. In summer, some Asian pollution, raised by convection to the upper troposphere, passes southward into the tropics and to the Southern Hemisphere. In winter, subsidence keeps the pollution at low altitudes where it moves over the ocean towards the Inter-Tropical Convergence Zone (ITCZ), with photochemical destruction and secondary pollutant generation occurring en route. Convection raises this modified air to the upper troposphere, where some re may enter the stratosphere. Thus winter Asian pollution may at have a smaller direct influence on the global atmosphere than it would if injected at other longitudes and seasons.

The need for accurate long-term measurements of water vapor in the upper troposphere and lower stratosphere with global coverage.

PubMed

Müller, Rolf; Kunz, Anne; Hurst, Dale F; Rolf, Christian; Krämer, Martina; Riese, Martin

2016-02-01

Water vapor is the most important greenhouse gas in the atmosphere although changes in carbon dioxide constitute the "control knob" for surface temperatures. While the latter fact is well recognized, resulting in extensive space-borne and ground-based measurement programs for carbon dioxide as detailed in the studies by Keeling et al. (1996), Kuze et al. (2009), and Liu et al. (2014), the need for an accurate characterization of the long-term changes in upper tropospheric and lower stratospheric (UTLS) water vapor has not yet resulted in sufficiently extensive long-term international measurement programs (although first steps have been taken). Here, we argue for the implementation of a long-term balloon-borne measurement program for UTLS water vapor covering the entire globe that will likely have to be sustained for hundreds of years.

Infrared spectroscopic detection of sulfur hexafluoride (SF6) in the lower stratosphere and upper troposphere

NASA Technical Reports Server (NTRS)

Rinsland, C. P.; Brown, L. R.; Farmer, C. B.

1990-01-01

This paper reports the detection and identification of the unresolved SF6 nu-3 band Q branch at 947.9/cm in high-resolution solar occultation spectra of the lower stratosphere and upper troposphere, which was made from the analysis of data recorded on April 30 to May 1, 1985 by the spaceborne Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer as part of the Spacelab 3 mission. On the basis of SF6 line-by-line parameters obtained from the laboratory studies of Bobin et al. (1987) and Schatz and Hornig (1953), the measured absorption was analyzed to deduce SF6 volume mixing ratios in the altitude range 12-22 km. It was found that, in this altitude range, the SF6 volume mixing ratio is independent of altitude, with an average measured value of 1.42 parts per trillion by volume (pptv) at 31 deg N latitude.

SABER (TIMED) and MLS (UARS) Temperature Observations of Mesospheric and Stratospheric QBO and Related Tidal Variations

NASA Technical Reports Server (NTRS)

Huang, Frank T.; Mayr, Hans G.; Reber, Carl A.; Russell, James; Mlynczak, Marty; Mengel, John

2006-01-01

More than three years of temperature observations from the SABER (TIMED) and MLS WARS) instruments are analyzed to study the annual and inter-annual variations extending from the stratosphere into the upper mesosphere. The SABER measurements provide data from a wide altitude range (15 to 95 km) for the years 2002 to 2004, while the MLS data were taken in the 16 to 55 km altitude range a decade earlier. Because of the sampling properties of SABER and MLS, the variations with local solar time must be accounted for when estimating the zonal mean variations. An algorithm is thus applied that delineates with Fourier analysis the year-long variations of the migrating tides and zonal mean component. The amplitude of the diurnal tide near the equator shows a strong semiannual periodicity with maxima near equinox, which vary from year to year to indicate the influence from the Quasi-biennial Oscillation (QBO) in the zonal circulation. The zonal mean QBO temperature variations are analyzed over a range of latitudes and altitudes, and the results are presented for latitudes from 48"s to 48"N. New results are obtained for the QBO, especially in the upper stratosphere and mesosphere, and at mid-latitudes. At Equatorial latitudes, the QBO amplitudes show local peaks, albeit small, that occur at different altitudes. From about 20 to 40 km, and within about 15" of the Equator, the amplitudes can approach 3S K for the stratospheric QBO or SQBO. For the mesospheric QBO or MQBO, we find peaks near 70 km, with temperature amplitudes reaching 3.5"K, and near 85 km, the amplitudes approach 2.5OK. Morphologically, the amplitude and phase variations derived from the SABER and MLS measurements are in qualitative agreement. The QBO amplitudes tend to peak at the Equator but then increase again pole-ward of about 15" to 20'. The phase progression with altitude varies more gradually at the Equator than at mid-latitudes. A comparison of the observations with results from the Numerical Spectral Model (NSM) reveals that there is qualitative agreement. The NSM generates the QBO extending from the stratosphere into the upper mesosphere, with temperature variations extending to mid latitudes, but the predicted amplitudes are smaller than those observed.

The Evolution of the Stratopause during the 2006 Major Warming: Satellite Data and Assimilated Meteorological Analyses

NASA Technical Reports Server (NTRS)

Manney, Gloria L.; Krueger, Kirstin; Pawson, Steven; Minschwaner, Ken; Schwartz, Michael J.; Daffer, William H.; Livesey, Nathaniel J.; Mlynczak, Martin G.; Remsberg, Ellis E.; Russell, James M., III;

Stratospheric water vapor and ozone evaluation in reanalyses as part of the SPARC Reanalysis Intercomparison Project (S-RIP)

NASA Astrophysics Data System (ADS)

Davis, S. M.; Hegglin, M. I.; Fujiwara, M.; Manney, G. L.; Dragani, R.; Nash, E.; Tegtmeier, S.; Kobayashi, C.; Harada, Y.; Long, C. S.; Wargan, K.; Rosenlof, K. H.

2017-12-01

Reanalyses are widely used to understand atmospheric processes and past variability, and are often used to stand in as "observations" for comparisons with climate model output. Because of the central role of water vapor (WV) and ozone (O3) in climate change, it is important to understand how accurately and consistently these species are represented in existing global reanalyses. Here we present the results of WV and O3 intercomparisons that have been performed as part of the SPARC (Stratosphere-troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The comparisons cover a range of timescales and evaluate both inter-reanalysis and observation-reanalysis differences. The assimilation of total column ozone (TCO) observations in newer reanalyses results in realistic representations of TCO in reanalyses except when data coverage is lacking, such as during polar night. The vertical distribution of ozone is also relatively well represented in the stratosphere in reanalyses, particularly given the relatively weak constraints on ozone vertical structure provided by most assimilated observations and the simplistic representations of ozone photochemical processes in most of the reanalysis forecast models. For times when vertically resolved observations are not assimilated, biases in the vertical distribution of ozone are found in the upper troposphere and lower stratosphere in all reanalyses. In contrast to O3, reanalysis stratospheric WV fields are not directly constrained by assimilated data. Observations of atmospheric humidity are typically used only in the troposphere, below a specified vertical level at or near the tropopause. The fidelity of reanalysis stratospheric WV products is therefore dependent on the reanalyses' representation of processes that influence stratospheric WV, such as tropical tropopause layer temperatures and methane oxidation. The lack of assimilated observations and known deficiencies in the representation of stratospheric transport in reanalyses result in much poorer agreement amongst observational and reanalysis estimates of stratospheric WV. Hence, stratospheric WV products from the current generation of reanalyses should generally not be used in scientific studies.

Using CFC-12 and HCl to quantify the annual cycle of the stratospheric contribution to ozone in the Arctic troposphere

NASA Astrophysics Data System (ADS)

Liang, Q.; Douglass, A. R.; Duncan, B. N.; Stolarski, R. S.; Witte, J. C.

2007-12-01

In this study, we use CFC-12 and hydrochloric acid (HCl) to quantify the annual cycle of stratosphere-to- troposphere transport of O3 to the Arctic troposphere. To do so, we analyze results from a 5-year stratosphere and troposphere simulation from the Global Modeling Initiative (GMI) Chemical Transport Model (CTM) for 1994- 1998 and a 10-year simulation using the GEOS Chemistry Climate Model (GEOS CCM) for 1995-2004. The later includes a tagged CFC-12 tracer to track the transport of aged stratospheric air into the troposphere. We compare the simulated CFC-12 with 10 years surface CFC-12 measurements at two NOAA-GMD sites, Alert and Barrow. We compare O3 with 10 years of ozonesondes at Alert, Eureka, and Resolute. CFC-12, HCl and O3 are all compared with satellite observations from the Advanced Composition Explorer (ACE) and several MkIV balloon measurements in the Arctic. The GEOS CCM and GMI CTM simulations capture well the observed magnitude and annual cycle of CFC-12, HCl, and O3 in the stratosphere and troposphere. Since CFC-12 is emitted at the surface and destroyed in the stratosphere while HCl and O3 are produced in the stratosphere, the stratospheric air shows strong correlation between HCl and O3 and anti-correlation between CFC-12 and O3. We use the CFC-12 tagged tracer to track the transport from the stratosphere to the troposphere and the subsequent transport into the lower troposphere in the Arctic. HCl is paired with O3 to quantify the stratospheric contribution to O3 in the troposphere by applying a scaling factor to the simulated HCl using the HCl-O3 regression ratio. O3 and its annual cycle in the upper troposphere are dominated by stratospheric influence, which peaks in spring. The stratospheric contribution decreases as altitude decreases, accompanied by a delay in the phase of maximum. In the middle troposphere (2-6km), the stratospheric contribution peaks during the summer and is comparable to that of net photochemistry. Due to inefficient transport into the lower Arctic surface, the stratospheric contribution of O3 at the surface accounts for only a few (<5) ppbv.

Multimodel assessment of the upper troposphere and lower stratosphere: Tropics and global trends

NASA Astrophysics Data System (ADS)

Gettelman, A.; Hegglin, M. I.; Son, S.-W.; Kim, J.; Fujiwara, M.; Birner, T.; Kremser, S.; Rex, M.; AñEl, J. A.; Akiyoshi, H.; Austin, J.; Bekki, S.; Braesike, P.; Brühl, C.; Butchart, N.; Chipperfield, M.; Dameris, M.; Dhomse, S.; Garny, H.; Hardiman, S. C.; JöCkel, P.; Kinnison, D. E.; Lamarque, J. F.; Mancini, E.; Marchand, M.; Michou, M.; Morgenstern, O.; Pawson, S.; Pitari, G.; Plummer, D.; Pyle, J. A.; Rozanov, E.; Scinocca, J.; Shepherd, T. G.; Shibata, K.; Smale, D.; TeyssèDre, H.; Tian, W.

2010-01-01

The performance of 18 coupled Chemistry Climate Models (CCMs) in the Tropical Tropopause Layer (TTL) is evaluated using qualitative and quantitative diagnostics. Trends in tropopause quantities in the tropics and the extratropical Upper Troposphere and Lower Stratosphere (UTLS) are analyzed. A quantitative grading methodology for evaluating CCMs is extended to include variability and used to develop four different grades for tropical tropopause temperature and pressure, water vapor and ozone. Four of the 18 models and the multi-model mean meet quantitative and qualitative standards for reproducing key processes in the TTL. Several diagnostics are performed on a subset of the models analyzing the Tropopause Inversion Layer (TIL), Lagrangian cold point and TTL transit time. Historical decreases in tropical tropopause pressure and decreases in water vapor are simulated, lending confidence to future projections. The models simulate continued decreases in tropopause pressure in the 21st century, along with ˜1K increases per century in cold point tropopause temperature and 0.5-1 ppmv per century increases in water vapor above the tropical tropopause. TTL water vapor increases below the cold point. In two models, these trends are associated with 35% increases in TTL cloud fraction. These changes indicate significant perturbations to TTL processes, specifically to deep convective heating and humidity transport. Ozone in the extratropical lowermost stratosphere has significant and hemispheric asymmetric trends. O3 is projected to increase by nearly 30% due to ozone recovery in the Southern Hemisphere (SH) and due to enhancements in the stratospheric circulation. These UTLS ozone trends may have significant effects in the TTL and the troposphere.

Modelling trends in tropical column ozone with the UKCA chemistry-climate model

NASA Astrophysics Data System (ADS)

Keeble, James; Bednarz, Ewa; Banerjee, Antara; Abraham, Luke; Harris, Neil; Maycock, Amanda; Pyle, John

2016-04-01

Trends in tropical column ozone under a number of different emissions scenarios are explored with the UM-UKCA coupled chemistry climate model. A transient 1960-2100 simulation was run following the RCP6 scenario. Tropical averaged (10S-10N) total column ozone values decrease from the 1970s, reaching a minimum around 2000, and return to their 1980 values around 2040, consistent with the use and emission of ozone depleting substances, and their later controls under the Montreal Protocol. However, when the total column is subdivided into three partial columns, extending from the surface to the tropopause, the tropopause to 30km, and 30km to 50km, significant differences to the total column trend are seen. Modelled tropospheric column values increase from 1960-2000 before remaining steady throughout the 21st Century. Lower stratospheric column values decrease rapidly from 1960-2000, remain steady until 2050 before slowly decreasing to 2100, never recovering to their 1980s values. Upper stratospheric values decrease from 1960-2000, before rapidly increasing throughout the 21st Century, recovering to 1980s values by ~2020 and are significantly increased above the 1980s values by 2100. Using a series of idealised model simulations with varying concentrations of greenhouse gases and ozone depleting substances, we assess the physical processes driving the partial column response in the troposphere, lower stratosphere and upper stratosphere, and assess how these processes change under different emissions scenarios. Finally, we present a simple, linearised model for predicting tropical column ozone values based on greenhouse gas and ozone depleting substance scenarios.

A dynamical perspective on the energetic particles precipitation-middle atmosphere interaction

NASA Astrophysics Data System (ADS)

Karami, Khalil; Sinnhuber, Miriam; Versick, Stefan; Braesicke, Peter

2015-04-01

Energetic particles including protons, electrons and heavier ions, enter the Earth's atmosphere over polar region of both hemispheres, where the geomagnetic lines are considered to be open and connected to the interplanetary medium. This condition allows direct access for energetic particles of solar or galactic origin to directly deposit their own energy into the middle and upper atmosphere. Such particle precipitations can greatly disturb the chemical composition of the upper and middle atmosphere. At polar latitudes, these particles have the potential to penetrate from thermosphere deep into the mesosphere and in rare occasions into the stratosphere. The most important are changes to the budget of atmospheric nitric oxides, NOy, and to atmospheric reactive hydrogen oxides, HOx, which both contribute to ozone loss in the stratosphere and mesosphere. The chemistry-climate general circulation model ECHAM5/MESSy is used to investigate the impact of changed ozone concentration due to energetic particles precipitation on temperatures and wind fields. The simulated anomalies of both zonal mean temperature and zonal wind suggest that these changes are very unlikely to be caused in situ by ozone depletion and indirect dynamical condition is important. The results of our simulations suggests that ozone perturbation is a starting point for a chain of processes resulting in temperature and circulation changes in many areas of the atmosphere. Different dynamical analysis (e.g., frequency of sudden stratospheric warming, dates of stratospheric final warming, divergence of Eliassen-Palm flux and refractive index of planetary waves) are performed to investigate the impact of ozone anomaly originated from high energetic particle precipitation on middle atmospheric temperature and circulation.

Rate coefficient measurements for the ClO radical self-reaction as a function of pressure and temperature

NASA Astrophysics Data System (ADS)

Burkholder, J. B.; Feierabend, K.

2010-12-01

Halogen chemistry plays an important role in polar stratospheric ozone loss. The ClO dimer (Cl2O2) catalytic ozone destruction cycle accounts for the vast majority of winter/spring polar stratospheric ozone loss. A key step in the dimer catalytic cycle is the pressure and temperature dependent self-reaction of the ClO radical. The rate coefficient for the ClO self-reaction has been measured in previous laboratory studies but uncertainties persist, particularly at atmospherically relevant temperatures and pressures. In this laboratory study, rate coefficients for the ClO self-reaction were measured over a range of temperature (200 - 296 K) and pressure (50 - 600 Torr, He and N2 bath gases). ClO radicals were produced by pulsed laser photolysis of Cl2O at 248 nm. The ClO radical temporal profile was measured using dual wavelength cavity ring-down spectroscopy (CRDS) near 280 nm. The absolute ClO radical concentration was determined using the ClO UV absorption cross sections and their temperature dependence measured as part of this work. The results from this work will be compared with previous studies and the discrepancies discussed. Possible explanations for deviations of the reaction rate coefficient from the simple Falloff kinetic behavior currently recommended for use in atmospheric model calculations will be discussed.

Stratospheric O3 changes during 2001-2010: The small role of solar flux variations in a CTM

NASA Astrophysics Data System (ADS)

Dhomse, Sandip; Chipperfield, Martyn; Feng, Wuhu; Ball, William; Unruh, Yvonne; Haigh, Joanna; Krivova, Natalie; Solanki, Sami

2013-04-01

Solar spectral fluxes (or irradiance) measured by the SOlar Radiation and Climate Experiment (SORCE) shows different variability at ultraviolet (UV) wavelengths compared to other irradiance measurements and models (e.g. NRL, SATIRE-S). Some modelling studies have suggested that stratospheric O3 changes during solar cycle 23 (1996-2008) can only be reproduced if SORCE solar fluxes are used. We have used a 3-D chemical transport model (CTM), forced by meteorology from the European Centre for Medium-Range Weather Forecasts (ECMWF), to simulate stratospheric O3 using 3 different solar flux datasets (SORCE, NRL-SSI and SATIRE-S). Simulated O3 changes are compared with Microwave Limb Sounder (MLS) and Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite data. Modelled O3 anomalies using all solar flux datasets show good agreement with the observations, despite the different flux variations. A notable feature during this period is a robust positive solar signal in the tropical middle stratosphere. The CTM reproduces these changes through dynamical information contained in the analyses. Changes in the upper stratosphere cannot be used to discriminate between solar flux datasets due to large uncertainties in the O3 observations. Overall this study suggests that the UV variations detected by SORCE are not necessary to reproduce observed stratospheric O3 changes during 2001-2010.

Interhemispheric differences in polar stratospheric HNO3, H2O, ClO, and O3

NASA Technical Reports Server (NTRS)

Santee, M. L.; Read, W. G.; Waters, J. W.; Froidevaux, L.; Manney, G. L.; Flower, D. A.; Jarnot, R. F.; Harwood, R. S.; Peckham, G. E.

1995-01-01

Simultaneous global measurements of nitric acid (HNO3), water (H2O), chlorine monoxide (ClO), and ozone (O3) in the stratosphere have been obtained over complete annual cycles in both hemispheres by the Microwave Limb Sounder on the Upper Atmosphere Research Satellite. A sizeable decrease in gas-phase HNO3 was evident in the lower stratospheric vortex over Antarctica by early June 1992, followed by a significant reduction in gas-phase H2O after mid-July. By mid-August, near the time of peak ClO, abundances of gas-phase HNO3 and H2O were extremely low. The concentrations of HNO3 and H2O over Antarctica remained depressed into November, well after temperatures in the lower stratosphere had risen above the evaporation threshold for polar stratospheric clouds, implying that denitrification and dehydration had occurred. No large decreases in either gas-phase HNO3 or H2O were observed in the 1992-1993 Arctic winter vortex. Although ClO was enhanced over the Arctic as it was over the Antarctic, Arctic O3 depletion was substantially smaller than that over Antarctica. A major factor currently limiting the formation of an Arctic ozone 'hole' is the lack of denitrification in the northern polar vortex, but future cooling of the lower stratosphere could lead to more intense denitrification and consequently larger losses of Arctic ozone.

ENSO effects on stratospheric ozone: A nudged model perspective

NASA Astrophysics Data System (ADS)

Braesicke, Peter; Kirner, Oliver; Versick, Stefan; Joeckel, Patrick

2015-04-01

The El Niño/Southern Oscillation (ENSO) phenomenon is an important pacemaker for interannual variability in the Earth's atmosphere. ENSO impacts on ozone have been observed and modelled for the stratosphere and the troposphere. It is well recognized that attribution of ENSO variability is important for trend detection. ENSO impacts in low latitudes are easier to detect, because the response emerges close (temporally and spatially) to the forcing. Moving from low to high latitudes it becomes increasingly difficult to isolate ENSO driven variability, due to time-lags involved and many other modes of variability playing a role as well. Here, we use a nudged version of the EMAC chemistry-climate model to evaluate ENSO impacts on ozone over the last 35 years. In the nudged mode configuration EMAC is not entirely free running. The tropospheric meteorology is constrained using ERA-Interim data. Only the upper stratosphere and the composition (including ozone) are calculated without additional observational constraints. Using lagged correlations and supported by additional idealised modelling, we describe the ENSO impact on tropospheric and stratospheric ozone in the EMAC system. We trace the ENSO signal from the tropical lower troposphere to the polar lower and middle stratosphere. Instead of distinguishing tropospheric and stratospheric responses, we present a coherent approach detecting the ENSO signal as a function of altitude, latitude and time, and demonstrate how a concise characterisation of the ENSO impact aids improved trend detection.

The molecular physics of photolytic fractionation of sulfur and oxygen isotopes in planetary atmospheres (Invited)

NASA Astrophysics Data System (ADS)

Johnson, M. S.; Schmidt, J. A.; Hattori, S.; Danielache, S.; Meusinger, C.; Schinke, R.; Ueno, Y.; Nanbu, S.; Kjaergaard, H. G.; Yoshida, N.

2013-12-01

Atmospheric photochemistry is able to produce large mass independent anomalies in atmospheric trace gases that can be found in geological and cryospheric records. This talk will present theoretical and experimental investigations of the molecular mechanisms producing photolytic fractionation of isotopes with special attention to sulfur and oxygen. The zero point vibrational energy (ZPE) shift and reflection principle theories are starting points for estimating isotopic fractionation, but these models ignore effects arising from isotope-dependent changes in couplings between surfaces, excited state dynamics, line densities and hot band populations. The isotope-dependent absorption spectra of the isotopologues of HCl, N2O, OCS, CO2 and SO2 have been examined in a series of papers and these results are compared with experiment and ZPE/reflection principle models. Isotopic fractionation in planetary atmospheres has many interesting applications. The UV absorption of CO2 is the basis of photochemistry in the CO2-rich atmospheres of the ancient Earth, and of Mars and Venus. For the first time we present accurate temperature and isotope dependent CO2 absorption cross sections with important implications for photolysis rates of SO2 and H2O, and the production of a mass independent anomaly in the Ox reservoir. Experimental and theoretical results for OCS have implications for the modern stratospheric sulfur budget. The absorption bands of SO2 are complex with rich structure producing isotopic fractionation in photolysis and photoexcitation.

Nitrogen oxides in the arctic stratosphere: Implications for ozone abundances. Ph.D. Thesis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Slusser, J.R.

1994-01-01

In the high latitude winter stratosphere, NO2 sequesters chlorine compounds which are extremely efficient at destroying ozone. During the nighttime, NO2 reacts with ozone to form N2O5 which acts as a reservoir of NO2. Under heavy aerosol loading, N2O5 may react with water on aerosol surfaces to form HNO3, a reservoir more resistant to photolysis. This heterogeneous reaction results in reduced NO2 concentration when the sun returns at the end of the winter. A spectrograph system has been developed to measure scattered zenith skylight and thereby determine stratospheric NO2 slant column abundance. Conversion of the measured slant column abundance tomore » vertical column abundance requires dividing by the air mass. The air mass is the enhancement in the optical path for the scattered twilight as compared to a vertical path. Air mass values determined using a multiple scattering radiative transfer code have been compared to those derived using a Monte Carlo code and were found to agree to within 6% at a 90 deg solar zenith angle for a stratospheric absorber. Six months of NO2 vertical column abundance measured over Fairbanks during the winter 1992-93 exhibited the daylight diminished and increased as the sunlight hours lengthened. The overall seasonal behavior was similar to high-latitude measurements made in the Southern Hemisphere. The ratios of morning to evening column abundance were consistent with predictions based on gas-phase chemistry. The possible heterogeneous reaction of N2O5 on sulfate aerosols was investigated using FTIR Spectrometer measurements of HNO3 column abundance and lidar determinations of the aerosol profile. Using an estimated N2O5 column abundance and aerosol profile as input to a simple model, significant HNO3 production was expected. No increase in HNO3 column abundance was measured. From this set of data, it was not possible to determine whether significant amounts of N2O5 were converted to HNO3 by this heterogeneous reaction.« less

Assessing the long-term variability of acetylene and ethane in the stratosphere of Jupiter

NASA Astrophysics Data System (ADS)

Melin, Henrik; Fletcher, L. N.; Donnelly, P. T.; Greathouse, T. K.; Lacy, J. H.; Orton, G. S.; Giles, R. S.; Sinclair, J. A.; Irwin, P. G. J.

2018-05-01

Acetylene (C2H2) and ethane (C2H6) are both produced in the stratosphere of Jupiter via photolysis of methane (CH4). Despite this common source, the latitudinal distribution of the two species is radically different, with acetylene decreasing in abundance towards the pole, and ethane increasing towards the pole. We present six years of NASA IRTF TEXES mid-infrared observations of the zonally-averaged emission of methane, acetylene and ethane. We confirm that the latitudinal distributions of ethane and acetylene are decoupled, and that this is a persistent feature over multiple years. The acetylene distribution falls off towards the pole, peaking at ∼ 30°N with a volume mixing ratio (VMR) of ∼ 0.8 parts per million (ppm) at 1 mbar and still falling off at ± 70° with a VMR of ∼ 0.3 ppm. The acetylene distributions are asymmetric on average, but as we move from 2013 to 2017, the zonally-averaged abundance becomes more symmetric about the equator. We suggest that both the short term changes in acetylene and its latitudinal asymmetry is driven by changes to the vertical stratospheric mixing, potentially related to propagating wave phenomena. Unlike acetylene, ethane has a symmetric distribution about the equator that increases toward the pole, with a peak mole fraction of ∼ 18 ppm at about ± 50° latitude, with a minimum at the equator of ∼ 10 ppm at 1 mbar. The ethane distribution does not appear to respond to mid-latitude stratospheric mixing in the same way as acetylene, potentially as a result of the vertical gradient of ethane being much shallower than that of acetylene. The equator-to-pole distributions of acetylene and ethane are consistent with acetylene having a shorter lifetime than ethane that is not sensitive to longer advective timescales, but is augmented by short-term dynamics, such as vertical mixing. Conversely, the long lifetime of ethane allows it to be transported to higher latitudes faster than it can be chemically depleted.

Evaluation of the Ozone Fields in NASA's MERRA-2 Reanalysis

NASA Technical Reports Server (NTRS)

Wargan, Krzysztof; Labow, Gordon; Frith, Stacey; Pawson, Steven; Livesey, Nathaniel; Partyka, Gary

2017-01-01

We describe and assess the quality of the assimilated ozone product from the Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2) produced at NASAs Global Modeling and Assimilation Office (GMAO) spanning the time period from 1980 to present. MERRA-2 assimilates partial column ozone retrievals from a series of Solar Backscatter Ultraviolet (SBUV) radiometers on NASA and NOAA spacecraft between January 1980 and September 2004; starting in October 2004 retrieved ozone profiles from the Microwave Limb Sounder (MLS) and total column ozone from the Ozone Monitoring Instrument on NASAs EOS Aura satellite are assimilated. We compare the MERRA-2 ozone with independent satellite and ozonesonde data focusing on the representation of the spatial and temporal variability of stratospheric and upper tropospheric ozone and on implications of the change in the observing system from SBUV to EOS Aura. The comparisons show agreement within 10 (standard deviation of the difference) between MERRA-2 profiles and independent satellite data in most of the stratosphere. The agreement improves after 2004 when EOS Aura data are assimilated. The standard deviation of the differences between the lower stratospheric and upper tropospheric MERRA-2 ozone and ozonesondes is 11.2 and 24.5, respectively, with correlations of 0.8 and above, indicative of a realistic representation of the near-tropopause ozone variability in MERRA-2. The agreement improves significantly in the EOS Aura period, however MERRA-2 is biased low in the upper troposphere with respect to the ozonesondes. Caution is recommended when using MERRA-2 ozone for decadal changes and trend studies.

Evaluation of the Ozone Fields in NASA’s MERRA-2 Reanalysis

PubMed Central

Wargan, Krzysztof; Labow, Gordon; Frith, Stacey; Pawson, Steven; Livesey, Nathaniel; Partyka, Gary

2018-01-01

We describe and assess the quality of the assimilated ozone product from the Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2) produced at NASA’s Global Modeling and Assimilation Office (GMAO) spanning the time period from 1980 to present. MERRA-2 assimilates partial column ozone retrievals from a series of Solar Backscatter Ultraviolet (SBUV) radiometers on NASA and NOAA spacecraft between January 1980 and September 2004; starting in October 2004 retrieved ozone profiles from the Microwave Limb Sounder (MLS) and total column ozone from the Ozone Monitoring Instrument on NASA’s EOS Aura satellite are assimilated. We compare the MERRA-2 ozone with independent satellite and ozonesonde data focusing on the representation of the spatial and temporal variability of stratospheric and upper tropospheric ozone and on implications of the change in the observing system from SBUV to EOS Aura. The comparisons show agreement within 10 % (standard deviation of the difference) between MERRA-2 profiles and independent satellite data in most of the stratosphere. The agreement improves after 2004 when EOS Aura data are assimilated. The standard deviation of the differences between the lower stratospheric and upper tropospheric MERRA-2 ozone and ozonesondes is 11.2 % and 24.5 %, respectively, with correlations of 0.8 and above, indicative of a realistic representation of the near-tropopause ozone variability in MERRA-2. The agreement improves significantly in the EOS Aura period, however MERRA-2 is biased low in the upper troposphere with respect to the ozonesondes. Caution is recommended when using MERRA-2 ozone for decadal changes and trend studies. PMID:29527096

Evaluation of the Ozone Fields in NASA's MERRA-2 Reanalysis.

PubMed

Wargan, Krzysztof; Labow, Gordon; Frith, Stacey; Pawson, Steven; Livesey, Nathaniel; Partyka, Gary

2017-04-01

We describe and assess the quality of the assimilated ozone product from the Modern-Era Retrospective Analysis for Research and Applications, Version 2 (MERRA-2) produced at NASA's Global Modeling and Assimilation Office (GMAO) spanning the time period from 1980 to present. MERRA-2 assimilates partial column ozone retrievals from a series of Solar Backscatter Ultraviolet (SBUV) radiometers on NASA and NOAA spacecraft between January 1980 and September 2004; starting in October 2004 retrieved ozone profiles from the Microwave Limb Sounder (MLS) and total column ozone from the Ozone Monitoring Instrument on NASA's EOS Aura satellite are assimilated. We compare the MERRA-2 ozone with independent satellite and ozonesonde data focusing on the representation of the spatial and temporal variability of stratospheric and upper tropospheric ozone and on implications of the change in the observing system from SBUV to EOS Aura. The comparisons show agreement within 10 % (standard deviation of the difference) between MERRA-2 profiles and independent satellite data in most of the stratosphere. The agreement improves after 2004 when EOS Aura data are assimilated. The standard deviation of the differences between the lower stratospheric and upper tropospheric MERRA-2 ozone and ozonesondes is 11.2 % and 24.5 %, respectively, with correlations of 0.8 and above, indicative of a realistic representation of the near-tropopause ozone variability in MERRA-2. The agreement improves significantly in the EOS Aura period, however MERRA-2 is biased low in the upper troposphere with respect to the ozonesondes. Caution is recommended when using MERRA-2 ozone for decadal changes and trend studies.

Simulations of the Boreal Winter Upper Mesosphere and Lower Thermosphere With Meteorological Specifications in SD-WACCM-X

NASA Astrophysics Data System (ADS)

Sassi, Fabrizio; Siskind, David E.; Tate, Jennifer L.; Liu, Han-Li; Randall, Cora E.

2018-04-01

We investigate the benefit of high-altitude nudging in simulations of the structure and short-term variability of the upper mesosphere and lower thermosphere (UMLT) dynamical meteorology during boreal winter, specifically around the time of the January 2009 sudden stratospheric warming. We compare simulations using the Specified Dynamics, Whole Atmosphere Community Climate Model, extended version, nudged using atmospheric specifications generated by the Navy Operational Global Atmospheric Prediction System, Advanced Level Physics High Altitude. Two sets of simulations are carried out: one uses nudging over a vertical domain from 0 to 90 km; the other uses nudging over a vertical domain from 0 to 50 km. The dynamical behavior is diagnosed from ensemble mean and standard deviation of winds, temperature, and zonal accelerations due to resolved and parameterized waves. We show that the dynamical behavior of the UMLT is quite different in the two experiments, with prominent differences in the structure and variability of constituent transport. We compare the results of our numerical experiments to observations of carbon monoxide by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer to show that the high-altitude nudging is capable of reproducing with high fidelity the observed variability, and traveling planetary waves are a crucial component of the dynamics. The results of this study indicate that to capture the key physical processes that affect short-term variability (defined as the atmospheric behavior within about 10 days of a stratospheric warming) in the UMLT, specification of the atmospheric state in the stratosphere alone is not sufficient, and upper atmospheric specifications are needed.

Measurements of upper atmosphere water vapor made in situ with a new moisture sensor

NASA Technical Reports Server (NTRS)

Chleck, D.

1979-01-01

A new thin-film aluminum oxide sensor, Aquamax II, has been developed for the measurement of stratospheric and upper tropospheric water vapor levels. The sensor is briefly described with attention given to its calibration and performance. Data obtained from six balloon flights are presented; almost all the results show a constant water vapor mixing ratio, in agreement with other data from midlatitude regions.

Observed Temporal Evolution of Global Mean Age of Stratospheric Air for the 2002 to 2010 Period

NASA Astrophysics Data System (ADS)

Stiller, G. P.; von Clarmann, T.; Haenel, F.; Funke, B.; Glatthor, N.; Grabowski, U.; Kellmann, S.; Kiefer, M.; Linden, A.; Lossow, S.; Lopez-Puertas, M.

2011-12-01

According to model calculations, the meridional circulation is expected to intensify as a result of climate change, and mean age of stratospheric air is expected to decrease. However, an observational data set presented recently (Engel et al., 2009) and consisting of 27 balloon samples of the age of air tracers carbon dioxide and sulfur hexafluoride covering the years 1975 to 2005 did not confirm the model predictions. As a contribution to the ongoing discussion, an extensive observational data set, consisting of more than 1 Million SF6 vertical profiles distributed globally is presented here. It has been derived from the MIPAS instrument covering the period 2002 to 2010 and has been converted into mean age of stratospheric air by referring to a combined data set of in-situ and flask global mean tropospheric SF6 measurements provided by NOAA/ESRL. During conversion into age of air, the non-linearity of tropospheric SF6 increase has been corrected for by convolution with the age spectrum within an iterative approach. Monthly zonal means of mean age of air, binned at 10 deg latitude and 1-2 km altitude, were analyzed with respect to their temporal variation by fitting a regression model consisting of a constant and a linear increase term, 2 proxies for the QBO variation, sinusoidal terms for the seasonal and semi-annual variation and overtones for the correction of the shapes to the observed data set. The impact of subsidence of mesospheric SF6-depleted air and in-mixing into non-polar latitudes on mid-latitudinal absolute age of air and the age-of-air linear increase was assessed and found to be small. The linear increase of mean age of stratospheric air was found to be positive and partly larger than the trend derived by Engel et al. (2009) for most of the Northern mid-latitudes, the middle stratosphere in the tropics, and parts of the Southern mid-latitudes, as well as for the Southern polar upper stratosphere. Multi-year decrease of age of air was found for the lowermost and the upper stratospheric tropics, for parts of Southern mid-latitudes, and for the Northern polar regions. Analysis of the amplitudes and phases of the seasonal variation shed light on the coupling of stratospheric regions to each other. In particular, the Northern mid-latitude stratosphere is well coupled to the tropics, while the Northern lowermost mid-latitudinal stratosphere is decoupled, confirming the separation of the shallow branch of the Brewer-Dobson circulation from the deep branch. We suggest an overall increased tropical upwelling, together with weakening of mixing barriers, especially in the Northern hemisphere, as a hypothetical model to explain the observed pattern of linear multi-year increase/decrease, and amplitudes and phase shifts of the seasonal variation. Reference: Engel, A., Möbius, T., Bönisch, H., Schmidt, U., Heinz, R., Levin, I., Atlas, E., Aoki, S., Nakazawa, T., Sugawara, S., Moore, F., Hurst, D., Elkins, J., Schauffler, S., Andrews, A., and Boering, K.: Age of stratospheric air unchanged within uncertainties over the past 30 years, Nature Geosci., 2, 28--31, doi:10.1038/ngeo388, 2009.

EOF analysis of COSMIC observations on the global zonal mean temperature structure of the Upper Troposphere and Lower Stratosphere from 2007 to 2013

NASA Astrophysics Data System (ADS)

Salinas, Cornelius Csar Jude H.; Chang, Loren C.

2018-06-01

This work presents the results of a Conventional Empirical Orthogonal Function Analysis on daily global zonal mean temperature profiles in the Upper Troposphere and Lower Stratosphere (15-35 km), as measured by the FORMOSAT-3/COSMIC mission from January 2007 to June 2013. For validation, results were compared with ERA-Interim reanalysis. Results show that, the leading global EOF mode (27%) from COSMIC is consistent with temperature anomalies due to the tropical cooling associated with boreal winter Sudden Stratospheric Warmings (SSW). The second global EOF mode from COSMIC (15.3%) is consistent with temperature anomalies due to the Quasi-biennial Oscillation (QBO). The third global mode from COSMIC (10.9%) is consistent with temperature anomalies due to the El Nino Southern Oscillation. This work also shows that the second northern hemisphere EOF mode from COSMIC (16.8%) is consistent with temperature anomalies due Rossby-wave breaking (RWB) which is expected to only be resolved by a high vertical and temporal resolution dataset like COSMIC. Our work concludes that the use of a high vertical and temporal resolution dataset like COSMIC yields non-seasonal EOF modes that are consistent with relatively more intricate temperature anomalies due to the SSW, QBO, ENSO and RWB.

Nitrous Oxide In The Antarctic Stratosphere

NASA Technical Reports Server (NTRS)

Podolske, J. R.; Loewenstein, M.; Strahan, S. E.; Chan, K. R.

1991-01-01

Paper reports on measurements of nitrous oxide (N2O) in upper atmosphere of Southern Hemisphere, made by tunable-laser absorption spectrometer on airplane. Measurements fill gap in information about distribution of N2O over Antarctic while ozone hole forming.

The Diurnal Variation of Hydrogen, Nitrogen, and Chlorine Radicals: Implications for the Heterogeneous Production of HNO2

NASA Technical Reports Server (NTRS)

Salawitch, R. J.; Wofsy, S. C.; Wennberg, P. O.; Cohen, R. C.; Anderson, J. G.; Fahey, D. W.; Gao, R. S.; Keim, E. R.; Woodbridge, E. L.; Stimpfle, R. M.;

Does shortwave absorption by methane influence its effectiveness?

NASA Astrophysics Data System (ADS)

Modak, Angshuman; Bala, Govindasamy; Caldeira, Ken; Cao, Long

2018-01-01

In this study, using idealized step-forcing simulations, we examine the effective radiative forcing of CH4 relative to that of CO2 and compare the effects of CH4 and CO2 forcing on the climate system. A tenfold increase in CH4 concentration in the NCAR CAM5 climate model produces similar long term global mean surface warming ( 1.7 K) as a one-third increase in CO2 concentration. However, the radiative forcing estimated for CO2 using the prescribed-SST method is 81% that of CH4, indicating that the efficacy of CH4 forcing is 0.81. This estimate is nearly unchanged when the CO2 physiological effect is included in our simulations. Further, for the same long-term global mean surface warming, we simulate a smaller precipitation increase in the CH4 case compared to the CO2 case. This is because of the fast adjustment processes—precipitation reduction in the CH4 case is larger than that of the CO2 case. This is associated with a relatively more stable atmosphere and larger atmospheric radiative forcing in the CH4 case which occurs because of near-infrared absorption by CH4 in the upper troposphere and lower stratosphere. Within a month after an increase in CH4, this shortwave heating results in a temperature increase of 0.8 K in the lower stratosphere and upper troposphere. In contrast, within a month after a CO2 increase, longwave cooling results in a temperature decrease of 3 K in the stratosphere and a small change in the upper troposphere. These fast adjustments in the lower stratospheric and upper tropospheric temperature, along with the adjustments in clouds in the troposphere, influence the effective radiative forcing and the fast precipitation response. These differences in fast climate adjustments also produce differences in the climate states from which the slow response begins to evolve and hence they are likely associated with differing feedbacks. We also find that the tropics and subtropics are relatively warmer in the CH4 case for the same global mean surface warming because of a larger longwave clear-sky and shortwave cloud forcing over these regions in the CH4 case. Further investigation using a multi-model intercomparison framework would permit an assessment of the robustness of our results.

Diagnostic Comparison of Meteorological Analyses during the 2002 Antarctic Winter

NASA Technical Reports Server (NTRS)

Manney, Gloria L.; Allen, Douglas R.; Kruger, Kirstin; Naujokat, Barbara; Santee, Michelle L.; Sabutis, Joseph L.; Pawson, Steven; Swinbank, Richard; Randall, Cora E.; Simmons, Adrian J.;

The impact of cut-off lows on ozone in the upper troposphere and lower stratosphere over Changchun from ozonesonde observations

NASA Astrophysics Data System (ADS)

Song, Yushan; Lü, Daren; Li, Qian; Bian, Jianchun; Wu, Xue; Li, Dan

2016-02-01

In situ measurements of the vertical structure of ozone were made in Changchun (43.53°N, 125.13°E), China, by the Institute of Atmosphere Physics, in the summers of 2010-13. Analysis of the 89 validated ozone profiles shows the variation of ozone concentration in the upper troposphere and lower stratosphere (UTLS) caused by cut-off lows (COLs) over Changchun. During the COL events, an increase of the ozone concentration and a lower height of the tropopause are observed. Backward simulations with a trajectory model show that the ozone-rich airmass brought by the COL is from Siberia. A case study proves that stratosphere-troposphere exchange (STE) occurs in the COL. The ozone-rich air mass transported from the stratosphere to the troposphere first becomes unstable, then loses its high ozone concentration. This process usually happens during the decay stage of COLs. In order to understand the influence of COLs on the ozone in the UTLS, statistical analysis of the ozone profiles within COLs, and other profiles, are employed. The results indicate that the ozone concentrations of the in-COL profiles are significantly higher than those of the other profiles between ±4 km around the tropopause. The COLs induce an increase in UTLS column ozone by 32% on average. Meanwhile, the COLs depress the lapse-rate tropopause (LRT)/dynamical tropopause height by 1.4/1.7 km and cause the atmosphere above the tropopause to be less stable. The influence of COLs is durable because the increased ozone concentration lasts at least one day after the COL has passed over Changchun. Furthermore, the relative coefficient between LRT height and lower stratosphere (LS) column ozone is -0.62, which implies a positive correlation between COL strength and LS ozone concentration.

Modeling the effects of UV variability and the QBO on the troposphere-stratosphere system. Part II: The troposphere

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rind, D.; Balachandran, N.K.

1995-08-01

Results of experiments with a GCM involving changes in UV input ({plus_minus} 25%, {plus_minus}5% at wavelengths below 0.3 {mu}) and simulated equatorial QBO are presented, with emphasis on the tropospheric response. The QBO and UV changes alter the temperature in the lower stratosphere/upper troposphere warms, tropospheric eddy energy is reduced, leading to extratropical tropospheric cooling of some 0.5{degrees}C on the zonal average, and surface temperature changes up to {plus_minus}5{degrees}C locally. Opposite effects occur when the extratropical lower stratosphere/upper troposphere cools. Cooling or warming of the comparable region in the Tropics decreases/increases static stability, accelerating/decelerating the Hadley circulation. Tropospheric dynamical changesmore » are on the order of 5%. The combined UV/QBO effect in the troposphere results from its impact on the middle atmosphere; in the QBO east phase, more energy is refracted to higher latitudes, due to the increased horizontal shear of the zonal wind, but with increased UV, this energy propagates preferentially out of the polar lower stratosphere, in response to the increased vertical shear of the zonal winds; therefore, it is less effective in warming the polar lower stratosphere. Due to their impacts on planetary wave generation and propagation, all combinations of UV and QBO phases affect the longitudinal patterns of tropospheric temperatures and geopotential heights. The modeled perturbations often agree qualitatively with observations and are of generally similar orders of magnitude. The results are sensitive to the forcing employed. In particular, the nature of the tropospheric response depends upon the magnitude (and presumably wavelength) of the solar irradiance perturbation. The results of the smaller UV variations ({plus_minus}5%) are more in agreement with observations, showing clear differences between the UV impact in the east and west QBO phase. 34 refs., 15 figs., 3 tabs.« less

Establishing the Dependence of [HO2]/[OH] on Temperature, Halogen Loading, O3, and NO(x) Based on in Situ Measurements from the NASA ER-2

NASA Technical Reports Server (NTRS)

Lanzendorf, E. J.; Hanisco, T. F.; Wennberg, P. O.; Cohen, R. C.; Stimpfle, R. M.; Anderson, J. G.; Gao, R. S.; Margitan, J. J.; Bui, T. P.

2001-01-01

In situ observations of OH and HO2 from the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA), Stratospheric TRacers of Atmospheric Transport (STRAT), and Polar Ozone Loss in the Arctic Region in Summer (POLARIS) NASA ER-2 field campaigns are used to examine the partitioning of HO(x) in the lower stratosphere (tropopause to approx.21 km) and upper troposphere (approx.10 km to tropopause). These measurements span a latitude range from 70degS to 90degN and a variety of atmospheric conditions as a result of seasonal changes and altitude. The response of the observed [HO2]/[OH] to changes in temperature, [03], [CO], [NO], [CIO], and [BrO] is investigated. The measured ratio is accurately described (approx.+/-10%) by a steady-state model constrained by the measured mixing ratios of O3, CO, NO, CIO, and BrO, where the model is valid for conditions of HO(x) cycling much faster than HO(x) production and loss. The concentration of HO2 depends on [OH], which, to first order, has been observed to be a simple function of the solar zenith angle in the lower stratosphere. The partitioning between OH and HO2 is controlled by the local chemistry between the HO, radicals and O3, CO, NO, CIO, and BrO. The response of [HO(x)] to changes in [NO(x)] and [O3] is demonstrated. Further observations are necessary to illustrate the response of HO(x) to changes in halogen concentrations. A quantitative understanding of [HO2]/[OH] is important, since many of the reactions that control this ratio are directly involved in catalytic removal of O3 in the lower stratosphere and production of O3 in the upper troposphere.

Nitrous oxide in the tropical middle atmosphere, observed by ground-based mm-wave spectrometry

NASA Technical Reports Server (NTRS)

Connor, Brian J.; De Zafra, R. L.; Solomon, P. M.; Parrish, Solomon A.; Barrett, J. W.

1987-01-01

Measurements of stratospheric N2O were made from Mauna Kea in Hawaii in June 1983, and in May and June 1986, by observing thermal emission of the molecule in a rotational transition at about 1 mm wavelength. Analyses of the data yield altitude profiles in the middle and upper stratosphere. Useful measurements of N2O may be made in one to two hours. The N2O profiles agree reasonably well with model predictions and with published satellite data, though significantly more N2O is reported near the stratopause than shown by the satellite measurement, and significantly more N2O in the middle stratosphere than in one of the models. The discrepancy between these data and the satellite measurement may be due in part to variations induced by the solar cycle.

Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

NASA Technical Reports Server (NTRS)

Perkins, P. J.; Papathakos, L. C.

1977-01-01

The Global Atmospheric Sampling Program (GASP) by NASA is collecting and analyzing data on gaseous and aerosol trace species in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Advances were made in airborne sampling instrumentation. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei and mass concentrations of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to uniquely identify the source of the air mass as being typically tropospheric or stratospheric. A quantitative understanding of the tropospheric-stratospheric exchange processes leads to better knowledge of the atmospheric impact of pollution through the development of improved simulation models of the atmosphere.

The Chemistry of Meteoric Metals in the Upper Atmosphere

NASA Astrophysics Data System (ADS)

Balasubramanian, Rajasekhar

The metals Na, Li, K, Ca and Fe have been observed around 90 km in the earth's upper atmosphere. Meteoric ablation is believed to be the source of these metals. The mesospheric chemistry of these metals and their impact on the general chemistry of the atmosphere are poorly understood. Therefore, a detailed investigation of processes affecting the gas -phase chemistry of these metals was undertaken. Both kinetic and photochemical studies were carried out using the techniques of pulsed photolysis of a suitable metal precursor and laser induced fluorescence of the resulting metal atoms. Ab initio calculations were also carried out to study the geometries of the metallic species and calculate their thermochemical properties. Kinetic investigations on the recombination reactions of the alkali metals with O_2 were performed over an extended temperature range (230-1100 K) in an attempt to understand their different seasonal behavior. The three reactions have very similar temperature dependences over the experimental temperature range. Use of the Troe formalism indicates that this dependency will continue into the mesospheric temperature range (140-240 K). The similarity suggests that differences in the temperature dependence of these reactions are not responsible for the different seasonal behavior of the alkali metals. The lower limits for the bond energies of the alkali superoxides were estimated from the kinetic decays obtained at 1100 K, and then combined with ab initio calculations to yield recommended bond energies. These values are of use in the Troe formalism and the mesospheric models. To assess the effectiveness of NaO_2 as a daytime sink, the absolute cross-section for photodissociation of NaO_2 was measured at 230 K. The photolysis rate of NaO_2 was derived above 70 km. The results indicate that above 85 km the reaction between NaO_2 and O is a more important loss term for NaO _2 than daytime photolysis and that between 80 and 65 km the photolysis of NaO_2 is the dominant loss term. From the photolysis experiment, an atmospherically important new Na species, NaO _4, was identified. The bimolecular reactions of Na with HCl/DCl, N_2O, and Li with H_2 O were investigated. The possible role of the reaction between NaCl and H in the chlorine catalyzed destruction of O_3 was explored. Finally, the role of the reactions of dissociative electron attachment to NaHCO_3 and NaCO_3 in the formation of sudden sodium layers above 90 km was examined by ab initio and thermochemical calculations. The results indicate that NaHCO_3, an unreactive species in the mesosphere, can result in the formation of SSLs on collision with energetic auroral electrons.

Present state of knowledge of the upper atmosphere: An assessment report

NASA Technical Reports Server (NTRS)

1984-01-01

A program of research, technology, and monitoring of the phenomena of the upper atmosphere, to provide for an understanding of and to maintain the chemical and physical integrity of the Earth's upper atmosphere was developed. NASA implemented a long-range upper atmospheric science program aimed at developing an organized, solid body of knowledge of upper atmospheric processes while providing, in the near term, assessments of potential effects of human activities on the atmosphere. The effects of chlorofluorocarbon (CFC) releases on stratospheric ozone were reported. Issues relating the current understanding of ozone predictions and trends and highlights recent and future anticipated developments that will improve our understanding of the system are summarized.

UARS MLS Observations of Lower Stratospheric ClO in the 1992-93 and 1993-94 Arctic Winter Vortices

NASA Technical Reports Server (NTRS)

Waters, J. W.; Manney, G. L.; Read, W. G.; Froidevaux, L.; Flower, D. A.; Jarnot, R. F.

1995-01-01

UARS (Upper Atmosphere Research Satellite) MLS (Microwave Limb Sounder) measurements of lower stratospheric ClO during the 1992-93 and 1993-94 Arctic winters are presented. Enhanced ClO in the 1992-93 winter was first observed in early December, and extensively during February when temperatures were continually low enough for PSCs. Sporadic episodes of enhanced ClO were observed for most of the 1993-94 winter as minimum temperatures hovered near the PSC threshold, with largest ClO amounts occurring in early March after a sudden deep cooling in late February.

Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

NASA Technical Reports Server (NTRS)

Perkins, P. J.; Papathakos, L. C.

1978-01-01

The Global Atmospheric Sampling Program (GASP) is collecting and analyzing data on gaseous and aerosol trace contaminants in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei, and mass concentration of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to identify the source of the air mass as being typically tropospheric or stratospheric.

Measurement of HO2 and other trace gases in the stratosphere using a high resolution far-infrared spectrometer at 28 km

NASA Technical Reports Server (NTRS)

Traub, Wesley A.; Chance, Kelly V.; Johnson, David G.; Jucks, Kenneth W.; Wofsy, Steven C.

1993-01-01

This report covers the time period 1 January 1993 to 30 June 1993. During this reporting period we had our third Upper Atmosphere Research Satellite (UARS) correlative balloon flight and submitted the results from this flight to the Central Data Handling Facility (CDHF). We made a number of improvements in our data processing software in preparation for a new analysis of our old balloon data sets. Finally, we continue to analyze the data obtained during the second Airborne Arctic Stratospheric Expedition (AASE 2).

Radiation chemistry in the Jovian stratosphere - Laboratory simulations

NASA Technical Reports Server (NTRS)

Mcdonald, Gene D.; Thompson, W. R.; Sagan, Carl

1992-01-01

The results of the present low-pressure/continuous-flow laboratory simulations of H2/He/CH4/NH3 atmospheres' plasma-induced chemistry indicate radiation yields of both hydrocarbon and N2-containing organic compounds which increase with decreasing pressure. On the basis of these findings, upper limits of 1 million-1 billion molecules/sq cm/sec are established for production rates of major auroral-chemistry species in the Jovian stratosphere. It is noted that auroral processes may account for 10-100 percent of the total abundances of most of the observed polar-region organic species.

Cirrus and Polar Stratospheric Cloud Studies using CLAES Data

NASA Technical Reports Server (NTRS)

Mergenthaler, John L.; Douglass, A. (Technical Monitor)

2001-01-01

We've concluded a 3 year (Period of Performance- January 21, 1998 to February 28, 2001) study of cirrus and polar stratospheric clouds using CLAES (Cryogenic Limb Array Etalon Spectrometer) data. We have described the progress of this study in monthly reports, UARS (Upper Atmosphere Research Satellite) science team meetings, American Geophysical Society Meetings, refereed publications and collaborative publications. Work undertaken includes the establishment of CLAES cloud detection criteria, the refinement of CLAES temperature retrieval techniques, compare the findings of CLAES with those of other instruments, and present findings to the larger community. This report describes the progress made in these areas.

Stratospheric Ozone Distribution and Tropospheric General Circulation: Interconnections in the UTLS Region

NASA Astrophysics Data System (ADS)

Barodka, S.; Krasovsky, A.; Shalamyansky, A.

2014-12-01

The height of the tropopause, which divided the stratosphere and the troposphere, is a result of two rival categories of processes: the tropospheric vertical convection and the radiative heating of the stratosphere resulting from the ozone cycle. Hence, it is natural that tropospheric and stratospheric phenomena can have effect each other in manifold processes of stratosphere-troposphere interactions. In the present study we focus our attention to the "top-down" side of the interaction: the impact of stratospheric ozone distribution on the features of tropospheric circulation and the associated weather patterns and regional climate conditions. We proceed from analyzes of the observational data performed at the A.I. Voeikov Main Geophysical Observatory, which suggest a distinct correlation between stratospheric ozone distribution, synoptic formations and air-masses boundaries in the upper troposphere and the temperature field of the lower stratosphere [1]. Furthermore, we analyze local features of atmospheric general circulation and stratospheric ozone distribution from the atmospheric reanalyses and general circulation model data, focusing our attention to instantaneous positions of subtropical and polar stationary atmospheric fronts, which define regional characteristics of the general circulation cells in the troposphere and separate global tropospheric air-masses, correspond to distinct meteorological regimes in the TOC field [2, 3]. We assume that by altering the tropopause height, stratospheric ozone-related processes can have an impact on the location of the stationary atmospheric fronts, thereby exerting influence on circulation processes in troposphere and lower stratosphere. For midlatitudes, the tropopause height controls the position of the polar stationary front, which has a direct impact on the trajectory of motion of active vortices on synoptic tropospheric levels, thereby controlling weather patterns in that region and the regional climate. This mechanism is particularly important for the formation of blocking events. [1] A.M. Shalamyansky - Proceedings of Voeikov Main Geophysical Observatory, V. 568, pp. 173-194, 2013 (in Russian) [2] R.D. Hudson et al - J. Atmos. Sci., V. 60, pp. 1669-1677, 2003. [3] R.D. Hudson et al - Atmos. Chem. Phys., V. 6, pp. 5183-5191, 2006.

Impact of the Asian monsoon on the extratropical lower stratosphere: trace gas observations during TACTS over Europe 2012

NASA Astrophysics Data System (ADS)

Müller, Stefan; Hoor, Peter; Bozem, Heiko; Gute, Ellen; Vogel, Bärbel; Zahn, Andreas; Bönisch, Harald; Keber, Timo; Krämer, Martina; Rolf, Christian; Riese, Martin; Schlager, Hans; Engel, Andreas

2016-08-01

The transport of air masses originating from the Asian monsoon anticyclone into the extratropical upper troposphere and lower stratosphere (Ex-UTLS) above potential temperatures Θ = 380 K was identified during the HALO aircraft mission TACTS in August and September 2012. In situ measurements of CO, O3 and N2O during TACTS flight 2 on 30 August 2012 show the irreversible mixing of aged stratospheric air masses with younger (recently transported from the troposphere) ones within the Ex-UTLS. Backward trajectories calculated with the trajectory module of CLaMS indicate that these tropospherically affected air masses originate from the Asian monsoon anticyclone. These air masses are subsequently transported above potential temperatures Θ = 380 K from the monsoon circulation region into the Ex-UTLS, where they subsequently mix with stratospheric air masses. The overall trace gas distribution measured during TACTS shows that this transport pathway had affected the chemical composition of the Ex-UTLS during boreal summer and autumn 2012. This leads to an intensification of the tropospheric influence on the extratropical lower stratosphere with PV > 8 pvu within 3 weeks during the TACTS mission. During the same time period a weakening of the tropospheric influence on the lowermost stratosphere (LMS) is determined. The study shows that the transport of air masses originating from the Asian summer monsoon region within the lower stratosphere affects the change in the chemical composition of the Ex-UTLS over Europe and thus contributes to the flushing of the LMS during summer 2012.

Asymmetries in ozone depressions between the polar stratospheres following a solar proton event

NASA Technical Reports Server (NTRS)

Maeda, K.; Heath, D. F.

1978-01-01

Ozone depletions in the polar stratosphere during the energetic solar proton event on 4 August 1972 were observed by the backscattered ultraviolet (BUV) experiments on the Nimbus 4 satellite. The observed ozone contents, the ozone depressions and their temporal variations above the 4 mb level exhibited distinct asymmetries between the northern and southern hemispheres. Since the ozone destroying solar particles precipitate rather symmetrically into the two polar atmospheres, due to the geomagnetic dipole field, it is suggested that these asymmetries may be explained in terms of the differences in dynamics between the summer and the winter polar atmospheres. In the summer (northern) hemisphere, the stratospheric and mesospheric ozone depletion and recovery are smooth functions of time due to the preponderance of undistributed orderly flow in this region. On the other hand, the temporal variation of the upper stratospheric ozone in the winter polar atmosphere (southern hemisphere) exhibits large amplitude irregularities. These characteristic differences between the two polar atmospheres are also evident in the vertical distributions of temperatures and winds observed by balloons and rocket soundings.

3D General Circulation Model of the Middle Atmosphere of Jupiter

NASA Astrophysics Data System (ADS)

Zube, Nicholas Gerard; Zhang, Xi; Li, Cheng; Le, Tianhao

2017-10-01

The characteristics of Jupiter’s large-scale stratospheric circulation remain largely unknown. Detailed distributions of temperature and photochemical species have been provided by recent observations [1], but have not yet been accurately reproduced by middle atmosphere general circulation models (GCM). Jupiter’s stratosphere and upper troposphere are influenced by radiative forcing from solar insolation and infrared cooling from hydrogen and hydrocarbons, as well as waves propagating from the underlying troposphere [2]. The relative significance of radiative and mechanical forcing on stratospheric circulation is still being debated [3]. Here we present a 3D GCM of Jupiter’s atmosphere with a correlated-k radiative transfer scheme. The simulation results are compared with observations. We analyze the impact of model parameters on the stratospheric temperature distribution and dynamical features. Finally, we discuss future tracer transport and gravity wave parameterization schemes that may be able to accurately simulate the middle atmosphere dynamics of Jupiter and other giant planets.[1] Kunde et al. 2004, Science 305, 1582.[2] Zhang et al. 2013a, EGU General Assembly, EGU2013-5797-2.[3] Conrath 1990, Icarus, 83, 255-281.