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NASA NTRS2011

Reactive Nitrogen, Ozone and Ozone Production in the Arctic Troposphere and the Impact of Stratosphere-Troposphere Exchange

We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of approximately 60 ppbv and NOx of approximately 25 pptv throughout spring and summer with CO decreases from approximately 145 ppbv in spring to approximately 100 ppbv in summer. These observed CO, NOx and O3 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 the past two decades in processes that could have changed the 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 concentration of 140-160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (approximately 800 pptv in spring and approximately 1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of approximately 120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the 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.

Liang, Q.↗

NASA NTRS1976

Atmospheric ozone measurements made from B-747 AIRLINERS: Spring 1975

Atmospheric ozone in the upper troposphere and lower stratosphere north of the equator has been registered aboard two commercial B-747 airliners. The composite ozone, flight and meteorological data are reported. Attention is drawn particularly to the vertical profiles of atmospheric ozone mixing ratio as a function of both distance from the tropopause and curvature of the streamlines. The GASP observations suggest that ozone levels typical of the lower stratosphere are often embedded in the upper troposphere, principally during occassions when cyclonic wind curvature was noted.

Falconer, P. D.↗

NASA NTRS2000

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

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.

Kurylo, M. J.↗

NASA NTRS1990

Halocarbon ozone depletion and global warming potentials

Concern over the global environmental consequences of fully halogenated chlorofluorocarbons (CFCs) has created a need to determine the potential impacts of other halogenated organic compounds on stratospheric ozone and climate. The CFCs, which do not contain an H atom, are not oxidized or photolyzed in the troposphere. These compounds are transported into the stratosphere where they decompose and can lead to chlorine catalyzed ozone depletion. The hydrochlorofluorocarbons (HCFCs or HFCs), in particular those proposed as substitutes for CFCs, contain at least one hydrogen atom in the molecule, which confers on these compounds a much greater sensitivity toward oxidation by hydroxyl radicals in the troposphere, resulting in much shorter atmospheric lifetimes than CFCs, and consequently lower potential for depleting ozone. The available information is reviewed which relates to the lifetime of these compounds (HCFCs and HFCs) in the troposphere, and up-to-date assessments are reported of the potential relative effects of CFCs, HCFCs, HFCs, and halons on stratospheric ozone and global climate (through 'greenhouse' global warming).

Cox, Richard A.↗

NASA NTRS1994

Venus climate stability and volcanic resurfacing rates

The climate of Venus is to a large degree controlled by the radiative properties of its massive atmosphere. In addition, outgassing due to volcanic activity, exospheric escape processes, and surface/atmosphere interactions may all be important in moderating the abundances of atmospheric CO2 and other volatiles. We have developed an evolutionary climate model for Venus using a systems approach that emphasizes feedbacks between elements in the climate system. Modules for atmospheric radiative transfer, surface/atmosphere interactions, tropospheric chemistry, and exospheric escape processes have so far been developed. Climate feedback loops result from interconnections between modules, in the form of the environmental parameters pressure, temperature, and atmospheric mixing ratios. The radiative transfer module has been implemented by using Rosseland mean opacities in a one dimensional grey radiative-convective model. The model has been solved for the static (time independent) case to determine climate equilibrium points. The dynamics of the model have also been explored by employing reaction/diffusion kinetics for possible surface atmosphere heterogeneous reactions over geologic timescales. It was found that under current conditions, the model predicts that the climate of Venus is at or near an unstable equilibrium point. The effects of constant rate volcanism and corresponding exsolution of volatiles on the stability of the climate model were also explored.

Bullock, M. A.↗

NASA NTRS2013

Three Decades of Global Methane Sources and Sinks

Methane is an important greenhouse gas, responsible for about 20 of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios which differ in fossil fuel and microbial emissions to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.

periodic variations↗

NASA NTRS1989

The global consequences of increasing tropospheric ozone concentrations

Recent analyses of long term records of tropospheric ozone measurements in the Northern Hemisphere suggest that it is increasing at a rate of 1 to 2 percent per year. Because of this, it is argued that the amount of atmospheric warming due to increasing tropospheric ozone is comparable to, or possibly even greater than, the amount of warming due to the increase of carbon dioxide. Unlike all other climatically important trace gases, ozone is toxic, and increases in its concentration will result in serious environmental damage, as well as impairment of human health.

Fishman, Jack↗

NASA NTRS1991

The global consequences of increasing tropospheric ozone concentrations

Recent analyses of long-term records of tropospheric ozone measurements in the Northern Hemisphere suggest that it is increasing at a rate of 1 to 2 percent per year. Because of this, it is argued that the amount of atmospheric warming due to increasing tropospheric ozone is comparable to, or possibly even greater than, the amount of warming due to the increase of carbon dioxide. Unlike all other climatically important trace gases, ozone is toxic, and increases in its concentration will result in serious environmental damage, as well as impairment of human health.

Fishman, Jack↗

NASA NTRS1993

The meteorological environment of the tropospheric ozone maximum over the tropical South Atlantic Ocean

Atmospheric flow patterns are examined over the South Atlantic Ocean where a maximum of tropospheric ozone has been observed just west of southern Africa. We investigate the flow climatology during October and perform a case study for six days during October 1989. Horizontal and vertical motions are examined and used to prepare 3D backward trajectories from the region of greatest ozone. An initially zonally symmetric distribution of ozone is treated as a passive tracer and advected by 3D flows forecast by the global model. Results from the passive tracer simulation indicate that 3D advection alone can produce a maximum of tropospheric ozone in the observed location. In addition, the trajectories suggest that by-products of biomass burning could be transported to the area of maximum ozone. Low-level flow from commonly observed regions of burning in Africa streams westward to the area of interest. Over Brazil, if the burning by-products are carried into the upper troposphere by convective process, they then could be transported eastward to the ozone feature in approximately five days. There is considerable subsidence over the tropical southern Atlantic, such that stratospheric influences also are a factor in producing the ozone maximum. Both planetary-scale and transient synoptic-scale circulation features play major roles in the various transport processes that influence the region. In summary, the observed tropospheric ozone maximum appears to be caused by a complex set of horizontal and vertical advections, transport from regions of biomass burning, and stratospheric influences.

Krishnamurti, T. N.↗

NASA NTRS2000

A New Interferometer for Monitoring Atmospheric Phase Fluctuations

Water vapor in the Earth's troposphere introduces an extra electrical path in the propagation of radio signals through the atmosphere. The distribution of water vapor is irregular and distorts the wavefronts of incoming radio waves, limiting the angular resolution that can be achieved with ground-based telescopes. The level of fluctuations depends both on the location of the site ,and on the prevailing atmospheric conditions. The ability to measure the fluctuations is therefore important when choosing a site for a new instrument, and for scheduling observations of existing telescopes. Existing phase monitors are radio interferometers that monitor monochromatic beacon tones from geostationary communications satellites at a frequency of about 12 GHz. They have a classical heterodyne design based on two satellite receiving antennas; each has a front-end for amplifying and down-converting the incoming signals using a local oscillator that is phase-locked to a common reference frequency. In addition to multiple phase-locked loops these instruments require expensive phase-stable cabling to reduce the effects of thermal drift. The new system uses two consumer 18" digital satellite TV dishes to monitor satellite TV broadcast signals over a bandwidth of 500 MHz (12.2 to 12.7 GHz). The novel design eliminates the need for phase-locked loops and thermally stable components, and uses a pair of Gilbert Cell multipliers to perform the broadband correlation. A phase monitor has been been built and deployed at the site of the Berkeley-Illinois-Maryland Association Millimeter Array in Northern California, and has been operating successfully since June 1998, measuring the difference in electrical path length for parallel lines of sight to the satellite separated by a baseline of 100 m. With a hardware cost of approximately $4000, it is much cheaper than previous instruments, and the low power requirements and high reliability make the system suitable for site testing in remote locations.

Lay, Oliver↗

NASA NTRS2023

Stratospheric Water Vapor Affecting Atmospheric Circulation

Water vapor plays an important role in many aspects of the climate system, by affecting radiation, cloud formation, atmospheric chemistry and dynamics. Even the low stratospheric water vapor content provides an important climate feedback, but current climate models show a substantial moist bias in the lowermost stratosphere. Here we report crucial sensitivity of the atmospheric circulation in the stratosphere and troposphere to the abundance of water vapor in the lowermost stratosphere. We show from a mechanistic climate model experiment and inter-model variability that lowermost stratospheric water vapor decreases local temperatures, and thereby causes an upward and poleward shift of subtropical jets, a strengthening of the stratospheric circulation, a poleward shift of the tropospheric eddy-driven jet and regional climate impacts. The mechanistic model experiment in combination with atmospheric observations further shows that the prevailing moist bias in current models is likely caused by the transport scheme, and can be alleviated by employing a less diffusive Lagrangian scheme. The related effects on atmospheric circulation are of similar magnitude as climate change effects. Hence, lowermost stratospheric water vapor exerts a first order effect on atmospheric circulation and improving its representation in models offers promising prospects for future research.

stratosphere↗

NASA NTRS1984

Vertical displacement of the mid-tropospheric water vapor boundary in the tropics derived from the VISSR Atmospheric Sounder (VAS) 6.7-micron channel

A technique for locating areas of upward or downward motion of the upper boundary of the midtropospheric water-vapor envelope over tropical oceans on the basis of GOES Visible/IR Spin-Scan Radiometer (VISSR) Atmospheric Sounder (VAS) 6.7-micron brightness temperatures is developed and demonstrated. The technique employs an analogy to the method developed by Schoeberl and Krueger (1983) for the bottom of the ozone layer and depends on the relationship investigated by Chesters and Uccellini (1982) between 6.7-micron brightness temperature and the pressure of the water-vapor upper boundary. The results of analysis of VAS data for the North Atlantic (20-40 deg N and 35-75 deg W) on September 5-7, 1982, are presented in maps which are shown to be physically consistent and in agreement with conventional upper-air measurements. Refinement of the method to account for horizontal advection and diffusion is suggested.

Stout, J.↗

NASA NTRS1994

Aerosol particles in the upper troposphere and lower stratosphere: Elemental composition and morphology of individual particles in northern midlatitudes

Atmospheric particles were collected in the midlatitude upper troposphere (UT) and lower stratosphere (LS) by inetrial impaction for subsequent electron microscopy and individual particle element analysis. More than 97% of particles analyzed on impactor substrates exposed in the LS contained only O and S in detectable quantities; these particles are believed to be acidic sulfate. Nonsulfate materials seen in the remaining particles included soot, other c-rich substances and crustal materials. Although not predominantly sulfate, usually carried a sulfer-rich coating in the LS. Samples collected very near and just below the tropopause were also dominated by sulfates. The fraction of sulfate particles analyzed on impactor substrates exposed in the UT was 91-94% of the total particle concentration. Nonsulfate substances observed in the UT samples included crustal-type material, hydrated marine salts, carbon-rich materials of several types, and metal-containing substances of uncertain origin. Most of these UT particles were not coated with detectable quantitites of sulfate.

Sheridan, Patrick J.↗

NASA NTRS2009

The Seasonal Response of Titan's Troposphere and Stratosphere

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

Flasar, F. M.↗

NASA NTRS1979

The evolution and variability of atmospheric ozone over geological time

The rise of atmospheric O3 as a function of the evolution of O2 has been investigated using a one-dimensional steady-state photochemical model based on the chemistry and photochemistry of Ox(O3, O, O(1D)), N2O, NOx(NO, NO2, HNO3), H2O, and HOx(H, OH, HO2, H2O2) including the effect of vertical eddy transport on the species distribution. The total O3 column density was found to maximize for an O2 level of 0.1 present atmospheric level (PAL) and exceeded the present total O3 column by about 40%. For that level of O2, surface and tropospheric O3 densities exceeded those of the present atmosphere by about an order of magnitude. Surface and tropospheric OH densities of the paleoatmosphere exceeded those of the present atmosphere by orders of magnitude. It was also found that in the O2-deficient paleoatmosphere, N2O (even at present atmospheric levels) produces much less NOx than it does in the present atmosphere.

Levine, J. S.↗

NASA NTRS2018

Impacts of Snow Darkening Effects by Light Absorbing Aerosols on Hydroclimate of Eurasia During Boreal Spring and Summer

In this study, we used the NASA GEOS-5 climate model to investigate the impact of snow darkening by light-absorbing aerosols on the hydro-climate if Eurasia during boreal spring and summer. Two sets of 10-member ensemble model integrations with prescribed sea surface temperature were carried out for 10 simulated years (2002-2011); one includes snow-darkening effects (SDE) by light-absorbing aerosols, and one does not (NSDE). Differences between the two experiments in the hydro-climates over Eurasia were evaluated. Results show that SDE warming is most pronounced during the melting season due to strong snow-albedo feedback in the vicinity of the retreating seasonal snowline. SDE spurs a Wet-First-Dry-Later (WFDL) modulation of the surface energy and water balances, characterized by an accelerated (days-to-weeks) snowmelt along with excessive runoff and a warming and wetting of the land during the early part of the melting season. The fast snowmelt is followed by a prolonged (> months) warming and desiccation of the land, stemming from a deficit of late-season snowmelt water and increased surface evaporation. The prolonged warming and drying of the land atmosphere system persist through the summer, sustained by atmospheric conditions favorable for the development of atmospheric blocking, i.e., higher mid-to-upper tropospheric geopotential height, lower relative humidity, reduced cloudiness and enhanced atmospheric subsidence. Overall, SDE by light absorbing aerosols leads to a warmer and drier boreal summer hydro-climate, increasing the frequency of the top 5% and 1% extreme hot days (as defined by NSDE statistics) over western and northern Eurasia by approximately three-fold and tenfold, respectively.

Snow darkening↗

NASA NTRS1976

Evaluation of upwelling infrared radiance from the earth's troposphere

Basic equations for calculating the upwelling atmospheric radiance are presented. Theoretical formulation of the transmittance models (line-by-line and quasi-random band) and computational procedures for the evaluation of transmittance and radiance are discussed. This information is useful in the interpretation of the data obtained from measuring gaseous pollutants in the troposphere.

Tiwari, S. N.↗

NASA NTRS1977

Possible variations in atmospheric methane

A model coupling photochemistry and vertical transport in the troposphere has been used to investigate the magnitude of possible future perturbations to atmospheric CH4. The response of atmospheric CH4 to an increase in the concentration of CO or to a variation in stratospheric O3 is studied. Both of the above mechanisms, which could be caused by man's activities, arise because a change in the concentration of tropospheric OH will lead to a change in the CH4 abundance. The calculations imply that a perturbation of about 30-40% in atmospheric CH4 could occur if stratospheric O3 were perturbed by 10% or if man-made CO continued to increase. The possible consequences of a CH4 perturbation may entail a perturbation in stratospheric photochemistry or in the thermal balance of the atmosphere.

Chameides, W. L.↗