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At least 217 records · Page 12

The reservoir of ozone in the boundary layer of the eastern United States and its potential impact on the global tropospheric ozone budget

An analysis of available ozone data in the eastern two-thirds of the United States indicates that a substantial reservoir of ozone is present in the summertime. Five-year mean concentrations range from 40 to 65 ppbv. The reservoir covered an area of several million square kilometers and extends vertically from the surface to 1 to 2 km. The vertical distribution of ozone in the reservoir during midday supports a transport of additional ozone from the boundary layer to the free troposphere. Data are presented demonstrating the potential effect of transport by convective clouds and by the sea breeze circulation - mechanisms by which ozone may be transported out of the boundary layer into the free troposphere. The potential impact of this reservoir on the tropospheric ozone budget is discussed. It is shown that if less than half of the ozone mass in this reservoir is transported to the free troposphere, then the amount of ozone transported out of the boundary layer approximates the amount of ozone transported downward during a tropopause fold event.

Vukovich, F. M.↗

The photochemistry of methane and carbon monoxide in the troposphere in 1950 and 1985

The roughly 1 percent/year increase in tropospheric methane and roughly 2 percent/year increase in tropospheric carbon monoxide deduced from recent analyses of ground-based solar infrared spectra recorded in 1950 and 1951 have very important implications for the photochemistry and chemistry of the troposphere. Photochemical calculations indicate that as a result of the increase of methane and carbon monoxide since 1950-51, levels of the hydroxyl radical, the key species in the photochemistry of the troposphere, may have decreased by about 25 percent.

Levine, J. S.↗

Space opportunities for tropospheric chemistry research

The use of the Space Shuttle to measure tropospheric trace species is examined. Factors which affect the measurement of tropospheric trace species are discussed. The Academy of Sciences 1985 report categorized the trace species into levels: first-level gases include water vapor, O3, CO, and CH4, and the second-level gases are N2O, NO2, NH3, SO2, chlorofluoromethanes, and HCl. The effects of first-level gases on the earth's climate, the photochemistry/chemistry of the troposphere, and the photochemical/chemical production and destruction of the hydroxyl radical are studied; the distribution and magnitude of the hydroxyl radical in the troposphere are analyzed in terms of water vapor, O3, CO, and CH4.

Levine, Joel S.↗

Nonmethane hydrocarbons in the troposphere - Impact on the odd hydrogen and odd nitrogen chemistry

A one-dimensional model is utilized to study the role of nonmethane hydrocarbons (NMHCs) in tropospheric chemistry. The effects of NMHCs on tropospheric peroxyacetyl nitrate (PAN) formation are analyzed; the global distribution and seasonal variability of PAN in the troposphere of the Northern and Southern Hemispheres are examined. The NMHC-PAN measurements obtained by model simulations are compared to the photochemical theory. The seasonal cycles in NMHC abundances are predicted, and their effects on other tropospheric species are investigated.

Kasting, James F.↗

Chlorine-hydrocarbon photochemistry in the marine troposphere and lower stratosphere

The role of chlorine atoms in the oxidation of methane and nonmethane hydrocarbons (NMHCs) in the marine troposphere and lower stratosphere was investigated using a one-dimensional photochemical model that incorporated the chemistry of CH4, NMHCs, NO(x), O(x), and HO(x), as well as organic and inorganic halogens in the troposphere and lower stratosphere. The model predicted that chlorine atoms are present in the marine troposphere at the concentrations of about 1000/cu cm, mostly as a product of the reaction between OH and HCl released from sea spray. The results indicate that Cl atoms cause 20 to 40 percent of NMHC oxidation in the troposphere and 40 to 90 percent in the lower stratosphere. At 15 km, the NMHC-Cl reactions account for nearly 80 percent of the PAN produced. Where available, experimental data confirmed the model predictions.

Singh, H. B.↗

On the transfer of stratospheric ozone into the troposphere near the North Pole

A series of nearly daily ozone vertical profiles obtained at station T-3 on Fletcher's Ice Island (about 85 deg N, about 90 deg W) during the period January-March 1971 shows several significant ozone intrusions into the troposphere. These intrusions are not only associated with enhanced ozone amounts in the stratosphere but also require tropopause folding events to transport ozone into the troposphere. These folds in the arctic tropopause appear to be capable of contributing significantly to the ozone budget of the arctic troposphere during the late winter and spring seasons. The importance of tropopause folding for bringing ozone into the troposphere seen in the daily ozone profiles confirms the results found in the Arctic Gas and Aerosol Sampling Program aircraft flights.

Oltmans, Samuel J.↗

Troposphere-stratosphere interactions in a one-dimensional model of Jovian photochemistry

The case of a chemically unreactive species flowing downward through the stratosphere and troposphere with a constant flux is presently treated by a one-dimensional Jovian atmosphere model which encompasses the coupling between a rapidly mixed troposphere and a stagnant stratosphere, so that the contrast between the peak stratosphere and tropopause concentrations is reflective of the variation between the lower stratosphere and upper troposphere eddy diffusion coefficients. Numerical simulations of unreactive CO and C2H6 species indicate that upper troposphere abundances may possess a substantial photochemical contribution. The implications of these modeling results for higher spectral resolution observations are noted.

Landry, Bridget↗

Satellite observations of variations in tropical cyclone convection caused by upper-tropospheric troughs

Satellite observations and numerical model results have been used to study the relationship between upper-tropospheric forcing and the oscillation of convection of tropical cyclones Florence (1988) and Irene (1981) during their mature stage over open warm oceans (SST greater than or equal to 26 C). It is suggested that the initiation and maintenance of intense convective outbreaks in tropical cyclones are related to the channeling and strengthening of their outflow by upper-tropospheric troughs. It is possible to enhance the convection in response to the outflow jet-induced import of eddy relative angular momentum and ascending motion associated with the thermally direct circulation. Both Florence and Irene are found to intensify after the onset of these convective episodes. It is also suggested that the cessation in the convection of the two tropical cyclones occurs when the upper-tropospheric troughs move near or over the tropical cyclones, resulting in the weakening of their outflow and the entrainment of dry upper-tropospheric air into their inner core.

Rodgers, Edward B.↗

Measured and calculated optical property profiles in the mixed layer and free troposphere

Nearly simultaneous measurements of the physical and optical properties of mixed layer and free tropospheric aerosols near Boulder, Colorado, were made on several occasions using aircraft, balloon, and ground-based sensors. This effort (Front Range Lidar, Aircraft, and Balloon experiment (FRLAB)) was conducted with the purpose of obtaining a diverse, self-consistent data set that could be used for testing optical model calculations based on measured physical characteristics such as apparent size distribution, composition, and shape. It was found that even with the uncertainties involved, the model predictions are in good agreement with the measurements in the visible and near infrared wavelength regions. At CO2 lidar wavelengths there is considerably more uncertainty in both the calculated and measured values; however, within the estimated errors there appears to be satisfactory agreement except for the highest free tropospheric layer studied. The results also indicate that during FRLAB the aerosol in the boundary layer and free troposphere behaved as spherical particles for optical modeling purposes. The utility of the observations for determining the extinction-to-backscatter ratio relevant to aerosols in the boundary layer and free troposphere is described with typical measured values being in the 20 to 30 sr range.

Rosen, James M.↗

Large-scale variability of ozone and aerosols in the summertime Arctic and sub-Arctic troposphere

The results of mesoscale and large-scale studies of the distribution of aerosols and O3 using primarily an airborne DIAL system are reported. The tropospheric composition at high latitudes is found to be strongly influenced by stratospheric intrusions. Regions of low-aerosol scattering and enhanced O3 mixing ratios are correlated with descending air from the lower stratosphere. Over 37 percent of the troposphere along the flight track at latitudes higher than 57 deg N had significantly enhanced O3 levels due to stratospheric intrusions, and in the 4-6 km latitude range the tropospheric extent of the enhanced O3 exceeded 56 percent. Ozone mixing ratios of 80 ppbv at 6 km are common, with vertical O3 gradients of over 11 ppbv/km observed across the base of strong intrusions. In the mixed layer over the tundra, O3 was in the 25-35 ppbv range with a gradient of 5.5 ppbv/km, while in the continental polar air masses, the average gradient in the lower troposphere is 7.4 ppbv/km, indicating more downward transport of O3 at higher latitudes.

Browell, E. V.↗

Propagation of planetary waves between the troposphere and stratosphere

The propagation of planetary waves between the troposphere and stratosphere is investigated using a linear, time-dependent, primitive equation model. It is found that the tropopause acts like a valve for the propagation of planetary waves. The key parameters controlling the valve are the vertical gradient of buoyancy frequency and the vertical shear of the zonal winds at the tropopause. For a given wind profile smaller gradient of buoyancy frequency enhances the propagation of planetary waves. For a given profile of buoyancy frequency the larger the shear, the more the wave activity is trapped in the troposphere, and therefore, there is less left to propagate into the stratosphere. The transmission across the tropopause is, however, not sensitive to zonal winds in the upper stratosphere. The propagation of planetary waves is very sensitive to transience. More transient waves propagate more vertically within the troposphere, and for more transient waves, more wave activity is transferred into the stratosphere from the troposphere.

Chen, Ping↗

The use of satellite data to determine the distribution of ozone in the troposphere

Measurements from two independent satellite data sets have been used to derive the climatology of the integrated amount of ozone in the troposphere. These data have led to the finding that large amounts of ozone pollution are generated by anthropogenic activity originating from both the industrialized regions of the Northern Hemisphere and from the southern tropical regions of Africa. To verify the existence of this ozone anomaly at low latitudes, an ozonesonde capability has been established at Ascension Island (8 deg S, 15 deg W) since July 1990. According to the satellite analyses, Ascension Island is located downwind of the primary source region of this ozone pollution, which likely results from the photochemical oxidation of emissions emanating from the widespread burning of savannas and other biomass. These in situ measurements confirm the existence of large amounts of ozone in the lower atmosphere. A summary of these ozonesonde data to date will be presented. In addition, we will present some ozone profile measurements from SAGE II which can be used to provide upper tropospheric ozone measurements directly in the tropical troposphere. A preliminary comparison between the satellite observations and the ozonesonde profiles in the upper troposphere and lower stratosphere will also be presented.

Fishman, Jack↗

Radon measurements in the lower tropical stratosphere - Evidence for rapid vertical transport and dehydration of tropospheric air

During the tropical experiment of NASA's Stratosphere-Troposphere Exchange Program (STEP), in situ radon and other trace constituent measurements were made aboard a NASA ER-2 high-altitude research aircraft to investigate the mechanisms of irreversible transfers from the troposphere into the tropical stratosphere. Observations made in and downwind of the cirrus shields of three large tropical cyclones and downwind of the cirrus anvil of a large cumulonimbus cloud cluster showed several clear instances of elevated radon activity occurring simultaneously with low total water mixing ratios. These observations are unambiguous evidence of an effective dehydration process, capable of reducing total water vapor mixing ratios to less than 2.5 ppmv, occurring in conjunction with troposphere-to-stratosphere transport and indicate that rapid localized convection, rather than slow regional mean motions, was responsible for the observed transports and associated with the accompanying dehydration. Radon activities measured in regions of active or recent troposphere-to-stratosphere transport were consistent with the 17 pCi/scm mean value needed to support the observed abundance of stratospheric 210 Pb.

Kritz, Mark A.↗

Reactive nitrogen and its correlation with ozone in the lower stratosphere and upper troposphere

High resolution in situ measurements of reactive nitrogen (NO(y)) and O3 were made in the upper troposphere and lower stratosphere at a variety of latitudes and seasons. In the lower stratosphere, NO(y) and O3 are very highly positively correlated at all times and spatial scales sampled. The ratio NO(y)/NO3 is much less variable than either species measured separately. The ratio has a much weaker gradient with altitude than the mixing ratios of O3 or NO(y). The ratio is smaller and decreases more rapidly with altitude in the tropics than at midlatitudes. In the upper troposphere NO(y) and O3 are only weakly correlated. Their ratio in the tropical upper troposphere is about 0.005-0.025 and the ratio in the midlatitude upper troposphere is about 0.004-0.010. The NO(y) in the upper troposhere is probably partly due to lightning.

Murphy, D. M.↗

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.↗

Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming

The paper examines the tropospheric aerosol record obtained over the period 1971 to 1990, during which high-altitude balloons with optical particle counters were launched at Laramie, Wyoming, in a long-term study of the stratospheric sulfate aerosol layer. All aerosol particle size ranges display pronounced seasonal variations, with the condensation nuclei concentration and the optically active component showing a summer maximum throughout the troposphere. Mass estimates, assuming spherical sulfate particles, indicate an average column mass between altitudes of 2.5 and 10 km of about 4 and 16 mg/sq m in winter and summer, respectively. Calculated optical depths vary between 0.01 and 0.04 from winter to summer; the estimated mass scattering cross section is about 3 sq m/g throughout the troposphere. There is evidence for a decreasing trend of 1.6-1.8 percent/yr in the optically active tropospheric aerosol over the past 20 yr, which may be related to a similar reduction in SO2 emission in the U.S. over this period.

Hofmann, David J.↗

The coupling of the troposphere and stratosphere

A linear, time-dependent, primitive-equation, 3D numerical model is used to investigate the dynamical coupling between the troposphere and stratosphere through the vertical propagation of planetry waves. Attention is given to the roles of the tropopause in affecting the propagation of planetary waves and to the extent to which the stratosphere can determine its own wave driving, i.e., the sensitivity of the generation of the wave activity in the troposphere to the change of zonal wind in the stratosphere. Two maxima in Eliassen-Palm (EP) flux convergence are found for wave 1 in high latitudes, one in the upper stratosphere and the other in the upper troposphere. For wave 2 there is a third maximum north of the zero wind line in the tropical stratosphere. The formation of the maximum in EP-flux convergence in the upper troposphere is related to the dissipation of non-WKBJ waves near a local maximum of the refractive index. The existence of the local maximum in refractive index at the tropopause is a result of the great gradient of the buoyancy frequency as well as the vertical shear of the zonal flow there.

Chen, Ping↗

The Feasibility of Tropospheric and Total Ozone Determination Using a Fabry-perot Interferometer as a Satellite-based Nadir-viewing Atmospheric Sensor

Monitoring of the global distribution of tropospheric ozone (O3) is desirable for enhanced scientific understanding as well as to potentially lessen the ill-health impacts associated with exposure to elevated concentrations in the lower atmosphere. Such a capability can be achieved using a satellite-based device making high spectral resolution measurements with high signal-to-noise ratios; this would enable observation in the pressure-broadened wings of strong O3 lines while minimizing the impact of undesirable signal contributions associated with, for example, the terrestrial surface, interfering species, and clouds. The Fabry-Perot Interferometer (FPI) provides high spectral resolution and high throughput capabilities that are essential for this measurement task. Through proper selection of channel spectral regions, the FPI optimized for tropospheric O3 measurements can simultaneously observe a stratospheric component and thus the total O3 column abundance. Decreasing stratospheric O3 concentrations may lead to an increase in biologically harmful solar ultraviolet radiation reaching the earth's surface, which is detrimental to health. In this research, a conceptual instrument design to achieve the desired measurement has been formulated. This involves a double-etalon fixed-gap series configuration FPI along with an ultra-narrow bandpass filter to achieve single-order operation with an overall spectral resolution of approximately .068 cm(exp -1). A spectral region of about 1 cm(exp -1) wide centered at 1054.73 cm(exp -1) within the strong 9.6 micron ozone infrared band is sampled with 24 spectral channels. Other design characteristics include operation from a nadir-viewing satellite configuration utilizing a 9 inch (diameter) telescope and achieving horizontal spatial resolution with a 50 km nadir footprint. A retrieval technique has been implemented and is demonstrated for a tropical atmosphere possessing enhanced tropospheric ozone amounts. An error analysis assessing the impact on retrieved O3 amounts of the most significant uncertainties associated with this particular measurement has been performed for several different types of atmospheres. Results show the proposed instrumentation to enable a good measurement of absolute ozone amounts and an even better determination of relative changes, with a range of accuracy to within 7.55 to 20.6 percent for integrated tropospheric amounts (and 1.99 to 4.02 percent for total O3 column abundance) and a corresponding range in precision to within 7.73 to 10.4 percent (and 3.30 to 3.95 percent for total O3 column abundance), for the atmospheric conditions considered.

Larar, Allen Maurice↗