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Logan, J. A.

Publications and source records attributed to Logan, J. A..

At least 19 records

Activities of NASA's Global Modeling Initiative (GMI) in the Assessment of Subsonic Aircraft Impact

The Intergovernmental Panel on Climate Change estimated a peak increase in ozone ranging from 7-12 ppbv (zonal and annual average, and relative to a baseline with no aircraft), due to the subsonic aircraft in the year 2015, corresponding to aircraft emissions of 1.3 TgN/year. This range of values presumably reflects differences in model input (e.g., chemical mechanism, ground emission fluxes, and meteorological fields), and algorithms. The model implemented by the Global Modeling Initiative allows testing the impact of individual model components on the assessment calculations. We present results of the impact of doubling the 1995 aircraft emissions of NOx, corresponding to an extra 0.56 TgN/year, utilizing meteorological data from NASA's Data Assimilation Office (DAO), the Goddard Institute for Space Studies (GISS), and the Middle Atmosphere Community Climate Model, version 3 (MACCM3). Comparison of results to observations can be used to assess the model performance. Peak ozone perturbations ranging from 1.7 to 2.2 ppbv of ozone are calculated using the different fields. These correspond to increases in total tropospheric ozone ranging from 3.3 to 4.1 Tg/Os. These perturbations are consistent with the IPCC results, due to the difference in aircraft emissions. However, the range of values calculated is much smaller than in IPCC.

Rodriquez, J. M.

Ozone Climatological Profiles for Version 8 TOMS and SBUV Retrievals

A new altitude dependent ozone climatology has been produced for use with the latest Total Ozone Mapping Spectrometer (TOMS) and Solar Backscatter Ultraviolet (SBUV) retrieval algorithms. The climatology consists of monthly average profiles for ten degree latitude zones covering from 0 to 60 km. The climatology was formed by combining data from SAGE II (1988 to 2000) and MLS (1991-1999) with data from balloon sondes (1988-2002). Ozone below about 20 km is based on balloons sondes, while ozone above 30 km is based on satellite measurements. The profiles join smoothly between 20 and 30 km. The ozone climatology in the southern hemisphere and tropics has been greatly enhanced in recent years by the addition of balloon sonde stations under the SHADOZ (Southern Hemisphere Additional Ozonesondes) program. A major source of error in the TOMS and SBUV retrieval of total column ozone comes from their reduced sensitivity to ozone in the lower troposphere. An accurate climatology for the retrieval a priori is important for reducing this error on the average. The new climatology follows the seasonal behavior of tropospheric ozone and reflects its hemispheric asymmetry. Comparisons of TOMS version 8 ozone with ground stations show an improvement due in part to the new climatology.

McPeters, R. D.

Quasibiennial Oscillation in Tropical Ozone as Revealed by Ozonesonde and Satellite Data

We present an analysis of the quasi-biennial oscillation (QBO) in tropical ozone using recent in situ measurements made by ozonesondes, supplemented by satellite profile and column data. The first in situ equatorial ozone profiles reveal the dramatic change in shape of the profile that accompanies the descent of the westerly shear zone. The partial pressure maximum in ozone increases by -25% in 5-6 months as it descends from 17.5 to 24 hPa. The amplitude of the QBO anomaly that extends from 15 to 80 hPa is found to exceed *20%, larger than indicated by earlier analyses of satellite data. The influence of the QBO on equatorial ozone is dominant between 10 and 45 hPa, but the seasonal cycle is more important below 50 hPa. The equatorial ozone anomalies are influenced by El Niiio-Southern Oscillation (ENSO) in the lowest part of the stratosphere. The ozone anomaly in the lower stratosphere at 20"s lags that at the equator by only a few months during the easterlies from 1994 to 1998, contrary to the previous picture of the subtropical and equatorial anomalies being out of phase.

Logan, J. A.

SAGE (version 5.96) Ozone Trends in the Lower Stratosphere

Ozone retrievals from Stratospheric Aerosol and Gas Experiment (SAGE) II version 5.96 (v5.96) below approx. 25 km altitude are discussed. This version of the algorithm includes improved constraints on the wavelength dependence of aerosol extinctions based on the ensemble of aerosol size distribution measurements. This results in a reduction of SAGE ozone errors in the 2 years after the Mount Pinatubo eruption. However, SAGE ozone concentrations are still approx. 10% larger than ozonesonde and Halogen Occultation Experiment (HALOE) measurements below 20 km altitude under nonvolcanic conditions (and by more than this in the tropics). The analysis by Steele and Turco suggests that the SAGE ozone overpredictions are in the wrong direction to be explained by aerosol extinction extrapolation errors. Moreover, preliminary SAGE 11 v6.0a retrievals suggest that they are partially accounted for by geometric difficulties at low altitudes in v5.96 and prior retrievals. SAGE ozone trends for the 1979-1996 and 1984-1996 periods are calculated and compared, and the sources of trend errors are discussed. These calculations are made after filtering out ozone data during periods of high, local aerosol extinctions. In the lower stratosphere, below approx. 28 km altitude, there is shown to be excellent agreement in the altitudinal structure of ozone decreases at 45 deg N between SAGE and ozonesondes with the largest decrease in both between 1979 and 1996 having occurred below 20 km altitude, amounting to 0.9 +/- 0.7% yr (2sigma) at 16 km altitude. However, in contrast to the fairly steady decreases at 45 deg N, both SAGE measurements and Lauder ozonesondes show ozone increases at 45 deg S over the period from the mid-1980s to 1996 of 0.2 +/- 0.5%/yr (2sigma) from 15 to 20 km altitude. The SAGE data suggest that this increase is a wintertime phenomenon which occurs in the 15-20 km height range. Changes in dynamics are suggested as the most likely cause of this increase. These hemispheric differences in ozone trends are supported by ozone column measurements by the Total Ozone Mapping Spectrometer (TOMS).

Cunnold, D. M.

Ozone in the Pacific Troposphere from Ozonesonde Observations

Ozone vertical profile measurements obtained from ozonesondes flown at Fiji, Samoa, Tahiti and the Galapagos are used to characterize ozone in the troposphere over the tropical Pacific. There is a significant seasonal variation at each of these sites. At sites in both the eastern and western Pacific, ozone is highest at almost all levels in the troposphere during the September-November season and lowest during, March-May. There is a relative maximum at all of the sites in the mid-troposphere during all seasons of the year (the largest amounts are usually found near the tropopause). This maximum is particularly pronounced during, the September-November season. On average, throughout the troposphere at all seasons, the Galapagos has larger ozone amounts than the western Pacific sites. A trajectory climatology is used to identify the major flow regimes that are associated with the characteristic ozone behavior at various altitudes and seasons. The enhanced ozone seen in the mid-troposphere during September-November is associated with flow from the continents. In the western Pacific this flow is usually from southern Africa (although 10-day trajectories do not always reach the continent), but also may come from Australia and Indonesia. In the Galapagos the ozone peak in the mid-troposphere is seen in flow from the South American continent and particularly from northern Brazil. The time of year and flow characteristics associated with the ozone mixing ratio peaks seen in both the western and eastern Pacific suggest that these enhanced ozone values result from biomass burning. In the upper troposphere low ozone amounts are seen with flow that originates in the convective western Pacific.

Oltmans, S. J.

Origin of Ozone NO(x) in the Tropical Troposphere: A Photochemical Analysis of Aircraft Observations Over the South Atlantic Basin

The photochemistry of the troposphere over the South Atlantic basin is examined by modeling of aircraft observations up to 12-km altitude taken during the TRACE A expedition in September-October 1992. A close balance is found in the 0 to 12-km column between photochemical production and loss Of O3, with net production at high altitudes compensating for weak net loss at low altitudes. This balance implies that O3 concentrations in the 0-12 km column can be explained solely by in situ photochemistry; influx from the stratosphere is negligible. Simulation of H2O2, CH3OOH, and CH2O concentrations measured aboard the aircraft lends confidence in the computations of O3 production and loss rates, although there appears to be a major gap in current understanding of CH2O chemistry in the marine boundary layer. The primary sources of NO(x) over the South Atlantic Basin appear to be continental (biomass burning, lightning, soils). There is evidence that NO(x) throughout the 0 to 12-km column is recycled from its oxidation products rather than directly transported from its primary sources. There is also evidence for rapid conversion of HNO3 to NO(x) in the upper troposphere by a mechanism not included in current models. A general representation of the O3 budget in the tropical troposphere is proposed that couples the large scale Walker circulation and in situ photochemistry. Deep convection in the rising branches of the Walker circulation injects NO(x) from combustion, soils, and lightning to the upper troposphere, leading to O3 production; eventually, the air subsides and net O3 loss takes place in the lower troposphere, closing the O3 cycle. This scheme implies a great sensitivity of the oxidizing power of the atmosphere to NO(x) emissions in the tropics.

Jacob, D. J.

Tropospheric OH in a three-dimensional chemical tracer model - An assessment based on observations of CH3CCl3

The paper introduces the representation of tropospheric chemistry allowing for calculation of chemical reaction rates within a chemical tracer model (CTM) simulation with the accuracy comparable to that of a detailed chemical model. The global distribution of tropospheric OH is calculated as a function of time, atmospheric composition, temperature, and solar irradiance. The globally integrated OH concentration weighted by frequency of reaction with CH3CCl3 is evaluated, along with the feasibility of using the observed latitudinal distribution of CH3CCl3 as a test for computed concentrations of OH. Seasonal variations of CH3CCl3 are also considered as a potential test for computed concentrations of OH. It is demonstrated that annual cycles of CH3CCl3 are controlled, or strongly influenced, by dynamical processes at latitudes northward of 25 deg South.

Spivakovsky, C. M.

Seasonal variations of troposheric ozone at Natal, Brazil

An analysis of ozone measurements from Natal, Brazil (6 deg S, 35 W), with a focus on the seasonal behavior in the troposphere, is presented. The amplitude of seasonal cycle at Natal is much larger than at Panama (9 deg N), the only other tropical site for which similar data are available. Concentrations of ozone in the middle troposphere in the southern spring are unexpectedly high, 60-70 ppb, similar to values found at northern midlatitudes in summer, and larger by 20-30 ppb than values found at Panama and at southern midlatitudes. It is suggested that photochemical production of ozone associated with emissions of CO, hydrocarbons, and NO(x) from biomass burning may contribute significantly to the high values of ozone, but note that stratospheric intrusions could also play a role. The data available at present do not permit a definitive evaluation of the relative importance of these two sources of ozone. The data from Natal, in combination with recent aircraft and surface data, show that tropical ozone exhibits strong spatial and temporal inhomogeneities. The distribution of tropospheric ozone appears to be considerably more complex than the traditional view, which suggested a northern midlatitude maximum and north/-south hemispheric asymmetry. The seasonal cycle in the total column of ozone at Natal appears to mirror the behavior of the tropospheric contribution to the ozone column rather than the stratospheric contribution, and this may account for differences in the annual cycle of the total column at Natal versus other tropical locations.

Logan, J. A.

Reductions of Antarctic ozone due to synergistic interactions of chlorine and bromine

The vertical column density of ozone observed in October over Antarctica has fallen precipitously over the past 10 yr. The concentration at Halley Bay (76 deg S, 27 deg W), expressed conventionally in Dobson units (DU), has dropped from about 300 DU in 1975 to less than 200 DU in 1984. Values in 1985 were even lower, comparable with the lowest values recorded anywhere on earth. It is suggested here that the loss of O3 in Antarctica may be attributed to catalysis of O3 recombination by a scheme in which the rate-limiting step is defined by the reaction of ClO + BrO - Cl + Br + O2. Concentrations of NO2 must be low and heterogeneous reactions involving particles in the polar stratospheric clouds must be an important element of the relevant chemistry. Industrial sources make important contributions to the contemporary budgets of both BrO and ClO and are likely to grow significantly in the future.

Mcelroy, M. B.

Tropospheric ozone - Seasonal behavior, trends, and anthropogenic influence

In the present analysis of tropospheric ozone data, attention is given to spatial and temporal variations. Two modes of seasonal behavior are noted for surface ozone at mid-latitudes: a broad summer maximum within a few hundred km of industrial/urban areas in Europe and the U.S., and a minimum in summer or autumn in sparcely populated regions that are remote from industrial activity. These and limited historical data indicate that summertime concentrations of ozone near the surface in the rural areas of Europe and the U.S. may have increased between 20 and 100 percent since the 1940s. It is suggested that the summer maximum in ozone and other observed trends are due to photochemical production associated with anthropogenic emissions of NO(x), hydrocarbons, and CO from fossil fuel combustion.

Logan, J. A.

Oxygen species

The spatial distribution of ozone, as predicted by numerical models, is compared with observations. A set of reference ozone profiles was developed against which to compare current numerical calculations. Most of the analyses will focus on ozone between 30 and 70 km altitude.

Brasseur, G.

Tropospheric trace gases

Trace gas concentrations in the atmosphere reflect in part the overall metabolism of the biosphere, and in part the broad range of human activities such as agriculture, production of industrial chemicals, and combustion of fossil fuels and biomass. There is compelling evidence that the composition of the atmosphere is now changing. Observed trends in trace gas levels are reviewed and implications for the chemistry of the atmosphere are discussed. Throughout the discussion, particular emphasis is given to those species which are now increasing in the atmosphere.

Gammon, R.

Tropospheric chemistry

The chemistry of the background troposphere, the source region, and the transition regions are discussed. The troposphere is governed by heterogeneous chemistry far more so than the stratosphere. Heterogeneous processes of interest involve scavenging of trace gases by aerosols, cloud and precipitation elements leading to aqueous phase chemical reactions and to temporary and permanent removal of material from the gas phase. Dry deposition is a major removal process for ozone, as well as for other gases of importance in tropospheric photochemistry. These processes are also discussed.

Mohnen, V. A.

Nitrogen oxides in the troposphere - Global and regional budgets

The cycle of nitrogen oxides in the troposphere is discussed from both global and regional perspectives. Global sources for NO(x) are estimated to be of magnitude 50 (+ or - 25) x 10 to the 12th gm N/yr. Nitrogen oxides are derived from combustion of fossil fuels (40 percent) and biomass burning (25 percent) with the balance from lightning and microbial activity in soils. Estimates for the rate of removal of NOx based on recent atmospheric and precipitation chemistry data are consistent with global source strengths derived here. Industrial and agricultural activities provide approximately two thirds of the global source for NOx. In North America, sources from combustion of fossil fuels exceed natural sources by a factor of 3-13. Wet deposition removes about one third of the combustion source of NOx over North America, while dry deposition removes a similar amount. The balance is exported from the continent. Deposition of nitrate in precipitation over eastern Canada and the western Atlantic is clearly influenced by sources of NOx in the eastern United States.

Logan, J. A.

Tropospheric chemistry - A global perspective

Processes that affect the concentration of tropospheric OH are considered, taking into account linkages between the chemistry of OH and the chemistry of H, HO2, and H2O2. A review is presented of observational data of special relevance to OH, notably the distributions of CO, CH4, O3, H2O, HNO3, NO, and NO2. Most of the results presented in connection with the description of the model were obtained by solving time-dependent continuity equations. Rates for photolytic processes were allowed to vary diurnally with insolation. It is found that a well-calibrated and reliable model for OH places important constraints on global budgets for a variety of gases including CH4, H2, and CH3Cl in addition to CO. Accurate measurements of species such as CH3CCl3 can provide valuable checks on global models that must integrate over a variety of atmospheric conditions. However, emission rates for the relevant gases must be adequately quantified.

Logan, J. A.

Oxidation of CS2 and COS - sources for atmospheric SO2

The oxidation of COS and CS2 by reaction with hydroxyl radicals is investigated as a possible source of atmospheric SO2 in remote marine regions. Calculations of the vertical profiles of SO2 were performed based on a one-dimensional photochemical model of the formation and destruction of SO2 by various processes for observed O3, CO, CH4 and H2O profiles at 15 deg S. Variations in the rate of SO2 destruction, the chosen deposition velocity and the loss due to aerosols are shown to lead to similar SO2 profiles, which indicate higher mixing ratios at high altitude, while the oxidation of dimethyl sulfide or hydrogen sulfide can not account for the profiles observed. Possible diffuse sources of CS2 and COS are indicated, and it is concluded that the oxidation of COS and possibly CS2 may provide an explanation for the existence of a uniform background level of SO2.

Logan, J. A.

Atmospheric chemistry - Response to human influence

Global atmospheric chemistry is surveyed, and the agreement of models with observed distribution of gases is considered. The influence of human perturbations due to combustion, agriculture, and chloro-carbon releases is examined with emphasis on ozone. Effects of combustion-related releases of CO on the abundances of other gases as well as possible effects of CO on tropospheric ozone are discussed. Other topics include the contribution of the chlorocarbon industry to stratospheric chloride and the recombination of nitrogen fixed by agriculture and combustion.

Logan, J. A.