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Ko, Malcolm K. W.

Publications and source records attributed to Ko, Malcolm K. W..

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Coupling Processes between Atmospheric Chemistry and Climate

This is the fourth semi-annual report for NAS5-97039, covering the time period July through December 1998. The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling tools for this work are the Atmospheric and Environmental Research (AER) two-dimensional chemistry-transport model, the AER two-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry. For this six month period, we report on a modeling study of new rate constant which modify the NOx/NOy ratio in the lower stratosphere; sensitivity to changes in stratospheric water vapor in the future atmosphere; a study of N2O and CH4 observations which has allowed us to adjust diffusion in the 2-D CTM in order to obtain appropriate polar vortex isolation; a study of SF6 and age of air with comparisons of models and measurements; and a report on the Models and Measurements II effort.

Ko, Malcolm K. W.↗

Coupling Processes Between Atmospheric Chemistry and Climate

The overall objective of this project is to improve the understanding of coupling processes between atmospheric chemistry and climate. Model predictions of the future distributions of trace gases in the atmosphere constitute an important component of the input necessary for quantitative assessments of global change. We will concentrate on the changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The key modeling tools for this work are the AER 2-dimensional chemistry-transport model, the AER 2-dimensional stratospheric sulfate model, and the AER three-wave interactive model with full chemistry. We will continue developing our three-wave model so that we can help NASA determine the strength and weakness of the next generation assessment models.

Ko, Malcolm K. W.↗

HSCT Assessment Calculations with the AER 2-D Model: Sensitivities to Transport Formulation, PSC Formulation, Interannual Temperature Variation

The summary are: (1) Some chemical differences in background atmosphere are surprisingly large (NOY). (2) Differences in model transport explain a majority of the intertnodel differences in the absence of PSCs. (3) With PSCS, large differences exist in predicted O3 depletion between models with the same transport. (4) AER/LLNL model calculates more O3 depletion in NH than LLNL. (5) AER/GSFC model cannot match calculated O3 depletion of GSFC model in SH. and (6) Results sensitive to interannual temperature variations (at least in NH).

Weisenstein, Debra K.↗

On the Relation between Stratospheric Chlorine/Bromine Loading and Short-Lived Tropospheric Source Gases

Current methods for estimating the concentrations of inorganic chlorine/bromine species Cl(y)/Br(y) in the stratosphere due to decomposition of tropospheric source gases assume that the Cl(y)/Br(y) concentration in the stratosphere is determined mainly by the balance between production from in situ oxidation of the source gases in the stratosphere and removal by transport of Cl(y)/Br(y) out of the stratosphere. The rationale being that for source gases whose lifetimes are of the order of several months or longer the concentration of Cl(y)/Br(y) in the troposphere is small because they are produced at a relatively slow rate and also removed efficiently by washout processes. As a result of the small concentration, the rate at which Cl(y)/Br(y) is transported to the stratosphere is expected to be small compared to the in situ stratospheric production. Thus the transport of Cl(y)/Br(y) from the troposphere contributes little to the stratospheric concentration. In contrast, the origin of stratospheric Cl(y)/Br(y) from reactive source gases with tropospheric lifetimes comparable to the washout lifetime of Cl(y)/Br(y) (of the order of 10-30 days) in the troposphere is distinctly different. The in situ source in the stratosphere is expected to be significantly smaller because only a small portion of the source gas is expected to survive the troposphere to be transported into this region. At the same time these short-lived source gases produce appreciable amounts of Cl(y)/Br(y) in the troposphere such that transport to the stratosphere offers a larger source for stratospheric Cl(y)/Br(y) than in situ production. Thus, for reactive source species, simple methods of estimating the concentration of stratospheric Cl(y)/Br(y) that ignore the tropospheric contribution will seriously underestimate the loading. Therefore estimation of the stratospheric Cl(y)/Br(y) loading requires not only measurements of tropospheric source gases but also measurements of Cl(y)/Br(y) at the tropopause. This paper illustrates the mechanism by using results from a two-dimensional chemistry-transport model. However, in view of the importance of tropospheric transport on stratospheric loading the detailed values should be further evaluated using a three-dimensional model with appropriate treatment of convective transport.

Ko, Malcolm K. W.↗

A Three-Wave Model of the Stratosphere with Coupled Dynamics, Radiation and Photochemistry

A zonal mean chemistry transport model (2-D CTM) coupled with a semi-spectral dynamical model is used to simulate the distributions of trace gases in the present day atmosphere. The zonal-mean and eddy equations for the velocity and the geopotential height are solved in the semi-spectral dynamical model. The residual mean circulation is derived from these dynamical variables and used to advect the chemical species in the 2- D CTM. Based on a linearized wave transport equation, the eddy diffusion coefficients for chemical tracers are expressed in terms of the amplitude, frequency and growth rate of dynamical waves; local chemical loss rates; and a time constant parameterizing small scale mixing. The contributions to eddy flux are from the time varying wave amplitude (transient eddy), chemical reactions (chemical eddy) and small scale mixing. In spite of the high truncation in the dynamical module (only three longest waves are resolved), the model has simulated many observed characteristics of stratospheric dynamics and distribution of chemical species including ozone. Compared with the values commonly used in 2-D CTMs, the eddy diffusion coefficients for chemical species calculated in this model are smaller, especially in the subtropics. It is also found that the chemical eddy diffusion has only a small effects in determining the distribution of most slow species, including ozone in the stratosphere.

Shia, Run-Lie↗

An Estimation of the Climatic Effects of Stratospheric Ozone Losses during the 1980s

In order to study the potential climatic effects of the ozone hole more directly and to assess the validity of previous lower resolution model results, the latest high spatial resolution version of the Atmospheric and Environmental Research, Inc., seasonal radiative dynamical climate model is used to simulate the climatic effects of ozone changes relative to the other greenhouse gases. The steady-state climatic effect of a sustained decrease in lower stratospheric ozone, similar in magnitude to the observed 1979-90 decrease, is estimated by comparing three steady-state climate simulations: 1) 1979 greenhouse gas concentrations and 1979 ozone, II) 1990 greenhouse gas concentrations with 1979 ozone, and III) 1990 greenhouse gas concentrations with 1990 ozone. The simulated increase in surface air temperature resulting from nonozone greenhouse gases is 0.272 K. When changes in lower stratospheric ozone are included, the greenhouse warming is 0.165 K, which is approximately 39% lower than when ozone is fixed at the 1979 concentrations. Ozone perturbations at high latitudes result in a cooling of the surface-troposphere system that is greater (by a factor of 2.8) than that estimated from the change in radiative forcing resulting from ozone depiction and the model's 2 x CO, climate sensitivity. The results suggest that changes in meridional heat transport from low to high latitudes combined with the decrease in the infrared opacity of the lower stratosphere are very important in determining the steady-state response to high latitude ozone losses. The 39% compensation in greenhouse warming resulting from lower stratospheric ozone losses is also larger than the 28% compensation simulated previously by the lower resolution model. The higher resolution model is able to resolve the high latitude features of the assumed ozone perturbation, which are important in determining the overall climate sensitivity to these perturbations.

MacKay, Robert M.↗

Bromine-Chlorine Coupling in the Antarctic Ozone Hole

The contribution from the chlorine and bromine species in the formation of the Antarctic ozone hole is evaluated. Since chlorine and bromine compounds are of different industrial origin, it is desirable, from a policy point of view, to be able to attribute chlorine-catalyzed loss of ozone with those reactions directly involving chlorine species, and likewise for bromine-catalyzed loss. In the stratosphere, however, most of the chemical families are highly coupled, and, for example, changes in the chlorine abundance will alter the partitioninig in other families and thus the rate of ozone loss. This modeling study examines formation of the Antarctic ozone hole for a wide range of bromine concentrations (5 - 25 pptv) and for chlorine concentrations typical of the last two decades (1.5, 2.5 and 3.5 ppbv). We follow the photochemical evolution of a single parcel of air, typical of the inner Antarctic vortex (50 mbar, 70 deg. S, NO(sub y) = 2 ppbv, with Polar Stratospheric Clouds(PSC)) from August 1 to November 1. For all of these ranges of chlorine and bromine loading, we would predict a substantial ozone hole (local depletion greater than 90%) within the de-nitrified, PSC- perturbed vortex. The contributions of the different catalytic cycles responsible for ozone loss are tabulated. The deep minimum in ozone is driven primarily by the chlorine abundance. As bromine levels decrease, the magnitude of the chlorine-catalyzed ozone loss increases to take up the slack. This is because bromine suppresses ClO by accelerating the conversion of ClO an Cl2O2 back to HCI. For this range of conditions, the local relative efficiency of ozone destruction per bromine atom to that per chlorine atom (alpha-factor) ranges from 33 to 55, decreasing with increase of bromine.

Danilin, Michael Y.↗

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

UARS data sets provide global coverage for the distributions of trace gases, which gives us an excellent chance to utilize the data set for model-data intercomparison studies. In the past three months, we have been working on the comparisons of the UARS data between 1992 (a half year after the Pinatubo eruption) and 1993 (one and a half year after the eruption) in an attempt to see how the Pinatubo volcanic eruption may have impacted stratospheric chemistry.

Rodriquez, Jose M.↗

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

We proposed model-data intercomparison studies for UARS data. In the past three months, we have been working on constructing analysis tools to diagnose the UARS data. The 'Trajectory mapping' technique, which was developed by Morris (1994), is adaptable to generate synoptic maps of trace gas data from asynoptic observations. An in-house trajectory model (kinematic methods following Merrill et al., 1986 and Pickering et al., 1994) has been developed in AER under contract with NASA/ACMAP and the trajectory mapping tool has been applied to analyze UARS measurement.

Rodriquez, Jose M.↗

Effects on stratospheric ozone from high-speed civil transport: Sensitivity to stratospheric aerosol loading

The potential impact of high-speed civil transport (HSCT) aircraft emissions on stratospheric ozone and the sensitivity of these results to changes in aerosol loading are examined with a two-dimensional model. With aerosols fixed at background levels, calculated ozone changes due to HSCT aircraft emissions range from negligible up to 4-6% depletions in column zone at northern high latitudes. The magnitude of the ozone change depends mainly on the NO(x) increase due to aircraft emissions, which depends on fleet size, cruise altitude, and engine design. The partitioning of the odd nitrogen species in the lower stratosphere among NO, NO2, N2O5, is strongly dependent on the concentration of sulfuric acid aerosol particles, and thus the sensitivity of O3 to NO(x) emissions changes when the stratospheric aerosol loading changes. Aerosol concentrations 4 times greater than background levels have not been unusual in the last 2 decades. Our model results show that a factor of 4 increase in aerosol loading would significantly reduce the calculated ozone depletion due to HSCT emissions. Because of the neutral variabiltiy of stratospheric aerosols, the possible impact of HSCT emissions on ozone must be viewed as a range of possible results.

Weisenstein, Debra K.↗

A two-dimensional model with coupled dynamics, radiation, and photochemistry. 1: Simulation of the middle atmosphere

Spatial and seasonal distribution of ozone and other trace gases are simulated using a interactive two-dimensional model of the stratosphere updated to include full gas phase chemistry. The model consists of a primitive equation dynamics module, a full radiative transfer scheme, and a comprehensive gas phase chemistry module. The circulation is derived from heating rates in the stratosphere that are calculated using model-generated ozone. In the troposphere, parameterized heating rates are adopted. The eddy momentum flux divergence in the zonal mean momentum equation is given by the eddy fluxes of potential vorticity. Eddy fluxes of potential vorticity and tracers are parameterized using a set of predetermined diffusion coefficients. The adopted values for K(sub yy), show a hemispherical asymmetry in that the values in the lower stratosphere are consistently smaller in the southern hemisphere. The asymmetry in K(sub yy) and in the parameterization of the tropospheric heating rate results in an asymmetry in the circulation giving rise to unique signatures in the trace gas distributions. The model successfully simulates the observed asymmetry in the column abundance of the springtime ozone maxima between northern and southern hemisphere. Results for other trace gases are in agreement with the gross observed features although specific differences exist.

Ko, Malcolm K. W.↗

A two-dimensional model with coupled dynamics, radiative transfer, and photochemistry. 2: Assessment of the response of stratospheric ozone to increased levels of CO2, N2O, CH4, and CFC

The impact of increased levels of carbon dioxide (CO2), chlorofluorocarbons (CFCs), and other trace gases on stratospheric ozone is investigated with an interactive, two-dimensional model of gas phase chemistry, dynamics, and radiation. The scenarios considered are (1) a doubling of the CO2 concentration, (2) increases of CFCs, (3) CFC increases combined with increases of nitrous oxide (N2O) and methane CH4, and (4) the simultaneous increase of CO2, CFCs, N2O, and CH4. The radiative feedback and the effect of temperature and circulation changes are studied for each scenario. For the double CO2 calculations the tropospheric warming was specified. The CO2 doubling leads to a 3.1% increase in the global ozone content. Doubling of the CO2 concentrations would lead to a maximum cooling of about 12 C at 45 km if the ozone concentration were held fixed. The cooling of the stratosphere leads to an ozone increase with an associated increase in solar heating, reducing the maximum temperature drop by about 3 C. The CFC increase from continuous emissions at 1985 rate causes a 4.5% loss of ozone. For the combined perturbations a net loss of 1.3% is calculated. The structure of the perturbations shows a north-south asymmetry. Ozone losses (when expressed in terms of percent changes) are generally larger in the high latitudes of the southern hemisphere as a result of the eddy mixing being smaller than in the northern hemisphere. Increase of chlorine leads to ozone losses above 30 km altitude where the radiative feedback results in a cooler temperature and an ozone recovery of about one quarter of the losses predicted with a noninteractive model. In all the cases, changes in circulation are small. In the chlorine case, circulation changes reduce the calculated column depletion by about one tenth compared to offline calculations.

Schneider, Hans R.↗

Atmospheric sulfur hexafluoride - Sources, sinks and greenhouse warming

An estimate is obtained of worldwide production of SF6, from which a global emission rate is derived and extrapolated for the next 20 years. The atmospheric lifetime of SF6 is then estimated based on a known mechanism (e.g., photolysis and atmospheric oxidation) and/or on the mass balance method. Finally, the radiative forcing of SF6 is calculated based on recent laboratory IR absorption data, and the expected warming over the time period 1950-2010 is computed for several emission scenarios. Calculations showed that SF6 is 3 times more effective as a greenhouse gas compared to CFC 11 on a per-molecule basis. However, based on projected emission scenarios, the expected warming from SF6 through 2010 is small (0.004 C), compared to the warming from CO2 and other trace gases (0.8 C).

Ko, Malcolm K. W.↗

Interrelationships between mixing ratios of long-lived stratospheric constituents

Relationships between the simultaneously measured mixing ratios of certain stratospheric constituents that are sometimes linear are argued to be expected for species of sufficiently long lifetime. Species whose local lifetimes are longer than quasi-horizontal-transport time scales are in climatological slope equilibrium, i.e., they share surfaces of constant mixing ratio, and a scatter plot of the mixing ratio of one versus that of the other collapses to a compact curve whose slope at any point is the ratio of the net global fluxes of the two species through the corresponding surface of constant mixing ratio. Species whose local lifetimes are greater than vertical transport time scales are in gradient equilibrium and their mixing ratios display a linear relationship. These statements are illustrated using results from a 2D chemistry-transport model.

Plumb, R. A.↗

The chlorine budget of the present-day atmosphere - A modeling study

The contribution of source gases to the total amount of inorganic chlorine (ClY) is examined analytically with a time-dependent model employing 11 source gases. The source-gas emission data are described, and the modeling methodology is set forth with attention given to the data interpretation. The abundances and distributions are obtained for all 11 source gases with corresponding ClY production rates and mixing ratios. It is shown that the ClY production rate and the ClY mixing ratio for each source gas are spatially dependent, and the change in the relative contributions from 1950 to 1990 is given. Ozone changes in the past decade are characterized by losses in the polar and midlatitude lower stratosphere. The values for CFC-11, CCl4, and CH3CCl3 suggest that they are more evident in the lower stratosphere than is suggested by steady-state estimates based on surface concentrations.

Weisenstein, Debra K.↗

The Atmospheric Effects of Stratospheric Aircraft: a First Program Report

Studies have indicated that, with sufficient technology development, high speed civil transport aircraft could be economically competitive with long haul subsonic aircraft. However, uncertainty about atmospheric pollution, along with community noise and sonic boom, continues to be a major concern; and this is addressed in the planned 6 yr HSRP begun in 1990. Building on NASA's research in atmospheric science and emissions reduction, the AESA studies particularly emphasizing stratospheric ozone effects. Because it will not be possible to directly measure the impact of an HSCT aircraft fleet on the atmosphere, the only means of assessment will be prediction. The process of establishing credibility for the predicted effects will likely be complex and involve continued model development and testing against climatological patterns. Lab simulation of heterogeneous chemistry and other effects will continue to be used to improve the current models.

Prather, Michael J.↗

Ozone Response to Aircraft Emissions: Sensitivity Studies with Two-dimensional Models

Our first intercomparison/assessment of the effects of a proposed high-speed civil transport (HSCT) fleet on the stratosphere is presented. These model calculations should be considered more as sensitivity studies, primarily designed to serve the following purposes: (1) to allow for intercomparison of model predictions; (2) to focus on the range of fleet operations and engine specifications giving minimal environmental impact; and (3) to provide the basis for future assessment studies. The basic scenarios were chosen to be as realistic as possible, using the information available on anticipated developments in technology. They are not to be interpreted as a commitment or goal for environmental acceptability.

Ko, Malcolm K. W.↗

Role of heterogeneous conversion of N2O5 on sulphate aerosols in global ozone losses

The reaction rate of N2O5 on sulphate aerosols is included in a model to predict global ozone loss and the column abundances of atmospheric gases. Because the reaction of N2O5 and the aerosols can take place in the stratospheric sulphate aerosol layer, it is included in the 2D model so that the results can be compared to abundances derived from satellite data and ground-based measurements. The N2O5/sulphate reaction is the only heterogeneous reaction in the model, in which aerosol loading is assumed to be constant and only diurnal values are examined. The decadal ozone trends resulting from calculations based on the model are found to be closer to the observed values. An important conclusion is that measurements of OH, ClO, HNO3, NO, and NO2 in the region of about 14-25 km are needed to examine significant changes in their abundances resulting from the inclusion of the N2O5/sulphate aerosol reaction.

Rodriguez, Jose M.↗