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Sze, Nien-Dak

Publications and source records attributed to Sze, Nien-Dak.

Coupling Processes Between Atmospheric Chemistry and Climate

This is the final report. The overall objective of this project is to improve the understanding of coupling processes among atmospheric chemistry, aerosol and climate, all important for quantitative assessments of global change. Among our priority are changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The work emphasizes two important aspects: (1) AER's continued participation in preparation of, and providing scientific input for, various scientific reports connected with assessment of stratospheric ozone and climate. These include participation in various model intercomparison exercises as well as preparation of national and international reports. and (2) Continued development of the AER three-wave interactive model to address how the transport circulation will change as ozone and the thermal properties of the atmosphere change, and assess how these new findings will affect our confidence in the ozone assessment results.

Ko, Malcolm K. W.↗

Coupling Processes Between Atmospheric Chemistry and Climate

This is the final report for NAS5-97039 for work performed between December 1996 and November 1999. The overall objective of this project is to improve the understanding of coupling processes among atmospheric chemistry, aerosol and climate, all important for quantitative assessments of global change. Among our priority are changes in ozone and stratospheric sulfate aerosol, with emphasis on how ozone in the lower stratosphere would respond to natural or anthropogenic changes. The work emphasizes two important aspects: (1) AER's continued participation in preparation of, and providing scientific input for, various scientific reports connected with assessment of stratospheric ozone and climate. These include participation in various model intercomparison exercises as well as preparation of national and international reports. (2) Continued development of the AER three-wave interactive model to address how the transport circulation will change as ozone and the thermal properties of the atmosphere change, and assess how these new findings will affect our confidence in the ozone assessment results.

Ko, Malcolm↗

Stratospheric Cooling and Arctic Ozone Recovery

We present sensitivity studies using the AER( box model for an idealized parcel in the lower stratosphere at 70 N during winter/spring with different assumed stratospheric coolings and chlorine loadings. Our calculations show that stratospheric cooling could further deplete ozone via increased polar stratospheric cloud (PSC) formation and retard its expected recovery even with the projected chlorine loading decrease. We introduce the concept of chlorine-cooling equivalent and show that a 1 K cooling could provide the same local ozone depletion as an increase of chlorine by 0.4-0.7 ppbv for the scenarios considered. Thus, sustained stratospheric cooling could further reduce Arctic ozone content and delay the anticipated ozone recovery in the Northern Hemisphere even with the realization of the Montreal Protocol and its Amendments.

Danilin, Michael Y.↗

Stratospheric Cooling and Arctic Ozone Recovery

We present sensitivity studies using the AER box model for an idealized parcel in the lower stratosphere at 70 deg N during winter/spring with different assumed stratospheric cooling and chlorine loadings. Our calculations show that stratospheric cooling could further deplete ozone via increased polar stratospheric cloud (PSC) formation and retard its expected recovery even with the projected chlorine loading decrease. We introduce the concept of chlorine-cooling equivalent and show that a 1 K Cooling could provide the same local ozone depletion as an increase of chlorine by 0.4-0.7 ppbv for the scenarios considered. Thus, sustained stratospheric cooling could further reduce Arctic ozone content and delay the anticipated ozone recovery in the Northern Hemisphere even with the realization of the Montreal Protocol and its Amendments.

Danilin, Michael Y.↗

Stratospheric Cooling and Arctic Ozone Recovery

We present sensitivity studies using the AER box model for an idealized parcel in the lower stratosphere at 70 deg N during winter/spring with different assumed stratospheric cooling and chlorine loadings. Our calculations show that stratospheric cooling could further deplete ozone via increased polar stratospheric cloud (PSC) formation and retard its expected recovery even with the projected chlorine loading decrease. We introduce the concept of chlorine-cooling equivalent and show that a 1 K cooling could provide the same local ozone depletion as an increase of chlorine by 0.4 - 0.7 ppbv for the scenarios considered. Thus, sustained stratospheric cooling could further reduce Arctic ozone content and delay the anticipated ozone recovery in the Northern Hemisphere even with the realization of the Montreal Protocol and its Amendments.

Danilin, Michael Y.↗

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↗

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.↗

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.↗

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 roles of dynamical and chemical processes in determining the stratospheric concentration of ozone in one-dimensional and two-dimensional models

The two-dimensional model of Ko et al. (1985) was used to calculate the stratospheric concentrations of ozone, to determine the principal modes of balance for different stratospheric regions. The results of this analysis show that the local concentration of ozone in different regions of stratosphere is determined by balances between different mechanisms. In the upper stratosphere, the ozone concentration is dominated by photochemical processes, whereas in the mid-lower stratosphere, the bulk of ozone appears to be controlled by an interaction between the transport and the photochemical processes. The results point to the limitations of one-dimensional models, which fail to properly account for the effect of transport in the lower stratosphere.

Ko, Malcolm K. W.↗

Photochemical modeling of the Antarctic stratosphere: Observational constraints from the airborne Antarctic ozone experiment and implications for ozone behavior

The rapid decrease in O3 column densities observed during Antarctic spring has been attributed to several chemical mechanisms involving nitrogen, bromine, or chlorine species, to dynamical mechanisms, or to a combination of the above. Chlorine-related theories, in particular, predict greatly elevated concentrations of ClO and OClO and suppressed abundances of NO2 below 22 km. The heterogeneous reactions and phase transitions proposed by these theories could also impact the concentrations of HCl, ClNO3 and HNO3 in this region. Observations of the above species have been carried out from the ground by the National Ozone Expedition (NOZE-I, 1986, and NOZE-II, 1987), and from aircrafts by the Airborne Antarctic Ozone Experiment (AAOE) during the austral spring of 1987. Observations of aerosol concentrations, size distribution and backscattering ratio from AAOE, and of aerosol extinction coefficients from the SAM-II satellite can also be used to deduce the altitude and temporal behavior of surfaces which catalyze heterogeneous mechanisms. All these observations provide important constraints on the photochemical processes suggested for the spring Antarctic stratosphere. Results are presented for the concentrations and time development of key trace gases in the Antarctic stratosphere, utilizing the AER photochemical model. This model includes complete gas-phase photochemistry, as well as heterogeneous reactions. Heterogeneous chemistry is parameterized in terms of surface concentrations of aerosols, collision frequencies between gas molecules and aerosol surfaces, concentrations of HCl/H2O in the frozen particles, and probability of reaction per collision (gamma). Values of gamma are taken from the latest laboratory measurements. The heterogeneous chemistry and phase transitions are assumed to occur between 12 and 22 km. The behavior of trace species at higher altitudes is calculated by the AER 2-D model without heterogeneous chemistry. Calculations are performed for solar illumination conditions typical of 60, 70, and 80 S, from July 15 to October 31.

Rodriguez, Jose M.↗

Antarctic ozone decrease: Possible impact on the seasonal and latitudinal distribution of total ozone as simulated by a 2-D model

Satellite borne instruments, the Total Ozone Mapping Spectrometer (TOMS) and the Solar Backscatter Ultraviolet spectrometer (SBUV), show that total column ozone has decreased by more than 5 percent in the neighborhood of 60 S at all seasons since 1979. This is considerably larger than the decrease calculated by 2-D models which take into account solar flux variation and increases of trace gas concentrations over the same period. The meteorological conditions (warmer temperature and the apparent lack of polar stratospheric clouds) at these latitudes do not seem to favor heterogeneous chemistry as the direct cause for the observed ozone reduction. A mechanism involving the seasonal transport of ozone-poor air mass from within the polar vortex to lower latitudes (the so-called dilution effect) is proposed as a possible explanation for the observed year-round ozone reduction in regions away from the vortex.

Ko, Malcolm K. W.↗