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Wuebbles, D. J.

Publications and source records attributed to Wuebbles, D. J..

An Intercomparative Study of the Effects of Aircraft Emissions on Surface Air Quality

This study intercompares, among five global models, the potential impacts of all commercial aircraft emissions worldwide on surface ozone and particulate matter (PM (sub 2.5)). The models include climate-response models (CRMs) with interactive meteorology, chemical-transport models (CTMs) with prescribed meteorology, and models that integrate aspects of both. Model inputs are harmonized in an effort to achieve a consensus about the state of understanding of impacts of 2006 commercial aviation emissions. Models find that aircraft increase near-surface ozone (0.3 to 1.9 percent globally), with qualitatively similar spatial distributions, highest in the Northern Hemisphere. Annual changes in surface-level PM (sub 2.5) in the CTMs (0.14 to 0.4 percent) and CRMs (-1.9 to 1.2 percent) depend on differences in nonaircraft baseline aerosol fields among models and the inclusion of feedbacks between aircraft emissions and changes in meteorology. The CTMs tend to result in an increase in surface PM (sub 2.5) primarily over high-traffic regions in the North American midlatitudes. The CRMs, on the other hand, demonstrate the effects of aviation emissions on changing meteorological fields that result in large perturbations over regions where natural emissions (e.g., soil dust and sea spray) occur. The changes in ozone and PM (sub 2.5) found here may be used to contextualize previous estimates of impacts of aircraft emissions on human health.

Air quality

Our Globally Changing Climate

Since the Third U.S. National Climate Assessment (NCA3) was published in May 2014, new observations along multiple lines of evidence have strengthened the conclusion that Earth's climate is changing at a pace and in a pattern not explainable by natural influences. While this report focuses especially on observed and projected future changes for the United States, it is important to understand those changes in the global context (this chapter). The world has warmed over the last 150 years, especially over the last six decades, and that warming has triggered many other changes to Earth's climate. Evidence for a changing climate abounds, from the top of the atmosphere to the depths of the oceans. Thousands of studies conducted by tens of thousands of scientists around the world have documented changes in surface, atmospheric, and oceanic temperatures; melting glaciers; disappearing snow cover; shrinking sea ice; rising sea level; and an increase in atmospheric water vapor. Rainfall patterns and storms are changing, and the occurrence of droughts is shifting.

Wuebbles, D. J.

Model study of atmospheric transport using carbon 14 and strontium 90 as inert tracers

The observed excess carbon 14 in the atmosphere from 1963 to 1970 provides unique, but limited, data up to an altitude of about 35 km for testing the air motions calculated by 11 multidimensional atmospheric models. Strontium 90 measurements in the atmosphere from 1964 to mid-1967 provide data that have more latitude coverage than those of carbon 14 and are useful for testing combined models of air motions and aerosol settling. Model calculations for carbon 14 begin at October 1963, 9 months after the conclusion of the nuclear bomb tests; the initial conditions for the calculations are derived by three methods, each of which agrees fairly well with measured carbon 14 in October 1963 and each of which has widely different values in regions of the stratosphere where there were no carbon 14 measurements. The model results are compared to the stratospheric measurements, not as if the observed data were absolute standards, but in an effort to obtain new insight about the models and about the atmosphere. The measured carbon 14 vertical profiles at 31 deg N are qualitatively different from all of the models; the measured vertical profiles show a maximum mixing ratio in the altitude range of 20 to 25 km from October 1963 through July 1966, but all modeled profiles show mixing ratio maxima that increase in altitude from 20 km in October 1963 to greater than 40 km by April 1966. Both carbon 14 and strontium 90 data indicate that the models differ substantially among themselves with respect to stratosphere-troposphere exchange rate, but the modeled carbon 14 stratospheric residence times indicate that differences among the models are small with respect to transport rate between the middle stratosphere and the lower stratosphere. Strontium 90 data indicate that aerosol settling is important up to at least 35 km altitude. Relative to the measurements, about three quarters of the models transport carbon 14 from the lower stratosphere to the troposphere too rapidly, and all models with all three sets of initial conditions appear to sweep carbon 14 out of the midstratosphere (above 28 km) much more slowly than was observed from 1963 to 1970. Atmospheric dynamicists should seriously consider that the carbon 14 measurements imply with respect to advection in the midstratosphere.

Kinnison, D. E.

Observations of lower-stratospheric ClONO2, HNO3, and aerosol by the UARS CLAES experiment between January 1992 and April 1993

This paper discusses simultaneous measurements of stratospheric ClONO2, HNO3, temperature, and aerosol extinction coefficient by the Cryogenic Limb Array Etalon Spectrometer (CLAES) on the NASA Upper Atmosphere Research Satellite (UARS), obtained over the period 9 January 1992 through 23 April 1993. The discussion concentrates on the stratosphere region near 21 km of particular interest to heterogeneously driven ozone depletion. For periods between 12 June and 1 September 1992 at latitudes poleward of about 60 deg S, when temperatures were below type I polar stratospheric cloud (PSC) formation thresholds throughout the lower stratosphere, CLAES observed high levels of PSCs coincident with highly depleted fields of both HNO3 and ClONO2. By 17 September, the incidence of PSCs had greatly diminished in the lower stratosphere, but both CLONO2 and HNO3 remained highly depleted. These observations are consistent with the removal of gaseous HNO3 through the formation of nitric acid trihydrate (NAT) particles and the removal of ClONO2 through heterogeneous reactions on the particle surfaces. They also suggest substantial denitrification of the lower Antarctic vortex through sedimentation of PSC particles. In the Northern Hemisphere winter of 1992/93 far fewer PSCs were observed in the Arctic lower-stratosphere vortex, which had shorter periods and more localized regions of cold temperatures. Both HNO3 and ClONO2 maintained much higher levels inside the Arctic vortex than seen in the Antarctic throughout the winter/spring period. Following 28 February 1993 when Arctic vortex temperatures rose above 195 K, ClONO2 was observed in large quantities (greater than 2.1 ppbv near 21 km) inside the vortex. The persistence of relatively high levels of HNO3 inside the Arctic spring vortex compared with the low levels seen in the Antarctic spring vortex suggest a much lower level of denitrification in the Arctic.

Roche, A. E.

Effect of vibrationally excited oxygen on ozone production in the stratosphere

Photolysis of vibrationally excited oxygen produced by ultraviolet photolysis of ozone in the upper stratosphere is incorporated into the Lawrence Livermore National Laboratory two-dimensional zonally averaged chemical-radiative-transport model of the troposphere and stratosphere. The importance of this potential contributor of odd oxygen to the concentration of ozone is evaluated based on recent information on vibrational distributions of excited oxygen and on preliminary studies of energy transfer from the excited oxygen. When energy transfer rate constants similar to those of Toumi et al. (1991) are assumed, increases in model ozone concentrations of up to 4.0% in the upper stratosphere are found, and the model ozone concentrations are found to agree slightly better with measurements, including recent data from the Upper Atmosphere Research Satellite. However, the ozone increase is only 0.3% when the larger energy transfer rate constants indicated by recent experimental work are applied to the model. An ozone increase of 1% at 50 km requires energy transfer rate constants one-twentieth those of the preliminary observations. As a result, vibrationally excited oxygen processes probably do not contribute enough ozone to be significant in models of the upper stratosphere.

Patten, K. O., Jr.

Model predictions of ozone changes

The predictions of several one-dimensional models were examined for a number of prescribed scenarios in steady-state or time-dependent approximations. A small number of two-dimensional steady-state calculations for a limited number of scenarios were compared with the results of one-dimensional models. The sensitivity of the calculated predictions to the values of input parameters were examined in order to assess recognized uncertainties in these predictions.

Johnston, H. S.

Rate of reaction of OH with HNO3

Measurements of the kinetics of the reaction of OH with HNO3, and mechanisms of HNO3 removal from the stratosphere, are reported. Bimolecular rate constants were determined at temperatures between 224 and 366 K by monitoring the concentrations of OH radicals produced by HNO3 photolysis and HNO3 according to their resonance fluorescence and 184.9-nm absorption, respectively. The rate constant measured at 298 K is found to be somewhat faster than previously accepted values, with a negative temperature dependence. Calculations of a one-dimensional transport-kinetic atmospheric model on the basis of the new rate constant indicate reductions in O3 depletion due to chlorofluoromethane release and NOx injection, of magnitudes dependent on the nature of the reaction products.

Wine, P. H.

On the theoretical model for vertical ozone density distributions in the mesosphere and upper stratosphere.

Calculations based on an improved, time-dependent theoretical model for the vertical ozone density distribution in the upper atmosphere are shown to clarify the cause and determine the appearance precondition for the depression at the 70-85 km altitude region in the ozone density distribution suggested by several theoretical models and only sometimes experimentally observed. It is concluded that the depression develops at night through the effects of hydrogen-oxygen and nitrogen-oxygen reactions, as well as those of eddy diffusion transports.

Shimazaki, T.