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Yung, Yuk L.

Publications and source records attributed to Yung, Yuk L..

At least 37 records · Page 2

Chemistry and Transport in a Multi-Dimensional Model

Our work has two primary scientific goals, the interannual variability (IAV) of stratospheric ozone and the hydrological cycle of the upper troposphere and lower stratosphere. Our efforts are aimed at integrating new information obtained by spacecraft and aircraft measurements to achieve a better understanding of the chemical and dynamical processes that are needed for realistic evaluations of human impact on the global environment. A primary motivation for studying the ozone layer is to separate the anthropogenic perturbations of the ozone layer from natural variability. Using the recently available merged ozone data (MOD), we have carried out an empirical orthogonal function EOF) study of the temporal and spatial patterns of the IAV of total column ozone in the tropics. The outstanding problem about water in the stratosphere is its secular increase in the last few decades. The Caltech/PL multi-dimensional chemical transport model (CTM) photochemical model is used to simulate the processes that control the water vapor and its isotopic composition in the stratosphere. Datasets we will use for comparison with model results include those obtained by the Total Ozone Mapping Spectrometer (TOMS), the Solar Backscatter Ultraviolet (SBUV and SBUV/2), Stratosphere Aerosol and Gas Experiment (SAGE I and II), the Halogen Occultation Experiment (HALOE), the Atmospheric Trace Molecular Spectroscopy (ATMOS) and those soon to be obtained by the Cirrus Regional Study of Tropical Anvils and Cirrus Layers Florida Area Cirrus Experiment (CRYSTAL-FACE) mission. The focus of the investigations is the exchange between the stratosphere and the troposphere, and between the troposphere and the biosphere.

Yung, Yuk L.↗

Interannual Variability of Snow and Ice and Impact on the Carbon Cycle

The goal of this research is to assess the impact of the interannual variability in snow/ice using global satellite data sets acquired in the last two decades. This variability will be used as input to simulate the CO2 interannual variability at high latitudes using a biospheric model. The progress in the past few years is summarized as follows: 1) Albedo decrease related to spring snow retreat; 2) Observed effects of interannual summertime sea ice variations on the polar reflectance; 3) The Northern Annular Mode response to Arctic sea ice loss and the sensitivity of troposphere-stratosphere interaction; 4) The effect of Arctic warming and sea ice loss on the growing season in northern terrestrial ecosystem.

Yung, Yuk L.↗

A Mechanism For Solar Forcing of Climate: Did the Maunder Minimum Cause the Little Ice Age?

The mechanism we wish to demonstrate exploits chemical, radiative, and dynamical sensitivities in the stratosphere to affect the climate of the troposphere. The sun, while its variability in total radiative output over the course of the solar cycle is on the order of 0.1%, exhibits variability in the UV output on the order of 5%. We expect to show that a substantially decreased solar UV output lessened the heating of the Earth's stratosphere during the Maunder Minimum, through decreased radiative absorption by ozone and oxygen. These changes in stratospheric heating would lead to major changes in the stratospheric zonal wind pattern which would in turn affect the propagation characteristics of planetary-scale waves launched in the winter hemisphere. Until recently, there was no quantitative data to relate the changes in the stratosphere to those at the surface. There is now empirical evidence from the NCEP Reanalysis data that a definitive effect of the solar cycle on climate in the troposphere exists. Our recent work is summarized as follows (see complete list of publications in later part of this report).

Yung, Yuk L.↗

Photochemical Studies of Chemistry in the Outer Solar System

The goal of the proposed science investigation is to gain a quantitative understanding of chemical processes and their coupling with atmospheric dynamics in the reducing atmospheres of the outer solar system, with a particular focus on Infrared Space Observatory (ISO) observations and future experiments such as the Cassini Mission to Saturn and Titan. The proposed work is divided into two related tasks. We have carried out a systematic comparison between atmospheric models for every giant planet and Titan, which employ a consistent set of photochemical reactions. Combined with recent observations of hydrocarbon species by ISO, this can provide the most rigorous test of our current understanding of the photochemistry of hydrocarbon in the outer solar system. The emphasis will be on the methyl radical (CH3), first detected by IS0 in the atmospheres of Saturn and Neptune (Bezard et al. 1998). CH3 is one of the most important radicals in the hydrocarbon photochemistry because it is the primary product of methane photolysis and plays an essential role in forming C2H6, the most abundant and stable C2 species. A fundamental understanding of the distribution of CH3 provides unique insights into the chemistry of hydrocarbons as well as comparative planetology.

Yung, Yuk L.↗

Variability of Clouds Over a Solar Cycle

One of the most controversial aspects of climate studies is the debate over the natural and anthropogenic causes of climate change. Historical data strongly suggest that the Little Ice Age (from 1550 to 1850 AD when the mean temperature was colder by about 1 C) was most likely caused by variability of the sun and not greenhouse molecules (e.g., CO2). However, the known variability in solar irradiance and modulation of cosmic rays provides too little energy, by many orders of magnitude, to lead to climate changes in the troposphere. The conjecture is that there is a 'trigger mechanism'. This idea may now be subjected to a quantitative test using recent global datasets. Using the best available modern cloud data from International Satellite Cloud Climatology Project (ISCCP), Svensmark and Friis-Christensen found a correlation of a large variation (3-4%) in global cloud cover with the solar cycle. The work has been extended by Svensmark and Marsh and Svensmark. The implied forcing on climate is an order of magnitude greater than any previous claims. Are clouds the long sought trigger mechanism? This discovery is potentially so important that it should be corroborated by an independent database, and, furthermore, it must be shown that alternative explanations (i.e., El Nino) can be ruled out. We used the ISCCP data in conjunction with the Total Ozone Mapping Spectrometer (TOMS) data to carry out in in depth study of the cloud trigger mechanism.

Yung, Yuk L.↗

Chemistry and Transport In a Multi-Dimensional Model

The focus of the work funded under this proposal is the exchange between the stratosphere and the troposphere, and between the troposphere and the blaspheme. These two interfaces represent the frontiers of atmospheric chemistry. It is the combination of exchange processes at both interfaces that ultimately controls how the blaspheme (including human activities) affects the ozone layer. The modeling work was motivated by and attempts to integrate information obtained by aircraft, spacecraft, shuttle and oceanic measurements. The model development and research activities accomplished in the past three years provide a technical and intellectual basis for the research in this group. The innovative part of our research program is related to the IAV of ozone and the hydrological cycle. Other related but independently supported work include the study of isotopic fractionation of atmospheric species, e.g., N2O and CO2. Our theory suggests that we now have the ability to probe the middle atmosphere at a level of sensitivity where subtle details such as the isotopic composition of simple molecules can yield measurable systematic effects. This creates the possibility for probing the chemistry and dynamics of the middle atmosphere using all of the N2O and CO2 isotopologues. In the following we will briefly describe the model development and review the highlights of recent accomplishments.

Yung, Yuk L.↗

Study of Tropospheric Ozone and UV Reflectivity Using TOMS Data

Perhaps the single most important result from the study of Chuang and Yung is that the interannual variability of the Earth's albedo (especially in Spring) on land is dominated by snow/ice, and not by clouds. This interannual variability could be the major driver of changes in the atmosphere and the biosphere. It is plausible that the interannual variability of snow/ice, through interactions with the atmosphere and biosphere, is responsible for the interannual variability of atmospheric CO2. By carefully studying the albedo variations off the Peru coast, we found evidence for indirect aerosol effect on clouds. Based on a detailed analysis of the cloud data obtained by the International Satellite Cloud Climatology Project (SCCP) in the years 1983-1991, we show that besides the reported 3 % variation in global cloudiness, the global mean cloud optical thickness (MCOT) also has significant variation which is out of phase with that of the global cloudiness. The combined effect of the two opposing variations may be a null effect on the cloud reflectivity. These results are consistent with the Total Ozone Mapping Spectrometer (TOMS) reflectively measurements. The MCOT variation is further shown to be correlated with both the solar cycle and the ENSO (El Nino Southern Oscillation) cycle. Our present analysis cannot distinguish which of the above two provides better correlation, although independent data from the High resolution Infrared Radiation Sounder (HIRS) from 1990 to 1996 favor the solar cycle. Future data are needed to identify the true cause of these changes.

Yung, Yuk L.↗

Photochemical Modeling of CH3 Abundances in the Outer Solar System

Recent measurements of methyl radicals (CH3) in the upper atmospheres of Saturn and Neptune by the Infrared Space Observatory (ISO) provide new constraints to photochemical models of hydrocarbon chemistry in the outer solar system. The derived column abundances of CH3 on Saturn above 10 mbar and Neptune above the 0.2 mbar pressure level are (2.5 - 6.0) x 10(exp 13) / sq cm and (0.7 - 2.8) x 10(exp 13) / sq cm, respectively. We use the updated Caltech/Jet Propulsion Laboratory photochemical model, which incorporates hydrocarbon photochemistry, vertical molecular and bulk atmospheric eddy diffusion, and realistic radiative transfer modeling, to study the CH3 abundances in the upper atmosphere of the giant planets and Titan. We identify the key reactions that control the concentrations of CH3 in the model, such as the three-body recombination reaction, CH3 + CH3 + M yields C2H6 + M. We evaluate and extrapolate the three-body rate constant of this reaction to the low-temperature limit (1.8 x 10(exp -16) T(sup -3.75) e(sup -300/T), T < 300 K) and compare methyl radical abundances in five atmospheres: Jupiter, Saturn, Uranus, Neptune, and Titan. The sensitivity of our models to the rate coefficients for the reactions H + CH3 + M yields CH4 + M, H + C2H3 yields C2H2 + H2, (sup 1)CH2 + H2 yields CH3 + H, and H + C2H5 yields 2CH3, the branching ratios of CH4 photolysis, vertical mixing in the five atmospheres, and Lyman alpha photon enhancement at the orbit of Neptune have all been tested. The results of our model CH3 abundances for both Saturn (5.1 x 10(exp 13) / sq cm) and Neptune (2.2 x 10(exp 13) / sq cm) show good agreement with ISO Short Wavelength Spectrometer measurements. Using the same chemical reaction set, our calculations also successfully generate vertical profiles of stable hydrocarbons consistent with Voyager and ground-based measurements in these outer solar system atmospheres. Predictions of CH3 column concentrations (for p <= 0.2 mbar) in the atmospheres of Jupiter (3.3 x 10(exp 13) /sq cm), Uranus (2.5 x 10(exp 12) / sq cm), and Titan (1.9 x 10(exp 15) / sq cm) may be checked by future observations.

Lee, Anthony Y. T.↗

ATMOS Stratospheric Deuterated Water and Implications for Tropospheric-Stratospheric Transport

Measurements of the isotopic composition of stratospheric water by the ATMOS instrument are used to infer the convective history of stratospheric air. The average water vapor entering the stratosphere is found to be highly depleted of deuterium, with delta-D(sub w) of -670 +/- 80 (67% deuterium loss). Model calculations predict, however, that under conditions of thermodynamic equilibrium, dehydration to stratospheric mixing ratios should produce stronger depletion to delta-D(sub w) of -800 to 900 (80-90% deuterium loss). Deuterium enrichment of water vapor in ascending parcels can occur only in conditions of rapid convection; enrichments persisting into the stratosphere require that those conditions continue to near-tropopause altitudes. We conclude that either the predominant source of water vapor to the uppermost troposphere is enriched convective water, most likely evaporated cloud ice, or troposphere-stratosphere transport occurs closely associated with tropical deep convection.

Moyer, Elisabeth J.↗

Heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(s)

The heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) (eq 1) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(S) (eq 2) were investigated over the temperature range 223-296 K in a flow-tube reactor coupled to a quadrupole mass spectrometer. Either a chemical ionization mass spectrometer (CIMS) or an electron-impact ionization mass spectrometer (EIMS) was used to provide suitable detection sensitivity and selectivity. In order to mimic atmospheric conditions, partial pressures of HNO3 and N2O5 in the range 6 x 10(exp -8) - 2 x 10(exp -6) Torr were used. Granule sizes and surface roughness of the solid NaCl substrates were determined by using a scanning electron microscope. For dry NaCl substrates, decay rates of HNO3 were used to obtain gamma(1) = 0.013 +/- 0.004 (1sigma) at 296 K and > 0.008 at 223 K, respectively. The error quoted is the statistical error. After all corrections were made, the overall error, including systematic error, was estimated to be about a factor of 2. HCl was found to be the sole gas-phase product of reaction 1. The mechanism changed from heterogeneous reaction to predominantly physical adsorption when the reactor was cooled from 296 to 223 K. For reaction 2 using dry salts, gamma(2) was found to be less than 1.0 x 10(exp -4) at both 223 and 296 K. The gas-phase reaction product was identified as ClNO2 in previous studies using an infrared spectrometer. An enhancement in reaction probability was observed if water was not completely removed from salt surfaces, probably due to the reaction of N2O5(g) + H2O(s) yields 2HNO3(g). Our results are compared with previous literature values obtained using different experimental techniques and conditions. The implications of the present results for the enhancement of the hydrogen chloride column density in the lower stratosphere after the El Chichon volcanic eruption and for the chemistry of HCl and HNO3 in the marine troposphere are discussed.

Leu, Ming-Taun↗

(abstract) Odd Hydrogen in the Atmospheres of Earth and Mars

The Martian atmosphere has many features in common with the terrestrial mesosphere. Both share similar pressure and temperature ranges, and much of the same chemistry operates in each. For example, the radical species H, OH, and H(sub 2)O, which comprise the odd hydrogen family, are of central importance in the catalytic destruction of CO and O(sub 3) in both atmospheres. The inclusion of recent chemical kinetics data, specifically temperature dependent CO(sub 2) absorption cross-sections, into our one dimensional photochemical model of the Martial atmosphere shows that oxidation of CO by odd hydrogen is too efficient. The incorporation of smaller cross sections for CO(sub 2) leads to an enhanced photolysis rate of water vapor, increasing odd hydrogen to the point where the predicted mixing ratio of CO in our model is substantially less than the observed value of 6.5 x 10(sup -4). Interestingly, most photochemical models of the terrestrial mesosphere underestimate the CO and O(sub 3) densities using currently accepted photodissociation and kinetic rate coefficients. This has also been attributed to an overabundance of odd hydrogen in the models. We shall show that agreement between models and observations of CO in the Martian atmosphere as well as of CO and O(sub 3) in the terrestrial mesosphere can be achieved by revising the rate constants for the reactions OH + HO(sub 2) and CO + OH within their published uncertainties. The fact that similar revisions alleviate discrepancies in both the terrestrial and Martian atmospheres warrants a re-evaluation of these key rate constants at the appropriate temperatures and pressures.

dioxide ozone odd hydrogen family pressure tempera↗

Quantitative understanding of the cycles of oxidized and reduced sulfur on Venus

The evolution of the Venus atmosphere is determined by the supply of gases from the interior of the planet and outer space, and by the loss of particles to space over time. In particular, questions pertaining to the initial inventory of water and the current and past rates of outgassing can be addressed by studying the loss rates of H, D, He3 and He4. The photochemistry of the H2SO4 clouds may also have played an important role in regulating the amount of water above the cloud tops, and hence limit the rate of escape of hydrogen from the planet. Thus the problems of evolution and chemistry are intimately related. In our proposal the principal tasks we undertook to advance our understanding of the origin and evolution of water on Venus included: (1) escape of light atoms from Venus and (2) develop a photochemical model of sulfate formation. In the last two years we have made progress on Task 1 regarding how light atoms can escape from the exosphere of Venus with the development of a Monte Carlo program and in Task 2 have developed a thorough update on the SO2 photochemistry that had been previously carried out.

Yung, Yuk L.↗

Fractionation of hydrogen and deuterium on Venus due to collisional ejection

The collisional ejection process for hydrogen on Venus is reanalyzed. Improved values for the efficiency of H and D escape as a function of the ionospheric temperature are reported. It is proposed that the reduction of the hydrogen flux for collisional ejection be reduced from 8 to 3.5 x 10 exp 6/sq cm/s, and a revised D/H fractional factor of 0.47 due to collisional ejection is suggested. The resulting deuterium flux is 3.1 x 10 exp 4/sq cm/s, roughly six times the flux due to charge exchange, making collisional ejection the dominant escape mechanism for deuterium on Venus.

Gurwell, Mark A.↗

Chemistry and transport in a multi-dimensional model

The focus of our research program is the achievement of a quantitative understanding of the spatial distribution and temporal variation of chemical species in the terrestrial middle atmosphere, with emphasis on ozone. Although not directed at assessments of anthropogenic impacts, our activities contribute to a refinement of model descriptions of chemical and dynamical processes that are needed for assessment tasks. A unique feature of our research effort is a close interaction with the chemical kinetics group at JPL and the field measurement groups at JPL. The principal tools used in our investigations are l-D and 2-D photochemical models. The advective component of the meridional transport in these models is approximated by the diabatic circulation, which is derived diagnostically from the net radiative heating rates. We are developing accurate radiative transfer algorithms to find the net heating rates and the diabatic circulation for use in the 2-D model.

Yung, Yuk L.↗

The relative abundance of ethane to acetylene in the Jovian stratosphere

The inclusion of the results of laboratory kinetics studies on the reaction of C2H3 and H2 to yield C2H4, which is suggestive of an efficient chemical mechanism for the hydrogenation of C2H2 to C2H6, can be included in a comprehensive model of the Jupiter atmosphere hydrocarbon photochemistry to explain the observed altitude variation of the C2H6/C2H2 ratio. The sensitivity of these results to uncertainties in key low-temperature rate constants is demonstrated. These key reaction-rate constants decrease with falling temperature.

Allen, Mark↗

Hydrocarbon nucleation and aerosol formation in Neptune's atmosphere

The present theoretical analysis of particle formation mechanisms at conditions relevant to the troposphere and stratosphere of Neptune indicates that the hydrocarbon-nucleation process in the lower stratosphere is very inefficient, because saturation ratios much greater than unity are required in the cases of aerosol formation by homogeneous, heterogeneous, and ion-induced nucleation. The latter two of these, however, should be possible on Neptune for most of the complex hydrocarbon species in question. The relative effectiveness of heterogeneous and ion-induced nucleation depends on the physical and thermodynamic properties of the species in question, condensable-species abundance, supersaturation temperatures, and the number and type of available condensation ions or nuclei.

Moses, Julianne I.↗

Solar control of the upper atmosphere of Triton

If the upper atmosphere and ionosphere of Triton are controlled by precipitation of electrons from Neptune's magnetosphere as previously proposed, Triton could have the only ionosphere in the solar system not controlled by solar radiation. However, a new model of Triton's atmosphere, in which only solar radiation is present, predicts a large column of carbon atoms. With an assumed, but reasonable, rate of charge transfer between N2(+) and C, a peak C(+) abundance results that is close to the peak electron densities measured by Voyager in Triton's ionosphere. These results suggest that Triton's upper atmospheric chemistry may thus be solar-controlled. Measurement of key reaction rate constants, currently unknown or highly uncertain at Triton's low temperatures, would help to clarify the chemical and physical processes occurring in Triton's atmosphere.

Lyons, James R.↗

Enhancement of atmospheric radiation by an aerosol layer

The presence of a stratospheric haze layer may produce increases in both the actinic flux and the irradiance below this layer. Such haze layers result from the injection of aerosol-forming material into the stratosphere by volcanic eruptions. Simple heuristic arguments show that the increase in flux below the haze layer, relative to a clear sky case, is a consequence of 'photon trapping'. The magnitude of these flux perturbations, as a function of aerosol properties and illumination conditions, is explored with a new radiative transfer model that can accurately compute fluxes in an inhomogeneous atmosphere with nonconservative scatterers having arbitrary phase function. One calculated consequence of the El Chichon volcanic eruption is an increase in the midday surface actinic flux at 20 deg N latitude, summer, by as much as 45 percent at 2900 A. This increase in flux in the UV-B wavelength range was caused entirely by aerosol scattering, without any reduction in the overhead ozone column.

Michelangeli, Diane V.↗