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In this talk I will present several experimental techniques currently used to investigate gas-surface interaction related to acid rain, photochemical smog, and polar ozone depletion.
In mid-March 2005 the northern lower stratospheric polar vortex experienced a severe stretching episode, bringing a large polar filament far south of Alaska toward Hawaii. This meridional intrusion of rare extent, coinciding with the polar vortex final warming and breakdown, was followed by a zonal stretching in the wake of the easterly propagating subtropical main flow. This caused polar air to remain over Hawaii for several days before diluting into the subtropics. After being successfully forecasted to pass over Hawaii by the high-resolution potential vorticity advection model Modele Isentrope du transport Meso-echelle de l'Ozone Stratospherique par Advection (MIMOSA), the filament was observed on isentropic surfaces between 415 K and 455 K (17-20 km) by the Jet Propulsion Laboratory stratospheric ozone lidar measurements at Mauna Loa Observatory, Hawaii, between 16 and 19 March 2005. It was materialized as a thin layer of enhanced ozone peaking at 1.6 ppmv in a region where the climatological values usually average 1.0 ppmv. These values were compared to those obtained by the three dimensional Chemistry-Transport Model MIMOSA-CHIM. Agreement between lidar and model was excellent, particularly in the similar appearance of the ozone peak near 435 K (18.5 km) on 16 March, and the persistence of this layer at higher isentropic levels for the following three days. Passive ozone, also modeled by MIMOSA-CHIM, was at about 3-4 ppmv inside the filament while above Hawaii. A detailed history of the modeled chemistry inside the filament suggests that the air mass was still polar ozone- depleted when passing over Hawaii. The filament quickly separated from the main vortex after its Hawaiian overpass. It never reconnected and, in less than 10 days, dispersed entirely in the subtropics.
The long-term evolution of the Antarctic ozone hole is studied based on the TOMS data and the JMA data-set of stratospheric temperature in relation with the possible role of polar stratospheric clouds (PSC's). The effective mass of depleted ozone in the ozone hole at its annual mature stage reached a historical maximum of 55 Mt in 1991, 4.3 times larger than in 1981. The ozone depletion rate during 30 days before the mature ozone hole does not show any appreciable long-term trend but the interannual fluctuations do, ranging from 0.169 to 0.689 Mt/day with the average of 0.419 Mt/day for the period of 1979 - 1991. The depleted ozone mass has the highest correlation with the region below 195 K on the 30 mb surface in June, whereas the ozone depletion rate correlates most strongly with that in August. The present result strongly suggests that the long-term evolution of the mature ozone hole is caused both by the interannual change of the latitudinal coverage of the early PSC's, which may control the latitude and date of initiation of ozone decrease, and by that of the spatial coverage of the mature PSC's which may control the ozone depletion rate in the Antarctic spring.
The polar motion excitation caused by variations in major natural lakes, the impoundment in artificial reservoirs, and the depletion of a major groundwater aquifer is calculated. It is found that the annual water mass variation in natural lakes contributes a significant fraction in the total hydrological excitation of the annual wobble and that the hydrological reservoirs have been negligible in the Chandler wobble excitation. It is also shown that the contribution of hydrological reservoirs to the total secular polar drift has been negligible in the century due to fortuitous cancellation among reservoirs.
We present the first spatially resolved polarized scattered light H-band detection of the DoAr 28 transitional disk. Our two epochs of imagery detect the scattered light disk from our effective inner working angle of 0 double prime.10 (13 AU) out to 0double prime.50 (65 AU). This inner working angle is interior to the location of the system's gap inferred by previous studies using spectral energy distribution modeling (15 AU). We detected a candidate point source companion 1 double prime.08 northwest of the system; however, our second epoch of imagery strongly suggests that this object is a background star. We constructed a grid of Monte Carlo Radiative Transfer models of the system, and our best fit models utilize a modestly inclined (50 degrees), 0.01 solar mass disk that has a partially depleted inner gap from the dust sublimation radius out to approximately 8 AU. Subtracting this best fit, axi-symmetric model from our polarized intensity data reveals evidence for two small asymmetries in the disk, which could be attributable to a variety of mechanisms.
The molecular origins of homochirality on Earth is not understood well, particularly how enantiomerically enriched molecules of astrobiological significance like sugars and amino acids might have been synthesized on icy grains in space preceding their delivery to Earth. Polycyclic aromatic hydrocarbons (PAHs) identified in carbonaceous chondrites could have been processed in molecular clouds by circularly polarized light prior to the depletion of enantiomerically enriched helicenes onto carbonaceous grains resulting in chiral islands. However, the fundamental low temperature reaction mechanisms leading to racemic helicenes are still unknown. Here, by exploiting synchrotron based molecular beam photoionization mass spectrometry combined with electronic structure calculations, we provide compelling testimony on barrierless, low temperature pathways leading to racemates of [5] and [6]helicene. Astrochemical modeling advocates that gas-phase reactions in molecular clouds lead to racemates of helicenes suggesting a pathway for future astronomical observation and providing a fundamental understanding for the origin of homochirality on early Earth.
A new platform has been developed for the 1-MA COBRA generator to investigate the physical processes affecting the formation, collimation, and stability of high-speed outflows in magnetically driven laboratory plasma jets. Such experiments serve as diagnostically accessible surrogates for astrophysical jets under the assumption that the underlying dynamics are scale invariant. In contrast to previous current driven high energy density laboratory jet experiments that use radial/conical wire arrays or foils, the platform described here uses azimuthally symmetric gas-puff injection. This avoids the ablation phase from a solid target, allowing the jets to develop earlier and be driven longer without depleting their mass source and disrupting. A permanent magnet provides an initial poloidal magnetic field, which links the two concentric electrodes and mimics the boundary conditions of a star-accretion disk system. Extended magnetohydrodynamic effects can be assessed using a polarity convolute, which allows for reversal of the electrode bias. The resulting plasma jets exhibit remarkable stability, persisting for hundreds of nanoseconds and achieving aspect ratios ≳30:1.
The role that the cleft/cusp has in ionosphere-magnetosphere coupling makes it a dynamic and important region. It is directly exposed to the solar wind, making it possible for the entry of electromagnetic energy and precipitating electrons and ions from dayside reconnection and other dayside events. It is also a significant source of ionospheric plasma, contributing largely to the mass loading of the magnetosphere with large fluxes of outflowing ions. Crossing the cusp/cleft near 5100 km, the Polar instruments observe the common correlation of downward Poynting flux, ion energization, soft electron precipitation, broadband extremely low-frequency (BB-ELF) emissions, and density depletions. The dominant power in the BB-ELF emissions is now identified to be from spatially broad, low frequency Alfv nic structures. For a cusp crossing, we determine using the Electric Field Investigation (EFI), that the electric and magnetic field fluctuations are Alfv nic and the electric field gradients satisfy the inequality for stochastic acceleration. With all the Polar 1996 horizontal crossings of the cusp, we determine the O+ heating rate using the Thermal Ion Dynamics Experiment (TIDE) and Plasma Wave Investigation (PWI). We then compare this heating rate to other heating rates assuming the electric field gradient criteria exceeds the limit for stochastic acceleration for the remaining crossings. The comparison suggests that a stochastic acceleration mechanism is operational and the heating is controlled by the transverse spatial scale of the Alfvenic waves.
The thermal and suprathermal ion populations present in the refilling regions after a magnetic storm are examined using retarding ion mass spectrometer (RIMS) data from the Dynamics Explorer 1 spacecraft. The RIMS instrument is described, and data are presented and discussed in detail for the outer plasmasphere, plasmapause, depleted dayside magnetosphere, and dayside cusp. Three distinct populations were observed: thermal ions, warm anisotropic plasma, and the polar wind. The characteristics of these populations are considered, including the densities, temperatures, and density ratios. Aspects of the ionospheric plasma outflow are discussed, including the field-aligned flow speed, the ionospheric plasma escape flux, plasmaspheric refilling, and wave-particle phenomena.
The Antarctic ozone hole develops each year and culminates by early spring (late September - early October). The severity of the hole has been assessed from satellites using the minimum total ozone value from the October monthly mean (depth of the hole), calculating the average area coverage during this September-October period, and by estimating ozone mass deficit. Profile information shows that ozone is completely destroyed in the 14-2 1 km layer by early October. Ozone is mainly destroyed by halogen (chlorine and bromine) catalytic cycles, and these losses are modulated by temperature variations. Because atmospheric halogen levels are responding to international agreements that limit or phase out production, the amount of halogens in the stratosphere should decrease over the next few decades. Both models and projections of ozone depleting substances (ODSs) into the 21St century reveal that polar ozone levels should recover in the 2060- 2070 period. In this talk, we will review current projections of polar ozone recovery. Using models and ODs projections, we explore both the past, near future (2008-2025), and far future (> 2025) levels of polar ozone. Finally, we will discuss various factors that complicate recovery such as greenhouse gas changes (e.g., cooling in the upper stratosphere) and the acceleration of the Brewer-Dobson circulation.
A novel mass spectrometer designed to measure simultaneously positive ion composition in the mesosphere, was successfully launched during the NLC-91 project. Instruments supporting the mass spectrometer were a probed to measure both electrons and positive ions as well as a wave propagation experiment. The location of the Noctilucent Clouds (NLC) was determined by a particle impact sensor to detect secondary electrons and ions from the impact of NLC particle. The density of proton hydrates and of the related total ions is depleted in the NLC region at 83 km. An improved detection limit of 5 x 10(exp 4)/cu m for positive ions and improved height resolution revealed for the first time large gradients in the O2(+), H(+)(H2O)2 and H(+)(H2O)6 densities within a small height range of the order of 50 m. Such gradients at the altitude of NLC and Polar Mesospheric Summer Echoes (PMSE) are associated with strong variability of mesospheric water vapor, temperature and neutral air density.
The origin of the material ejected during a white-light coronal transient on August 26 and 27, 1973, is investigated using simultaneous observations of a slowly ascending prominence and the more rapid accompanying coronal transient. Nearly identical simultaneous images of the prominence were obtained over a six-hour period in the H-alpha and He II (304 A) emission lines; contemporaneous Skylab coronograph observations over approximately 1.5 hours showed that the mass-ejection coronal transient rose above the ascending prominence. Based on analysis of these observations, it is concluded that: (1) the bulk of the ejected material originated in the lower corona, despite the lack of an observed depletion there; (2) the material in the transient was at coronal temperature and was visible in polarized radiation due to Thomson scattering of photospheric light by free electrons; and (3) the total event was far larger, more energetic, and longer lasting than would have been inferred from the prominence observations alone.
We use satellite ozone records and Global Modeling Initiative (GMI) chemistry transport model (CTM) simulations integrated with MERRA2 meteorology to identify a metric that accurately captures the trend in Antarctic ozone attributable to the decline in ozone depleting substances (ODSs). The GMI CTM Baseline simulation with realistically varying ODS levels closely matches observed interannual to decadal scale variations in Antarctic September ozone over the past 4 decades. The expected increase or recovery trend is obtained from the differences between the Baseline simulation and one with identical meteorology and fixed 1995 ODS levels. The differences show that vortex-averaged column O3 has the greatest sensitivity to ODS change from 1-20 Sep. The observed vortex-averaged column O3 during this period produces a trend consistent with the expected recovery attributable to ODS decline. Trends from dates after 20 Sep have smaller sensitivity to ODS decline and are more uncertain due to transport variability. Simulations show that the greatest decrease in O3 loss (i.e., recovery) occurs inside the vortex near the edge. The polar cap metrics have vortex size-dependent bias and do not consistently sample this region. Because the 60-90oS 220 DU O3 mass deficit (OMD) metric does not sample the edge region, its trend is lower than the expected trend; this is improved by area weighting. The 250 DU OMD metric samples more of the edge region, which increases its trend. Approximately 25% of the September Antarctic O3 increase is due to higher O3 levels in June prior to winter depletion.
This paper reports on the measurements of reaction probabilities for heterogeneous reaction of N2O5 with H2O and HCl on ice surfaces at 195 K, using a fast-flow reactor coupled with a quadrupole mass spectrometer. The reaction probability for N2O5 on pure-water ice was found to be 0.028 + or - 0.011, with nitric acid in the solid phase as the sole product. In the presence of HCl in ice, the probability of N2O5 reaction was enhanced (to 0.037); the reaction produced, besides solid-phase nitric acid, ClNO2 and ClONO which were released into the gas phase within a few milliseconds. The latter two compounds can be readily photolyzed in the austral spring to form active chlorine which would remove stratospheric ozone. It is suggested that, since the polar stratospheric clouds are believed to contain HCl-ice mixture on the surface, the reactions of N2O5 on H2O/HCl particles is a major factor in the Antarctic springtime ozone depletion.
A theoretical study of the thermospheric circulation and composition at polar latitudes is presented. It is suggested that the observed motions and density perturbations in N2, O and He can be understood in terms of electric field momentum coupling, Joule heating, and interactions between these two processes. It is found that the vortex type double cell polar circulation is primarily driven by collisional momentum transfer from electric field induced ion convection. Because of the thermospheric low pass filter, a large time independent component is produced by Joule heating. Due to wind induced diffusion, the N2 is concentrated where the O and He are depleted and vice versa. The electric field driven vortex circulation redistributes the mass and energy in the time independent density and temperature variations, producing primarily diurnal variations in the temperature and composition near the pole and at auroral latitudes.
Composition data obtained by the quadrupole mass spectrometer (NACS) carried aboard the DE-B satellite were examined for variations in the polar regions during magnetically quiet conditions. The corresponding predictions of the MSIS-83 model are often used for comparison. The MSIS-83 model is used to emphasize the variations of interest by suppressing all other variations. A persistent enhancement of N2 density and a depletion of He density are present in the vicinity of the magnetic poles with maximum density response in the morning hours (magnetic) on average. A universal time (UT) variation in average density levels is evident near both the geographic and magnetic poles. There are systematic morphology changes with UT and between summer and winter which are qualitatively consistent with the simple concept that thermospheric heating effects are shifted or spread in the downwind direction of the global circulation systems driven by EUV and magnetospheric sources. The magnitude of the UT variations is larger in the southern hemisphere and is larger in local winter than summer.
Contents include the following: A Model for Multiple Populations of Presolar Diamonds. Characterization of Martian North Polar Geologic Units Using Mars Odyssey THEMIS Data. Effect of Flow on the Internal Structure of the Martian North Polar Layered Deposits. Elemental Abundance Distributions in Basalt Clays and Meteorites: Is It a Biosignature? Early Results on the Saturn System from the Composite Infrared Spectrometer. NanoSIMS D/H Imaging of Isotopically Primitive Interplanetary Dust Particles. Presolar (Circumstellar and Interstellar) Phases in Renazzo: The Effects of Parent Body Processing. Catastrophic Disruption of Hydrated Targets: Implications for the Hydrated Asteroids and for the Production of Interplanetary Dust Particles. Chemical and Mineralogical Analyses of Particles from the Stratospheric Collections Coinciding with the 2002 Leonid Storm and the 2003 Comet Grigg-Skjellerup Trail Passage. An Analysis of the Solvus in the CaS-MnS System. ESA s SMART-1 Mission at the Moon: First Results, Status and Next Steps. Europa Analog Ice-splitting Measurements and Experiments with Ice-Hunveyor on the Frozen Balaton-Lake, Hungary. Chromium on Eros: Further Evidence of Ordinary Chondrite Composition. Dust Devil Tracks on Mars: Observation and Analysis from Orbit and the Surface. Spatial Variation of Methane and Other Trace Gases Detected on Mars: Interpretation with a General Circulation Model. Mars Water Ice and Carbon Dioxide Seasonal Polar Caps: GCM Modeling and Comparison with Mars Express Omega Observations. Component Separation of OMEGA Spectra with ICA. Clathrate Formation in the Near-Surface Environment of Titan. Space Weathering: A Proposed Laboratory Approach to Explaining the Sulfur Depletion on Eros. Sample Collection from Small Airless Bodies: Examination of Temperature Constraints for the TGIP. Sample Collector for the Hera Near-Earth Asteroid Sample Return Mission. A Rugged Miniature Mass-Spectrometer for Measuring Aqueous Geochemistry on Mars. Martian and Lunar Pyroxene Microstructures Studied by Single-Crystal X-Ray Diffraction.
Preliminary results are reported of the direct measurement of accommodation coefficients for HNO3, N2O5 and HCl on water drops, aqueous sulfuric acid drops and ice particles. The heterogeneous chemistry of these species together with ClONO2 has been implicated in the ozone depletion observed in the Antarctic stratosphere during the spring in the last eight years. The most plausible chemical mechanism involves the removal of nitrogen oxide species via condensation on ice particles in polar stratospheric clouds resulting in a increase in the active chlorine species responsible for the ozone depletion. The observation of low NO2 and high ClO densities in the Antarctic stratosphere last summer appear to be consistent with such a mechanism.