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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.↗

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.↗

Study of a Solar X-Ray Telescope

The highly structured nature of the outer solar atmosphere seems to be intimately linked to the presence, at the solar surface, of magnetic fields that have been generated inside the Sun and have emerged to the surface. The corona is brightest (and also hottest) at just those locations where the magnetic field has emerged from inside the Sun. Dynamo theory predicts that strong magnetic fields will be generated deep in the solar interior and that bundles or 'ropes' of magnetic flux will float to the surface. When this happens, a magnetically bipolar region will become visible, extending above the surface in a three-dimensional structure. The field lines penetrate through the surface, showing two magnetic poles, and also exhibit a three-dimensional structure above the surface. The structure created by the field emergence is rooted in the (relatively) cool photosphere and extends through the chromosphere and transition region to the corona. Thus, the magnetic field creates a region, called an active region, which contains portions at temperatures from less than 10(exp 4) K to greater than 10(exp 6) K, and is therefore visible at wavelengths from the infrared through x-rays. The locations where the magnetic field leaves and reenters the visible surface are called the 'footpoints' of the coronal structures associated with the magnetic field. The magnetic fields themselves are not directly visible. However, the hot coronal plasma is, for the most part, constrained to follow the direction of the magnetic field lines in the atmosphere. Now, 100 years after the discovery of x-rays by Wilhelm Roentgen in 1896, we can routinely make observations of the solar corona from outside the Earth's atmosphere in this region of the electromagnetic spectrum. As shown by comparing x-ray images with magnetograms, the bright corona over these bipolar magnetic regions consists of closed structures that seem to follow the orientation of the magnetic field. Although we can see down to the photosphere at x-ray wavelengths when observing the disk of the Sun, this part of the solar atmosphere emits so little that far from the peak of its Planck curve it appears dark in x-ray images. This impression of hot plasma following the magnetic field direction is further strengthened by quantitative studies that calculate coronal magnetic field strength and direction based on photospheric measurements and compare them with the observed brightness and location of the x-ray emitting structures. Such comparisons make it clear that, for the most part, the hot plasma conforms to the geometry of the magnetic field and that the coronal brightness is strongly linked to the strength of the magnetic fields which have erupted to the solar surface from the interior. It is also the case that the larger-scale, fainter corona, as well as coronal holes, are strongly influenced by the large-scale solar magnetic field. We may get a small hint of the reason that the coronal plasma outlines the direction of B by examining the thermal conductivity of a hot plasma in the presence of a magnetic field. This quantity has enormously different values in the directions parallel and perpendicular to the field for a coronal temperature of 10(exp 6) K, a particle density of 10(exp 9)/cu cm and a magnetic field strength of 100 G, the conductivity along the field is approximately 13 orders of magnitude greater than that perpendicular to the field. It is therefore not surprising that a parcel of plasma which is locally heated would conduct that heat preferentially in the direction of the field. We also note that the thermal conductivity parallel to the magnetic field increases with temperature T, while the perpendicular conductivity decreases. To the extent that the loop aspect ratio, i.e., the ratio of loop length to loop width, is determined by the thermal conductivity, we would expect that higher temperature loops are longer and thinner than cooler ones. However, if the loop width becomes smaller than the spatial resolution of the observing instrument, this effect will not be directly observable. For organizational purposes, we provide a listing of some scientific objectives for a Solar-B x-ray telescope, arranged in terms of identifiable features in the corona.

Golub, Leon↗

Stratospheric Heterogeneous Chemistry and Microphysics: Model Development, Validation and Applications

The objectives of this project are to: define the chemical and physical processes leading to stratospheric ozone change that involve polar stratospheric clouds (PSCS) and the reactions occurring on the surfaces of PSC particles; study the formation processes, and the physical and chemical properties of PSCS, that are relevant to atmospheric chemistry and to the interpretation of field measurements taken during polar stratosphere missions; develop quantitative models describing PSC microphysics and heterogeneous chemical processes; assimilate laboratory and field data into these models; and calculate the extent of chemical processing on PSCs and the impact of specific microphysical processes on polar composition and ozone depletion. During the course of the project, a new coupled microphysics/physical-chemistry/ photochemistry model for stratospheric sulfate aerosols and nitric acid and ice PSCs was developed and applied to analyze data collected during NASA's Arctic Airborne Stratospheric Expedition-II (AASE-II) and other missions. In this model, detailed treatments of multicomponent sulfate aerosol physical chemistry, sulfate aerosol microphysics, polar stratospheric cloud microphysics, PSC ice surface chemistry, as well as homogeneous gas-phase chemistry were included for the first time. In recent studies focusing on AASE measurements, the PSC model was used to analyze specific measurements from an aircraft deployment of an aerosol impactor, FSSP, and NO(y) detector. The calculated results are in excellent agreement with observations for particle volumes as well as NO(y) concentrations, thus confirming the importance of supercooled sulfate/nitrate droplets in PSC formation. The same model has been applied to perform a statistical study of PSC properties in the Northern Hemisphere using several hundred high-latitude air parcel trajectories obtained from Goddard. The rates of ozone depletion along trajectories with different meteorological histories are presently being systematically evaluated to identify the principal relationships between ozone loss and aerosol state. Under this project, we formulated a detailed quantitative model that predicts the multicomponent composition of sulfate aerosols under stratospheric conditions, including sulfuric, nitric, hydrochloric, hydrofluoric and hydrobromic acids. This work defined for the first time the behavior of liquid ternary-system type-1b PSCS. The model also allows the compositions and reactivities of sulfate aerosols to be calculated over the entire range of environmental conditions encountered in the stratosphere (and has been incorporated into a trajectory/microphysics model-see above). Important conclusions that derived from this work over the last few years include the following: the HNO3 content of liquid-state aerosols dominate PSCs below about 195 K; the freezing of nitric acid ice from sulfate aerosol solutions is likely to occur within a few degrees K of the water vapor frost point; the uptake and reactions of HCl in liquid aerosols is a critical component of PSC heterogeneous chemistry. In a related application of this work, the inefficiency of chlorine injection into the stratosphere during major volcanic eruptions was explained on the basis of nucleation of sulfuric acid aerosols in rising volcanic plumes leading to the formation of supercooled water droplets on these aerosols, which efficiently scavenges HCl via precipitation.

Turco, Richard P.↗

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.↗

Implications of Large Scale Shifts in Tropospheric NO(x) Levels in the Remote Tropical Pacific

A major observation recorded during NASA's western Pacific Exploratory Mission (PEM-West B) was the large shift in tropical NO levels as a function of geographical location. High-altitude NO levels exceeding 100 pptv were observed during portions of tropical flights 5-8, while values almost never exceeded 20 pptv during tropical flights 9 and 10. The geographical regions encompassing these two flight groupings are here labeled "high" and "low" NOx regimes. A comparison of these two regimes, based on back trajectories and chemical tracers, suggests that air parcels in both were strongly influenced by deep convection. The low NO(x) regime appears to have been predominantly impacted by marine convection, whereas the high NO(x) regime shows evidence of having been more influenced by deep convection over a continental land mass. DMSP satellite observations point strongly toward lightning as the major source of NOx in the latter regime. Photochemical ozone formation in the high NOx regime exceeded that for low NO(x) by factors of 2 to 6, whereas O3 destruction in the low NO(x)regime exceeded that for high NOx by factors of up to 3. Taking the tropopause height to be 17 km, estimates of the net photochemical effect on the O3 column revealed that the high NO(x) regime led to a small net production. By contrast, the low NOx regime was shown to destroy O3 at the rate of 3.4 % per day. One proposed mechanism for off-setting this projected large deficit would involve the transport of 03 rich midlatitude air into the tropics. Alternatively, it is suggested that O3 within the tropics may be overall near self-sustaining with respect to photochemical activity. This scenario would require that some tropical regions, unsampled at the time of PEM-B, display significant net column O3 production, leading to an overall balanced budget for the "greater" tropical Pacific basin. Details concerning the chemical nature of such regimes are discussed.

Crawford, J. H.↗

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.↗

A Quantitative Investigation of Entrainment and Detrainment in Numerically Simulated Convective Clouds: Simulations of Cumulonimbus Clouds - Pt. 2

Deep cumulonimbus clouds are simulated using a model that makes accurate diagnoses of entrainment and detrainment rates and of the properties of entrained and detrained air. Clouds generated by a variety of initial thermodynamic soundings are compared. In the simulations, updraft entrainment rates are large near and above cloud base, through the entire depth of the conditionally unstable layer. Stronger updrafts in a more unstable environment are better able to entrain relatively undisturbed environmental air, while weaker updrafts can entrain only air that has been modified by the clouds. When the maximum buoyancy is large, the updraft includes parcels with a wide range of buoyancies, while weaker clouds are more horizontally uniform. Strong downdrafts originate from levels at which updrafts detrain, and their mass flux depends on the mass flux of the updraft. The magnitude of mixing between cloud and environment, not the entrainment rate, varies inversely with the cloud radius. How much of the mixed air is entrained depends on the buoyancy.

Cohen, Charles↗

Investigation of the Physical Processes Governing Large-scale Tracer Transport in the Stratosphere and Troposphere

This report reviews the second year of a three-year research program to investigate the physical mechanisms which underlie the transport of trace constituents in the stratosphere- troposphere system. The primary scientific goal of the research is to identify the processes which transport air masses within the lower stratosphere, particularly between the tropics and middle latitudes. The SASS program seeks to understand the impact of the present and future fleets of conventional jet traffic on the upper troposphere and lower stratosphere, while complementary airborne observations under UARP seek to understand the complex interactions of dynamical and chemical processes that affect the ozone layer. The present investigation contributes to the goals of each of these by diagnosing the history of air parcels intercepted by NASA research aircraft in UARP and AEAP campaigns.

Selkirk, Henry B.↗

Dehydration and Denitrification in the Arctic Polar Vortex During the 1995-1996 Winter

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (theta about 450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(sub y)) had also been removed, with layers of enhanced (sub y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (about 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 micron) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range of theta is estimated to have been dehydrated in this event.

Hintsa, E. J.↗

Dehydration and Denitrification in the Arctic Polar Vortex During the 1995-1996 Winter

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (0-450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(y)) had also been removed, with layers of enhanced NO(y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (approximately 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 microns) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range of 0 is estimated to have been dehydrated in this event.

Hintsa, E. J.↗

The Life Cycle of Stratospheric Aerosol Particles

This paper describes the life cycle of the background (nonvolcanic) stratospheric sulfate aerosol. The authors assume the particles are formed by homogeneous nucleation near the tropical tropopause and are carried aloft into the stratosphere. The particles remain in the Tropics for most of their life, and during this period of time a size distribution is developed by a combination of coagulation, growth by heteromolecular condensation, and mixing with air parcels containing preexisting sulfate particles. The aerosol eventually migrates to higher latitudes and descends across isentropic surfaces to the lower stratosphere. The aerosol is removed from the stratosphere primarily at mid- and high latitudes through various processes, mainly by isentropic transport across the tropopause from the stratosphere into the troposphere.

Hamill, Patrick↗

Simulation of Tropical Biomass Burning

The work proposed was carried out as planned. The work described in this final report formed the basis for a follow-on research grant research grant from NASA Ames Research Center. The research objectives that were achieved during the course of our studies include the following: (1) the evaluation of several components of MM5 (Meteorological Model 5 version 2) and the Global/Regional Atmospheric Chemistry Event Simulator (GRACES) combined modeling system; (2) improved calculations of the transport of tracers for both NASA airborne missions, Study of Ozone and Nitrogen oxides experiment (SONEX) and Pacific Exploratory MIssion in the Tropics (PEM-Tropics); (3) improved source strength estimates for isoprene, dust and similar emissions from the Earth's surface. This required the use of newly available databases on the Earth's surface and vegetation; (4) completed atmospheric chemistry simulations of radicals and nitrogen oxide species; (5)improved the handling of cumulonimbus convection by modifying the existing scheme; (6) identified the role of the African Intertropical Front, using MM5's nesting capability to refine model resolution in crucial areas; modified the MM5 trajectory program to allow it to work much better for a parcel crossing the west/east boundaries.

Hamill, Patrick↗

A Lagrangian Simulation of Subsonic Aircraft Exhaust Emissions

To estimate the effect of subsonic and supersonic aircraft exhaust on the stratospheric concentration of NO(y), we employ a trajectory model initialized with air parcels based on the standard release scenarios. The supersonic exhaust simulations are in good agreement with 2D and 3D model results and show a perturbation of about 1-2 ppbv of NO(y) in the stratosphere. The subsonic simulations show that subsonic emissions are almost entirely trapped below the 380 K potential temperature surface. Our subsonic results contradict results from most other models, which show exhaust products penetrating above 380 K, as summarized. The disagreement can likely be attributed to an excessive vertical diffusion in most models of the strong vertical gradient in NO(y) that forms at the boundary between the emission zone and the stratosphere above 380 K. Our results suggest that previous assessments of the impact of subsonic exhaust emission on the stratospheric region above 380 K should be considered to be an upper bound.

Schoeberl, M. R.↗

Sensitivity of Cirrus Simulations in Idealized Situations: The WG2 Test Cases

GCSS Cirrus Cloud Systems Working Group (WG2) is presently conducting a comparison of cirrus cloud models for idealized initial conditions. The experiments involve binary (off/on) tests of model sensitivity to infrared radiative processes, and thermal stratification, and vertical wind shear for situations of weakly forced (3 cm/s uplift) cold (-60 to -70 C) and warm (-35 to -50 C) cirrus clouds. A range of model types are involved including parcel, SCM, 2-D CRM, 3-D CRM and LES models. The test cases will be described and results from 2-dimensional cirrus cloud models with bulk microphysics (implicit second moment scheme) and explicit bin microphysics will be compared. Vertical ice mass flux (particle fall speed) is a critical model component leading to significant intermodel differences. Efforts are ongoing to better quantify this aspect. Future plans of WG2 will also be briefly described and include model comparisons for a well-observed case of cold (ARM IOP) cirrus and of warm (EUCREX) cirrus, as well as, a joint activity with WG4 to consider the treatment of anvil cirrus in a variety of models.

Starr, David OC.↗

Dehydration and Denitrification in the Arctic Polar Vortex During the 1995-1996 Winter

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (theta approximately 450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(y)) had also been removed, with layers of enhanced NO(y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (approximately 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 micrometers) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range Transport of theta is estimated to have been dehydrated in this event.

Hintsa, E. J.↗

SONEX Airborne Mission and Coordinated POLINAT-2 Activity: Overview and Accomplishments

The SASS (Subsonic Assessment) Ozone and NO(x) Experiment (SONEX) was an airborne field campaign conducted in October-November 1997 in the vicinity of the North Atlantic Flight Corridor Lo study the impact of aircraft emissions on NOx and ozone (03). A fully instrumented NASA DC-8 aircraft was used as the primary SONEX platform. SONEX activities were closely coordinated with the European POLINAT-2 (Pollution from Aircraft Emissions in the North Atlantic Flight Corridor) program, which used a Falcon-20 aircraft and an instrumented in-service Swissair B-747. Both campaigns focused on the upper troposphere/"lowermost" stratosphere (UT/LS) as the region of greatest interest. Specific sampling goals were achieved with the aid of a state-of-the art modeling and meteorological support system, which allowed targeted sampling of air parcels with desired characteristics. A substantial impact of aircraft emissions on NO(x) and O3 in the UT/LS of the study region is shown to be present. It is further shown that the NO(x)- HO(x)-O3 relationships are highly nonlinear and must be accurately simulated to make meaningful future predictions with global models. SONEXIPOLINAT-2 results are being published in Special Sections of GRL and JGR. Here we provide a brief overview of SONEX design, implementation, and expected results to provide a context within which these publications can be understood.

Singh, Hanwant B.↗

A "Stratospheric Drain" over the Maritime Continent

Evidence is presented from operational rawinsonde data surrounding the maritime continent that the net mass flux near the tropopause is downward over this region, contrary to the behavior of current numerical models. The air is descending year-round, despite mean upward motion below and above the descending layer. This sinking implies the existence of a significant energy-removing process, which is argued to be the injection of cold air by overshooting convective clouds. The mass, energy, and horizontal momentum budgets are examined in reaching these conclusions. The implied cooling effect of convective overshoots can be simulated with a simple, parcel-sorting convective mixing model. The findings contradict the common view that the mean flow enters the stratosphere in this strongly-convecting region, and have important implications for transport of water vapor and other gases into the stratosphere.

Sherwood, Steve↗