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The Sensitivity of Arctic Ozone Loss to Polar Stratospheric Cloud Volume and Chlorine and Bromine Loading in a Chemistry and Transport Model

The sensitivity of Arctic ozone loss to polar stratospheric cloud volume (V(sub PSC)) and chlorine and bromine loading is explored using chemistry and transport models (CTMs). A simulation using multi-decadal output from a general circulation model (GCM) in the Goddard Space Flight Center (GSFC) CTM complements one recycling a single year s GCM output in the Global Modeling Initiative (GMI) CTM. Winter polar ozone loss in the GSFC CTM depends on equivalent effective stratospheric chlorine (EESC) and polar vortex characteristics (temperatures, descent, isolation, polar stratospheric cloud amount). Polar ozone loss in the GMI CTM depends only on changes in EESC as the dynamics repeat annually. The GSFC CTM simulation reproduces a linear relationship between ozone loss and Vpsc derived from observations for 1992 - 2003 which holds for EESC within approx.85% of its maximum (approx.1990 - 2020). The GMI simulation shows that ozone loss varies linearly with EESC for constant, high V(sub PSC).

Douglass, A. R.↗

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.↗

Decadal-Scale Responses in Middle and Upper Stratospheric Ozone From SAGE II Version 7 Data

Stratospheric Aerosol and Gas Experiment (SAGE II) version 7 (v7) ozone profiles are analyzed for their decadal-scale responses in the middle and upper stratosphere for 1991 and 1992-2005 and compared with those from its previous version 6.2 (v6.2). Multiple linear regression (MLR) analysis is applied to time series of its ozone number density vs. altitude data for a range of latitudes and altitudes. The MLR models that are fit to the time series data include a periodic 11 yr term, and it is in-phase with that of the 11 yr, solar UV (Ultraviolet)-flux throughout most of the latitude/ altitude domain of the middle and upper stratosphere. Several regions that have a response that is not quite in-phase are interpreted as being affected by decadal-scale, dynamical forcings. The maximum minus minimum, solar cycle (SClike) responses for the ozone at the low latitudes are similar from the two SAGE II data versions and vary from about 5 to 2.5% from 35 to 50 km, although they are resolved better with v7. SAGE II v7 ozone is also analyzed for 1984-1998, in order to mitigate effects of end-point anomalies that bias its ozone in 1991 and the analyzed results for 1991-2005 or following the Pinatubo eruption. Its SC-like ozone response in the upper stratosphere is of the order of 4%for 1984-1998 vs. 2.5 to 3%for 1991-2005. The SAGE II v7 results are also recompared with the responses in ozone from the Halogen Occultation Experiment (HALOE) that are in terms of mixing ratio vs. pressure for 1991-2005 and then for late 1992- 2005 to avoid any effects following Pinatubo. Shapes of their respective response profiles agree very well for 1992-2005. The associated linear trends of the ozone are not as negative in 1992-2005 as in 1984-1998, in accord with a leveling off of the effects of reactive chlorine on ozone. It is concluded that the SAGE II v7 ozone yields SC-like ozone responses and trends that are of better quality than those from v6.2.

Remsberg, E. E.↗

Meridional Variations of C2H2 and C2H6 in Jupiter's Atmosphere from Cassini CIRS Infrared Spectra

Hydrocarbons such as acetylene (C2H2) and ethane (C2H6) are important tracers in Jupiter's atmosphere, constraining our models of the chemical and dynamical processes. However, our knowledge of the vertical and meridional variations of their abundances has remained sparse. During the flyby of the Cassini spacecraft in December 2000, the Composite Infrared Spectrometer (CIRS) instrument was used to map the spatial variation of emissions from 10-1400 cm(sup -1) (1000-7 microns). In this paper we analyze a zonally-averaged set of CIRS spectra taken at the highest (0.5 cm(sup -1)) resolution, to infer atmospheric temperatures in the stratosphere at 0.5-20 mbar via the v4 band of CH4, and in the troposphere at 150-400 mbar, via the H2 absorption at 600-800 cm(sup -1). Simultaneously, we retrieve the abundances of C2H2 and C2H6 via the v5 and vg bands respectively. Tropospheric absorption and stratospheric emission are highly anti-correlated at the CIRS resolution, introducing a non-uniqueness into the retrievals, such that vertical gradient and column abundance cannot both be found without additional constraints. Assuming profile gradients from photochemical calculations, we show that the column abundance of C2H2 decreases sharply towards the poles by a factor approximately 4, while C2H6 is unchanged in the north and increasing in the south, by a factor approximately 1.8. An explanation for the meridional trends is proposed in terms of a combination of photochemistry and dynamics. Poleward, the decreasing UV flux is predicted to decrease the abundances of C2H2 and C2H6 by factors 2.7 and 3.5 respectively at a latitude 70 deg. However, the lifetime of C2H6 in the stratosphere (5 x 10(exp 9)) is much longer than the dynamical timescale for meridional motions inferred from SL-9 debris (5 x 10(exp 8 s)), and therefore the constant or rising abundance towards high latitudes likely indicates that meridional mixing dominates over photochemical effects. For C2H2, the opposite occurs, with the relatively short photochemical lifetime (3 x 10(exp 7 s)), compared to meridional mixing times, ensuring that the expected photochemical trends are visible.

Nixon, C. A.↗

Abundance Measurements of Titan's Stratospheric HCN, HC3N, C3H4, and CH3CN from ALMA Observations

Previous investigations have employed more than 100 close observations of Titan by the Cassini orbiter to elucidate connections between the production and distribution of Titan's vast, organic-rich chemical inventory and its atmospheric dynamics. However, as Titan transitions into northern summer, the lack of incoming data from the Cassini orbiter presents a potential barrier to the continued study of seasonal changes in Titan's atmosphere. In our previous work, we demonstrated that the Atacama Large Millimeter/submillimeter Array (ALMA) is well suited for measurements of Titan's atmosphere in the stratosphere and lower mesosphere (~100 - 500 km) through the use of spatially resolved (beam sizes <1") flux calibration observations of Titan. Here, we derive vertical abundance profiles of four of Titan's trace atmospheric species from the same 3 independent spatial regions across Titan's disk during the same epoch (2012-2015): HCN, HC3N, C3H4, and CH3CN. We find that Titan's minor constituents exhibit large latitudinal variations, with enhanced abundances at high latitudes compared to equatorial measurements; this includes CH3CN, which eluded previous detection by Cassini in the stratosphere, and thus spatially resolved abundance measurements were unattainable. Even over the short 3-year period, vertical profiles and integrated emission maps of these molecules allow us to observe temporal changes in Titan's atmospheric circulation during northern spring. Our derived abundance profiles are comparable to contemporary measurements from Cassini infrared observations, and we find additional evidence for subsidence of enriched air onto Titan's south pole during this time period. Continued observations of Titan with ALMA beyond the summer solstice will enable further study of how Titan's atmospheric composition and dynamics respond to seasonal changes.

Thelen, Alexander E.↗

Temperature dependence of the HNO3 UV absorption cross sections

The temperature dependence of the HNO3 absorption cross sections between 240 and 360 K over the wavelength range 195 to 350 nm has been measured using a diode array spectrometer. Absorption cross sections were determined using both (1) absolute pressure measurements at 298 K and (2) a dual absorption cell arrangement in which the absorption spectrum at various temperatures is measured relative to the room temperature absorption spectrum. The HNO3 absorption spectrum showed a temperature dependence which is weak at short wavelengths but stronger at longer wavelengths which are important for photolysis in the lower stratosphere. The 298 K absorption cross sections were found to be larger than the values currently recommended for atmospheric modeling (DeMore et al., 1992). Our absorption cross section data are critically compared with the previous measurements of both room temperature and temperature-dependent absorption cross sections. Temperature-dependent absorption cross sections of HNO3 are recommended for use in atmospheric modeling. These temperature dependent HNO3 absorption cross sections were used in a two-dimensional dynamical-photochemical model to demonstrate the effects of the revised absorption cross sections on loss rate of HNO3 and the abundance of NO2 in the stratosphere.

Burkholder, James B.↗

Comment on "Observation of Large and All-Season Ozone Losses Over the Tropics" [AIP Advances 12, 075066 (2022)]

As discussed above, and supported by extensive literature, there is no robust, credible observational evidence for substantial ozone depletion (i.e., an “ozone hole”) in the tropics. It is well known that climatological total ozone in the tropics is much lower than that in the mid-latitudes (e.g., Sahai et al., 2000; Weber et al., 2022). Satellite and ozonesonde measurements indicate a 3%–5% per decade decline of tropical lower stratosphere ozone prior to 2000, far smaller than that reported by L2022. The stronger decline reported by L2022 is caused by inappropriate use of the gap-filled version of the TOST ozone dataset, which is based on sparse tropical ozone sondes before the 1990s. This misuse of data (TOST and total column ozone) shows the importance of collaboratively engaging with groups who obtain the measurements and create climatological datasets before performing such analyses. Furthermore, the study by L2022 has multiple flaws in its discussion of atmospheric chemistry and dynamics, particularly in the proposed, and previously refuted (see Sec. III A), cosmicray- driven electron induced (CRE) mechanism. Evidence for the occurrence of tropical stratospheric clouds, as needed for the tropical CRE mechanism, is lacking, nor do CFC-12 observations show signatures of depletion in the tropical lower stratosphere, which could be associated with dissociative electron attachment-induced loss of CFC-12 on particulate matter (i.e., the CRE mechanism). Finally, it is worth reiterating that the CRE mechanism is also not responsible for polar LS ozone depletion. Polar ozone loss can be well explained by the gas phase and heterogeneous chemistry, based on extensive observations and modeling studies documented in many thousands of scientific papers on the topic [e.g., see WMO (2018) and references therein], which is not acknowledged by L2022. L2022’s research paper is a severely flawed one. There is no tropical ozone hole, and the CRE mechanism does not explain observed changes in stratospheric ozone either in the polar regions or in the tropics.

Quality assurance↗

The Polar Vortex and Extreme Weather: The Beast from the East in Winter 2018

Public attention has recently focused on high-impact extreme weather events in midlatitudes that originate in the sub-Arctic. We investigate movements of the stratospheric polar vortex (SPV) and related changes in lower atmospheric circulation during the February-March 2018 “Beast from the East” cold winter event that dramatically affected much of Europe and north-central North America. This study demonstrates that the movement of the SPV is a key linkage in late winter subarctic and northern midlatitude extreme weather events. February–March 2018 saw two types of subarctic-midlatitude weather connections. In the first type, the SPV was displaced from the pole to lower latitudes over North America in February and then was found over northern Siberia in March. Mid-February and mid-March are examples of persistent near vertically aligned geopotential height structures of the atmospheric circulation. These structures over North America and Eurasia advected cold Arctic air southward. The second type of cold surface event was associated with a weak regional SPV and a sudden stratospheric warming event over Europe during the second half of February. These late winter linkage events that arise through dynamic instabilities of the SPV are more common in the last decade, but the potential role of enhanced Arctic amplification is uncertain.

54 ENVIRONMENTAL SCIENCES↗

Nitric acid forecast experiments

Results of two three-dimensional forecasts of the time evolution of the distribution of HNO3 in the stratosphere are reported. The first is for the February 1979 stratospheric warming, and the second is for a period in March, 1979 when the relative importance of photochemistry and dynamics is thought to be rapidly changing. The zonal mean results of the model calculations are in general qualitative agreement with the LIMS HNO3 observations. However, the calculated three-dimensional fields show significant differences from the observations. The results provide insight into what must be done to form a successful constituent forecast model and provide information on the modeling technique and the self-consistency of the observed dynamical and constituent fields.

Rood, Richard B.↗

Investigation of atmospheric waves on Neptune

This document constitutes the final report for grant NAGW-2442 of the Neptune Data Analysis Program, which supported research concerning atmospheric dynamics on Neptune. Professor Von R. Eshleman was the principal investigator. David P. Hinson was a Co-Investigator. The grant covered the period 1 March 1991 through 31 August 1994, including a six month no-cost extension. Funding from this grant resulted in publication of one journal article and one book chapter as well as presentation of results at two conferences and in numerous seminars. A complete bibliography is given below. A copy of the journal article is attached along with abstracts from the book chapter and the conference presentations. With support from this grant we extended our analysis and interpretation of the Voyager Project. This research contributed to an improvement in our basic understanding of atmospheric dynamics on Neptune. The highlight was the discovery and characterization of inertio-gravity waves in the troposphere and stratosphere. Results include measures of basic wave properties, such as amplitudes and vertical wavelengths, as well as estimates of the effect of the waves on the photochemistry and momentum balance of the stratosphere. This investigation also yielded a better understanding of the potential of radio occultation experiments for studies of atmospheric waves. At the same time we developed new methods of data analysis for exploiting these capabilities. These are currently being applied to radio occultation data obtained with the Magellan spacecraft to study waves in the atmosphere of Venus. Future planetary missions, such as Mars Global Surveyor and Cassini, will benefit from these accomplishments.

Eshleman, Von R.↗

Tracer evolution in winds generated by a global spectral mechanistic model

The lower boundary of a spectral mechanistic model is prescribed with 100 hPa geopotentials, and its performance during a November 1989 through March 1990 integration is compared with National Meteorological Center observations. Although the stratopause temperatures quickly become biased near the pole in both hemispheres, the model develops a residual mean circulation which shows significant descent over the winter pole and ascent in the tropics and over the summer pole at pressures less than 10 hPa. The daily correspondence of observed to modeled features in the upper stratosphere and mesosphere degrades after one month. However, the long-term variability qualitatively follows the observations. The results of off-line transport experiments are also described. A passive tracer is instantaneously injected into the flow over the poles and evolves in a manner which is consistent with the residual mean circulation. It demonstrates a significant cross-equatorial flux in the mesosphere near solstice, and air which originates in the southern hemisphere polar mesosphere can be found descending deep into the nothern polar stratosphere at the end of the integration. Nitrous oxide is also transported, and its ability to act as a dynamical tracer is evaluated by comparison to the evolution of the passive tracer.

Nielsen, J. E.↗

Analysis of observations of the middle atmosphere from satellites

Satellite data are being used to investigate problems in middle atmosphere chemistry and dynamics. Efforts have been focused primarily on studies to determine the quality of observed distributions of trace species and derived dynamical quantities. Those data have been used as diagnostics for model-derived constituent profiles and fields and for improving our understanding of some of the fundamental processes occurring in the middle atmosphere. Temperatures and derived winds from Nimbus 7 Limb Infrared Monitoring of the Stratosphere (LIMS) data were compared with long-time series of rawinsonde data at Invercargill, New Zealand, and Berlin, West Germany, and the results are excellent for both quantities. It was also demonstrated that more highly-derived dynamical quantities can be obtained reliably from those LIMS fields. Furthermore, both the diabatic and residual-mean circulations derived using LIMS data agree qualitatively with changes in the distribution of trace species determined independently with the Nimbus 7 SAMS and LIMS experiments. Subsequently, an examination of LIMS data at mid to high latitudes of the Southern Hemisphere has revealed a synoptic-scale, upper stratospheric instability during late autumn that is associated with the development of the stratospheric polar jet. Investigation of this phenomenon continues with Stratospheric Sounding Unit (SSU) data sets.

Remsberg, Ellis E.↗

Radiative Forcing of the Stratosphere by SO(sub 2) Gas, Silicate Ash, and H(sub 2)SO(sub 4) Aerosols Shortly after the 1982 Eruptions of El Chichon

The 1982 eruptions of El Chichon Volcano injected large quantities of sulfur dioxide gas and silicate ash into the stratosphere. Several studies have shown that the long-lived sulfuric acid aerosols derived from these volcanic effluents produced measurable changes in the radiative heating rates and the global circulation. The radiative and dynamical perturbations associated with the short-lived, but more strongly absorbing sulfur dioxide and ash clouds have received much less attention. We therefore used an atmospheric radiative transfer model and observations collected by satellites, aircraft, and ground based observers to estimate the amplitudes of the stratospheric radiative heating rate perturbations produced by each of these components during the first few weeks after the El Chichon eruption. One week after the April 4, 1982 eruption, net radiative heating rate perturbations exceeding 20 Kelvin per day were found at altitudes near 26 km.

El Chichon↗

Balloon Borne Arc-Second Pointer Feasibility Study

For many years scientists have been utilizing stratospheric balloons as low-cost platforms on which to conduct space science experiments. A major hurdle in extending the range of experiments for which these vehicles are useful has been the imposition of the gondola dynamics on the accuracy with which an instrument can be kept pointed at a celestial target. A significant number of scientists have sought the ability to point their instruments with jitter in the arc-second range. This paper presents the design and analysis of a stratospheric balloon borne pointing system that is able to meet this requirement. The foundation for a high fidelity controller simulation is presented. The flexibility of the flight train is represented through generalized modal analysis. A multiple controller scheme is introduced for coarse and fine pointing. Coarse azimuth pointing is accomplished by an established pointing system, with extensive flight history, residing above the gondola structure. A pitch-yaw gimbal mount is used for fine pointing, providing orthogonal axes when nominally on target. Fine pointing actuation is from direct drive dc motors, eliminating backlash problems. An analysis of friction nonlinearities and a demonstration of the necessity in eliminating static fiction are provided. A unique bearing hub design is introduced that eliminates static fiction from the system dynamics. A control scheme involving linear accelerometers for enhanced disturbance rejection is also presented. Results from a linear analysis of the total system and the high fidelity simulation are given. This paper establishes that the proposed control strategy can be made robustly stable with significant design margins. Also demonstrated is the efficacy of the proposed system in rejecting disturbances larger than those considered realistic. Finally, we see that sub arc-second pointing stability can be achieved for a large instrument pointing at an inertial target.

Ward, Philip R.↗

The global distribution and variability of stratospheric constituents measured by LIMS

The purpose of the Nimbus 7 LIMS experiment was to sound the composition and structure of the upper atmosphere and provide data for study of photochemistry, radiation, and dynamics processes. Vertical profiles were measured of temperature and ozone (O3) over the 10-km to 65-km range and water vapor, nitrogen dioxide, and nitric acid over the 10-km to 50-km range. Latitude coverage extended from 64 deg S to 84 deg N. Several general features of the atmosphere have emerged from data analyzes thus far. Nitrogen dioxide exhibits rapid latitudinal variations in winter and shows hemispheric asymmetry with generally higher vertical column amount in the summer hemisphere. HNO3 data show that this gas is highly variable with altitude, latitude, and season. Smallest mixing ratios occur in the tropics, and the largest values occur in the high latitude winter hemisphere. The results show that O3, NO2, and HNO3 are strongly affected during a stratospheric warming.

Russell, J. M., III↗

Simulations of Water Vapor in the Upper Troposphere and Lower Stratosphere

A detailed study of the water vapor budget in the upper troposphere and lower stratosphere of the "Finite Volume CCM3" (FVCCM3) model is presented. The model is based on a combination of a finite-volume dynamical core (developed by Lin and Rood) and the physical package from Version 3 of the Community Climate Model (CCM3, developed at NCAR). The model was used with a horizontal resolution of 2 by 2.5 degrees and 55 levels, with the upper boundary at 0.0lhPa and a vertical resolution of about 1.2km near the tropopause. Most results presented are from a 17-year simulation performed for the Atmospheric Model Intercomparison Project. It is shown that the model simulates a realistic thermal structure in the tropical tropopause region and that water vapor distributions are in qualitative accord with observations (which are uncertain). The longitudinal structure of the tropical atmosphere is slightly too asymmetric, compared to reasonable estimates of the truth. The processes leading to the horizontal and vertical transport of water vapor in the tropopause region are analyzed in detail. Special attention is given to the realism of horizontal transport events (the ability of the model to retain sharply defined features) and to the role of localized vertical motions in transporting air (and water vapor) between the troposphere and stratosphere. It is shown that the vertical transport of water vapor in the tropical lower stratosphere occurs at about the same rate as that observed, while in many other models this vertical transport is too fast.

Pawson, Steven↗

Strategic Ozone Sounding Networks: Review of Design and Accomplishments

Ozone soundings are used to integrate models, satellite, aircraft and ground-based measurements for better interpretation of ozone variability, including atmospheric losses (predominantly in the stratosphere) and pollution (troposphere). A well-designed network of ozonesonde stations gives information with high vertical and horizontal resolution on a number of dynamical and chemical processes, allowing us to answer questions not possible with aircraft campaigns or current satellite technology. Strategic ozonesonde networks are discussed for high, mid- and low latitude studies. The Match sounding network was designed specifically to follow ozone depletion within the polar vortex; the standard sites are at middle to high northern hemisphere latitudes and typically operate from December through mid-March. Three mid-latitude strategic networks (the IONS series) operated over North America in July-August 2004, March-May and August 2006, and April and June-July-2008. These were designed to address questions about tropospheric ozone budgets and sources, including stratosphere-troposphere transport, and to validate satellite instruments and models. A global network focusing on processes in the equatorial zone, SHADOZ (Southern Hemisphere Additional Ozonesondes), has operated since 1998 in partnership with NOAA, NASA and the Meteorological Services of host countries. Examples of important findings from these networks are described,

Thompson, Anne M.↗

Testing the Equivalence Principle in an Einstein Elevator: Detector Dynamics and Gravity Perturbations

We discuss specific, recent advances in the analysis of an experiment to test the Equivalence Principle (EP) in free fall. A differential accelerometer detector with two proof masses of different materials free falls inside an evacuated capsule previously released from a stratospheric balloon. The detector spins slowly about its horizontal axis during the fall. An EP violation signal (if present) will manifest itself at the rotational frequency of the detector. The detector operates in a quiet environment as it slowly moves with respect to the co-moving capsule. There are, however, gravitational and dynamical noise contributions that need to be evaluated in order to define key requirements for this experiment. Specifically, higher-order mass moments of the capsule contribute errors to the differential acceleration output with components at the spin frequency which need to be minimized. The dynamics of the free falling detector (in its present design) has been simulated in order to estimate the tolerable errors at release which, in turn, define the release mechanism requirements. Moreover, the study of the higher-order mass moments for a worst-case position of the detector package relative to the cryostat has led to the definition of requirements on the shape and size of the proof masses.

Hubbard, Dorthy↗