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At least 73 records · Page 4

The Influence of Extremely Large Solar Proton Events in a Changing Stratosphere. Stratospheric Influence of Solar Proton Events

Two periods of extremely large solar proton events (SPEs) occurred in the past thirty years, which forced significant long-term polar stratospheric changes. The August 2-10, 1972 and October 19-27, 1989 SPEs happened in stratospheres that were quite different chemically. The stratospheric chlorine levels were relatively small in 1972 (approximately 1.2 ppbv) and were fairly substantial in 1989 at about (approximately 3 ppbv). Although these SPEs produced both HO(x) and NO(y) constituents in the mesosphere and stratosphere, only the NO(y) constituents had lifetimes long enough to affect ozone for several months to years past the events. Our recently improved two-dimensional chemistry and transport atmospheric model was used to compute the effects of these gigantic SPEs in a changing stratosphere. Significant upper stratospheric ozone depletions > 10% are computed to last for a few months past these SPEs. The long-lived SPE-produced NO(y) constituents were transported to lower levels during winter after these huge SPEs and caused impacts in the middle and lower stratosphere. During periods of high halogen loading these impacts resulted in interference with the chlorine and bromine loss cycles for ozone destruction. The chemical state of the atmosphere, including the stratospheric sulfate aerosol density, substantially affected the predicted stratospheric influence of these extremely large SPEs.

Jackman, Charles H.↗

Toward a Combined SAGE II-HALOE Aerosol Climatology: An Evaluation of HALOE Version 19 Stratospheric Aerosol Extinction Coefficient Observations

Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 microns is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 microns is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 micron aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40micronaerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 micron channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

Thomason, L. W.↗

OMI Measurements of Bromine Monoxide and Implications for Missing Sources of Polar Bromine in GEOS-Chem

The OMI satellite instrument provides total column measurements of bromine monoxide (BrO) with daily global coverage. Reactive bromine compounds (Br and BrO) catalytically destroy ozone in both the stratosphere and troposphere. The current emission scheme of brominated source gases in the GEOS-Chem chemical transport model well represents the stratospheric burden of bromine. However, halogen research in GEOS-Chem has largely focused on the influence of halogens on the tropospheric oxidative capacity. In the troposphere, the distribution of brominated compounds is more variable and significant uncertainties remain in the chemical processes governing the sources and sinks of reactive bromine compounds. In this study, we use GEOS-Chem simulated stratospheric columns of BrO to separate the tropospheric signal of BrO from the OMI total column measurements. The resulting tropospheric BrO columns are used to identify seasonal and regional anomalies in tropospheric BrO not currently represented in GEOS-Chem. In particular, periods of elevated tropospheric BrO during polar spring are observable by OMI, and past studies have connected these so-called "bromine explosion" events to near complete removal of surface ozone. Due to significant uncertainties in the springtime polar source of reactive bromine, many global models, including GEOS-Chem, do not simulate these tropospheric ozone depletion events. Consequently, OMI-based tropospheric columns of BrO are useful tool for investigating the impact of bromine explosion events on tropospheric ozone depletion episodes as well as background air quality.

Wales, Pamela↗

Stratospheric Temperature and Ozone Impacts of the Hunga Tonga-Hunga Ha'apai Water Vapor Injection

The January 2022 eruption of the Hunga Tonga-Hunga Ha'apai underwater volcano injected a large amount of water vapor into the mid-stratosphere. This study uses model simulations to investigate the resulting stratospheric impacts out to 2031. Maximum radiatively-driven model temperature changes occur in the Southern Hemisphere (SH) subtropics in April–May 2022, with warming of ∼1 K in the lower stratosphere and cooling of 3 K in the mid-stratosphere. The radiative cooling combined with adiabatic cooling driven by the quasi-biennial oscillation meridional circulation explains the near-record cold anomaly observed in the SH subtropical mid-stratosphere. Projected ozone responses maximize in 2023–2024 as the water vapor plume is transported globally throughout the stratosphere and mesosphere. The excess H2O increases the OH radical, causing a negative global ozone response (2%–10%) in the upper stratosphere and mesosphere due to increased odd hydrogen-ozone loss, and a small positive ozone response (0.5%–1%) in the mid-stratosphere due to interference of the NOx catalytic loss cycle by the additional OH. In the lower stratosphere, the excess H2O is projected to increase polar stratospheric clouds and springtime halogen-ozone loss, enhancing the Antarctic ozone hole by 25–30 DU in 2023. Arctic impact is small, with maximum additional ozone loss of 4–5 DU projected in spring 2024. These responses diminish after 2024 to be quite small by 2031, as the excess H2O is removed from the stratosphere with a 2.5-year e-folding time. Given the year-to-year variability of the stratosphere, the magnitudes of these ozone responses may be below the threshold of detectability in observations.

stratosphere↗

A kinetics investigation of several reactions involving chlorine containing compounds

The technique of flash photolysis-resonance fluorescence was utilized to study nine reactions of stratospheric importance. The tropospheric degradation reactions of seven halogenated hydrocarbons were studied to assess their possible influx into the stratosphere. There are reactions of either Cl, OH, or O(3P) species with hydrogenated species, O3 or chlorinated compounds. Apart from the kinetic measurements, the quantum yield for the production of O(1D) from O3 in the crucial wavelength region of 293 to 316.5 nm was studied by utilizing a narrow wavelength laser as the photolysis source. The product formation was monitored by measuring the fluorescence of NO2 formed through O(1D) reaction with N2O followed by NO reaction with O3 to give NO2.

Davis, D. D.↗

Using Kalman Filter Chemical Data Assimilation to Study Ozone Catalytic Loss Cycles in January 1992

This paper presents for the first time a global study of the ozone catalytic destruction cycles operating in the stratosphere using a stratospheric analyses for January 1992. The chemical analyses were produced using a Kalman filter data assimilation system. Because a major component of the variability of trace gases is due to the atmospheric motions the analyses have been cast in a flow-tracking coordinate system that moves with the large scale flow pattern. Particular attention is paid to the kinetic aspects of these cycles such as the rate limiting step and chain length. Although it is an important kinetic parameter, the chain length of the various cycles is seldom considered when the various catalytic cycles are discussed. This survey highlights that in the low stratosphere the cycles involving HO2 and halogens (notably bromine) are particularly important. In approximate order of effectiveness the most important ozone loss cycles in the polar lower stratosphere are the BrO/ClO, HO2/BrO, and OH/HO2 cycles. The ClO/ClO cycle clearly delineates the regions of chlorine activation. The chain length of the HO2/ClO, OH/HO2, Br/BrO, and ClO/NO2, clearly delineate the vortex edge region. The chain length of the BrO/NO2 and Cl/NO2 cycles highlight the regions of chemical processing outside the vortex where streamers of chemically processed air are stripped-off and transported away from the vortex. This is also true in the very low stratosphere for the Cl/ClO and BrO/ClO cycles.

Lary, David J.↗

Trends from the Long-term Data Record and Models: What Do They Tell Us About our Ability to Predict Ozone Recovery?

Our industrial society has performed an experiment on the stratospheric ozone layer over the last several decades. The initial part of this experiment was the rapidly increasing release of halogen-containing compounds that carry chlorine and bromine to the stratosphere where they can cause a loss of ozone. The present part of this experiment is the implementation of the Montreal Protocol, which has led to a leveling off of these halogen compounds and the beginning of their slow removal from the atmosphere. The observation and attribution of ozone response to the halogens has been a particularly important and difficult task because of the impact of solar cycle uv variation, two major volcanic eruptions (El Chichon and Pinatubo), and interannual dynamic variability of the stratosphere. We have run 3 different simulations of the chemistry and transport of ozone and the minor constituents that affect ozone to help evaluate our understanding of the causes of ozone change and to assess our ability to predict ozone recovery with the removal of halogens from the stratosphere. One simulation, using the Goddard chemical transport model (CTM), had interannual variability in the dynamics for the entire 50 years of simulation, which included the past 3 decades (1974-2004) and the next 2 decades to 2022. The other two simulations used the Global Modeling Initiative (GMI) CTM with no dynamical variability: one used a the winds and temperatures from a repeating warm Arctic winter and the other used a repeating cold Arctic winter. All simulations included the effects of aerosol surfaces from volcanic eruptions on chemical reactions as well as the variation in UV over the 11-year solar cycle.

Strahan, Susan↗

Chlorine-hydrocarbon photochemistry in the marine troposphere and lower stratosphere

The role of chlorine atoms in the oxidation of methane and nonmethane hydrocarbons (NMHCs) in the marine troposphere and lower stratosphere was investigated using a one-dimensional photochemical model that incorporated the chemistry of CH4, NMHCs, NO(x), O(x), and HO(x), as well as organic and inorganic halogens in the troposphere and lower stratosphere. The model predicted that chlorine atoms are present in the marine troposphere at the concentrations of about 1000/cu cm, mostly as a product of the reaction between OH and HCl released from sea spray. The results indicate that Cl atoms cause 20 to 40 percent of NMHC oxidation in the troposphere and 40 to 90 percent in the lower stratosphere. At 15 km, the NMHC-Cl reactions account for nearly 80 percent of the PAN produced. Where available, experimental data confirmed the model predictions.

Singh, H. B.↗

Evaluation of Upper-Tropospheric and Lower-Stratospheric Ozone Profiles from a Global Ozone Data Assimilation System

The Data Assimilation Office at NASA's Goddard Space Flight Center provides global 3D ozone fields at six-hour time intervals. Data from Total Ozone Mapping Spectrometer (TOMS) and the Solar Backscatter Ultraviolet (SBUV) instrument are used in the assimilation. TOMS provides total column information and SBUV provides profile information, primarily above the ozone peak. Information below the ozone peak comes from the model. This paper will explore the realism of the assimilated ozone in the upper troposphere and lower stratosphere through validation with ozonesondes, Halogen Occultation Experiment (HALOE), and Polar Ozone and Aerosol Measurement (POAM) observations. This work is in preparation of using the assimilated ozone in the radiative calculation for the meteorological assimilation as well as in the derivation of tropospheric ozone.

Rood, Richard B.↗

Properties of Stratospheric Aerosol Estimated from HALOE Data

Extinction coefficients for stratospheric aerosols at 8 HALOE (HALogen Occultation Experiment) wavelengths are determined by comparing transmittances data for two adjacent solar occultation measurements, where one limb path is loaded with aerosols but the other path is free of aerosols. These extinction coefficients are used to infer the aerosol properties such as composition and size distribution parameters. Mie theory has been used to calculate the extinction coefficients, and a nonlinear least square method is applied to determine the aerosol properties. Sixteen cases are selected for the retrieval in southern hemisphere at latitudes from 21 to 48 deg S for the period of 29 Mar - 31 May 1992. Retrieved size width ranges from 1.1 to 1.5 and radius ranges from 0.25 to 0.45 micrometers. These size parameters are within the ranges of in situ measurements at Laramie, Wyoming. Retrieved weight percent of H2SO4 is larger than the equilibrium value by about 5 to approximately 10 weight percent, similar to the results for northern hemisphere at latitudes 20 to 55 deg N for the period from Nov 1991 to Feb. 1992.

Lee, Kwang-Mog↗

A New Formulation of Equivalent Effective Stratospheric Chlorine (EESC)

Equivalent effective stratospheric chlorine (EESC) is a convenient parameter to quantify the effects of halogens (chlorine and bromine) on ozone depletion in the stratosphere. We show and discuss a new formulation of EESC that now includes the effects of age-of-air dependent fractional release values and an age-of-air spectrum. This new formulation provides quantitative estimates of EESC that can be directly related to inorganic chlorine and bromine throughout the stratosphere. Using this EESC formulation, we estimate that human-produced ozone depleting substances will recover to 1980 levels in 2041 in the midlatitudes, and 2067 over Antarctica. These recovery dates are based upon the assumption that the international agreements for regulating ozone-depleting substances are adhered to. In addition to recovery dates, we also estimate the uncertainties in the estimated time of recovery. The midlatitude recovery of 2041 has a 95% confidence uncertainty from 2028 to 2049, while the 2067 Antarctic recovery has a 95% confidence uncertainty from 2056 to 2078. The principal uncertainties are from the estimated mean age-of-air, and the assumption that the mean age-of-air and fractional release values are time independent. Using other model estimates of age decrease due to climate change, we estimate that midlatitude recovery may be accelerated from 2041 to 2031.

Newman, P. A.↗

Effect of the HITRAN 92 spectral data on the retrieval of NO2 mixing ratios from Nimbus 7 LIMS

To ensure spectral consistency when comparing Nimbus 7 Limb Infrared Monitor of the Stratosphere Experiment (LIMS) NO2 distributions with those from Atmosphere Trace Molecule Spectroscopy (ATMOS) and Upper Atmosphere Research Satellite Experiments (UARS), 1 day (May 5, 1979) of LIMS measurements were reprocessed using the NO2 line list on the HITRAN 92 tape compiled by the Airforce Geophysics Laboratory (AFGL). The revised NO2 mixing ratios are smaller by up to 20%. The decrease is not constant with height, latitude, or time of day but depends on the absolute amount of NO2 in the profile, as a result of a change in the degree of saturation for the strong NO2 spectral lines. The revised NO2 agrees better with correlative measurements and with NO2 distributions from the Stratospheric Aerosol and Gas Experiment (SAGE) and Halogen Occultation Experiment (HALOE) satellite experiments but not with those from ATMOS 85. Profiles of the day/night ratio of revised NO2 are now larger near 5 hPa. There is also some improvement between observed and modeled ozone in the upper stratosphere, when the revised nighttime NO2 profile is used as the estimate of NO(y) for the model calculations.

Remsburg, Ellis E.↗

Multi-Model Assessment of the Factors Driving the Ozone Evolution Over the 21st Century

The evolution of ozone from 1960 to 2100 is examined in simulations from fourteen chemistry-climate models. There is general agreement among the models at the broadest levels, with all showing column ozone decreasing at all latitudes from 1960 to around 2000, then increasing at all latitudes over the first half of the 21 st century (21 C), and latitudinal variations in the rate of increase and date of return to historical values. In the second half of the century, ozone is projected to carry on increasing, level off or even decrease depending on the latitude, resulting in variable dates of return to historical values at latitudes where column ozone has declined below those levels. Separation into partial column above and below 20 hPa reveals that these latitudinal differences are almost completely due to differences in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21 C and returns to 1960 levels before the end of the century, although there is a spread among the models in dates that ozone returns to historical values. Using multiple linear regression the upper stratospheric ozone increase comes from almost equal contributions due to decrease in halogens and cooling from increased greenhouse gas concentrations. The evolution of lower stratospheric ozone differs with latitude. In the tropical lower stratosphere an increase in tropical upwelling causes a steady decrease in ozone through the 21C, and total column ozone does not return to 1960 levels in all models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21 C and returns to 1960 levels. For all models there is an earlier return for ozone to historical levels in the northern hemisphere. This is thought to be due to interhemispheric differences in transport.

Oman, L.↗

Long-term Ozone Changes and Associated Climate Impacts in CMIP5 Simulations

Ozone changes and associated climate impacts in the Coupled Model Intercomparison Project Phase 5 (CMIP5) simulations are analyzed over the historical (1960-2005) and future (2006-2100) period under four Representative Concentration Pathways (RCP). In contrast to CMIP3, where half of the models prescribed constant stratospheric ozone, CMIP5 models all consider past ozone depletion and future ozone recovery. Multimodel mean climatologies and long-term changes in total and tropospheric column ozone calculated from CMIP5 models with either interactive or prescribed ozone are in reasonable agreement with observations. However, some large deviations from observations exist for individual models with interactive chemistry, and these models are excluded in the projections. Stratospheric ozone projections forced with a single halogen, but four greenhouse gas (GHG) scenarios show largest differences in the northern midlatitudes and in the Arctic in spring (approximately 20 and 40 Dobson units (DU) by 2100, respectively). By 2050, these differences are much smaller and negligible over Antarctica in austral spring. Differences in future tropospheric column ozone are mainly caused by differences in methane concentrations and stratospheric input, leading to approximately 10DU increases compared to 2000 in RCP 8.5. Large variations in stratospheric ozone particularly in CMIP5 models with interactive chemistry drive correspondingly large variations in lower stratospheric temperature trends. The results also illustrate that future Southern Hemisphere summertime circulation changes are controlled by both the ozone recovery rate and the rate of GHG increases, emphasizing the importance of simulating and taking into account ozone forcings when examining future climate projections.

tropospheric ozone↗

Changing composition of the global stratosphere

The current understanding of stratospheric chemistry is reviewed with particular attention to the influence of human activity. Models are in good agreement with measurements for a variety of species in the mid-latitude stratosphere, with the possible exception of ozone (O3) at high altitude. Rates calculated for loss of O3 exceed rates for production by about 40 percent at 40 kilometers, indicating a possible but as yet unidentified source of high-altitude O3. The rapid loss of O3 beginning in the mid-1970s at low altitudes over Antarctica in the spring is due primarily to catalytic cycles involving halogen radicals. Reactions on surfaces of polar stratospheric clouds play an important role in regulating the abundance of these radicals. Similar effects could occur in northern polar regions and in cold regions of the tropics. It is argued that the Antarctic phenomenon is likely to persist: prompt drastic reduction in the emission of industrial halocarbons is required if the damage to stratospheric O3 is to be reversed.

Mcelroy, Michael B.↗

Evidence for slowdown in stratospheric ozone loss: First stage of ozone recovery

Global ozone trends derived from the Stratospheric Aerosol and Gas Experiment I and II (SAGE I/II) combined with the more recent Halogen Occultation Experiment (HALOE) observations provide evidence of a slowdown in stratospheric ozone losses since 1997. This evidence is quantified by the cumulative sum of residual differences from the predicted linear trend. The cumulative residuals indicate that the rate of ozone loss at 35- 45 km altitudes globally has diminished. These changes in loss rates are consistent with the slowdown of total stratospheric chlorine increases characterized by HALOE HCI measurements. These changes in the ozone loss rates in the upper stratosphere are significant and constitute the first stage of a recovery of the ozone layer.

Newchurch, M. J.↗