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The Influence of Large Solar Proton Events on the Atmosphere

Solar proton events (SPEs) can cause changes in constituents in the Earth s polar middle atmosphere. A number of large SPEs have occurred over the past 50 years and tend to happen most frequently near solar maximum. The highly energetic protons cause ionizations, excitations, dissociations, and dissociative ionizations of the background constituents. Complicated ion chemistry leads to HOx (H, OH, HO2) production and dissociation of N2 leads to NOy (N, NO, NO2, NO3, N2O5, HNO3, HO2NO2, ClONO2, BrONO2) production. Both the HOx and NOy increases can result in changes to ozone in the stratosphere and mesosphere. The HOx increases lead to short-lived (~days) ozone decreases in the mesosphere and upper stratosphere. The NOy increases lead to long-lived (~several months) stratospheric ozone changes because of the long lifetime of NOy constituents in this region. UARS HALogen Occultation Experiment (HALOE) instrument observations showed SPE-caused polar stratospheric NOx (NO+NO2) increases over 10 ppbv in September 2000 due to the very large SPE of July 2000, which are reasonably well simulated with the Whole Atmosphere Community Climate Model (WACCM). WACCM-computed SPE-caused polar stratospheric ozone decreases >10% continued for up to 5 months past the largest events in the past 50 years, however, SPE-caused total ozone changes were not found to be statistically significant. Small polar middle atmospheric temperature changes of <4 K have also been predicted to occur as a result of the larger SPEs. The polar atmospheric effects of large SPEs during solar cycle 23 and 24 will be emphasized in this presentation.

Jackman, Charles H.↗

Long-term Evolution of Upper Stratospheric Ozone at Selected Stations of the Network for the Detection of Stratospheric Change (NDSC)

The long-term evolution of upper stratospheric ozone has been recorded by lidars and microwave radiometers within the ground-based Network for the Detection of Stratospheric Change (NDSC), and by the space-borne Solar Backscatter Ultra-Violet instruments (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE), and Halogen Occultation Experiment (HALOE). Climatological mean differences between these instruments are typically smaller than 5% between 25 and 50 km. Ozone anomaly time series from all instruments, averaged from 35 to 45 km altitude, track each other very well and typically agree within 3 to 5%. SBUV seems to have a slight positive drift against the other instruments. The corresponding 1979 to 1999 period from a transient simulation by the fully coupled MAECHAM4-CHEM chemistry climate model reproduces many features of the observed anomalies. However, in the upper stratosphere the model shows too low ozone values and too negative ozone trends, probably due to an underestimation of methane and a consequent overestimation of ClO. The combination of all observational data sets provides a very consistent picture, with a long-term stability of 2% or better. Upper stratospheric ozone shows three main features: (1) a decline by 10 to 15% since 1980, due to chemical destruction by chlorine; (2) two to three year fluctuations by 5 to 10%, due to the Quasi-Biennial Oscillation (QBO); (3) an 11-year oscillation by about 5%, due to the 11-year solar cycle. The 1979 to 1997 ozone trends are larger at the southern mid-latitude station Lauder (45 S), reaching 8%/decade, compared to only about 6%/decade at Table Mountain (35 N), Haute Provence/Bordeaux (approximately equal to 45 N), and Hohenpeissenberg/Bern(approximately equal to 47 N). At Lauder, Hawaii (20 N), Table Mountain, and Haute Provence, ozone residuals after subtraction of QBO- and solar cycle effects have levelled off in recent years, or are even increasing. Assuming a turning point in January 1997, the change of trend is largest at southern mid-latitude Lauder, +11%/decade, compared to +7%/decade at northern mid-latitudes. This points to a beginning recovery of upper stratospheric ozone. However, chlorine levels are still very high and ozone will remain vulnerable. At this point the most northerly mid-latitude station, Hohenpeissenberg/Bern differs from the other stations, and shows much less clear evidence for a beginning recovery, with a change of trend in 1997 by only +3%/decade. In fact, record low upper stratospheric ozone values were observed at Hohenpeissenberg/Bern, and to a lesser degree at Table Mountain and Haute Provence, in the winters 2003/2004 and 2004/2005.

Steinbrecht, W.↗

Evidence for a Continuous Decline in Lower Stratospheric Ozone Offsetting Ozone Layer Recovery

Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer-Dobson circulation (BDC), forming a protective "ozone layer" around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60degS and 60degN outside the polar regions (60-90deg). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60degS and 60degN has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60degS and 60degN. We find that total column ozone between 60degS and 60degN appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.

Stratospheric Ozone↗

Methane as a Diagnostic Tracer of Changes in the Brewer-Dobson Circulation of the Stratosphere

This study makes use of time series of methane (CH4/ data from the Halogen Occultation Experiment (HALOE) to detect whether there were any statistically significant changes of the Brewer-Dobson circulation (BDC) within the stratosphere during 1992-2005. The HALOE CH4 profiles are in terms of mixing ratio versus pressure altitude and are binned into latitude zones within the Southern Hemisphere and the Northern Hemisphere. Their separate time series are then analyzed using multiple linear regression (MLR) techniques. The CH4 trend terms for the Northern Hemisphere are significant and positive at 10 N from 50 to 7 hPa and larger than the tropospheric CH4 trends of about 3%decade(exp -1) from 20 to 7 hPa. At 60 N the trends are clearly negative from 20 to 7 hPa. Their combined trends indicate an acceleration of the BDC in the middle stratosphere of the Northern Hemisphere during those years, most likely due to changes from the effects of wave activity. No similar significant BDC acceleration is found for the Southern Hemisphere. Trends from HALOE H2O are analyzed for consistency. Their mutual trends with CH4 are anti-correlated qualitatively in the middle and upper stratosphere, where CH4 is chemically oxidized to H2O. Conversely, their mutual trends in the lower stratosphere are dominated by their trends upon entry to the tropical stratosphere. Time series residuals for CH4 in the lower mesosphere also exhibit structures that are anti-correlated in some instances with those of the tracer-like species HCl. Their occasional aperiodic structures indicate the effects of transport following episodic, wintertime wave activity. It is concluded that observed multi-year, zonally averaged distributions of CH4 can be used to diagnose major instances of wave-induced transport in the middle atmosphere and to detect changes in the stratospheric BDC.

Remsberg, E. E.↗

An Overview of the NASA Spring/Summer 2008 Arctic Campaign - ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites)

ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) is a major NASA led airborne field campaign being performed in the spring and summer of 2008 at high latitudes (http://cloud1.arc.nasa.gov/arctas/). ARCTAS is a part of the International Polar Year program and its activities are closely coordinated with multiple U. S. (NOAA, DOE), Canadian, and European partners. Observational data from an ensemble of aircraft, surface, and satellite sensors are closely integrated with models of atmospheric chemistry and transport in this experiment. Principal NASA airborne platforms include a DC-8 for detailed atmospheric composition studies, a P-3 that focuses on aerosols and radiation, and a B-200 that is dedicated to remote sensing of aerosols. Satellite validation is a central activity in all these platforms and is mainly focused on CALIPSO, Aura, and Aqua satellites. Major ARCTAS themes are: (1) Long-range transport of pollution to the Arctic including arctic haze, tropospheric ozone, and persistent pollutants such as mercury; (2) Boreal forest fires and their implications for atmospheric composition and climate; (3) Aerosol radiative forcing from arctic haze, boreal fires, surface-deposited black carbon, and other perturbations; and (4) Chemical processes with focus on ozone, aerosols, mercury, and halogens. The spring deployment (April) is presently underway and is targeting plumes of anthropogenic and biomass burning pollution and dust from Asia and North America, arctic haze, stratosphere-troposphere exchange, and ozone photochemistry involving HOx and halogen radicals. The summer deployment (July) will target boreal forest fires and summertime photochemistry. The ARCTAS mission is providing a critical link to enhance the value of NASA satellite observations for Earth science. In this talk we will discuss the implementation of this campaign and some preliminary results.

Jacob, Daniel J.↗

High resolution infrared spectroscopy of the sun and the earth's atmosphere from space

The FFT spectrometer used in the atmospheric trace molecule spectroscopy (ATMOS) experiment, flown for the first time aboard the Shuttle Spacelab 3 mission (in April 1985), is described together with the instrument's design parameters, the ATMOS's science objectives, and observational techniques used. The ATMOS experiment acquired more than 1000 atmospheric spectra with an equal number of 'solar only' scans, yielding absorption spectra of some 400 different atmospheric constituents. Data were obtained on such key reservoir species as COF2, HNO4, and N2O5; simultaneous vertical distributions of the minor gases from 5 to 140 km; the entire odd-nitrogen family in the stratosphere; and on most of the halogen-source gases with their corresponding reservoir and sink species.

Farmer, Crofton B.↗

Model calculations of the relative effects of CFCs and their replacements on stratospheric ozone

Because chlorine has been linked to the destruction of stratospheric ozone, the use of many fully halogenated compounds, such as the chlorofluorocarbons CFC-11 and -12, is restricted by international agreement. Hydrohalocarbons are under intensive development as replacements for CFCs. Because they contain hydrogen, these gases are susceptible to tropospheric destruction which significantly shortens their atmospheric lifetimes,. Model calculations show that chlorine-containing hydrohalocarbons have less effect on ozone, by an order of magnitude, than their regulated counterparts.

Fisher, Donald A.↗

A Reference Model for Middle Atmosphere Ozone in 1992-1993

An ozone climatology for the period April 1992 to March 1993 and covering pressures from 0.1 to 100 hPa and from 80 deg N to 80 deg S is derived from satellite-based measurements by the Stratospheric Aerosol and Gas Experiment (SAGE), the Halogen Occultation Experiment (HALOE), and the Microwave Limb Sounder (MLS). At pressures less than 1 hPa, separate distributions are given for daytime and nighttime conditions. From 0.46 to 32 hPa the accuracy of the distribution is estimated to be 5%, and the precision is also approx. 5%. Estimates of atmospheric variability are provided on the basis of standard deviations of the measurements within months. Distributions of ozone monthly means and standard deviations are also given in a potential temperature, equivalent latitude coordinate system. This data set is included in the UARS reference atmosphere, and it is accessible through that web site.

Wang, H. J.↗

A Reference Model for Middle Atmosphere Ozone in 1992/1993: Differences from That of Keating et al (1996)

Ozone distributions have been derived from recent satellite-based measurements by the Stratospheric Aerosol and Gas Experiment (SAGE), the Halogen Occultation Experiment (HALOE) and the Microwave Limb Sounder (MLS). An ozone distribution for the period April 1992 to March 1993 and covering pressures from 0.1 to 100 mb and from 80 deg N to 80 deg S is summarized. At pressures less than 1 mb, separate distributions are given for daytime and nighttime conditions. The resulting distributions extend to somewhat higher latitudes and lower altitudes than previous COSPAR reference atmosphere distributions for ozone. Differences versus the most recent COSPAR distribution by Keating et al are illustrated.

Wang, H. J.↗

Solar Occultation Satellite Data and Derived Meteorological Products: Sampling Issues and Comparisons with Aura MLS

Derived Meteorological Products (DMPs, including potential temperature (theta), potential vorticity, equivalent latitude (EqL), horizontal winds and tropopause locations) have been produced for the locations and times of measurements by several solar occultation (SO) instruments and the Aura Microwave Limb Sounder (MLS). DMPs are calculated from several meteorological analyses for the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer, Stratospheric Aerosol and Gas Experiment II and III, Halogen Occultation Experiment, and Polar Ozone and Aerosol Measurement II and III SO instruments and MLS. Time-series comparisons of MLS version 1.5 and SO data using DMPs show good qualitative agreement in time evolution of O3, N2O, H20, CO, HNO3, HCl and temperature; quantitative agreement is good in most cases. EqL-coordinate comparisons of MLS version 2.2 and SO data show good quantitative agreement throughout the stratosphere for most of these species, with significant biases for a few species in localized regions. Comparisons in EqL coordinates of MLS and SO data, and of SO data with geographically coincident MLS data provide insight into where and how sampling effects are important in interpretation of the sparse SO data, thus assisting in fully utilizing the SO data in scientific studies and comparisons with other sparse datasets. The DMPs are valuable for scientific studies and to facilitate validation of non-coincident measurements.

Manney, Gloria↗

Mechanisms and Feedbacks Causing Changes in Upper Stratospheric Ozone in the 21st Century

Stratospheric ozone is expected to increase during the 21st century as the abundance of halogenated ozone-depleting substances decrease to 1960 values. However, climate change will likely alter this "recovery" of stratospheric ozone by changing stratospheric temperatures, circulation, and abundance of reactive chemical species. Here we quantity the contribution of different mechanisms to changes in upper stratospheric ozone from 1960 to 2100 in the Goddard Earth Observing System Chemistry-Climate Model (GEOS CCM), using multiple linear regression analysis applied to simulations using either Alb or A2 greenhouse gas (GHG) scenarios. In both these scenarios upper stratospheric ozone has a secular increase over the 21st century. For the simulation using the Alb GHG scenario, this increase is determined by the decrease in halogen amounts and the greenhouse gas induced cooling, with roughly equal contributions from each mechanism. There is a larger cooling in the simulation using the A2 GHG scenario, but also enhanced loss from higher NOy and HOx concentrations, which nearly offsets the increase due to cooler temperatures. The resulting ozone evolutions are similar in the A2 and Alb simulations. The response of ozone due to feedbacks from temperature and HOx changes, related to changing halogen concentrations, are also quantified using simulations with fixed halogen concentrations.

Oman, Luke↗

Halogens and the Chemistry of the Free Troposphere

The role of halogens in both the marine boundary layer and the stratosphere has long been recognized, while their role in the free troposphere is often not considered in global chemical models. However, a careful examination of free-tropospheric chemistry constrained by observations using a full chemical data assimilation system shows that halogens do play a significant role in the free troposphere. In particular, the chlorine initiation of methane oxidation in the free troposphere can contribute more than 10%, and in some regions up to 50%, of the total rate of initiation. The initiation of methane oxidation by chlorine is particularly important below the polar vortex and in northern mid-latitudes. Likewise, the hydrolysis of BrONO2 alone can contribute more than 35% of the HNO3 production rate in the free-troposphere.

Lary, David John↗

TOMS and SBUV Data: Comparison to 3D Chemical-Transport Model Results

We have updated our merged ozone data (MOD) set using the TOMS data from the new version 8 algorithm. We then analyzed these data for contributions from solar cycle, volcanoes, QBO, and halogens using a standard statistical time series model. We have recently completed a hindcast run of our 3D chemical-transport model for the same years. This model uses off-line winds from the finite-volume GCM, a full stratospheric photochemistry package, and time-varying forcing due to halogens, solar uv, and volcanic aerosols. We will report on a parallel analysis of these model results using the same statistical time series technique as used for the MOD data.

Stolarski, Richard S.↗

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.↗

On the Observed Changes in Upper Stratospheric and Mesospheric Temperatures from UARS HALOE

Temperature versus pressure or T(p) time series from the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite (UARS) have been extended and re-analyzed for the period of 1991-2005 and for the upper stratosphere and mesosphere in 10-degree wide latitude zones from 60S to 60N. Even though sampling from a solar occultation experiment is somewhat limited, it is shown to be quite adequate for developing both the seasonal and longer-term variations in T(p). Multiple linear regression (MLR) techniques were used in the re-analyses for the seasonal and the significant interannual, solar cycle (SC-like or decadal-scale), and linear trend terms. A simple SC-like term of 11-yr period was fitted to the time series residuals after accounting for the seasonal and interannual terms. Highly significant SC-like responses were found for both the upper mesosphere and the upper stratosphere. The phases of these SC-like terms were checked for their continuity with latitude and pressure-altitude, and in almost all cases they are directly in-phase with that of standard proxies for the solar flux variations. The analyzed, max minus min, responses at low latitudes are of order 1 K, while at middle latitudes they are as large as 3 K in the upper mesosphere. Highly significant, linear cooling trends were found at middle latitudes of the middle to upper mesosphere (about -2 K/decade), at tropical latitudes of the middle mesosphere (about -1 K/decade), and at 2 hPa (or order -1 K/decade).

Remsberg, Ellis E.↗

The Impact of New Estimates of Mixing Ratio and Flux-based Halogen Scenarios on Ozone Evolution

The evolution of ozone in the 21st century has been shown to be mainly impacted by the halogen emissions scenario and predicted changes in the circulation of the stratosphere. New estimates of mixing ratio and flux-based emission scenarios have been produced from the SPARC Lifetime Assessment 2013. Simulations using the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM) are conducted using this new A1 2014 halogen scenario and compared to ones using the A1 2010 scenario. This updated version of GEOSCCM includes a realistic representation of the Quasi-Biennial Oscillation and improvements related to the break up of the Antarctic polar vortex. We will present results of the ozone evolution over the recent past and 21st century to the A1 2010, A1 2014 mixing ratio, and an A1 2014 flux-based halogen scenario. Implications of the uncertainties in these estimates as well as those from possible circulation changes will be discussed.

Chemistry-Climate Models↗

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements: Evaluation of Aerosol Measurements from SAGE II, HALOE, and Balloonborne Optical Particle Counters

Stratospheric aerosol measurements from the University of Wyoming balloonborne optical particle counters (OPCs), the Stratospheric Aerosol and Gas Experiment (SAGE) II, and the Halogen Occultation Experiment (HALOE) were compared in the period 1982-2000, when measurements were available. The OPCs measure aerosol size distributions, and HALOE multiwavelength (2.45-5.26 micrometers) extinction measurements can be used to retrieve aerosol size distributions. Aerosol extinctions at the SAGE II wavelengths (0.386-1.02 micrometers) were computed from these size distributions and compared to SAGE II measurements. In addition, surface areas derived from all three experiments were compared. While the overall impression from these results is encouraging, the agreement can change with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount was low, SAGE II and HALOE extinctions were higher than the OPC estimates, while the SAGE II surface areas were lower than HALOE and the OPCS. Under high loading conditions all three instruments mutually agree to within 50%.

Hervig, Mark↗

Spring dehydration in the Antarctic stratospheric vortex observed by HALOE

The distribution of dehydrated air in the middle and lower stratosphere during the 1992 Southern Hemisphere spring is investigated using Halogen Occultation Experiment (HALOE) observations and trajectory techniques. Comparisons between previously published Version 9 and the improved Version 16 retrievals on the 700-K isentropic surface show very slight (0.05 ppmv) increases in Version 16 CH4 relative to Version 9 within the polar vortex. Version 16 H2O mixing ratios show a reduction of 0.5 ppmv relative to Version 9 within the polar night jet and a reduction of nearly 1.0 ppmv in middle latitudes when compared to Version 9. The version 16 HALOE retrievals show low mixing ratios of total hydrogen (2CH4 + H2O) within the polar vortex on both 700 and 425 K isentropic surfaces relative to typical middle-stratospheric 2CH4 + H2O mixing ratios. The low 2CH4 + H2O mixing ratios are associated with dehydration. Slight reductions in total hydrogen, relative to typical middle-stratospheric values, are found at these levels throughout the Southern Hemisphere during this period. Trajectory calculations show that middle-latitude air masses are composed of a mixture of air from within the polar night jet and air from middle latitudes. A strong kinematic barrier to large-scale exchange is found on the poleward flank of the polar night jet at 700 K. A much weaker kinematic barrier is found at 425 K. The impact of the finite tangent pathlength of the HALOE measurements is investigated using an idealized tracer distribution. This experiment suggests that HALOE should be able to resolve the kinematic barrier, if it exists.

Pierce, R. Bradley↗