Changes in ozone over Europe: Analysis of ozone measurements from sondes, regular aircraft (MOZAIC) and alpine surface sites
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J. A. Logan↗
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Causes of Interannual Variability over the Southern Hemispheric Tropospheric Ozone Maximum
We examine the relative contribution of processes controlling the interannual variability (IAV) of tropospheric ozone over four sub-regions of the southern hemispheric tropospheric ozone maximum (SHTOM) over a 20-year period. Our study is based on hindcast simulations from the National Aeronautics and Space Administration Global Modeling Initiative chemistry transport model (NASA GMI-CTM) of tropospheric and stratospheric chemistry, driven by assimilated Modern Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Our analysis shows that over SHTOM region, the IAV of the stratospheric contribution is the most important factor driving the IAV of upper tropospheric ozone (270 hectopascals), where ozone has a strong radiative effect. Over the South Atlantic region, the contribution from surface emissions to the IAV of ozone exceeds that from stratospheric input at and below 430 hectopascals. Over the South Indian Ocean, the IAV of stratospheric ozone makes the largest contribution to the IAV of ozone with little or no influence from surface emissions at 270 and 430 hectopascals in austral winter. Over the tropical South Atlantic region, the contribution from IAV of stratospheric input dominates in austral winter at 270 hectopascals and drops to less than half but is still significant at 430 hectopascals. Emission contributions are not significant at these two levels. The IAV of lightning over this region also contributes to the IAV of ozone in September and December. Over the tropical southeastern Pacific, the contribution of the IAV of stratospheric input is significant at 270 and 430 hectopascals in austral winter, and emissions have little influence.
Global Modeling Initiative chemistry transport mod↗
Radiative Transfer and Retrievals in EOF Domain
The Infrared Atmospheric Sounding Interferometer (IASI) is a hyperspectral sensor with 8461 spectral channels and a nominal spectral resolution of 0.25 cm(sup -1). It is computationally intensive to perform radiative transfer calculations and inversions using all these channels. We will present a Principal Component-based Radiative Transfer Model (PCRTM) and a retrieval algorithm which perform all the necessary calculations in EOF domain. Since the EOFs are orthogonal to each other, only about 100 principal components are needed to represent the information content of the 8461 channels. The PCRTM provides the EOF coefficients and associated derivatives with respect to atmospheric and surface parameters needed by the inversion algorithm. The inversion algorithm is based on a non-linear Levenberg-Marquardt method with climatology covariance and a priori information as constraints. The retrieved parameters include atmospheric temperature, moisture and ozone profiles, cloud parameters, surface skin temperature, and surface emissivities. To make the retrieval system even more compact and stable. The atmospheric vertical profiles are compressed into the EOF space as well. The surface emissivities are also compressed into EOF space.
Liu, Xu↗
Solar radiation incident on the Martian surface
Calculations indicate that the maximum daily solar radiation reaching the Martian surface is about 325 cal/sq cm during southern hemisphere summer at latitude of about 40 deg S. In the ultraviolet region of the spectrum, the radiation reaching the surface at wavelengths greater than 2800 A is within 10% of the radiation incident on the atmosphere. There is significant extinction of radiation in the spectral region near 2500 A in mid and high latitudes due to absorption of radiation by ozone; radiation reaching the surface may be reduced to one one-thousandth of that incident on the atmosphere during winter. Virtually no radiation of wavelengths less than 1900 A reaches the surface because of absorption by the large column abundance of carbon dioxide. Daily and latitudinal distributions of radiation are presented for wavelengths of 3000, 2500 and 2000 A.
Kuhn, W. R.↗
Dynamical and Chemical Behavior of the Lower Stratosphere and Interactions with the Troposphere
Equivalent-barotropic calculations, in tandem with Lagrangian analyses, reveal how changes of total ozone follow from vertical and horizontal transport by planetary waves. Those calculations also throw light on how diabatic motions comprising the Brewer-Dobson circulation develop from quasi-horizontal advection by planetary waves. Potential temperature along a material surface indicates organized subsidence inside the polar-night vortex, resembling tracer observations from UARS. Lagrangian histories illustrate that this sinking motion follows in large part from parcels being driven out of thermodynamic equilibrium by planetary waves, especially at high latitudes. Irreversible heat transfer then produces a net drift of air across isentropic surfaces as parcels orbit about the displaced vortex. By driving mean-meridional overturning in the stratosphere, this downward drift is ultimately responsible for transferring ozone from the tropics to the extratropical lower stratosphere. It also introduces horizontal structure into the distribution of total ozone, which surfaces clearly in ozone trends. High-resolution global cloud imagery constructed from 6 satellites simultaneously observing the Earth was used to investigate the spectrum of equatorial waves generated by tropical convection and propagating vertically into the stratosphere. The results indicate that temperature variability is dominated by planetary-scale equatorial waves like the Kelvin mode, which agrees with satellite observations of the tropical stratosphere. However, the Kelvin mode accounts for only about 30 - 50% of the eastward momentum flux radiating into the stratosphere, the remainder coming from gravity waves. An algorithm was developed to determine 3-dimensional atmospheric motion from satellite tracer measurements. Based on Lagrangian constraints, the algorithm circumvents limitations of the traditional scheme for inferring motion from temperature measurements and determines the circulation in the tropics as reliably as elsewhere. A study of deep convection revealed that the highest towers (those penetrating into stratospheric air and controlling tropopause height and composition through convective mixing) occur in close association with the diurnal cycle of convection. Clouds colder than 220 K develop almost entirely in association with the diurnal cycle of convection over tropical landmasses and substantially in association with it even over maritime regions.
Salby, Murry L.↗
Contribution of TOMS to Earth Science- An Overview
The TOMS instrument was launched on the Nimbus-7 satellite in Oct 1978 with the goal of understanding the meteorological influences on the ozone column. The nominal lifetime of the instrument was 1 year. However, in response to the concern over possible man-made influences on the ozone layer NASA continued to nurse the instrument for 13.5 years and launched a major program to produce accurate trend quality dataset of ozone. Despite severe optical degradation and other significant anomalies that developed in the instrument over its lifetime, the effort turned out to be a tremendous success. In 1984, TOMS took center stage as the primary provider of Antarctic ozone hole maps to the world community; it continues to play that role until today. An unexpected benefit of the close attention paid to improving the TOMS data quality was that several atmospheric constituents that interfere with ozone measurement were also identified and meticulously converted into long-term datasets of their own. These constituents include clouds, volcanic S02, aerosols, and ocean phytoplankton. In addition, the high quality of the basic datasets made it possible to produce global maps of surface UV and tropospheric ozone. In most cases there are no other sources of these data sets. Advanced UV instruments currently under development in the US and Europe will continue to exploit the TOMS-developed techniques for several decades.
Bhartia, P. K.↗
Arctic Tropospheric Ozone: Assessment of Current Knowledge and Model Performance
As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.
Arctic↗
Sensitivity of surface temperature and atmospheric temperature to perturbations in the stratospheric concentration of ozone and nitrogen dioxide
A radiative-convective model is proposed for estimating the sensitivity of the atmospheric radiative heating rates and atmospheric and surface temperatures to perturbations in the concentration of O3 and NO2 in the stratosphere. Contribution to radiative energy transfer within the atmosphere from H2O, CO2, O3, and NO2 is considered. It is found that the net solar radiation absorbed by the earth-atmosphere system decreases with a reduction in O3; if the reduction of O3 is accompanied by an increase in NO2, there is a compensating effect due to solar absorption by NO2. The surface temperature and atmospheric temperature decrease with decreasing stratospheric O3. Another major conclusion is the strong sensitivity of surface temperature to the vertical distribution of O3 within the atmosphere. The results should be considered as reflecting the sensitivity of the proposed model rather than the sensitivity of the actual earth-atmosphere system.
Ramanathan, V.↗
The photochemistry of synoptic-scale ozone synthesis Implications for the global tropospheric ozone budget
The oxidation of nonmethane hydrocarbons represents a source of tropospheric ozone that is primarily confined to the boundary layers of several highly industrialized regions. (Each region has an area greater than one million km/sq cm). Using a photochemical model, the global tropospheric ozone budget is reexamined by including the in-situ production from these localized regimes. The results from these calculations suggest that the net source due to this photochemistry, which takes place on the synoptic scale, is approximately as large as the amount calculated for global scale photochemical processes which consider only the oxidation of methane and carbon monoxide. Such a finding may have a considerable impact on our understanding of the tropospheric ozone budget. The model results for ozone show reasonable agreement with the climatological summer distribution of ozone and the oxides of nitrogen at the surface and with the vertical distribution of ozone and nonmethane hydrocarbons obtained during a 1980 field program.
Fishman, J.↗
Aerosol-associated changes in tropical stratospheric ozone following the eruption of Mount Pinatubo
The large amount of sulfuric acid aerosol formed in the stratosphere by conversion of sulfur dioxide emitted by the eruption of Mount Pinatubo (15.14 deg N, 120.35 deg E) in the Philippines around June 15, 1991, has had a pronounced effect on lower stratospheric ozone in the tropics. Measurements of stratospheric ozone in the tropics using electrochemical concentration cell (ECC) sondes before and after the eruption and the airborne UV differential absorption lidar (DIAL) system after the eruption are compared with Stratospheric Aerosol and Gas Experiment II (SAGE II) measurements from several years before the eruption and ECC sonde measurements from the year prior to the eruption to determine the resulting changes. Ozone decreases of up to 33 % compared with SAGE II climatological values were found to be directly correlated with altitude regions of enhanced aerosol loading in the 16- to 28-km range. A maximum partial-column decrease of 29 +/- Dobson units (DU) was found over the 16- to 28-km range in September 1991 along with small increases (to 5.9 +/- 2 DU) from 28 to 31.5 km. A large decrease of ozone was also found at 4 deg to 8 deg S from May to August 1992, with a maximum decrease of 33 +/- 7 DU found above Brazzaville in July. Aerosol data form the visible channel of the advanced very high resolution radiometer (AVHRR) and the visible wavelength of the UV DIAL system were used to examine the relationship between aerosol (surface area) densities and ozone changes. The tropical stratospheric ozone changes we observed in 1991 and 1992 are likely be explained by a combination of dynamical (vertical transport) perturbations, radiative perturbations on ozone photochemistry, and heterogeneous chemistry.
Grant, William B.↗
Mars Ozone Absorption Line Shapes from Infrared Heterodyne Spectra Applied to GCM-Predicted Ozone Profiles and to MEX/SPICAM Column Retrievals
We present the application of infrared heterodyne line shapes of ozone on Mars to those produced by radiative transfer modeling of ozone profiles predicted by general circulation models (GCM), and to contemporaneous column abundances measured by Mars Express SPICAM. Ozone is an important tracer of photochemistry Mars' atmosphere, serving as an observable with which to test predictions of photochemistry-coupled GCMs. Infrared heterodyne spectroscopy at 9.5 microns with spectral resolving power >1,000,000 is the only technique that can directly measure fully-resolved line shapes of Martian ozone features from the surface of the Earth. Measurements were made with Goddard Space Flight Center's Heterodyne instrument for Planetary Wind And Composition (HIPWAC) at the NASA Infrared Telescope Facility (IRTF) on Mauna Kea, Hawaii on February 21-24 2008 UT at Ls=35deg on or near the MEX orbital path. The HIPWAC observations were used to test GCM predictions. For example, a GCM-generated ozone profile for 60degN 112degW was scaled so that a radiative transfer calculation of its absorption line shape matched an observed HIPWAC absorption feature at the same areographic position, local time, and season. The RMS deviation of the model from the data was slightly smaller for the GCM-generated profile than for a line shape produced by a constant-with-height profile, even though the total column abundances were the same, showing potential for testing and constraining GCM ozone-profiles. The resulting ozone column abundance from matching the model to the HIPWAC line shape was 60% higher than that observed by SPICAM at the same areographic position one day earlier and 2.5 hours earlier in local time. This could be due to day-to-day, diurnal, or north polar region variability, or to measurement sensitivity to the ozone column and its distribution, and these possibilities will be explored. This work was supported by NASA's Planetary Astronomy Program.
Fast, Kelly E.↗
Quantitative characterization of the Antarctic ozone hole
The long-term evolution of the Antarctic ozone hole is studied based on the TOMS data and the JMA data-set of stratospheric temperature in relation with the possible role of polar stratospheric clouds (PSC's). The effective mass of depleted ozone in the ozone hole at its annual mature stage reached a historical maximum of 55 Mt in 1991, 4.3 times larger than in 1981. The ozone depletion rate during 30 days before the mature ozone hole does not show any appreciable long-term trend but the interannual fluctuations do, ranging from 0.169 to 0.689 Mt/day with the average of 0.419 Mt/day for the period of 1979 - 1991. The depleted ozone mass has the highest correlation with the region below 195 K on the 30 mb surface in June, whereas the ozone depletion rate correlates most strongly with that in August. The present result strongly suggests that the long-term evolution of the mature ozone hole is caused both by the interannual change of the latitudinal coverage of the early PSC's, which may control the latitude and date of initiation of ozone decrease, and by that of the spatial coverage of the mature PSC's which may control the ozone depletion rate in the Antarctic spring.
Ito, T.↗
Climate Data Guide - Modern Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2)
The Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) is a global atmospheric reanalysis produced by the NASA Global Modeling and Assimilation Office (GMAO). It spans the satellite observing era from 1980 to the present. The goals of MERRA-2 are to provide a regularly-gridded, homogeneous record of the global atmosphere, and to incorporate additional aspects of the climate system including trace gas constituents (stratospheric ozone), and improved land surface representation, and cryospheric processes. MERRA-2 is also the first satellite-era global reanalysis to assimilate space-based observations of aerosols and represent their interactions with other physical processes in the climate system. The inclusion of these additional components are consistent with the overall objectives of an Integrated Earth System Analysis (IESA). MERRA-2 is intended to replace the original MERRA product, and reflects recent advances in atmospheric modeling and data assimilation. Modern hyperspectral radiance and microwave observations, along with GPS-Radio Occultation and NASA ozone datasets are now assimilated in MERRA-2. Much of the structure of the data files remains the same in MERRA-2. While the original MERRA data format was HDF-EOS, the MERRA-2 supplied binary data format is now NetCDF4 (with lossy compression to save space).
MERRA-2↗
Climatic consequences of observed ozone loss in the 1980s: Relevance to the greenhouse problem
Recently published findings using satellite and ground-based observations indicate a large winter and summertime decrease in the column abundance of ozone at high and middle latitudes during the last decade. Using a simple ozone depletion profile reflecting the observed decrease in ozone column abundance, Ramaswamy et al. (1992) showed that the negative radiative forcing that results from the ozone decrease between 1979 and 1990 approximately balanced the greenhouse climate forcing due to the chlorofluorocarbons emitted during the same period. Here, we extend the forcing analyses by calculating the equilibrium surface temperature response explicitly, using an updated version of the Atmospheric and Environmental Research two-dimensional radiative-dynamical seasonal model. The calculated steady state responses suggest that the surface cooling due to the ozone depletion in the lower stratosphere offsets about 30% of the surface warming due to greenhouse gases emitted during the same decade. The temperature offset is roughly a factor of 2 larger than the corresponding offset obtained from forcing intercomparisons. This result appears to be related to the climate feedback mechanisms operating in the model troposphere, most notably that associated with atmospheric meridional heat transport. Thus a comprehensive assessment of ozone change effects on the predicted greenhouse warming cannot be accomplished based on forcing evaluations alone. Our results also show that calculations adopting a seasonally and latitudinally dependent ozone depletion profile produce a negative forcing about 50% smaller than that calculated for the depletion profile used by Ramaswamy et al. (1992).
Molnar, G. I.↗
Surface Crystallization of Cloud Droplets: Implications for Climate Change and Ozone Depletion
The process of supercooled liquid water crystallization into ice is still not well understood. Current experimental data on homogeneous freezing rates of ice nucleation in supercooled water droplets show considerable scatter. For example, at -33 C, the reported freezing nucleation rates vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Until now, experimental data on the freezing of supercooled water has been analyzed under the assumption that nucleation of ice took place in the interior volume of a water droplet. Here, the same data is reanalyzed assuming that the nucleation occurred "pseudoheterogeneously" at the air (or oil)-liquid water interface of the droplet. Our analysis suggest that the scatter in the nucleation data can be explained by two main factors. First, the current assumption that nucleation occurs solely inside the volume of a water droplet is incorrect. Second, because the nucleation process most likely occurs on the surface, the rates of nuclei formation could differ vastly when oil or air interfaces are involved. Our results suggest that ice freezing in clouds may initiate on droplet surfaces and such a process can allow for low amounts of liquid water (approx. 0.002 g per cubic meters) to remain supercooled down to -40 C as observed in the atmosphere.
Tabazadeh, A.↗
Contributions to Future Stratospheric Climate Change: An Idealized Chemistry-Climate Model Sensitivity Study
Within the framework of an idealized model sensitivity study, three of the main contributors to future stratospheric climate change are evaluated: increases in greenhouse gas concentrations, ozone recovery, and changing sea surface temperatures (SSTs). These three contributors are explored in combination and separately, to test the interactions between ozone and climate; the linearity of their contributions to stratospheric climate change is also assessed. In a simplified chemistry-climate model, stratospheric global mean temperature is most sensitive to CO2 doubling, followed by ozone depletion, then by increased SSTs. At polar latitudes, the Northern Hemisphere (NH) stratosphere is more sensitive to changes in CO2, SSTs and O3 than is the Southern Hemisphere (SH); the opposing responses to ozone depletion under low or high background CO2 concentrations, as seen with present-day SSTs, are much weaker and are not statistically significant under enhanced SSTs. Consistent with previous studies, the strength of the Brewer-Dobson circulation is found to increase in an idealized future climate; SSTs contribute most to this increase in the upper troposphere/lower stratosphere (UT/LS) region, while CO2 and ozone changes contribute most in the stratosphere and mesosphere.
Hurwitz, M. M.↗
Defense meteorological satellite measurements of total ozone
A multichannel filter radiometer (MFR) on Defense Meteorological Satellites (DMS) that measured total ozone on a global-scale from March 1977 - February 1980 is described. The total ozone data measured by the MFR were compared with total ozone data taken by surfaced-based Dobson spectrophotometers. When comparisons were made for five months, the Dobson spectrophotometer measured 2-5% more total ozone than the MFR. Comparisons between the Dobson spectrophotometer and the MFR showed a reduced RMS difference as the comparisons were made at closer proximity. A Northern Hemisphere total ozone distribution obtained from MFR data is presented.
Lovill, J. E.↗
Radiative-photochemical response of the mesosphere to dynamical forcing
Combination of the chemical continuity equation for odd oxygen with the second law of thermodynamics yields analytic solutions which describe the coupled behavior of temperature and ozone perturbations in response to an externally specified forcing. The results appear in a form which allows easy physical interpretation of the coupling between radiative and photochemical processes. When the forcing is chosen to mimic a planetary scale wave, the theory shows that photochemical acceleration of radiative damping reduces the amplitude of the temperature perturbation by an amount which increases with the wave period. Although ozone fluctuations are anti-correlated with those in temperature, minima in ozone do not coincide exactly in longitude with temperature maxima. The percentage variation in ozone increases upward and is always larger than that in temperature at the same pressure. This demonstrates that variations in ozone on constant pressure surfaces may serve as a sensitive indicator of wave activity in the mesosphere.
Frederick, J. E.↗