Troposphere–Stratosphere Coupling Following Tropospheric Blocking and Extratropical Cyclones
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A new technique denoted cloud slicing has been developed for estimating tropospheric ozone profile information. All previous methods using satellite data were only capable of estimating the total column of ozone in the troposphere. Cloud slicing takes advantage of the opaque property of water vapor clouds to ultraviolet wavelength radiation. Measurements of above-cloud column ozone from the Nimbus 7 total ozone mapping spectrometer (TOMS) instrument are combined together with Nimbus 7 temperature humidity and infrared radiometer (THIR) cloud-top pressure data to derive ozone column amounts in the upper troposphere. In this study tropical TOMS and THIR data for the period 1979-1984 are analyzed. By combining total tropospheric column ozone (denoted TCO) measurements from the convective cloud differential (CCD) method with 100-400 hPa upper tropospheric column ozone amounts from cloud slicing, it is possible to estimate 400-1000 hPa lower tropospheric column ozone and evaluate its spatial and temporal variability. Results for both the upper and lower tropical troposphere show a year-round zonal wavenumber 1 pattern in column ozone with largest amounts in the Atlantic region (up to approx. 15 DU in the 100-400 hPa pressure band and approx. 25-30 DU in the 400-1000 hPa pressure band). Upper tropospheric ozone derived from cloud slicing shows maximum column amounts in the Atlantic region in the June-August and September-November seasons which is similar to the seasonal variability of CCD derived TCO in the region. For the lower troposphere, largest column amounts occur in the September-November season over Brazil in South America and also southern Africa. Localized increases in the tropics in lower tropospheric ozone are found over the northern region of South America around August and off the west coast of equatorial Africa in the March-May season. Time series analysis for several regions in South America and Africa show an anomalous increase in ozone in the lower troposphere around the month of March which is not observed in the upper troposphere. The eastern Pacific indicates weak seasonal variability of upper, lower, and total tropospheric ozone compared to the western Pacific which shows largest TCO amounts in both hemispheres around spring months. Ozone variability in the western Pacific is expected to have greater variability caused by strong convection, pollution and biomass burning, land/sea contrast and monsoon developments.
Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (+/-1 standard deviation) in RFs of +/-17%. Three different radiation schemes were used - we find differences in RFs between schemes (for the same ozone fields) of +/-10 percent. Applying two different tropopause definitions gives differences in RFs of +/-3 percent. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of +/-30 percent for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44+/-12 percent), nitrogen oxides (31 +/- 9 percent), carbon monoxide (15 +/- 3 percent) and non-methane volatile organic compounds (9 +/- 2 percent); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m(−2) DU(−1), a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m(−2); relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.
A new technique denoted cloud slicing has been developed for measuring upper tropospheric ozone. Cloud slicing takes advantage of the opaque property of water vapor clouds to ultraviolet wavelength radiation. Measurements of above-cloud column ozone from the Nimbus 7 total ozone mapping spectrometer (TOMS) instrument are combined together with Nimbus 7 temperature humidity and infrared radiometer (THIR) cloud-top pressure data to derive ozone column amounts in the upper troposphere. In this study tropical TOMS and THIR data for the period 1979-1984 are analyzed. By combining total tropospheric column ozone (denoted TCO) measurements from the convective cloud differential (CCD) method with 100-400 hPa upper tropospheric column ozone amounts from cloud slicing, it is possible to estimate 400-1000 hPa lower tropospheric column ozone and evaluate its spatial and temporal variability. Results for both the upper and lower tropical troposphere show a year-round zonal wave number 1 pattern in column ozone with largest amounts in the Atlantic region (up to 15 DU in the 100-400 hPa pressure band and around 25-30 DU in the 400-1000 hPa pressure band). Upper tropospheric ozone derived from cloud slicing shows maximum column amounts in the Atlantic region in the June-August and September-November seasons which is similar to the seasonal variability of CCD derived TCO in the region. For the lower troposphere, largest column amounts occur in the September-November season over Brazil in South America and also southern Africa. Localized increases in the tropics in lower tropospheric ozone are found over the northern region of South America around August and off the west coast of equatorial Africa in the March-May season. Time series analysis for several regions in South America and Africa show an anomalous increase in ozone in the lower troposphere around the month of March which is not observed in the upper troposphere. The eastern Pacific indicates weak seasonal variability of upper, lower, and total tropospheric ozone compared to the western Pacific which shows largest TCO amounts in both hemispheres around spring months. Ozone variability in the western Pacific is expected to have greater variability caused by strong convection, pollution and biomass burning, land/sea contrast and monsoon developments.
I ] The causes of trends in tropospheric ozone at Northern Hemisphere midlatitudes from 1970 to 1995 are investigated with the GEOS-CHEM model, a global three-dimensional model of the troposphere driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS). This model is used to investigate the sensitivity of tropospheric ozone with respect to (1) changes in the anthropogenic emission of nitrogen oxides and nonmethane hydrocarbons, (2) increases in methane concentrations, (3) variations in the stratospheric source of ozone, (4) changes in solar radiation resulting from stratospheric ozone depletion, and ( 5 ) increases in tropospheric temperatures. Model results indicate that local increases in NO, emissions have caused most of the increases seen in lower tropospheric ozone over Europe and Japan. Increases in methane are responsible for roughly one fifth of the anthropogenically induced increase in tropospheric ozone at northern midlatitudes. However, changes in ozone precursors do not adequately explain either the spatial differences in observed ozone trends across midlatitudes or the observed decreases in ozone over Canada throughout the troposphere. We argue that ozone depletion in the lowermost stratosphere is likely to have reduced the stratospheric source by as much as 30% from the early 1970s to the mid 1990s. Model simulations that account for such a reduction along with reported changes in anthropogenic emissions show steep declines of ozone in the upper troposphere and variable increases in the lower troposphere that are more consistent with observations. Differential temperature trends in summer between North America and Europe may account for at least some of the remaining spatial variation in tropospheric ozone trends. Increases in ultraviolet (UV) radiation due to stratospheric ozone depletion do not appear to significantly reduce tropospheric ozone, except at midlatitudes in the Southern Hemisphere following the breakup of the ozone hole.
We utilize the GISS Global Climate Middle Atmosphere Model and 8 different climate change experiments, many of them focused on stratospheric climate forcings, to assess the relative influence of tropospheric and stratospheric climate change on the extratropical circulation indices (Arctic Oscillation, AO; North Atlantic Oscillation, NAO). The experiments are run in two different ways: with variable sea surface temperatures (SSTs) to allow for a full tropospheric climate response, and with specified SSTs to minimize the tropospheric change. The results show that tropospheric warming (cooling) experiments and stratospheric cooling (warming) experiments produce more positive (negative) AO/NAO indices. For the typical magnitudes of tropospheric and stratospheric climate changes, the tropospheric response dominates; results are strongest when the tropospheric and stratospheric influences are producing similar phase changes. Both regions produce their effect primarily by altering wave propagation and angular momentum transports, but planetary wave energy changes accompanying tropospheric climate change are also important. Stratospheric forcing has a larger impact on the NAO than on the AO, and the angular momentum transport changes associated with it peak in the upper troposphere, affecting all wavenumbers. Tropospheric climate changes influence both the A0 and NAO with effects that extend throughout the troposphere. For both forcings there is often vertical consistency in the sign of the momentum transport changes, obscuring the difference between direct and indirect mechanisms for influencing the surface circulation.
In this study we use ozone and stratospheric ozone tracer simulations from the high-resolution (0.5°x0.5°) Goddard Earth Observing System, Version 5 (GEOS-5) in a replay mode to study the impact of stratospheric ozone on tropospheric ozone interannual variability (IAV). We use these simulations in conjunction with ozone sonde measurements from 1990 to 2016 during the winter and spring seasons. The simulations include a stratospheric ozone tracer (StratO3) to aid 15in the evaluation of the impact of stratospheric ozone IAV on the IAV of tropospheric ozone at different altitudes and location. The model is in good agreement with the observed interannual variation of tropospheric ozone, except for the post-Pinatubo period(1992-1994)over the region of North America. Ozone sonde data show a negative ozone anomaly in 1992-1994 following the Pinatubo eruption, with recovery thereafter. The simulated anomaly is only half the magnitude of that observed. Our analysis suggests that the simulated Stratosphere-troposphere exchange (STE)flux deduced from the analysis 20might be too strong over the North American (50°N-70°N) region after the Mt. Pinatubo eruption in the early 1990s,maskingthe impact of lower stratospheric ozone concentration on tropospheric ozone. European ozone sonde measurements show a similar but weaker ozone depletion after the Mt. Pinatubo eruption, which is fully reproduced by the model. Analysis based on the stratospheric ozone tracer (StratO3) identifies differences in strength and vertical extent of stratospheric ozone impact on the tropospheric ozone interannual variation (IAV)between North America and Europe. Over NorthAmerica25stations, the StratO3IAV has a significant impact on tropospheric ozone from the upper to lower troposphere and explains about 60% and 66% of the simulated ozone IAV at 400 hPa, and ~11% and 34% at 700 hPa in winter and spring respectively. Over European stations, the influence is limited to the middle to upper troposphere, and becomes much smaller at 700 hPa. The Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2)assimilated fields exhibit strong longitudinal variations over northern hemisphere (NH) mid-high latitudes, with lower tropopause height and 30lower geopotential height over North America than Europe. These variations associated with the relevant variations in the location of tropospheric jet flows are responsible for the longitudinal differences in the stratospheric ozone impact, with stronger effects over North America than over Europe
A key component of climate/chemistry modeling is how to handle the influx into (and egress from) the troposphere. This is especially important when considering tropospheric ozone, and its precursors (e.g., NO(x) from aircraft). A study has been conducted with various GISS models to determine the minimum requirements necessary for producing realistic troposphere-stratosphere exchange. Four on-line tracers are employed: CFC-11 and SF6 for mixing from the troposphere into the stratosphere, Rn222 for vertical mixing within the troposphere, and 14C for mixing from the stratosphere into the troposphere. Four standard models are tested, with varying vertical resolution, gravity wave drag and location of the model top, and additional subsidiary models are employed to examine specific features. The results show that proper vertical transport between the troposphere and stratosphere in the GISS models requires lifting the top of the model considerably out of the stratosphere, and including gravity wave drag in the lower stratosphere. Increased vertical resolution without these aspects does not improve troposphere-stratosphere exchange. The transport appears to be driven largely by the residual circulation within the stratosphere; associated E-P flux convergences require both realistic upward propagating energy from the troposphere, and realistic pass-through possibilities. A 23 layer version with a top at the mesopause and incorporating gravity wave drag appears to have reasonable stratospheric-tropospheric exchange, in terms of both the resulting tracer distributions and atmospheric mass fluxes.
Current methods for estimating the concentrations of inorganic chlorine/bromine species Cl(y)/Br(y) in the stratosphere due to decomposition of tropospheric source gases assume that the Cl(y)/Br(y) concentration in the stratosphere is determined mainly by the balance between production from in situ oxidation of the source gases in the stratosphere and removal by transport of Cl(y)/Br(y) out of the stratosphere. The rationale being that for source gases whose lifetimes are of the order of several months or longer the concentration of Cl(y)/Br(y) in the troposphere is small because they are produced at a relatively slow rate and also removed efficiently by washout processes. As a result of the small concentration, the rate at which Cl(y)/Br(y) is transported to the stratosphere is expected to be small compared to the in situ stratospheric production. Thus the transport of Cl(y)/Br(y) from the troposphere contributes little to the stratospheric concentration. In contrast, the origin of stratospheric Cl(y)/Br(y) from reactive source gases with tropospheric lifetimes comparable to the washout lifetime of Cl(y)/Br(y) (of the order of 10-30 days) in the troposphere is distinctly different. The in situ source in the stratosphere is expected to be significantly smaller because only a small portion of the source gas is expected to survive the troposphere to be transported into this region. At the same time these short-lived source gases produce appreciable amounts of Cl(y)/Br(y) in the troposphere such that transport to the stratosphere offers a larger source for stratospheric Cl(y)/Br(y) than in situ production. Thus, for reactive source species, simple methods of estimating the concentration of stratospheric Cl(y)/Br(y) that ignore the tropospheric contribution will seriously underestimate the loading. Therefore estimation of the stratospheric Cl(y)/Br(y) loading requires not only measurements of tropospheric source gases but also measurements of Cl(y)/Br(y) at the tropopause. This paper illustrates the mechanism by using results from a two-dimensional chemistry-transport model. However, in view of the importance of tropospheric transport on stratospheric loading the detailed values should be further evaluated using a three-dimensional model with appropriate treatment of convective transport.
The goals of the paper are to: (1) present tropospheric ozone (O3) climatologies in summer 2008 based on a large amount of measurements, during the International Polar Year when the Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport (POLARCAT) campaigns were conducted (2) investigate the processes that determine O3 concentrations in two different regions (Canada and Greenland) that were thoroughly studied using measurements from 3 aircraft and 7 ozonesonde stations. This paper provides an integrated analysis of these observations and the discussion of the latitudinal and vertical variability of tropospheric ozone north of 55oN during this period is performed using a regional model (WFR-Chem). Ozone, CO and potential vorticity (PV) distributions are extracted from the simulation at the measurement locations. The model is able to reproduce the O3 latitudinal and vertical variability but a negative O3 bias of 6-15 ppbv is found in the free troposphere over 4 km, especially over Canada. Ozone average concentrations are of the order of 65 ppbv at altitudes above 4 km both over Canada and Greenland, while they are less than 50 ppbv in the lower troposphere. The relative influence of stratosphere-troposphere exchange (STE) and of ozone production related to the local biomass burning (BB) emissions is discussed using differences between average values of O3, CO and PV for Southern and Northern Canada or Greenland and two vertical ranges in the troposphere: 0-4 km and 4-8 km. For Canada, the model CO distribution and the weak correlation ( 30) of O3 and PV suggests that stratosphere-troposphere exchange (STE) is not the major contribution to average tropospheric ozone at latitudes less than 70oN, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely over Greenland, significant STE is found according to the better O3 versus PV correlation ( 40) and the higher 75th PV percentile. A weak negative latitudinal summer ozone gradient -6 to -8 ppbv is found over Canada in the mid troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production due to the BB emissions at latitudes less than 65oN, while STE contribution is more homogeneous in the latitude range 55oN to 70oN. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long range transport from multiple mid-latitude sources (North America, Europe and even Asia for latitudes higher than 77oN).
Potential sources of a priori ozone (O3) profiles for use in Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite tropospheric O3 retrievals are evaluated with observations from multiple Tropospheric Ozone Lidar Network (TOLNet) systems in North America. An O3 profile climatology (tropopause-based O3 climatology (TB-Clim), currently proposed for use in the TEMPO O3 retrieval algorithm) derived from ozonesonde observations and O3 profiles from three separate models (operational Goddard Earth Observing System (GEOS-5) Forward Processing (FP) product, reanalysis product from Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA2), and the GEOS-Chem chemical transport model (CTM)) were: 1) evaluated with TOLNet measurements on various temporal scales (seasonally, daily, hourly) and 2) implemented as a priori information in theoretical TEMPO tropospheric O3 retrievals in order to determine how each a priori impacts the accuracy of retrieved tropospheric (0-10 km) and lowermost tropospheric (LMT, 0-2 km) O3 columns. We found that all sources of a priori O3 profiles evaluated in this study generally reproduced the vertical structure of summer-averaged observations. However, larger differences between the a priori profiles and lidar observations were observed when evaluating inter-daily and diurnal variability of tropospheric O3. The TB-Clim O3 profile climatology was unable to replicate observed inter-daily and diurnal variability of O3 while model products, in particular GEOS-Chem simulations, displayed more skill in reproducing these features. Due to the ability of models, primarily the CTM used in this study, on average to capture the inter-daily and diurnal variability of tropospheric and LMT O3 columns, using a priori profiles from CTM simulations resulted in TEMPO retrievals with the best statistical comparison with lidar observations. Furthermore, important from an air quality perspective, when high LMT O3 values were observed, using CTM a priori profiles resulted in TEMPO LMT O3 retrievals with the least bias. The application of time-specific (non-climatological) hourly/daily model predictions as the a priori profile in TEMPO O3 retrievals will be best suited when applying this data to study air quality or event-based processes as the standard retrieval algorithm will still need to use a climatology product. Follow-on studies to this work are currently being conducted to investigate the application of different CTM-predicted O3 climatology products in the standard TEMPO retrieval algorithm. Finally, similar methods to those used in this study can be easily applied by TEMPO data users to recalculate tropospheric O3 profiles provided from the standard retrieval using a different source of a priori.
The ozone mixing ratio spatiotemporal variability in the pristine South Pacific Ocean is studied, for the first time, using 21-year-long ozone (O3) records from the entire southern tropical and subtropical Pacific between 1994 and 2014. The analysis considered regional O3 vertical observations from ozonesondes, surface carbon monoxide (CO) observations from flasks, and three-dimensional chemistry-transport model simulations of the global troposphere. Two 21-year-long numerical simulations, with and without biomass burning emissions, were performed to disentangle the importance of biomass burning relative to stratospheric intrusions for ambient ozone levels in the region. Tagged tracers of O3 from the stratosphere and CO from various biomass burning regions have been used to track the impact of these different regions on the southern tropical Pacific O3 and CO levels. Patterns have been analyzed based on atmospheric dynamics variability. Considering the interannual variability in the observations, the model can capture the observed ozone gradients in the troposphere with a positive bias of 7.5 % in the upper troposphere/lower stratosphere (UTLS) as well as near the surface. Remarkably, even the most pristine region of the global ocean is affected by distant biomass burning emissions by convective outflow through the mid and high troposphere and subsequent subsidence over the pristine oceanic region. Therefore, the biomass burning contribution to tropospheric CO levels maximizes in the UTLS. The Southeast Asian open fires have been identified as the major contributing source to CO from biomass burning in the tropical South Pacific, contributing on average for the study period about 8.5 and 13 ppbv of CO at Rapa Nui and Samoa, respectively, at an altitude of around 12 km during the burning season in the spring of the Southern Hemisphere. South America is the second-most important biomass burning source region that influences the study area. Its impact maximizes in the lower troposphere (6.5 ppbv for Rapa Nui and 3.8 ppbv for Samoa). All biomass burning sources contribute about 15–23 ppbv of CO at Rapa Nui and Samoa and account for about 25 % of the total CO in the entire troposphere of the tropical and subtropical South Pacific. This impact is also seen on tropospheric O3, to which biomass burning O3 precursor emissions contribute only a few ppbv during the burning period, while the stratosphere–troposphere exchange is the most important source of O3 for the mid troposphere of the South Pacific Ocean, contributing about 15–20 ppbv in the subtropics.
Tropospheric ozone is a key chemically active trace gas and radiative forcer. Understanding its long-term changes is important to properly interpret observed changes in total column ozone and stratospheric ozone recovery. We investigate global and regional tropospheric ozone changes and their impact on total column ozone during 2005-2018 using satellite measurements and the NASA Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). Global total ozone increased ~4 DU during 2005-2018 (+0.28±0.06 DU yr(exp -1)) as inferred from Ozone Monitoring Instrument (OMI). Consistent with previous studies, the OMI/MLS (Microwave Limb Sounder) derived global tropospheric ozone increased 2.2 DU during this period, 60% of the global total column ozone increase. While GEOSCCM reproduces reasonably well the total column increase, it overestimates the stratospheric ozone increase and underestimates the tropospheric ozone increase. We find that the tropospheric ozone increases are likely attributed to a growth of regional emissions of key ozone precursors, especially volatile organic compounds (VOCs) as reflected by the positive trends in formaldehyde (CH2O). Although carbon monoxide (CO) has been decreasing everywhere around the globe, it has relatively small impact on the tropospheric ozone trend. Trends in nitrogen dioxide (NO2) vary with regions, and these changes counteract or reinforce the positive effects of CH2O on the tropospheric ozone increases. The model underestimates the observed tropospheric ozone increase, especially over the US and Europe, because of underestimated NO2 emissions changes used in the model. The stratospheric ozone contribution increases during this period in the Northern Hemisphere and contributes to the tropospheric ozone increase.
New products from the TOMS (Total Ozone Mapping Spectrometer) >satellite instrument can resolve pollution events in tropical and mid-latitudes, Over the past several years, we have developed tropospheric ozone data sets by two methods. The modified-residual technique [Hudson and Thompson, 1998; Thompson and Hudson, 1999] uses v. 7 TOMS total ozone and is applicable to tropical regimes in which the wave-one pattern in total ozone is observed. The TOMSdirect method [Hudson et at., 2000] represents a new algorithm that uses TOMS radiances to extract tropospheric ozone in regions of constant stratospheric ozone and tropospheric ozone displaying high mixing ratios and variability characteristic of pollution, Absorbing aerosols (dust and smoke; Herman et at., 1997 Hsu et al., 1999), a standard TOMS product, provide transport and/or source marker information to interpret tropospheric ozone. For the Nimbus 7/TOMS observing period (1979-1992), modified-residual TTO (tropical tropospheric ozone) appears as two maps/month at I-degree latitude 2-degree longitude resolution at a homepage and digital data are available (20S to 20N) by ftp at http://metosrv2. umd.edu/~tropo/ 14y_data.d. Preliminary modified-residual TTO data from the operational Earth-Probe/TOMS (1996- present) are posted in near-real-time at the same website. Analyses with the new tropospheric ozone and aerosol data are illustrated by the following (I)Signals in tropical tropospheric ozone column and smoke amount during ENSO (El Nino-Southern Oscillation) events, e.g. 1982-1983 and the intense ENSO induced biomass fires of 1997-1998 over the Indonesian region [Thompson et a[, 2000a, Thompson and Hudson, 1999]. (2) Trends in tropospheric ozone and smoke aerosols in various tropical regions (Atlantic, Pacific, Africa, Brazil). No significant trends were found for ozone from1980-1990 [Thompson and Hudson, 19991 although smoke aerosols increased during the period [Hsu et al.,1999]. (3) Temporal and spatial offsets ("paradoxes") in tropical tropospheric ozone and smoke aerosol in regions of greatest tropical biomass burning [Thompson et at., 1996;2000b]. (4) Trans-boundary pollution tracking. With an air parcel (trajectory) model, smoke aerosol and ozone and dust plumes can be tracked across oceans (e.g., Asia to North America; North America to Europe) and national boundaries, e.g. Indonesia to Singapore and Malaysia during the 1997 ENSO fires.
The variability of the horizontal circulation in the stratosphere and troposphere of the Northern Hemisphere (NH) is compared by using various approaches. Spatial degrees of freedom (dof) on different time scales were derived. Modes of variability were computed in geopotential height fields at the tropospheric and stratospheric pressure levels by applying multivariate statistical approaches. Features of the spatial and temporal variability of the winterly zonal wind were studied with the help of recurrence and persistence analyses. The geopotential height and zonally-averaged zonal wind at the 50-, 500- and 1000-hPa level are used to investigate the behavior of the horizontal circulation in the lower stratosphere, mid-troposphere and at the near surface level, respectively. It is illustrated that the features of the variability of the horizontal circulation are very similar in the mid-troposphere and at the near surface level. Due to the filtering of tropospheric disturbances by the stratospheric and upper tropospheric zonal mean flow, the variability of the stratospheric circulation exhibits less spatial complexity than the circulation at tropospheric pressure levels. There exist enormous differences in the number of degrees of freedom (or free variability modes) between both atmospheric layers. Results of the analyses clearly show that the concept of a zonally symmetric AO with a simple structure in the troposphere similar to the one in the stratosphere is not valid. It is concluded that the spatially filtered climate change signal can be detected earlier in the stratosphere than in the mid-troposphere or at the near surface level.
This study evaluates the spatial distributions and seasonal cycles in upper tropospheric ozone (pressure range 200-500 hPa) from low to high latitudes (60S to 60N) derived from the satellite retrieval method called "Cloud Slicing." Cloud Slicing is a unique technique for determining ozone profile information in the troposphere by combining co-located measurements of cloud-top, pressure and above-cloud column ozone. For upper tropospheric ozone, co-located measurements of Nimbus 7 Total Ozone Mapping Spectrometer (TOMS) above-cloud column ozone, and Nimbus 7 Temperature Humidity Infrared Radiometer (THIR) cloud-top pressure during 1979-1984 were incorporated. In the tropics, upper tropospheric ozone shows year-round enhancement in the Atlantic region and evidence of a possible semiannual variability. Upper tropospheric ozone outside the tropics shows greatest abundance in winter and spring seasons in both hemispheres with largest seasonal and largest amounts in the NH. These characteristics are similar to lower stratospheric ozone. Comparisons of upper tropospheric column ozone with both stratospheric ozone and a proxy of lower stratospheric air mass (i.e., tropopause pressure) from National Centers for Environmental Prediction (NCEP) suggest that stratosphere-troposphere exchange (STE) may be a significant source for the seasonal variability of upper tropospheric ozone almost everywhere between 60S and 60N except in low latitudes around 10S to 25N where other sources (e.g., tropospheric transport, biomass burning, aerosol effects, lightning, etc.) may have a greater role.
Tropospheric ozone is important to the environment, because it acts as a strong oxidant to control the concentrations of many reduced gases (methane, carbon monoxide, ... ), its radiative forcing plays a significant role in the greenhouse effect, and direct contact with ozone is harmful to human health. Tropospheric ozone, whose main sources are intrusion from the stratosphere and chemical production from source gases associated with urban pollution or biomass burning, varies on a wide range of spatial and temporal scales. Its transport and chemistry can be influenced by weather, seasonal, or multiannual variability. Despite the importance of tropospheric ozone, it contributes only about 10% of the total ozone loading in the atmosphere. Consequently, satellite instruments lose sensitivity below the stratospheric ozone peak, and provide little information about middle and lower tropospheric ozone. This talk will discuss recent modifications made to the satellite ozone data assimilation system at NASA's Data Assimilation Office (DAO) in order to provide better tropospheric ozone columns and profiles. We use a version of the system that assimilates only the data from the Solar Backscatter UltraViolet/2 (SBUV/2) instrument. The quality of the assimilated ozone in the tropical troposphere is evaluated by comparison with independent observations obtained from the Southern Hemispheric Additional Ozonesondes (SHADOZ) network. It is shown that the quality of ozone fields is sensitive to the winds used in the transport model. Increasing the vertical resolution of the model also has a beneficial impact. The assimilated ozone in the lower troposphere was substantially improved by inclusion of tropospheric ozone production, loss, and dry deposition rates from the Harvard GEOS-CHEM model. The mechanisms behind these results will be examined and the implications for our understanding of tropospheric ozone will be discussed.
We present the first directly retrieved global distribution of tropospheric column ozone from Global Ozone Monitoring Experiment (GOME) ultraviolet measurements during December 1996 to November 1997. The retrievals clearly show signals due to convection, biomass burning, stratospheric influence, pollution, and transport. They are capable of capturing the spatiotemporal evolution of tropospheric column ozone in response to regional or short time-scale events such as the 1997-1998 El Nino event and a 10-20 DU change within a few days. The global distribution of tropospheric column ozone displays the well-known wave-1 pattern in the tropics, nearly zonal bands of enhanced tropospheric column ozone of 36-48 DU at 20degS-30degS during the austral spring and at 25degN-45degN during the boreal spring and summer, low tropospheric column ozone of <30 DU uniformly distributed south of 35 S during all seasons, and relatively high tropospheric column ozone of >33 DU at some northern high-latitudes during the spring. Simulation from a chemical transport model corroborates most of the above structures, with small biases of <+/-5 DU and consistent seasonal cycles in most regions, especially in the southern hemisphere. However, significant positive biases of 5-20 DU occur in some northern tropical and subtropical regions such as the Middle East during summer. Comparison of GOME with monthly-averaged Measurement of Ozone and Water Vapor by Airbus in-service Aircraft (MOZAIC) tropospheric column ozone for these regions usually shows good consistency within 1 a standard deviations and retrieval uncertainties. Some biases can be accounted for by inadequate sensitivity to lower tropospheric ozone, the different spatiotemporal sampling and the spatiotemporal variations in tropospheric column ozone.