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TOMS Tropical Tropospheric Ozone Data Sets at the University of Maryland Website

Since 1997, shortly after the launch of the Earth-Probe TOMS (Total Ozone Mapping Spectrometer) satellite instrument, we have been processing data in near-real time to post maps of tropical tropospheric ozone at a website: metosrv2.umd.edu/-tropo. Daily, 3-day and 9-day averages of tropical tropospheric ozone column depth (TTO) are viewable from 10N to 10S. Data can be downloaded (running 9-day means) from 20N-30S. Pollution events are trackable along with dynamically-induced variations in tropospheric ozone column. TOMS smoke aerosol (toms.gsfc.nasa.gov) can be used to interpret biomass burning ozone, as for example, during the extreme ozone and smoke pollution period during the ENSO-related fires of August November 1997. During that time plumes of ozone and smoke were frequently decoupled and ozone from Indonesian fires and from Africa merged in one large feature by late October 1997. In addition to the Earth-Probe TOMS record, data as half-month averages and as daily 9-day means from the Nimbus 7 TOMS instrument are at the metosrv2.umd.edu/-tropo website. A guide to the website and examples of ozone time-series and maps will be shown.

Kochhar, A. K.↗

Plant biochemistry influences tropospheric ozone formation, destruction, deposition, and response

Tropospheric ozone (O 3 ) is among the most damaging air pollutant to plants. Plants alter the atmospheric O 3 concentration in two distinct ways: (i) by the emission of volatile organic compounds (VOCs) that are precursors of O 3 ; and (ii) by dry deposition, which includes diffusion of O 3 into vegetation through stomata and destruction by nonstomatal pathways. Isoprene, monoterpenes, and higher terpenoids are emitted by plants in quantities that alter tropospheric O 3 . Deposition of O 3 into vegetation is related to stomatal conductance, leaf structural traits, and the detoxification capacity of the apoplast. The biochemical fate of O 3 once it enters leaves and reacts with aqueous surfaces is largely unknown, but new techniques for the tracking and identification of initial products have the potential to open the black box.

59 BASIC BIOLOGICAL SCIENCES↗

Impact of Surface Emissions to the Zonal Variability of Tropical Tropospheric Ozone and Carbon Monoxide for November 2004

The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so called zonal 'wave-one' pattern, which is characterized by peak ozone concentrations (70-80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60-70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30-40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.

tropical tropospheric ozone↗

Tropical Tropospheric Ozone: A Multi-Satellite View From TOMS and Other Instruments

New tropospheric ozone and aerosol products from the TOMS (Total Ozone Mapping Spectrometer) satellite instrument can resolve episodic pollution events in the tropics and interannual and seasonal variability. Modified-residual (MR) Nimbus 7 tropical tropospheric ozone (TTO), two maps/month (1979-1992, 1-deg latitude by 2-deg longitude) within the region in which total ozone displays a tropical wave-one pattern (maximum 20S to 20N), are available in digital form at http://metosrv2.umd.edu/~tropo. Also available are preliminary 1996-1999 MR-TTO maps based on real-time Earth-Probe (EP)/TOMS observations. Examples of applications are given.

Thompson, Anne M.↗

Sensitivity of Assimilated Tropical Tropospheric Ozone to the Meteorological Analyses

Tropical tropospheric ozone fields from two different experiments performed with an off-line ozone assimilation system developed in NASA's Data Assimilation Office (DAO) are examined. Assimilated ozone fields from the two experiments are compared with the collocated ozone profiles from the Southern Hemispheric Additional Ozonesondes (SHADOZ) network. Results are presented for 1998. The ozone assimilation system includes a chemistry-transport model, which uses analyzed winds from the Goddard Earth Observing System (GEOS) Data Assimilation System (DAS). The two experiments use wind fields from different versions of GEOS DAS: an operational version of the GEOS-2 system and a prototype of the GEOS-4 system. While both versions of the DAS utilize the Physical-space Statistical Analysis System and use comparable observations, they use entirely different general circulation models and data insertion techniques. The shape of the annual-mean vertical profile of the assimilated ozone fields is sensitive to the meteorological analyses, with the GEOS-4-based ozone being closest to the observations. This indicates that the resolved transport in GEOS-4 is more realistic than in GEOS-2. Remaining uncertainties include quantification of the representation of sub-grid-scale processes in the transport calculations, which plays an important role in the locations and seasons where convection dominates the transport.

Hayashi, Hiroo↗

Direct measurements of tropospheric ozone using TOMS data

Fishman and Larsen have proposed a new algorithm, called 'tropospheric residual method,' which retrieves the climatological tropospheric ozone by using SAGE (Stratospheric Aerosol and Gas Experiment) and TOMS (Total Ozone Mapping Spectrometer) data. In this paper, we will examine the feasibility of detection for tropospheric ozone using only TOMS data. From a case study over the Atlantic Ocean off the coast of west Africa, it has been found that total ozone in the archived TOMS data has been overestimated over a region of marine-stratocumulus clouds.

Hudson, Robert D.↗

Ozone, Tropospheric

In the early part of the 20th century, ground-based and balloon-borne measurements discovered that most of atmosphere's ozone is located in the stratosphere with highest concentrations located between 15 and 30 km (9,3 and 18.6 miles). For a long time, it was believed that tropospheric ozone originated from the stratosphere and that most of it was destroyed by contact with the earth's surface. Ozone, O3, was known to be produced by the photo-dissociation of molecular oxygen, O2, a process that can only occur at wavelengths shorter than 242 nm. Because such short-wave-length radiation is present only in the stratosphere, no tropospheric ozone production is possible by this mechanism. In the 1940s, however, it became obvious that production of ozone was also taking place in the troposphere. The overall reaction mechanism was eventually identified by Arie Haagen-Smit of the California Institute of Technology, in highly polluted southern California. The copious emissions from the numerous cars driven there as a result of the mass migration to Los Angeles after World War 2 created the new unpleasant phenomenon of photochemical smog, the primary component of which is ozone. These high levels of ozone were injuring vegetable crops, causing women's nylons to run, and generating increasing respiratory and eye-irritation problems for the populace. Our knowledge of tropospheric ozone increased dramatically in the early 1950s as monitoring stations and search centers were established throughout southern California to see what could be done to combat this threat to human health and the environment.

Fishman, Jack↗

The meteorological environment of the tropospheric ozone maximum over the tropical South Atlantic Ocean

Atmospheric flow patterns are examined over the South Atlantic Ocean where a maximum of tropospheric ozone has been observed just west of southern Africa. We investigate the flow climatology during October and perform a case study for six days during October 1989. Horizontal and vertical motions are examined and used to prepare 3D backward trajectories from the region of greatest ozone. An initially zonally symmetric distribution of ozone is treated as a passive tracer and advected by 3D flows forecast by the global model. Results from the passive tracer simulation indicate that 3D advection alone can produce a maximum of tropospheric ozone in the observed location. In addition, the trajectories suggest that by-products of biomass burning could be transported to the area of maximum ozone. Low-level flow from commonly observed regions of burning in Africa streams westward to the area of interest. Over Brazil, if the burning by-products are carried into the upper troposphere by convective process, they then could be transported eastward to the ozone feature in approximately five days. There is considerable subsidence over the tropical southern Atlantic, such that stratospheric influences also are a factor in producing the ozone maximum. Both planetary-scale and transient synoptic-scale circulation features play major roles in the various transport processes that influence the region. In summary, the observed tropospheric ozone maximum appears to be caused by a complex set of horizontal and vertical advections, transport from regions of biomass burning, and stratospheric influences.

Krishnamurti, T. N.↗

Climate Impacts on Tropospheric Ozone and Hydroxyl

Climate change may influence tropospheric ozone and OH via several main pathways: (1) altering chemistry via temperature and humidity changes, (2) changing ozone and precursor sources via surface emissions, stratosphere-troposphere exchange, and light- ning, and (3) affecting trace gas sinks via the hydrological cycle and dry deposition. We report results from a set of coupled chemistry-climate model simulations designed to systematically study these effects. We compare the various effects with one another and with past and projected future changes in anthropogenic and natural emissions of ozone precursors. We find that white the overall impact of climate on ozone is probably small compared to emission changes, some significant seasonal and regional effects are apparent. The global effect on hydroxyl is quite large, however, similar in size to the effect of emission changes. Additionally, we show that many of the chemistry-climate links that are not yet adequately modeled are potentially important.

Shindell, Drew T.↗

Elevated Tropospheric Ozone over the Atlantic

Tropospheric column ozone (TCO) is derived from differential measurements of TOMS total column ozone and Microwave Limb Sounder stratospheric column ozone. It is shown that TCO during summer months over the Atlantic and Pacific Oceans in northern midlatitudes is about the same (50 to 60 Dobson Units) as over the continents of North America, Europe, and Asia, where surface emissions of nitrogen oxides from industrial sources, biomass and biofuel burning and biogenic emissions are significantly larger. This nearly uniform zonal variation in TCO is modulated by surface topography of the Rocky and Himalayan mountains, and Tibetan plateau where TCO is reduced by 20 to 30 Dobson Units. The zonal variation in TCO is well simulated by a global chemical transport model called MOZART-2 (Model of Ozone and Related Chemical Tracers, version 2). The model results are analyzed to delineate the relative importance of various processes contributing to observed zonal characteristics of TCO.

Chandra, S.↗

Accurate Satellite-Derived Estimates of Tropospheric Ozone Radiative Forcing

Estimates of the radiative forcing due to anthropogenically-produced tropospheric O3 are derived primarily from models. Here, we use tropospheric ozone and cloud data from several instruments in the A-train constellation of satellites as well as information from the GEOS-5 Data Assimilation System to accurately estimate the instantaneous radiative forcing from tropospheric O3 for January and July 2005. We improve upon previous estimates of tropospheric ozone mixing ratios from a residual approach using the NASA Earth Observing System (EOS) Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) by incorporating cloud pressure information from OMI. Since we cannot distinguish between natural and anthropogenic sources with the satellite data, our estimates reflect the total forcing due to tropospheric O3. We focus specifically on the magnitude and spatial structure of the cloud effect on both the shortand long-wave radiative forcing. The estimates presented here can be used to validate present day O3 radiative forcing produced by models.

Joiner, Joanna↗

Tropospheric Ozone Over a Tropical Atlantic Station in the Northern Hemisphere: Paramaribo, Surinam (6 deg N, 55 deg W)

We present an analysis of 2.5 years of weekly ozone soundings conducted at a new monitoring station in Paramaribo, Surinam (6 deg N,55 deg W). This is currently one of only three ozone sounding stations in the northern hemisphere (NH) tropics, and the only one in the equatorial Atlantic region. Paramaribo is part of the Southern Hemisphere ADditional Ozone Sounding program (SHADOZ). Due to its position close to the equator, the Inter Tropical Convergence Zone (ITCZ) passes over Paramaribo twice per year, which results in a semi-annual seasonality of many parameters including relative humidity and ozone. The dataset from Paramaribo is used to: (1) evaluate ozone variability relative to precipitation, atmospheric circulation patterns and biomass burning; (2) contrast ozone at the NH equatorial Atlantic with that at nearby southern hemisphere (SH) stations Natal (6 deg S,35 deg W) and Ascension (8 deg S,14 deg W); (3) compare the seasonality of tropospheric ozone with a satellite-derived ozone product: Tropical Tropospheric Ozone Columns from the Modified Residual method (MR-TTOC). We find that Paramaribo is a distinctly Atlantic station. Despite its position north of the equator, it resembles nearby SH stations during most of the year. Transport patterns in the lower and middle troposphere during February and March differ from SH stations, which leads to a seasonality of ozone with two maxima. MR-TTOC over Paramaribo does not match the observed seasonality of ozone due to the use of a SH ozone sonde climatology in the MR method. The Paramaribo ozone record is used to suggest an improvement for northern hemisphere MR-TTOC retrievals. We conclude that station Paramaribo shows unique features in the region, and clearly adds new information to the existing SHADOZ record.

Peters, W.↗

Analysis of the Latitudinal Variability of Tropospheric Ozone in the Arctic Using the Large Number of Aircraft and Ozonesonde Observations in Early Summer 2008

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).

climatologies↗

How Can TOLNet Help to Better Understand Tropospheric Ozone? A Satellite Perspective

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.

Satellite↗

Radiative Forcing Due to Enhancements in Tropospheric Ozone and Carbonaceous Aerosols Caused by Asian Fires During Spring 2008

Simulations of tropospheric ozone and carbonaceous aerosol distributions, conducted with the Real-time Air Quality Modeling System (RAQMS), are used to study the effects of major outbreaks of fires that occurred in three regions of Asia, namely Thailand, Kazakhstan, and Siberia, during spring 2008. RAQMS is a global scale meteorological and chemical modeling system. Results from these simulations, averaged over April 2008, indicate that tropospheric ozone column increases by more than 10 Dobson units (DU) near the Thailand region, and by lesser amounts in the other regions due to the fires. Widespread increases in the optical depths of organic and black carbon aerosols are also noted. We have used an off-line radiative transfer model to evaluate the direct radiative forcing due to the fire-induced changes in atmospheric composition. For clear sky, the monthly averaged radiative forcing at the top of the atmosphere (TOA) is mostly negative with peak values less than -12 W/sq m occurring near the fire regions. The negative forcing represents the increased outgoing shortwave radiation caused by scattering due to carbonaceous aerosols. At high latitudes, the radiative forcing is positive due to the presence of absorbing aerosols over regions of high surface albedo. Regions of positive forcing at TOA are more pronounced under total sky conditions. The monthly averaged radiative forcing at the surface is mostly negative, and peak values of less than -30 W/sq m occur near the fire regions. Persistently large negative forcing at the surface could alter the surface energy budget and potentially weaken the hydrological cycle.

Natarajan, Murali↗

Radiative forcing perturbation due to observed increases in tropospheric ozone at Hohenpeissenberg

The effect on surface temperature due to changes in atmospheric O3 depends highly on the latitude where the change occurs. Previous sensitivity calculations indicate that ozone changes in the upper troposphere and lower stratosphere are more effective in causing surface temperature change (Wang et al., 1980). Long term ground-based observations show that tropospheric ozone, especially at the tropopause region, has been increasing at middle and high latitudes in the Northern Hemisphere (NATO, 1988; Quadrennial Ozone Symposium, 1992). These increases will enhance the greenhouse effect and increase the radiative forcing to the troposphere-surface system, which is opposite to the negative radiative forcing calculated from the observed stratospheric ozone depletion recently reported in WMO (1992). We used more than two thousands regularly measured ozonesondes providing reliable vertical O3 distribution at Hohenpeissenberg (47N; 11E) for the 1967-1990 to study the instantaneous solar and longwave radiative forcing the two decades 1971-1990 and compare the forcing with those caused by increasing CO2, CH4, N2O, and CFCs. Calculations are also made to compare the O3 radiative forcing between stratospheric depletion and tropospheric increase. Results indicate that the O3 changes will induce a positive radiative forcing dominated by tropospheric O3 increase and the magnitude of the forcing is comparable to that due to CO2 increases during the two decades. The significant implications of the tropospheric O3 increase to the global climate are discussed.

Wang, Wei-Chyung↗

Chemistry-Transport Modeling of the Satellite Observed Distribution of Tropical Tropospheric Ozone

We have compared the 14-year record of satellite derived tropical tropospheric ozone columns (TTOC) from the NIMBUS-7 Total Ozone Mapping Spectrometer (TOMS) to TTOC calculated by a chemistry-transport model (CTM). An objective measure of error, based on the zonal distribution of TTOC in the tropics, is applied to perform this comparison systematically. In addition, the sensitivity of the model to several key processes in the tropics is quantified to select directions for future improvements. The comparisons indicate a widespread, systematic (20%) discrepancy over the tropical Atlantic Ocean, which maximizes during austral Spring. Although independent evidence from ozonesondes shows that some of the disagreement is due to satellite over-estimate of TTOC, the Atlantic mismatch is largely due to a misrepresentation of seasonally recurring processes in the model. Only minor differences between the model and observations over the Pacific occur, mostly due to interannual variability not captured by the model. Although chemical processes determine the TTOC extent, dynamical processes dominate the TTOC distribution, as the use of actual meteorology pertaining to the year of observations always leads to a better agreement with TTOC observations than using a random year or a climatology. The modeled TTOC is remarkably insensitive to many model parameters due to efficient feedbacks in the ozone budget. Nevertheless, the simulations would profit from an improved biomass burning calendar, as well as from an increase in NOX abundances in free tropospheric biomass burning plumes. The model showed the largest response to lightning NOX emissions, but systematic improvements could not be found. The use of multi-year satellite derived tropospheric data to systematically test and improve a CTM is a promising new addition to existing methods of model validation, and is a first step to integrating tropospheric satellite observations into global ozone modeling studies. Conversely,the CTM may suggest improvements to evolving satellite retrievals for tropospheric ozone.

Peters, Wouter↗

Tropospheric Ozone from Assimilation of Aura Data using Different Definitions of the Tropopause

Ozone data from Aura OMI and MLS instruments were assimilated into the general circulation model (GCM) constrained by assimilated meteorological fields from the Global Modeling and Assimilation Office at NASA Goddard. Properties of tropospheric ozone and their sensitivity to the definition of the tropopause are investigated. Three definitions of the tropopause are considered: (1) dynamical (using potential vorticity and potential temperature), (2) using temperature lapse rate, and (3) using a fixed ozone value. Comparisons of the tropospheric ozone columns using these tropopause definitions will be presented and evaluated against coincident profiles from ozone sondes. Assimilated ozone profiles are used to identify possible tropopause folding events, which are important for stratosphere-troposphere exchange. Each profile is searched for multiple levels at which ozone attains the value typical of the troposphere-stratosphere transition in order to identify possible tropopause folds. Constrained by the dynamics from a global model and by assimilation of Aura ozone data every 3-hours, this data set provides an opportunity to study ozone evolution in the upper troposphere and lower stratosphere with high temporal resolution.

Stajner, Ivanka↗