Transport analysis and source attribution of seasonal and interannual variability of CO in the tropical upper troposphere and lower stratosphere

We used the GEOS-Chem chemistry-transport model to investigate impacts of surface emissions and dynamical processes on the spatial and temporal patterns of CO observed by the Microwave Limb Sounder (MLS) in the upper troposphere (UT) and lower stratosphere (LS). Model simulations driven by GEOS-4 and GEOS-5 assimilated fields present many features of the seasonal and inter-annual variation of CO in the upper troposphere and lower stratosphere. Both model simulations and the MLS data show a transition from semi-annual variations in the UT to annual variations in the LS. Tagged CO simulations indicate that the semi-annual variation of CO in the UT is determined mainly by the temporal overlapping of surface biomass burning from different continents as well as the north-south shifts of deep convection. Both GEOS-4 and GEOS-5 have maximum upward transport in April and May with a minimum in July to September. The CO peaks from the Northern Hemisphere (NH) fires propagate faster to the LS than do those from the Southern Hemisphere (SH) fires. Thus the transition from a semi-annual to an annual cycle around 80 hPa is induced by a combination of the CO signal at the tropopause and the annual cycle of the Brewer-Dobson circulation. In GEOS-5, the shift to an annual cycle occurs at a lower altitude than in MLS CO, a result of inadequate upward transport. We deduce vertical velocities from MLS CO, and use them to evaluate the velocities derived from the archived GEOS meteorological fields. We find that GEOS-4 velocities are similar to those from MLS CO between 215 hPa and 125 hPa, while the velocities in GEOS-5 are too low in spring and summer. The mean tropical vertical velocities from both models are lower than those inferred from MLS CO above 100 hPa, particularly in GEOS-5, with mean downward, rather than upward motion in boreal summer. Thus the models' CO maxima from SH burning are transported less effectively than those in MLS CO above 147 hPa and almost disappear by 100 hPa. The strongest peaks in the CO tape-recorder are in late 2004, 2006, and 2010, with the first two resulting from major fires in Indonesia and the last from severe burning in South America, all associated with intense droughts

Analysis of CO in the tropical troposphere using Aura satellite data and the GEOS-Chem model: insights into transport characteristics of the GEOS meteorological products

We use the GEOS-Chem chemistry-transport model (CTM) to interpret the spatial and temporal variations of tropical tropospheric CO observed by the Microwave Limb Sounder (MLS) and the Tropospheric Emission Spectrometer (TES). In so doing, we diagnose and evaluate transport in the GEOS-4 and GEOS-5 assimilated meteorological fields that drive the model, with a particular focus on vertical mixing at the end of the dry season when convection moves over the source regions. The results indicate that over South America, deep convection in both GEOS-4 and GEOS-5 decays at too low an altitude early in the wet season, and the source of CO from isoprene in the model (MEGAN v2.1) is too large, causing a lag in the model's seasonal maximum of CO compared to MLS CO in the upper troposphere (UT). TES and MLS data reveal problems with excessive transport of CO to the eastern equatorial Pacific and lofting in the ITCZ in August and September, particularly in GEOS-4. Over southern Africa, GEOS-4 and GEOS-5 simulations match the phase of the observed CO variation from the lower troposphere (LT) to the UT fairly well, although the magnitude of the seasonal maximum is underestimated considerably due to low emissions in the model. A sensitivity run with increased emissions leads to improved agreement with observed CO in the LT and middle troposphere (MT), but the amplitude of the seasonal variation is too high in the UT in GEOS-4. Difficulty in matching CO in the LT and UT implies there may be overly vigorous vertical mixing in GEOS-4 early in the wet season. Both simulations and observations show a time lag between the peak in fire emissions (July and August) and in CO (September and October). We argue that it is caused by the prevailing subsidence in the LT until convection moves south in September, as well as the low sensitivity of TES data in the LT over the African Plateau. The MLS data suggest that too much CO has been transported from fires in northern Africa to the UT in the model during the burning season, as does MOZAIC aircraft data, perhaps as a result of the combined influence of too strong Harmattan winds in the LT and too strong vertical mixing over the Gulf of Guinea in the model

Global estimates of CO sources with high resolution by adjoint inversion of multiple satellite datasets (MOPITT, AIRS, SCIAMACHY, TES)

We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005) global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM) and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD), and aircraft (MOZAIC) are used for evaluation of the a posteriori solution. Using GEOS-Chem as a common intercomparison platform shows global consistency between the different satellite datasets and with the in situ data. Differences can be largely explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is 1350 Tg a<sup>−1</sup>. This is much higher than current bottom-up emission inventories. A large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes in winter and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. Implementing this seasonal variation of emissions solves the long-standing problem of models underestimating CO in the northern extratropics in winter-spring. A posteriori emissions also indicate a general underestimation of biomass burning in the GFED2 inventory. However, the tropical biomass burning constraints are not quantitatively consistent across the different datasets

First Directly Retrieved Global Distribution of Tropospheric Column Ozone from GOME: Comparison with the GEOS-CHEM Model

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 Niño 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 20°S–30°S during the austral spring and at 25°N–45°N during the boreal spring and summer, low 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 1σ 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.Earth and Planetary SciencesEngineering and Applied Science

Global Estimates of CO Sources with High Resolution by Adjoint Inversion of Multiple Satellite Datasets (MOPITT, AIRS, SCIAMACHY, TES)

We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005) global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM) and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD), and aircraft (MOZAIC) are used for evaluation of the a posteriori solution. Using GEOS-Chem as a common intercomparison platform shows global consistency between the different satellite datasets and with the in situ data. Differences can be largely explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is $1350 Tg a^{−1}$. This is much higher than current bottom-up emission inventories. A large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes in winter and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. Implementing this seasonal variation of emissions solves the long-standing problem of models underestimating CO in the northern extratropics in winter-spring. A posteriori emissions also indicate a general underestimation of biomass burning in the GFED2 inventory. However, the tropical biomass burning constraints are not quantitatively consistent across the different datasets.Engineering and Applied Science

Trends in the Vertical Distribution of Ozone: A Comparison of Two Analyses of Ozonesonde Data

We present the results of two independent analyses of ozonesonde measurements of the vertical profile of ozone. For most of the ozonesonde stations we use data that were recently reprocessed and reevaluated to improve their quality and internal consistency. The two analyses give similar results for trends in ozone. We attribute differences in results primarily to differences in data selection criteria and in utilization of data correction factors, rather than in statistical trend models. We find significant decreases in stratospheric ozone at all stations in middle and high latitudes of the northern hemisphere from 1970 to 1996, with the largest decreases located between 12 and 21 km, and trends of -3 to -10 %/decade near 17 km. The decreases are largest at the Canadian and the most northerly Japanese station, and are smallest at the European stations, and at Wallops Island, U.S.A. The mean mid-latitude trend is largest, -7 %/decade, from 12 to 17.5 km for 1970-96. For 1980-96, the decrease is more negative by 1-2 %/decade, with a maximum trend of -9 %/decade in the lowermost stratosphere. The trends vary seasonally from about 12 to 17.5 km, with largest ozone decreases in winter and spring. Trends in tropospheric ozone are highly variable and depend on region. There are decreases or zero trends at the Canadian stations for 1970-96, and decreases of -2 to -8 %/decade for the mid-troposphere for 1980-96; the three European stations show increases for 1970-96, but trends are close to zero for two stations for 1980-96 and positive for one; there are increases in ozone for the three Japanese stations for 1970-96, but trends are either positive or zero for 1980-96; the U.S. stations show zero or slightly negative trends in tropospheric ozone after 1980. It is not possible to define reliably a mean tropospheric ozone trend for northern mid-latitudes, given the small number of stations and the large variability in trends. The integrated column trends derived from the sonde data are consistent with trends derived from both surface based and satellite measurements of the ozone column

A quantitative assessment of uncertainties affecting estimates of global mean OH derived from methyl chloroform observations

We estimated the global abundance of OH by interpreting observations of methyl chloroform (MCF) from two networks using an inverse technique and a 3-D chemical transport model driven by assimilated meteorology. Our inversion approach optimized both the emissions of MCF and the abundance of OH. Because of an a priori overestimate of the latitudinal gradient by the model in the standard setup, the inversion lowers global emissions and the global sink due to OH. Optimized emissions are about 10 % lower than published inventories on average between 1988 and 1994, and the decrease in the sink suggested by the inversion implies an average lifetime for MCF (with respect to tropospheric OH) of about 6.9 years, 11-21 % longer than the 5.7-6.2 years reported in previous studies. Our results are driven by the need to match the observed latitudinal gradient of MCF while balancing the MCF budget. We find that these results depend on the a priori constraint placed on MCF emissions, the rate of interhemispheric mixing in the model, the interhemispheric distribution of OH assumed, and the model simulation of pollution events. Since these factors are highly uncertain, we believe that the level of understanding on global lifetimes of pollutants removed by OH is lower than might be implied by the narrow range of estimates for MCF lifetime in the literature. 2

The global budget of CO, 1988-1997: source estimates and validation with a global model

We present a model study of carbon monoxide for 1988-1997 using the GEOS-Chem 3-D model driven by assimilated meteorological data, with time-varying emissions from biomass burning and from fossil fuel and industry, overhead ozone columns, and methane. The hydroxyl radical is calculated interactively using a chemical parameterization to capture chemical feedbacks. We document the inventory for fossil fuels/industry and discuss major uncertainties and the causes of differences with other inventories that give significantly lower emissions. We find that emissions hardly change from 1988 to 1997, as increases in Asia are offset by decreases elsewhere. The model reproduces the 20% decrease in CO at high northern latitudes and the 10% decrease in the North Pacific, caused primarily by the decrease in European emissions. The model compares well with observations at sites impacted by fossil fuel emissions from North America, Europe, and east Asia suggesting that the emissions from this source are reliable to 25%, and we argue that bottom-up emission estimates are likely to be too low rather than too high. The model is too low at the seasonal maximum in spring in the southern tropics, except for locations in the Atlantic Ocean. This problem may be caused by an overestimate of the frequency of tropical deep convection, a common problem in models that use assimilated meteorological data. We argue that the yield of CO from methane oxidation is near unity, contrary to some other studies, based on removal rates of intermediate species