Decadal record of satellite carbon monoxide observations

Worden, H. M.; Deeter, M. N.; Frankenberg, Christian; George, M.; Nichitiu, F.; Worden, J.; Aben, I.; Bowman, K. W.; Clerbaux, Cathy; Coheur, Pierre‐François; Laat, A. T. J. de; Detweiler, Raymond; Drummond, J. R.; Edwards, D. P.; Gille, J. C.; Hurtmans, Daniel; Luo, M.; Martínez-Alonso, S.; Massie, Steven T.; Pfister, Gabriele; Warner, J. X.

doi:10.5194/acp-13-837-2013

Cited by 225 publications

(197 citation statements)

References 60 publications

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“…CO has a tropospheric lifetime of a few months, so the seasonal variations reflect the northern hemisphere seasonal CO background, which is driven by enhanced emission in cold seasons and accelerated oxidation in summer (Logan et al, 1981). Such maxima of CO in spring have been found at other remote sites (e.g., Macdonald et al (2011) and for the Northern Hemisphere in general (Worden et al, 2013). The average O 3 of NATL were 39, 31, and 33 ppbv for spring, summer, and fall, respectively.…”

Section: Transport Patterns and Associated Chemical Signaturesmentioning

confidence: 89%

Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic

Zhang

Owen

Perlinger

et al. 2017

Elementa: Science of the Anthropocene

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Ten-year observations of trace gases at Pico Mountain Observatory (PMO), a free troposphere site in the central North Atlantic, were classified by transport patterns using the Lagrangian particle dispersion model, FLEXPART. The classification enabled identifying trace gas mixing ratios associated with background air and long- range transport of continental emissions, which were defined as chemical signatures. Comparison between the chemical signatures revealed the impacts of natural and anthropogenic sources, as well as chemical and physical processes during long transport,on air composition in the remote North Atlantic. Transport of North American anthropogenic emissions(NA-Anthro) and summertime wildfire plumes (Fire) significantly enhanced CO and O3 at PMO. Summertime CO enhancements caused by NA-Anthro were found to have been decreasing by a rate of 0.67 ± 0.60 ppbv/year in the ten-year period, due possibly to reduction of emissions in North America. Downward mixing from the upper troposphere and stratosphere due to the persistent Azores-Bermuda anticyclone causes enhanced O3 and nitrogen oxides. The d[O3]/d [CO] value was used to investigate O3 sources and chemistry in different transport patterns. The transport pattern affected by Fire had the lowest d [O3]/d [CO], which was likely due to intense CO production and depressed O3 production in wildfire plumes. Slightly enhanced O3 and d [O3]/d [CO] were found in the background air, suggesting that weak downward mixing from the upper troposphere is common at PMO. Enhancements of both butane isomers were found during upslope flow periods, indicating contributions from local sources. The consistent ratio of butane isomers associated with the background air and NA-anthro implies no clear difference in the oxidation rates of the butane isomers during long transport. Based on observed relationships between non-methane hydrocarbons, the averaged photochemical age of the air masses at PMO was estimated to be 11 ± 4 days.

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Section: Transport Patterns and Associated Chemical Signaturesmentioning

confidence: 89%

Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic

Zhang

Owen

Perlinger

et al. 2017

Elementa: Science of the Anthropocene

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“…Note that for consistency with benchmarking procedures for the full chemistry simulation, we have included here only the aircraft data in the standard GEOS-Chem benchmark (all data are available at https://bitbucket.org/gcst/gc_1yr_benchmark/). This dataset does not include any recent aircraft campaigns, and we therefore do not expect a quantitative match to our simulations (which span 2009-2011), especially near anthropogenic source regions where emissions have changed dramatically over the last few decades (Worden et al, 2013; Model results are monthly means at the location of each site from the full chemistry (solid orange), base CO-only (dashed red), and improved CO-only (dashed purple) simulations. The main difference between the two CO-only simulations is the vertical distribution of the CO source from NMVOCs, which is three-dimensional in the improved simulation but only occurs in the surface layer in the base simulation.…”

Section: Implications For Global Evaluation With Observationsmentioning

confidence: 99%

Improved method for linear carbon monoxide simulation and source attribution in atmospheric chemistry models illustrated using GEOS-Chem v9

et al. 2017

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Abstract. Carbon monoxide (CO) simulation in atmospheric chemistry models is frequently used for source-receptor analysis, emission inversion, interpretation of observations, and chemical forecasting due to its computational efficiency and ability to quantitatively link simulated CO burdens to sources. While several methods exist for modeling CO source attribution, most are inappropriate for regions where the CO budget is dominated by secondary production rather than direct emissions. Here, we introduce a major update to the linear CO-only capability in the GEOS-Chem chemical transport model that for the first time allows sourceregion tagging of secondary CO produced from oxidation of non-methane volatile organic compounds. Our updates also remove fundamental inconsistencies between the CO-only simulation and the standard full chemistry simulation by using consistent CO production rates in both. We find that relative to the standard chemistry simulation, CO in the original CO-only simulation was overestimated by more than 100 ppb in the model surface layer and underestimated in outflow regions. The improved CO-only simulation largely resolves these discrepancies by improving both the magnitude and location of secondary production. Despite large differences between the original and improved simulations, however, model evaluation with the global dataset used to benchmark GEOS-Chem shows negligible change to the model's ability to match the observations. This suggests that the current GEOS-Chem benchmark is not well suited to evaluate model changes in regions influenced by biogenic emissions and chemistry, and expanding the dataset to include observations from biogenic source regions (including those from recent aircraft campaigns) should be a priority for the GEOSChem community. Using Australasia as a case study, we show that the new ability to geographically tag secondary CO production provides significant added value for interpreting observations and model results in regions where primary CO emissions are low. Secondary production dominates the CO budget across much of the world, especially in the Southern Hemisphere, and we recommend future model-observation and multi-model comparisons implement this capability to provide a more complete understanding of CO sources and their variability.

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“…As there have been only modestly decreasing trends observed in the concentrations of CO after the 1990s (FortemsCheiney et al, 2011;Worden et al, 2013), the sources and sinks of CO must be approximately in balance, except for some seasonal and interannual variations in the CO budget (Duncan and Logan, 2008). The few published estimates of the atmospheric CO burden date back to the 1990s, with 365-410 Tg (Granier et al, 1996), 380-470 Tg (Reichle and Connors, 1999), and 360 Tg (Prather et al, 2001).…”

Section: Introductionmentioning

confidence: 99%

On the wintertime low bias of Northern Hemisphere carbon monoxide found in global model simulations

Stein¹,

Schultz²,

et al. 2014

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Abstract. Despite the developments in the global modelling of chemistry and of the parameterization of the physical processes, carbon monoxide (CO) concentrations remain underestimated during Northern Hemisphere (NH) winter by most state-of-the-art chemistry transport models. The consequential model bias can in principle originate from either an underestimation of CO sources or an overestimation of its sinks. We address both the role of surface sources and sinks with a series of MOZART (Model for Ozone And Related Tracers) model sensitivity studies for the year 2008 and compare our results to observational data from ground-based stations, satellite observations, and vertical profiles from measurements on passenger aircraft. In our base case simulation using MACCity (Monitoring Atmospheric Composition and Climate project) anthropogenic emissions, the near-surface CO mixing ratios are underestimated in the Northern Hemisphere by more than 20 ppb from December to April, with the largest bias of up to 75 ppb over Europe in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOCs) is not able to reduce the annual course of the model bias and yields concentrations over the Southern Hemisphere which are too high. Raising global annual anthropogenic emissions with a simple scaling factor results in overestimations of surface mixing ratios in most regions all year round. Instead, our results indicate that anthropogenic CO and, possibly, VOC emissions in the MACCity inventory are too low for the industrialized countries only during winter and spring. Reasonable agreement with observations can only be achieved if the CO emissions are adjusted seasonally with regionally varying scaling factors. A part of the model bias could also be eliminated by exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes, which reduces the boreal winter dry deposition fluxes. The best match to surface observations, satellite retrievals, and aircraft observations was achieved when the modified dry deposition scheme was combined with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively). One reason for the apparent underestimation of emissions may be an exaggerated downward trend in the Representative Concentration Pathway (RCP) 8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot fully exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations on the modelled CO.

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Decadal record of satellite carbon monoxide observations

Cited by 225 publications

References 60 publications

Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic

Ten-year chemical signatures associated with long-range transport observed in the free troposphere over the central North Atlantic

Improved method for linear carbon monoxide simulation and source attribution in atmospheric chemistry models illustrated using GEOS-Chem v9

On the wintertime low bias of Northern Hemisphere carbon monoxide found in global model simulations

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