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We investigate the sensitivity of black carbon (BC) in the Arctic, including BC concentration in snow (BCsnow, ng g−1) and surface air (BCair, ng m−3), as well as emissions, dry deposition, and wet scavenging using the global three-dimensional (3-D) chemical transport model (CTM) GEOS-Chem. We find that the model underestimates BCsnow in the Arctic by 40 % on average (median = 11.8 ng g−1). Natural gas flaring substantially increases total BC emissions in the Arctic (by ∼ 70 %). The flaring emissions lead to up to 49 % increases (0.1–8.5 ng g−1) in Arctic BCsnow, dramatically improving model comparison with observations (50 % reduction in discrepancy) near flaring source regions (the western side of the extreme north of Russia). Ample observations suggest that BC dry deposition velocities over snow and ice in current CTMs (0.03 cm s−1 in the GEOS-Chem) are too small. We apply the resistance-in-series method to compute a dry deposition velocity (vd) that varies with local meteorological and surface conditions. The resulting velocity is significantly larger and varies by a factor of 8 in the Arctic (0.03–0.24 cm s−1), which increases the fraction of dry to total BC deposition (16 to 25 %) yet leaves the total BC deposition and BCsnow in the Arctic unchanged. This is largely explained by the offsetting higher dry and lower wet deposition fluxes. Additionally, we account for the effect of the Wegener–Bergeron–Findeisen (WBF) process in mixed-phase clouds, which releases BC particles from condensed phases (water drops and ice crystals) back to the interstitial air and thereby substantially reduces the scavenging efficiency of clouds for BC (by 43–76 % in the Arctic). The resulting BCsnow is up to 80 % higher, BC loading is considerably larger (from 0.25 to 0.43 mg m−2), and BC lifetime is markedly prolonged (from 9 to 16 days) in the Arctic. Overall, flaring emissions increase BCair in the Arctic (by ∼ 20 ng m−3), the updated vd more than halves BCair (by ∼ 20 ng m−3), and the WBF effect increases BCair by 25–70 % during winter and early spring. The resulting model simulation of BCsnow is substantially improved (within 10 % of the observations) and the discrepancies of BCair are much smaller during the snow season at Barrow, Alert, and Summit (from −67–−47 % to −46–3 %). Our results point toward an urgent need for better characterization of flaring emissions of BC (e.g., the emission factors, temporal, and spatial distribution), extensive measurements of both the dry deposition of BC over snow and ice, and the scavenging efficiency of BC in mixed-phase clouds. In addition, we find that the poorly constrained precipitation in the Arctic may introduce large uncertainties in estimating BCsnow. Doubling precipitation introduces a positive bias approximately as large as the overall effects of flaring emissions and the WBF effect; halving precipitation produces a similarly large negative bias.

A theoretical black carbon (BC) aging model is developed to account for three typical evolution stages, namely, freshly emitted aggregates, coated BC by soluble material, and BC particles undergoing further hygroscopic growth. The geometric-optics surface-wave (GOS) approach is employed to compute the BC single-scattering properties at each aging stage, which are subsequently compared with laboratory measurements. Theoretical calculations are consistent with measurements in extinction and absorption cross sections for fresh BC aggregates, but overestimate the scattering cross sections for BC mobility diameters of 155, 245, and 320 nm, because of uncertainties associated with theoretical calculations for small particles as well as laboratory scattering measurements. The measured optical cross sections for coated BC by sulfuric acid and for those undergoing further hygroscopic growth are captured by theoretical calculations using a concentric core-shell structure, with differences of less than 20 %. This suggests that the core-shell shape represents the realistic BC coating morphology reasonably well in this case, which is consistent with the observed strong structure compaction during aging. We find that the absorption and scattering properties of fresh BC aggregates vary by up to 60 % due to uncertainty in the BC refractive index, which, however, is a factor of two smaller in the case of coated BC particles. Sensitivity analyses on the BC morphology show that the optical properties of fresh BC aggregates are more sensitive to fractal dimension than primary spherule size. The absorption and scattering cross sections of coated BC particles vary by more than a factor of two due to different coating structures. We find an increase of 20–250 % in absorption and a factor of 3–15 in scattering during aging, significantly depending on coating morphology and aging stages. Applying the aging model to CalNex 2010 field measurements, we show that the resulting BC direct radiative forcing (DRF) first increases from 1.5 to 1.7 W m-2 and subsequently decreases to 1.0 W m-2 during the transport from the Los Angeles Basin to downwind regions, as a result of the competition between absorption enhancement due to coating and dilution of BC concentration. The BC DRF can vary by up to a factor of two due to differences in BC coating morphology. Thus, an accurate estimate of BC DRF requires the incorporation of a dynamic BC aging process that accounts for realistic morphology in climate models, particularly for the regional analysis with high atmospheric heterogeneity.

We estimate black carbon (BC) emissions in the western United States for July–September 2006 by inverting surface BC concentrations from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network using a global chemical transport model (GEOS-Chem) and its adjoint. Our best estimate of the BC emissions is 49.9 Gg at 2° × 2.5° (a factor of 2.1 increase) and 47.3 Gg at 0.5° × 0.667° (1.9 times increase). Model results now capture the observed major fire episodes with substantial bias reductions (~ 35 % at 2° × 2.5° and ~ 15 % at 0.5° × 0.667°). The emissions are ~ 20–50 % larger than those from our earlier analytical inversions (Mao et al., 2014). The discrepancy is especially drastic in the partitioning of anthropogenic versus biomass burning emissions. The August biomass burning BC emissions are 4.6–6.5 Gg and anthropogenic BC emissions 8.6–12.8 Gg, varying with the model resolution, error specifications, and subsets of observations used. On average both anthropogenic and biomass burning emissions in the adjoint inversions increase 2-fold relative to the respective {a priori} emissions, in distinct contrast to the halving of the anthropogenic and tripling of the biomass burning emissions in the analytical inversions. We attribute these discrepancies to the inability of the adjoint inversion system, with limited spatiotemporal coverage of the IMPROVE observations, to effectively distinguish collocated anthropogenic and biomass burning emissions on model grid scales. This calls for concurrent measurements of other tracers of biomass burning and fossil fuel combustion (e.g., carbon monoxide and carbon isotopes). We find that the adjoint inversion system as is has sufficient information content to constrain the total emissions of BC on the model grid scales.

We quantify source contributions to springtime (April 2008) surface black carbon (BC) in the Arctic by interpreting surface observations of BC at five receptor sites (Denali, Barrow, Alert, Zeppelin, and Summit) using a global chemical transport model (GEOS-Chem) and its adjoint. Contributions to BC at Barrow, Alert, and Zeppelin are dominated by Asian anthropogenic sources (40–43 %) before April 18 and by Siberian open biomass burning emissions (29–41 %) afterward. In contrast, Summit, a mostly free tropospheric site, has predominantly an Asian anthropogenic source contribution (24–68 %, with an average of 45 %). We compute the adjoint sensitivity of BC concentrations at the five sites during a pollution episode (April 20–25) to global emissions from March 1 to April 25. The associated contributions are the combined results of these sensitivities and BC emissions. Local and regional anthropogenic sources in Alaska are the largest anthropogenic sources of BC at Denali (63 %), and natural gas flaring emissions in the Western Extreme North of Russia (WENR) are the largest anthropogenic sources of BC at Zeppelin (26 %) and Alert (13 %). We find that long-range transport of emissions from Beijing-Tianjin-Hebei (also known as Jing-Jin-Ji), the biggest urbanized region in Northern China, contribute significantly (~ 10 %) to surface BC across the Arctic. On average it takes ~ 12 days for Asian anthropogenic emissions and Siberian biomass burning emissions to reach Arctic lower troposphere, supporting earlier studies. Natural gas flaring emissions from the WENR reach Zeppelin in about a week. We find that episodic, direct transport events dominate BC at Denali (87 %), a site outside the Arctic front, a strong transport barrier. The relative contribution of direct transport to surface BC within the Arctic front is much smaller (~ 50 % at Barrow and Zeppelin and ~ 10 % at Alert). The large contributions from Asian anthropogenic sources are predominately in the form of ‘chronic’ pollution (~ 40 % at Barrow and 65 % at Alert and 57 % at Zeppelin) on 1–2 month timescales. As such, it is likely that previous studies using 5- or 10-day trajectory analyses strongly underestimated the contribution from Asia to surface BC in the Arctic. Both finer temporal resolution of biomass burning emissions and accounting for the Wegener-Bergeron-Findeisen (WBF) process in wet scavenging improve the source attribution estimates.

We estimate biomass burning and anthropogenic emissions of black carbon (BC) in the western US for May–October 2006 by inverting surface BC concentrations from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network using a global chemical transport model. We first use active fire counts from the Moderate Resolution Imaging Spectroradiometer (MODIS) to improve the spatiotemporal distributions of the biomass burning BC emissions from the Global Fire Emissions Database (GFEDv2). The adjustment primarily shifts emissions from late to middle and early summer (a 33% decrease in September–October and a 56% increase in June–August) and leads to appreciable increases in modeled surface BC concentrations in early and middle summer, especially at the 1–2 and 2–3 km altitude ranges. We then conduct analytical inversions at both 2° × 2.5° and 0.5° × 0.667° (nested over North America) horizontal resolutions. The a posteriori biomass burning BC emissions for July–September are 31.7 Gg at 2° × 2.5° (an increase by a factor of 4.7) and 19.2 Gg at 0.5° × 0.667° (an increase by a factor of 2.8). The inversion results are rather sensitive to model resolution. The a posteriori biomass burning emissions at the two model resolutions differ by a factor of ~6 in California and the Southwest and by a factor of 2 in the Pacific Northwest. The corresponding a posteriori anthropogenic BC emissions are 9.1 Gg at 2° × 2.5° (a decrease of 48%) and 11.2 Gg at 0.5° × 0.667° (a decrease of 36%). Simulated surface BC concentrations with the a posteriori emissions capture the observed major fire episodes at most sites and the substantial enhancements at the 1–2 and 2–3 km altitude ranges. The a posteriori emissions also lead to large bias reductions (by ~30% on average at both model resolutions) in modeled surface BC concentrations and significantly better agreement with observations (increases in Taylor skill scores of 95% at 2° × 2.5° and 42 % at 0.5° × 0.667°).

In situ measurements of carbon monoxide (CO) and ozone (O3) at the Pico Mountain Observatory (PMO) located in the Azores, Portugal, are analyzed together with results from an atmospheric chemical transport model (GEOS-Chem) and satellite remote sensing data (AIRS (Atmospheric Infrared Sounder) for CO, and TES (Tropospheric Emission Spectrometer) for O3) to examine the evolution of free-troposphere CO and O3 over the North Atlantic for 2001–2011. GEOS-Chem captured the seasonal cycles for CO and O3 well but significantly underestimated the mixing ratios of CO, particularly in spring. Statistically significant (using a significance level of 0.05) decreasing trends were found for both CO and O3 based on harmonic regression analysis of the measurement data. The best estimates of the possible trends for CO and O3 measurements are −0.31 ± 0.30 (2-σ) ppbv yr−1 and −0.21 ± 0.11 (2-σ) ppbv yr−1, respectively. Similar decreasing trends for both species were obtained with GEOS-Chem simulation results. The most important factor contributing to the decreases in CO and O3 at PMO over the past decade is the decline in anthropogenic emissions from North America, which more than compensate for the impacts from increasing Asian emissions. It is likely that climate change in the past decade has also affected the intercontinental transport of O3.

Geoengineering applications by injection of sulfate aerosols into the stratosphere are under consideration as a measure of last resort to counter global warming. Here a potential regional-scale application to offset the impacts of heat waves is critically examined. Using the Weather Research and Forecasting model with fully coupled chemistry (WRF-Chem), the effect of regional-scale sulfate aerosol emission over California in each of two days of the July 2006 heat wave is used to quantify potential reductions in surface temperature as a function of emission rates in a layer at 12 km altitude. Local meteorological factors yield geographical differences in surface air temperature sensitivity. For emission rates of approximately 30 μg m−2 s−1 of sulfate aerosols (with standard WRF-Chem size distribution) over the region, temperature decreases of around 7 °C result during the middle part of the day over the Central Valley, one of the areas hardest hit by the heat wave. Regions more ventilated with oceanic air such as Los Angeles have slightly smaller reductions. The length of the hottest part of the day is also reduced. Advection effects on the aerosol cloud must be more carefully forecast for smaller injection regions. Verification of the impacts could be done via measurements of differences in reflected and surface downward shortwave. Such regional geoengineering applications with specific near-term target effects but smaller cost and side effects could potentially provide a means of testing larger scale applications. However, design considerations for regional applications, such as a preference for injection at a level of relatively low wind speed, differ from those for global applications. The size of the required injections and the necessity of injection close to the target region raise substantial concerns. The evaluation of this regional-scale application is thus consistent with global model evaluations, emphasizing that mitigation via reduction of fossil fuels remains preferable to considering geoengineering with sulfate aerosols.

A three-dimensional variational data assimilation (3-DVAR) algorithm for aerosols in a WRF/Chem model is presented. The WRF/Chem model uses the MOSAIC (Model for Simulating Aerosol Interactions and Chemistry) scheme, which explicitly treats eight major species (elemental/black carbon, organic carbon, nitrate, sulfate, chloride, ammonium, sodium and the sum of other inorganic, inert mineral and metal species) and represents size distributions using a sectional method with four size bins. The 3-DVAR scheme is formulated to take advantage of the MOSAIC scheme in providing comprehensive analyses of species concentrations and size distributions. To treat the large number of state variables associated with the MOSAIC scheme, this 3-DVAR algorithm first determines the analysis increments of the total mass concentrations of the eight species, defined as the sum of the mass concentrations across all size bins, and then distributes the analysis increments over four size bins according to the background error variances. The number concentrations for each size bin are adjusted based on the ratios between the mass and number concentrations of the background state. Additional flexibility is incorporated to further lump the eight mass concentrations, and five lumped species are used in the application presented. The system is evaluated using the analysis and prediction of PM2.5 in the Los Angeles basin during the CalNex 2010 field experiment, with assimilation of surface PM2.5 and speciated concentration observations. The results demonstrate that the data assimilation significantly reduces the errors in comparison with a simulation without data assimilation and improved forecasts of the concentrations of PM2.5 as well as individual species for up to 24 h. Some implementation difficulties and limitations of the system are discussed.

We systematically investigate the effects of Wegener-Bergeron-Findeisen (WBF) on BC scavenging efficiency, surface BCair, deposition flux, concentration in snow (BCsnow, ng g−1), and washout ratio using a global 3D chemical transport model (GEOS-Chem). We differentiate riming- versus WBF-dominated in-cloud scavenging based on liquid water content (LWC) and temperature. Specifically, we relate WBF to either temperature or ice mass fraction (IMF) in mixed-phase clouds. We find that at Jungfraujoch, Switzerland and Abisko, Sweden, where WBF dominates, the discrepancies of simulated BC scavenging efficiency and washout ratio are significantly reduced (from a factor of 3 to 10 % and from a factor of 4–5 to a factor of two). However, at Zeppelin, Norway, where riming dominates, simulation of BC scavenging efficiency, BCair, and washout ratio become worse (relative to observations) when WBF is included. There is thus an urgent need for extensive observations to distinguish and characterize riming- versus WBF-dominated aerosol scavenging in mixed-phase clouds and the associated BC scavenging efficiency. We find the reduction resulting from WBF to global BC scavenging efficiency varies substantially, from 8 % in the tropics to 76 % in the Arctic. The resulting annual mean BCair increases by up to 156 % at high altitudes and at northern high latitudes because of lower temperature and higher IMF. Overall, WBF halves the model-observation discrepancy (from −65 % to −30 %) of BCair across North America, Europe, China and the Arctic. Globally WBF increases BC burden from 0.22 to 0.29–0.35 mg m−2 yr−1, which partially explains the gap between observed and previous model simulated BC burdens over land. In addition, WBF significantly increases BC lifetime from 5.7 days to ~8 days. Additionally, WBF results in a significant redistribution of BC deposition in source and remote regions. Specifically, it lowers BC wet deposition (by 37–63 % at northern mid-latitudes and by 21–29 % in the Arctic) while increases dry deposition (by 3–16 % at mid-latitudes and by 81–159 % in the Arctic). The resulting total BC deposition is lower at mid-latitudes (by 12–34 %) but higher in the Arctic (by 2–29 %). We find that WBF decreases BCsnow at mid-latitudes (by ~15 %) but increases it in the Arctic (by 26 %) while improving model comparisons with observations. In addition, WBF dramatically reduces the model-observation discrepancy of washout ratios in winter (from a factor of 16 to 4). The remaining discrepancies in BCair, BCsnow and BC washout ratios suggest that in-cloud removal in mixed-phased clouds is likely still excessive over land.

The column abundance of NO3 was measured over Table Mountain Facility, CA (34.4° N, 117.7° W) from May 2003 through September 2004, using lunar occultation near full moon with a grating spectrometer. The NO3 column retrieval was performed with the differential optical absorption spectroscopy (DOAS) technique using both the 623 and 662 nm NO3 absorption bands. Other spectral features such as Fraunhofer lines and absorption from water vapor and oxygen were removed using solar spectra obtained at different airmass factors. We observed a seasonal variation, with nocturnally averaged NO3 columns between 5−7 × 1013 molec cm−2 during October through March, and 5−22 × 1013 molec cm−2 during April through September. A subset of the data, with diurnal variability vastly different from the temporal profile obtained from one-dimensional stratospheric model calculations, clearly has boundary layer contributions; this was confirmed by simultaneous long-path DOAS measurements. However, even the NO3 columns that did follow the modeled time evolution were often much larger than modeled stratospheric partial columns constrained by realistic temperatures and ozone concentrations. This discrepancy is attributed to substantial tropospheric NO3 in the free troposphere, which may have the same time dependence as stratospheric NO3.

We develop and examine a microphysics-based black carbon (BC) aerosol aging scheme that accounts for condensation, coagulation, and heterogeneous chemical oxidation processes in a global 3-D chemical transport model (GEOS-Chem) by interpreting the BC measurements from the HIAPER Pole-to-Pole Observations (HIPPO, 2009–2011) using the model. We convert aerosol mass in the model to number concentration by assuming lognormal aerosol size distributions and compute the microphysical BC aging rate (excluding chemical oxidation aging) explicitly from the condensation of soluble materials onto hydrophobic BC and the coagulation between hydrophobic BC and preexisting soluble particles. The chemical oxidation aging is tested in the sensitivity simulation. The microphysical aging rate is ∼ 4 times higher in the lower troposphere over source regions than that from a fixed aging scheme with an e-folding time of 1.2 days. The higher aging rate reflects the large emissions of sulfate–nitrate and secondary organic aerosol precursors hence faster BC aging through condensation and coagulation. In contrast, the microphysical aging is more than 5-fold slower than the fixed aging in remote regions, where condensation and coagulation are weak. Globally, BC microphysical aging is dominated by condensation, while coagulation contribution is largest over eastern China, India, and central Africa. The fixed aging scheme results in an overestimate of HIPPO BC throughout the troposphere by a factor of 6 on average. The microphysical scheme reduces this discrepancy by a factor of ∼ 3, particularly in the middle and upper troposphere. It also leads to a 3-fold reduction in model bias in the latitudinal BC column burden averaged along the HIPPO flight tracks, with largest improvements in the tropics. The resulting global annual mean BC lifetime is 4.2 days and BC burden is 0.25 mg m−2, with 7.3 % of the burden at high altitudes (above 5 km). Wet scavenging accounts for 80.3 % of global BC deposition. We find that, in source regions, the microphysical aging rate is insensitive to aerosol size distribution, condensation threshold, and chemical oxidation aging, while it is the opposite in remote regions, where the aging rate is orders of magnitude smaller. As a result, global BC burden and lifetime show little sensitivity (< 5 % change) to these three factors.

We estimate black carbon (BC) emissions in the Western United States (WUS) for July–September 2006 by inverting surface BC concentrations from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network using a global chemical transport model (GEOS-Chem) and its adjoint. Our best estimate of the BC emissions is 49.9 Gg at 2° × 2.5° (a factor of 2.1 increase) and 47.3 Gg at 0.5° × 0.667° (1.9 times increase). Model results now capture the observed major fire episodes with substantial bias reductions (∼35% at 2° × 2.5° and ∼15% at 0.5° × 0.667°). The emissions are ∼20–50% larger than those from our earlier analytical inversions (Mao et al., 2014). The discrepancy is especially drastic in the partitioning of anthropogenic vs. biomass burning emissions. The August biomass burning BC emissions are 4.6–6.5 Gg and anthropogenic BC emissions 8.6–12.8 Gg, varying with the model resolution, error specifications, and subsets of observations used. On average both increase twofold relative to the respective a priori emissions, in distinct contrast to the halving of the anthropogenic and tripling of the biomass burning emissions in the analytical inversions. We attribute these discrepancies to the inability of the inversion system, with limited spatiotemporal coverage of the IMPROVE observations, to effectively distinguish collocated anthropogenic and biomass burning emissions on model grid scales. This calls for concurrent measurements of other tracers of biomass burning and fossil fuel combustion (e.g., carbon monoxide and carbon isotopes). We find that the inversion system as is has sufficient information content to constrain the total emissions of BC on the model grid scales.

Atmospheric mineral dust particles exert significant direct radiative forcings and are critical drivers of climate change. Here, we use the GEOS-Chem global three-dimensional chemical transport model (3-D CTM) coupled online with the Fu-Liou-Gu (FLG) radiative transfer model (RTM) to investigate the dust radiative forcing and heating rates based on different dust vertical profiles. The coupled calculations using a realistic dust vertical profile simulated by GEOS-Chem minimize the physical inconsistencies between 3-D CTM aerosol fields and the RTM. The use of GEOS-Chem simulated aerosol optical depth (AOD) vertical profiles as opposed to the FLG prescribed AOD vertical profiles leads to greater and more spatially heterogeneous changes in estimated radiative forcing and heating rate produced by dust. Both changes can be attributed to a different vertical structure between dust and non-dust source regions. Values of the dust AOD are much larger in the middle troposphere, though smaller at the surface when the GEOS-Chem simulated AOD vertical profile is used, which leads to a much stronger heating rate in the middle troposphere. Compared to FLG vertical profile, the use of GEOS-Chem vertical profile reduces the solar radiative forcing effect by about 0.2–0.25 W m−2 and the Infrared (IR) radiative forcing over the African and Asia dust source regions by about 0.1–0.2 W m−2. Differences in the solar radiative forcing at the surface between using the GEOS-Chem vertical profile and the FLG vertical profile are most significant over the Gobi desert with a value of about 1.1 W m−2. The radiative forcing effect of dust particles is more pronounced at the surface over the Sahara and Gobi deserts by using FLG vertical profile, while it is less significant over the downwind area of Eastern Asia.

Concurrent tropospheric O 3 and CO vertical profiles from the Tropospheric Emission Spectrometer (TES) during the MILAGRO/INTEX-B aircraft campaigns over the Mexico City Metropolitan Area (MCMA) allow us to characterize mega-city pollution. Outflow from the MCMA occurred predominantly at 600–800 hPa, evident in O 3 , CO, and NO x enhancements in the in situ observations. We examined O 3 , CO, and their correlation at 600–800 hPa from TES retrievals, aircraft measurements, and GEOS-Chem model results over the aircraft coverage (within a radius of ~700 km around MCMA). The enhancements in O 3 and CO seen in the in situ measurements are not apparent in TES data, due to the lack of TES coverage during several strong pollution events. However, TES O 3 and CO data are consistent with the aircraft observations on a daily mean basis (50–60 ppbv and 100–130 ppbv for O 3 and CO respectively). The O 3 -CO correlation coefficients and enhancement ratios (ΔO 3 /ΔCO) derived from TES data are in good agreements with those derived from the aircraft observations and GEOS-Chem model results ( r : 0.5–0.9; ΔO 3 /ΔCO: 0.3–0.4), reflecting significant springtime photochemical production over MCMA and the surrounding region.

We present results from the first assimilation of carbon monoxide (CO) observations from the Tropospheric Emission Spectrometer (TES) into a global three-dimensional (3-D) chemistry and transport model (CTM). A sequential sub-optimal Kalman filter assimilation scheme (Khattatov et al., 2000) was applied to assimilate TES CO profiles during November 2004 into the GEOS-Chem global 3-D CTM. The assimilation results were compared with MOPITT and MOZAIC observations. The assimilation significantly improves model simulation of CO in the middle to upper troposphere, where the MOPITT versus model bias was reduced by up to two-thirds. Assimilation results show higher levels of CO in the southern tropics, consistent with MOPITT observations. We find good agreement between the TES assimilated model estimates of CO and in situ measurements from the MOZAIC program, which shows a negative bias of up to 10 ppbv in middle and upper tropospheric TES CO. The results demonstrate how assimilation can be used for non-coincident validation of TES CO profile retrievals.