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Validation of the Measurement of Pollution in the Troposphere (MOPITT) Experiment by Ground-Based Infrared Solar Spectroscopic Measurements of Carbon Monoxide (CO) and Methane (CH4)

The goal of the MOPITT experiment is to enhance our knowledge of the lower atmosphere system and particularly how it interacts with the surface/ocean/biomass systems. The particular focus is the distribution, transport, sources and sinks of carbon monoxide and methane in the troposphere. The MOPITT instrument was launched on EOS TERRA satellite December 18, 1999. After the launch and until March 22, 2000 the MOPITT instrument was in engineering and calibration mode. Beginning March 23, 2000 through May 6, 2001 the instrument was in a science measurement mode with some calibration breaks. On May 7, 2001 a criocooler on a side B died and channels 1 - 4 became inoperational. The MOPITT resumed its scientific measurements on August 25, 2001 with channels 5 - 8. With some calibration breaks the instrument currently provides the data. The project has three elements to it: hardware, data analysis and modeling. The MOPITT instrument, on the NASA EOS Terra satellite, measures the upwelling infrared radiance. Using the technique of correlation spectroscopy, information regarding the distribution of atmospheric CO and CH4 can be extracted. By using appropriate data analysis techniques, concentration profiles of CO are currently obtained on a global basis at a reasonably high horizontal (approximately 22km) and vertical resolution (approximately 3km). Column amounts of methane will be derived over the sunlit side of the orbit. These profiles are assimilated into models to study the chemistry and dynamics of CO, CH4 and other constituents of the lower atmosphere.

Pougatchev, Nikita

Measurements of Pollution In The Troposphere (MOPITT) Validation through 2006

Comparisons of aircraft measurements of carbon monoxide (CO) to the retrievals of CO using observations from the Measurements of Pollution in The Troposphere (MOPITT) instrument onboard the Terra satellite are presented. Observations made as part of the NASA INTEX-B and NSF MIRAGE field campaigns during March May 2006 are used to validate the MOPITT CO retrievals, along with routine samples from 2001 through 2006 from NOAA and the MOZAIC measurements from commercial aircraft. A significant positive bias, around 20% for total column CO, in MOPITT CO was found in the comparison to in situ measurements during 2006. Comparisons to the long-term records of measurements from NOAA and MOZAIC revealed an increasing bias in the V3 MOPITT CO retrievals over time. The impact of an instrumental drift is illustrated through retrieval simulations.

Emmons, L. K.

Southern Hemisphere Carbon Monoxide Inferannual Variability Observed by Terra/Measurement of Pollution in the Troposphere (MOPITT)

Biomass burning is an annual occurrence in the tropical southern hemisphere (SH) and represents a major source of regional pollution. Vegetation fires emit carbon monoxide (CO), which due to its medium lifetime is an excellent tracer of tropospheric transport. CO is also one of the few tropospheric trace gases currently observed from satellite and this provides long-term global measurements. In this paper, we use the 5 year CO data record from the Measurement Of Pollution In The Troposphere (MOPITT) instrument to examine the inter-annual variability of the SH CO loading and show how this relates to climate conditions which determine the intensity of fire sources. The MOPITT observations show an annual austral springtime peak in the SH zonal CO loading each year with dry-season biomass burning emissions in S. America, southern Africa, the Maritime Continent, and northwestern Australia. Although fires in southern Africa and S. America typically produce the greatest amount of CO, the most significant inter-annual variation is due to varying fire activity and emissions from the Maritime Continent and northern Australia. We find that this variation in turn correlates well with the El Nino Southern Oscillation precipitation index. Between 2000 and 2005, emissions were greatest in late 2002 and an inverse modeling of the MOPITT data using the MOZART chemical transport model estimates the southeast Asia regional fire source for the year August 2002 to September 2003 to be 52 Tg CO. Comparison of the MOPITT retrievals and NOAA surface network measurements indicate that the latter do not fully capture the inter-annual variability or the seasonal range of the CO zonal average concentration due to biases associated with atmospheric and geographic sampling.

Edwards, D. P.

Measurements of Pollution in the Troposphere (MOPITT) Validation Exercises During Summer 2004 Field Campaigns over North America

Measurements of carbon monoxide (CO) made as part of three aircraft experiments during the summer of 2004 over North America have been used for the continued validation of the CO retrievals from the Measurements of Pollution in the Troposphere (MOPITT) instrument on board the Terra satellite. Vertical profiles measured during the NASA INTEX-A campaign, designed to be coincident with MOPITT overpasses, as well as measurements made during the COBRA-2004 and MOZAIC experiments, provided valuable validation comparisons. On average, the MOPITT CO retrievals are biased slightly high for these North America locations. While the mean bias differs between the different aircraft experiments (e.g., 7.0 ppbv for MOZAIC to 18.4 ppbv for COBRA at 700 hPa), the standard deviations are quite large, so the results for the three data sets can be considered consistent. On average, it is estimated that MOPITT is 7- 14% high at 700 hPa and 03% high at 350 hPa. These results are consistent with the validation results for the Carr, Colorado, Harvard Forest, Massachusetts, and Poker Flats, Alaska, aircraft profiles for "phase 2" presented by Emmons et al. (2004) and are generally within the design criteria of 10% accuracy.

Emmons, L. K.

Direct Top-down Estimates of Biomass Burning CO Emissions Using TES and MOPITT Versus Bottom-up GFED Inventory

In this study, we utilize near-simultaneous observations from two sets of multiple satellite sensors to segregate Tropospheric Emission Spectrometer (TES) and Measurements of Pollution in the Troposphere (MOPITT) CO observations over active fire sources from those made over clear background. Hence, we obtain direct estimates of biomass burning CO emissions without invoking inverse modeling as in traditional top-down methods. We find considerable differences between Global Fire Emissions Database (GFED) versions 2.1 and 3.1 and satellite-based emission estimates in many regions. Both inventories appear to greatly underestimate South and Southeast Asia emissions, for example. On global scales, however, CO emissions in both inventories and in the MOPITT-based analysis agree reasonably well, with the largest bias (30%) found in the Northern Hemisphere spring. In the Southern Hemisphere, there is a one-month shift between the GFED and MOPITT-based fire emissions peak. Afternoon tropical fire emissions retrieved from TES are about two times higher than the morning MOPITT retrievals. This appears to be both a real difference due to the diurnal fire activity variations, and a bias due to the scarcity of TES data.

bias

MOPITT Mechanisms 16 Years In-Orbit Operation on TERRA

The 16th anniversary of the launch of NASA's Terra Spacecraft was marked on December 18, 2015, with the Measurements of Pollution in the Troposphere (MOPITT) instrument being a successful contributor to the NASA EOS flagship. MOPITT has been enabled by a large suite of mechanisms, allowing the instrument to perform long-duration monitoring of atmospheric carbon monoxide, providing global measurements of this important greenhouse gas for 16 years. Mechanisms have been successfully employed for scanning, cooling of detectors, and to optically modulate the gas path length within the instrument by means of pressure and gas cell length variation. The instrument utilizes these devices to perform correlation spectroscopy, enabling measurements with vertical resolution from the nadir view, and has thereby furthered understanding of source and global transport effects of carbon monoxide. Given the design requirement for a 5.25-year lifetime, the stability and performance of the majority of mechanisms have far surpassed design goals. With 16 continuously operating mechanisms in service on MOPITT, including 12 rotating mechanisms and 4 with linear drive elements, the instrument was an ambitious undertaking. The long life requirements combined with demands for cleanliness and optical stability made for difficult design choices including that of the selection of new lubrication processes. Observations and lessons learned with regards to many aspects of the mechanisms and associated monitoring devices are discussed here. Mechanism behaviors are described, including anomalies, long-term drive current/power, fill pressure, vibration and cold-tip temperature trends. The effectiveness of particular lubrication formulations and the screening method implemented is discussed in relation to continuous rotating mechanisms and stepper motors, which have exceeded 15 billon rotations and 2.5 billion steps respectively. Aspects of gas cell hermeticity, optical cleanliness, heater problems and SEU effects on accelerometers are also discussed.

Gibson, Andrew S.

MOPITT - A gas correlation spectrometer for tropospheric Earth observations

MOPITT (Measurement of Pollution in the Troposphere) is an instrument that will fly on the EOS AM-1 Polar Orbiting Platform, to be launched in mid-1998. The instrument accurately measures the concentration of carbon monoxide (CO) and methane (CH4) gas in the troposphere, using novel and conventional gas correlation spectroscopy techniques. These techniques are used to measure both the column amount and the vertical profile of the two gases in the troposphere. The instrument is nadir viewing and has cross-track scanning ability. It measures upwelling IR radiation through the atmosphere in the 4.6-micron and 2.3-micron bands for CO detection, and 2.2-micron for CH4. The instrument performance is enhanced using Stirling cycle mechanical coolers to maintain the IR detectors at less than 100 K. MOPITT has a total of eight detector channels to measure the total column of atmospheric CH4 gas to a precision of 1 percent, and to measure CO profiles to a precision of 10 percent. The instrument is self-calibrating to ensure data validity using internal targets and an external cold space view.

Drummond, James R.

Interpreting Space-Based Trends in Carbon Monoxide with Multiple Models

We use a series of chemical transport model and chemistry climate model simulations to investigate the observed negative trends in MOPITT CO over several regions of the world, and to examine the consistency of timedependent emission inventories with observations. We find that simulations driven by the MACCity inventory, used for the Chemistry Climate Modeling Initiative (CCMI), reproduce the negative trends in the CO column observed by MOPITT for 2000-2010 over the eastern United States and Europe. However, the simulations have positive trends over eastern China, in contrast to the negative trends observed by MOPITT. The model bias in CO, after applying MOPITT averaging kernels, contributes to the model-observation discrepancy in the trend over eastern China. This demonstrates that biases in a model's average concentrations can influence the interpretation of the temporal trend compared to satellite observations. The total ozone column plays a role in determining the simulated tropospheric CO trends. A large positive anomaly in the simulated total ozone column in 2010 leads to a negative anomaly in OH and hence a positive anomaly in CO, contributing to the positive trend in simulated CO. These results demonstrate that accurately simulating variability in the ozone column is important for simulating and interpreting trends in CO.

carbon monoxide

Asian Outflow and Trans-Pacific Transport of Carbon Monoxide and Ozone Pollution: An Integrated Satellite, Aircraft, and Model Perspective

Satellite observations of carbon monoxide (CO) from the Measurements of Pollution in the Troposphere (MOPITT) instrument are combined with measurements from the Transport and Chemical Evolution Over the Pacific (TRACE-P) aircraft mission over the northwest Pacific and with a global three-dimensional chemical transport model (GEOS-CHEM) to quantify Asian pollution outflow and its trans-Pacific transport during spring 2001. Global CO column distributions in MOPITT and GEOS-CHEM are highly correlated (R(exp 2) = 0.87), with no significant model bias. The largest regional bias is over Southeast Asia, where the model is 18% too high. A 60% decrease of regional biomass burning emissions in the model (to 39 Tg/yr) would correct the discrepancy; this result is consistent with TRACE-P observations. MOPITT and TRACE-P also give consistent constraints on the Chinese source of CO from fuel combustion (181 Tg CO/yr). Four major events of trans-Pacific transport of Asian pollution in spring 2001 were seen by MOPITT, in situ platforms, and GEOS-CHEM. One of them was sampled by TRACE-P (26-27 February) as a succession of pollution layers over the northeast Pacific. These layers all originated from one single event of Asian outflow that split into northern and southern plumes over the central Pacific. The northern plume (sampled at 6-8 km off California) had no ozone enhancement. The southern subsiding plume (sampled at 2-4 km west of Hawaii) contained a 8 - 17 ppbv ozone enhancement, driven by decomposition of peroxyacetylnitrate (PAN) to nitrogen oxides (NOx). This result suggests that PAN decomposition in trans-Pacific pollution plumes subsiding over the United States could lead to significant enhancements of surface ozone.

Heald, Colette L.

Evaluating Model Performance of an Ensemble-based Chemical Data Assimilation System During INTEX-B Field Mission

We present a global chemical data assimilation system using a global atmosphere model, the Community Atmosphere Model (CAM3) with simplified chemistry and the Data Assimilation Research Testbed (DART) assimilation package. DART is a community software facility for assimilation studies using the ensemble Kalman filter approach. Here, we apply the assimilation system to constrain global tropospheric carbon monoxide (CO) by assimilating meteorological observations of temperature and horizontal wind velocity and satellite CO retrievals from the Measurement of Pollution in the Troposphere (MOPITT) satellite instrument. We verify the system performance using independent CO observations taken on board the NSFINCAR C-130 and NASA DC-8 aircrafts during the April 2006 part of the Intercontinental Chemical Transport Experiment (INTEX-B). Our evaluations show that MOPITT data assimilation provides significant improvements in terms of capturing the observed CO variability relative to no MOPITT assimilation (i.e. the correlation improves from 0.62 to 0.71, significant at 99% confidence). The assimilation provides evidence of median CO loading of about 150 ppbv at 700 hPa over the NE Pacific during April 2006. This is marginally higher than the modeled CO with no MOPITT assimilation (-140 ppbv). Our ensemble-based estimates of model uncertainty also show model overprediction over the source region (i.e. China) and underprediction over the NE Pacific, suggesting model errors that cannot be readily explained by emissions alone. These results have important implications for improving regional chemical forecasts and for inverse modeling of CO sources and further demonstrate the utility of the assimilation system in comparing non-coincident measurements, e.g. comparing satellite retrievals of CO with in-situ aircraft measurements. The work described above also brought to light several short-comings of the data assimilation approach for CO profiles. Because of the limited vertical resolution of the measurement, the retrievals at different altitudes are correlated which can lead to problems with numerical error and overall efficiency. This has resulted in a manuscript that is about to be submitted to JGR:

Arellano, A. F., Jr.

EOS Terra Validation Program

The EOS Terra mission will be launched in July 1999. This mission has great relevance to the atmospheric radiation community and global change issues. Terra instruments include ASTER, CERES, MISR, MODIS and MOPITT. In addition to the fundamental radiance data sets, numerous global science data products will be generated, including various Earth radiation budget, cloud and aerosol parameters, as well as land surface, terrestrial ecology, ocean color, and atmospheric chemistry parameters. Significant investments have been made in on-board calibration to ensure the quality of the radiance observations. A key component of the Terra mission is the validation of the science data products. This is essential for a mission focused on global change issues and the underlying processes. The Terra algorithms have been subject to extensive pre-launch testing with field data whenever possible. Intensive efforts will be made to validate the Terra data products after launch. These include validation of instrument calibration (vicarious calibration) experiments, instrument and cross-platform comparisons, routine collection of high quality correlative data from ground-based networks, such as AERONET, and intensive sites, such as the SGP ARM site, as well as a variety field experiments, cruises, etc. Airborne simulator instruments have been developed for the field experiment and underflight activities including the MODIS Airborne Simulator (MAS), AirMISR, MASTER (MODIS-ASTER), and MOPITT-A. All are integrated on the NASA ER-2, though low altitude platforms are more typically used for MASTER. MATR is an additional sensor used for MOPITT algorithm development and validation. The intensive validation activities planned for the first year of the Terra mission will be described with emphasis on derived geophysical parameters of most relevance to the atmospheric radiation community. Detailed information about the EOS Terra validation Program can be found on the EOS Validation program homepage i/e.: http://ospso.gsfc.nasa.gov/validation/valpage.html).

Starr, David

EOS Terra Validation Program

The EOS Terra mission will be launched in July 1999. This mission has great relevance to the atmospheric radiation community and global change issues. Terra instruments include Advanced Spaceborne Thermal Emission and Reflection Radiometer (ASTER), Clouds and Earth's Radiant Energy System (CERES), Multi-Angle Imaging Spectroradiometer (MISR), Moderate Resolution Imaging Spectroradiometer (MODIS) and Measurements of Pollution in the Troposphere (MOPITT). In addition to the fundamental radiance data sets, numerous global science data products will be generated, including various Earth radiation budget, cloud and aerosol parameters, as well as land surface, terrestrial ecology, ocean color, and atmospheric chemistry parameters. Significant investments have been made in on-board calibration to ensure the quality of the radiance observations. A key component of the Terra mission is the validation of the science data products. This is essential for a mission focused on global change issues and the underlying processes. The Terra algorithms have been subject to extensive pre-launch testing with field data whenever possible. Intensive efforts will be made to validate the Terra data products after launch. These include validation of instrument calibration (vicarious calibration) experiments, instrument and cross-platform comparisons, routine collection of high quality correlative data from ground-based networks, such as AERONET, and intensive sites, such as the SGP ARM site, as well as a variety field experiments, cruises, etc. Airborne simulator instruments have been developed for the field experiment and underflight activities including the MODIS Airborne Simulator (MAS) AirMISR, MASTER (MODIS-ASTER), and MOPITT-A. All are integrated on the NASA ER-2 though low altitude platforms are more typically used for MASTER. MATR is an additional sensor used for MOPITT algorithm development and validation. The intensive validation activities planned for the first year of the Terra mission will be described with emphasis on derived geophysical parameters of most relevance to the atmospheric radiation community.

Starr, David

Transport and Chemical Evolution over the Pacific (TRACE-P)Aircraft Mission: Design, Execution, and First Results

The NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission was conducted in February-April 2001 over the NW Pacific (1) to characterize the Asian chemical outflow and relate it quantitatively to its sources and (2) to determine its chemical evolution. It used two aircraft, a DC-8 and a P-3B, operating out of Hong Kong and Yokota Air Force Base (near Tokyo), with secondary sites in Hawaii, Wake Island, Guam, Okinawa, and Midway. The aircraft carried instrumentation for measurements of long-lived greenhouse gases, ozone and its precursors, aerosols and their precursors, related species, and chemical tracers. Five chemical transport models (CTMs) were used for chemical forecasting. Customized bottom-up emission inventories for East Asia were generated prior to the mission to support chemical forecasting and to serve as a priori for evaluation with the aircraft data. Validation flights were conducted for the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument and revealed little bias (6 plus or minus 2%) in the MOPITT measurements of CO columns. A major event of transpacific Asian pollution was characterized through combined analysis of TRACE-P and MOPITT data. The TRACE-P observations showed that cold fronts sweeping across East Asia and the associated warm conveyor belts (WCBs) are the dominant pathway for Asian outflow to the Pacific in spring. The WCBs lift both anthropogenic and biomass burning (SE Asia) effluents to the free troposphere, resulting in complex chemical signatures. The TRACE-P data are in general consistent with a priori emission inventories, lending confidence in our ability to quantify Asian emissions from socioeconomic data and emission factors. However, the residential combustion source in rural China was found to be much larger than the a priori, and there were also unexplained chemical enhancements (HCN, CH3Cl, OCS, alkylnitrates) in Chinese urban plumes. The Asian source of CCl4 was found to be much higher than government estimates. Measurements of HCN and CH3CN indicated a dominant biomass burning source and ocean sink for both gases. Large fractions of sulfate and nitrate were found to be present in dust aerosols. Photochemical activity in the Asian outflow was strongly reduced by aerosol attenuation of UV radiation, with major implications for the concentrations of HOx, radicals. New particle formation, apparently from ternary nucleation involving NH3, was observed in Chinese urban plumes.

Jacob, Daniel J.

TERRA/MOPITT Measurements of Tropospheric Carbon Monoxide Distributions in Support of INTEX

Interaction with the ongoing satellite measurements programs was an important goal of INTEX- A. The Terra/MOPITT instrument had been making global measurements of the tropospheric carbon monoxide (CO) distribution for 4 years, and was in a unique position to provide valuable support during the field campaign. Remote sensing of CO directly addressed the scientific questions motivating the IXTEX-A strategy and deployment, and measurement of this gas was rated as being mission critical. CO is an important trace gas in tropospheric chemistry due to its role in determining the atmospheric oxidizing capacity, as an ozone precursor, and as an indicator and tracer of both natural and anthropogenic pollution arising from incomplete combustion. The satellite perspective provided the more general temporal and spatial context to the aircraft and ground-based measurements during the subsequent scientific analysis. We proposed to build on the experience of supplying MOPITT data to previous field campaigns, such as TRACE-P. We provided expedited MOPITT data processing in near real-time, along with basic analysis of the measurements to indicate, where possible, the origin of the CO plumes that impacted the regions of flight operations and other in situ measurement activities. To ensure maximum exploitation of the satellite information, we will also had a scientist in the field to present and interpret the MOPITT data for the INTEX team, and to help ensure its utility in flight planning.

Edwards, D. P.

High resolution assimilation of multiple satellite retrievals with emissions adjustment to improve air quality forecasting with WRF-Chem/DART

We will present results from medium (15km, 6hr cycling) and high (4 km, 6 hr cycling) spatiotemporal resolution applications of the WRF-Chem/DART ensemble, regional, air quality (AQ) forecast/assimilation system.The medium-resolution setup is applied to the Discover AQ/Front Range Air Pollution and Photochemistry Experiment (FRAPPE) domain from July 14 to July 29, 2014. The high-resolution setup is applied to a Colorado domain from July 14 to July 29, 2020. For the FRAPPE application, we assimilate MOPITT CO; IASI CO;MODIS AOD; OMI O3, NO2; and AirNow CO, O3, NO2, SO2, PM10, and PM2.5. For the Colorado application, we assimilate the same MOPITT, MODIS, and AirNow constituents as in the FRAPPE application and TROPOMI CO, O3, NO2; and synthetic TEMPO O3and NO2. WRF-Chem/DART integrates the Weather Research and Forecast (WRF) model with on-line chemistry (WRF-Chem) into the Data Assimilation Research Testbed (DART). It assimilates AirNow CO, O3, NO2, SO2, PM10, and PM2.5 measurements, MOPITT CO; IASI CO, O3; OMI O3, NO2, SO2; TROPOMI CO, O3, NO2, SO2; MODIS AOD; and synthetic TEMPO O3 and NO2 total/partial column and/or profile retrievals.WRF-Chem/DART uses: (i) the state augmentation method for adjusting emissions; (ii) state-space localization; and (iii) a near-real time scripting system. We use the medium-resolution FRAPPE application to demonstrate the incremental benefits from assimilating OMI observations with emissions adjustment and the high-resolution Colorado application to demonstrate the incremental benefits from assimilating syntheticTEMPO observations with emissions adjustment. For both applications, we expect that: (i) assimilating chemical observations will increaseAQ forecast skill; (ii) including emissions adjustment will increase forecast skill/predictability; and (iii) including assimilation of synthetic TEMPO observations will further increase forecast skill/predictability.

High resolution

Variability of Springtime Transpacific Pollution Transport During 2000-2006: The INTEX-5 Mission in the Context of Previous Years

We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part 8) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and .dynamics from changes in source strength. interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 113 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 213 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.

Pfister, G. G.

Description and Evaluation of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry Model (NMMB-MONARCH) Version 1.0: Gas-Phase Chemistry at Global Scale

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMBMONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT).We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3-0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error - RMSE - below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability).

atmospheric chemistry