Error Correlation Between CO2 and CO as Constraint for CO2 Flux Inversions Using Satellite Data

Inverse modeling of CO2 satellite observations to better quantify carbon surface fluxes requires a chemical transport model (CTM) to relate the fluxes to the observed column concentrations. CTM transport error is a major source of uncertainty. We show that its effect can be reduced by using CO satellite observations as additional constraint in a joint CO2-CO inversion. CO is measured from space with high precision, is strongly correlated with CO2, and is more sensitive than CO2 to CTM transport errors on synoptic and smaller scales. Exploiting this constraint requires statistics for the CTM transport error correlation between CO2 and CO, which is significantly different from the correlation between the concentrations themselves. We estimate the error correlation globally and for different seasons by a paired-model method (comparing GEOS-Chem CTM simulations of CO2 and CO columns using different assimilated meteorological data sets for the same meteorological year) and a paired-forecast method (comparing 48- vs. 24-h GEOS-5 CTM forecasts of CO2 and CO columns for the same forecast time). We find strong error correlations (r2>0.5) between CO2 and CO columns over much of the extra-tropical Northern Hemisphere throughout the year, and strong consistency between different methods to estimate the error correlation. Application of the averaging kernels used in the retrieval for thermal IR CO measurements weakens the correlation coefficients by 15% on average (mostly due to variability in the averaging kernels) but preserves the large-scale correlation structure. We present a simple inverse modeling application to demonstrate that CO2-CO error correlations can indeed significantly reduce uncertainty on surface carbon fluxes in a joint CO2-CO inversion vs. a CO2-only inversion.Earth and Planetary SciencesEngineering and Applied Science

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

International audienceWe 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

Detection and Attribution of Wildfire Pollution in the Arctic

The Arctic experiences poor air quality due to transport of pollutants from mid-latitudes, with wildfires providing an episodic source of trace gases and particulates. We present a multi-year time series of the total columns of CO, HCN, and C2H6 measured using Fourier transform infrared spectrometers at ten sites affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Six are high-latitude sites: Eureka, Ny Alesund, Thule, Kiruna, Poker Flat, and St. Petersburg, and four are mid-latitude sites: Zugspitze, Jungfraujoch, Toronto, and Rikubetsu. For each site, the inter-annual trends and seasonal variabilities of the CO total column time series are accounted for, allowing ambient concentrations to be determined. Enhancements above ambient levels are then used to identify possible wildfire pollution events. Since the abundance of each trace gas emitted in a wildfire event is specific to the type of vegetation burned and the burning phase, correlations of CO to the long-lived wildfire tracers HCN and C2H6 allow for further confirmation of the detection of wildfire pollution, while complementary measurements of aerosol optical depth from nearby AERONET sites confirms the presence of wildfire smoke. GEOS-Chem tagged CO simulations with Global Fire Assimilation System (GFAS) biomass burning emissions were used to determine the source attribution of CO concentrations at each site from 2003-2017. The influence of the various wildfire sources is found to differ between sites; however, North American and Eurasian boreal wildfires fires are found to be the greatest contributors to episodic CO enhancements in the summertime at all sites

Detection of wildfire pollution in the Arctic using a network of FTIR spectrometers and GEOS-Chem

Ground-based FTIR instruments provide simultaneous measurements of CO, HCN and C2H6 at high-latitudes. Detection of CO enhancements and strong correlations with HCN and C2H6 are indicative of wildfire pollution events. The GEOS-Chem tagged CO simulation provides attribution of CO sources to FTIR measurements from 2003-2017. At all FTIR sites, wildfire pollution events are detected annually and attributed to Boreal wildfires in North America and Asia

The Influence of Biomass Burning on the Arctic: Pan-Arctic FTIR Observations and Model Results

International audienceTransport of biomass burning emissions into the Arctic can cause episodic enhancements of multiple trace gas species. We present a multi-year time series of the total columns of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6) measured using Fourier Transform Infrared (FTIR) solar absorption spectroscopy at six high-latitude sites: Eureka, Nunavut; Ny Alesund, Norway; Thule, Greenland; Kiruna, Sweden; Poker Flat, Alaska; and St. Petersburg, Russia, and at three mid-latitude sites; Zugspitze, Germany; Jungfraujoch, Switzerland; and Toronto, Ontario. For each site, the inter-annual trends and seasonal variabilities of the CO total column time series are determined and enhancements above ambient levels are used to identify possible wildfire pollution events. Correlations of HCN and C2H6 with CO, back-trajectories from HYSPLIT and FLEXPART, and fire locations from the Moderate Resolution Spectroradiometer (MODIS) confirm the detections and identify the source regions. The GEOS-Chem chemical transport model is run in tagged mode to determine the relative contributions to the observed enhancements from continental-scale biomass burning source regions.Exceptional emissions of CO, HCN, C2H6, and ammonia (NH3) from the 2017 North American wildfires were measured at Eureka and Thule, indicating that wildfires may be a major source of NH3 in the summertime high Arctic. The enhancement ratios of the long- lived species HCN and C2H6 are found to be comparable between sites, but for NH3, the enhancement ratios are strongly dependent on the transport patterns of the smoke plumes. Satellite measurements of NH3 from the Infrared Atmospheric Sounding Instrument (IASI) and Cross-track Infrared Sounder (CrIS) are used to examine the spatial and temporal variabilities of NH3. Comparisons to a high-resolution (0.25° x 0.3125°) nested run of GEOS-Chem using emissions from the Global Fire Assimilation System (GFAS) are performed to evaluate the emission inventories and assess the long-range transport of NH3 to the high Arctic