Global CO_2 fluxes inferred from surface air-sample measurements and from TCCON retrievals of the CO_2 total column

We present the first estimate of the global distribution of CO_2 surface fluxes from 14 stations of the Total Carbon Column Observing Network (TCCON). The evaluation of this inversion is based on 1) comparison with the fluxes from a classical inversion of surface air-sample-measurements, and 2) comparison of CO_2 mixing ratios calculated from the inverted fluxes with independent aircraft measurements made during the two years analyzed here, 2009 and 2010. The former test shows similar seasonal cycles in the northern hemisphere and consistent regional carbon budgets between inversions from the two datasets, even though the TCCON inversion appears to be less precise than the classical inversion. The latter test confirms that the TCCON inversion has improved the quality (i.e., reduced the uncertainty) of the surface fluxes compared to the assumed or prior fluxes. The consistency between the surface-air-sample-based and the TCCON-based inversions despite remaining flaws in transport models opens the possibility of increased accuracy and robustness of flux inversions based on the combination of both data sources and confirms the usefulness of space-borne monitoring of the CO_2 column

Improvement of the retrieval algorithm for GOSAT SWIR XCO_2 and XCH_4 and their validation using TCCON data

The column-averaged dry-air mole fractions of carbon dioxide and methane (XCO_2 and XCH_4) have been retrieved from Greenhouse gases Observing SATellite (GOSAT) Short-Wavelength InfraRed (SWIR) observations and released as a SWIR L2 product from the National Institute for Environmental Studies (NIES). XCO_2 and XCH_4 retrieved using the version 01.xx retrieval algorithm showed large negative biases and standard deviations (−8.85 and 4.75 ppm for XCO_2 and −20.4 and 18.9 ppb for XCH_4, respectively) compared with data of the Total Carbon Column Observing Network (TCCON). Multiple reasons for these error characteristics (e.g., solar irradiance database, handling of aerosol scattering) are identified and corrected in a revised version of the retrieval algorithm (version 02.xx). The improved retrieval algorithm shows much smaller biases and standard deviations (−1.48 and 2.09 ppm for XCO_2 and −5.9 and 12.6 ppb for XCH_4, respectively) than the version 01.xx. Also, the number of post-screened measurements is increased, especially at northern mid- and high-latitudinal areas

Towards constraints on fossil fuel emissions from total column carbon dioxide

We assess the large-scale, top-down constraints on regional fossil fuel emissions provided by observations of atmospheric total column CO_2, X_CO_2. Using an atmospheric general circulation model (GCM) with underlying fossil emissions, we determine the influence of regional fossil fuel emissions on global X_CO_2 fields. We quantify the regional contrasts between source and upwind regions and probe the sensitivity of atmospheric X_CO_2 to changes in fossil fuel emissions. Regional fossil fuel X_CO_2 contrasts can exceed 0.7 ppm based on 2007 emission estimates, but have large seasonal variations due to biospheric fluxes. Contamination by clouds reduces the discernible fossil signatures. Nevertheless, our simulations show that atmospheric fossil X_CO_2 can be tied to its source region and that changes in the regional X_CO_2 contrasts scale linearly with emissions. We test the GCM results against X_CO_2 data from the GOSAT satellite. Regional X_CO_2 contrasts in GOSAT data generally scale with the predictions from the GCM, but the comparison is limited by the moderate precision of and relatively few observations from the satellite. We discuss how this approach may be useful as a policy tool to verify national fossil emissions, as it provides an independent, observational constraint

Balloon-borne radiometer measurement of Northern Hemisphere mid-latitude stratospheric HNO3 profiles spanning 12 years

Low-resolution atmospheric thermal emission spectra collected by balloon-borne radiometers over the time span of 1990–2002 are used to retrieve vertical profiles of HNO3, CFC-11 and CFC-12 volume mixing ratios between approximately 10 and 35 km altitude. All of the data analyzed have been collected from launches from a Northern Hemisphere mid-latitude site, during late summer, when stratospheric dynamic variability is at a minimum. The retrieval technique incorporates detailed forward modeling of the instrument and the radiative properties of the atmosphere, and obtains a best fit between modeled and measured spectra through a combination of onion-peeling and global optimization steps. The retrieved HNO3 profiles are consistent over the 12-year period, and are consistent with recent measurements by the Atmospheric Chemistry Experiment-Fourier transform spectrometer satellite instrument. This suggests that, to within the errors of the 1990 measurements, there has been no significant change in the HNO3 summer mid-latitude profile

The ACOS CO_2 retrieval algorithm – Part II: Global X_(CO_2) data characterization

Here, we report preliminary estimates of the column averaged carbon dioxide (CO_2) dry air mole fraction, X_(CO_2), retrieved from spectra recorded over land by the Greenhouse gases Observing Satellite, GOSAT (nicknamed "Ibuki"), using retrieval methods originally developed for the NASA Orbiting Carbon Observatory (OCO) mission. After screening for clouds and other known error sources, these retrievals reproduce much of the expected structure in the global X_(CO_2) field, including its variation with latitude and season. However, low yields of retrieved X_(CO_2) over persistently cloudy areas and ice covered surfaces at high latitudes limit the coverage of some geographic regions, even on seasonal time scales. Comparisons of early GOSAT X_(CO_2) retrievals with X_(CO_2) estimates from the Total Carbon Column Observing Network (TCCON) revealed a global, −2% (7–8 parts per million, ppm, with respect to dry air) X_(CO_2) bias and 2 to 3 times more variance in the GOSAT retrievals. About half of the global X_(CO_2) bias is associated with a systematic, 1% overestimate in the retrieved air mass, first identified as a global +10 hPa bias in the retrieved surface pressure. This error has been attributed to errors in the O_2 A-band absorption cross sections. Much of the remaining bias and spurious variance in the GOSAT X_(CO_2) retrievals has been traced to uncertainties in the instrument's calibration, oversimplified methods for generating O_2 and CO_2 absorption cross sections, and other subtle errors in the implementation of the retrieval algorithm. Many of these deficiencies have been addressed in the most recent version (Build 2.9) of the retrieval algorithm, which produces negligible bias in X_(CO_2) on global scales as well as a ~30% reduction in variance. Comparisons with TCCON measurements indicate that regional scale biases remain, but these could be reduced by applying empirical corrections like those described by Wunch et al. (2011b). We recommend that such corrections be applied before these data are used in source sink inversion studies to minimize spurious fluxes associated with known biases. These and other lessons learned from the analysis of GOSAT data are expected to accelerate the delivery of high quality data products from the Orbiting Carbon Observatory-2 (OCO-2), once that satellite is successfully launched and inserted into orbit

Emissions of greenhouse gases from a North American megacity

Atmospheric column abundances of carbon dioxide (CO_2), carbon monoxide (CO), methane (CH_4) and nitrous oxide (N_2O) have been measured above the South Coast air basin (SCB), a densely populated urban region of Southern California, USA, which includes Los Angeles and the surrounding suburbs. Large diurnal variations in CO and CH_4 are observed which correlate well with those in CO_2. Weaker correlations are seen between N_2O and CO_2, with large uncertainties. We compute yearly SCB emissions of CO and CH_4 to be 1.4 ± 0.3 Tg CO and 0.6 ± 0.1 Tg CH_4. We compare our calculated emissions to the California Air Resources Board (CARB) and the Emission Database for Global Atmospheric Research (EDGAR) estimates. Our measurements confirm that urban emissions are a significant source of CH_4 and in fact may be substantially higher than currently estimated. If our emissions are typical of other urban centers, these findings suggest that urban emissions could contribute 7–15% to the global anthropogenic budget of methane

Derivation of tropospheric methane from TCCON CH₄ and HF total column observations

The Total Carbon Column Observing Network (TCCON) is a global ground-based network of Fourier transform spectrometers that produce precise measurements of column-averaged dry-air mole fractions of atmospheric methane (CH₄). Temporal variability in the total column of CH₄ due to stratospheric dynamics obscures fluctuations and trends driven by tropospheric transport and local surface fluxes that are critical for understanding CH₄ sources and sinks. We reduce the contribution of stratospheric variability from the total column average by subtracting an estimate of the stratospheric CH₄ derived from simultaneous measurements of hydrogen fluoride (HF). HF provides a proxy for stratospheric CH₄ because it is strongly correlated to CH₄ in the stratosphere, has an accurately known tropospheric abundance (of zero), and is measured at most TCCON stations. The stratospheric partial column of CH₄ is calculated as a function of the zonal and annual trends in the relationship between CH₄ and HF in the stratosphere, which we determine from ACE-FTS satellite data. We also explicitly take into account the CH₄ column averaging kernel to estimate the contribution of stratospheric CH₄ to the total column. The resulting tropospheric CH₄ columns are consistent with in situ aircraft measurements and augment existing observations in the troposphere

Intercomparison of ground-based ozone and NO2 measurements during the MANTRA 2004 campaign

The MANTRA (Middle Atmosphere Nitrogen TRend Assessment) 2004 campaign took place in Vanscoy, Saskatchewan, Canada (52° N, 107° W) from 3 August to 15 September, 2004. In support of the main balloon launch, a suite of five zenith-sky and direct-Sun-viewing UV-visible ground-based spectrometers was deployed, primarily measuring ozone and NO2 total columns. Three Fourier transform spectrometers (FTSs) that were part of the balloon payload also performed ground-based measurements of several species, including ozone. Ground-based measurements of ozone and NO2 differential slant column densities from the zenith-viewing UV-visible instruments are presented herein. They are found to partially agree within NDACC (Network for the Detection of Atmospheric Composition Change) standards for instruments certified for process studies and satellite validation. Vertical column densities of ozone from the zenith-sky UV-visible instruments, the FTSs, a Brewer spectrophotometer, and ozonesondes are compared, and found to agree within the combined error estimates of the instruments (15%). NO2 vertical column densities from two of the UV-visible instruments are compared, and are also found to agree within combined error (15%)