We have developed an automated observatory for measuring atmospheric column abundances of CO2 and O2 using near‐infrared spectra of the Sun obtained with a high spectral resolution Fourier Transform ...Spectrometer (FTS). This is the first dedicated laboratory in a new network of ground‐based observatories named the Total Carbon Column Observing Network. This network will be used for carbon cycle studies and validation of spaceborne column measurements of greenhouse gases. The observatory was assembled in Pasadena, California, and then permanently deployed to northern Wisconsin during May 2004. It is located in the heavily forested Chequamegon National Forest at the WLEF Tall Tower site, 12 km east of Park Falls, Wisconsin. Under clear sky conditions, ∼0.1% measurement precision is demonstrated for the retrieved column CO2 abundances. During the Intercontinental Chemical Transport Experiment–North America and CO2 Boundary Layer Regional Airborne Experiment campaigns in summer 2004, the DC‐8 and King Air aircraft recorded eight in situ CO2 profiles over the WLEF site. Comparison of the integrated aircraft profiles and CO2 column abundances shows a small bias (∼2%) but an excellent correlation.
We retrieved column‐averaged dry air mole fractions of atmospheric carbon dioxide () from backscattered short‐wave infrared (SWIR) sunlight measured by the Japanese Greenhouse gases Observing ...SATellite (GOSAT). Over two years of retrieved from GOSAT is compared with inferred from collocated SWIR measurements by seven ground‐based Total Carbon Column Observing Network (TCCON) stations. The average difference between GOSAT and TCCON for individual TCCON sites ranges from −0.87 ppm to 0.77 ppm with a mean value of 0.1 ppm and standard deviation of 0.56 ppm. We find an average bias between all GOSAT and TCCON retrievals of −0.20 ppm with a standard deviation of 2.26 ppm and a correlation coefficient of 0.75. One year of was retrieved from GOSAT globally, which was compared to global 3‐D GEOS‐Chem chemistry transport model calculations. We find that the latitudinal gradient, seasonal cycles, and spatial variability of GOSAT and GEOS‐Chem agree well in general with a correlation coefficient of 0.61. Regional differences between GEOS‐Chem model calculations and GOSAT observations are typically less than 1 ppm except for the Sahara and central Asia where a mean difference between 2 to 3 ppm is observed, indicating regional biases in the GOSAT retrievals unobserved by the current TCCON network. Using a bias correction scheme based on linear regression these regional biases are significantly reduced, approaching the required accuracy for surface flux inversions.
Key Points
Bias and precision should be sufficient to allow improved surface flux estimates
Globally, regional differences are found to be small, except over desert regions
Retrievals should be useful for the inversion of CO2 surface fluxes
We compare two conceptually different methods for determining methane column‐averaged mixing ratios from Greenhouse Gases Observing Satellite (GOSAT) shortwave infrared (SWIR) measurements. These ...methods account differently for light scattering by aerosol and cirrus. The proxy method retrieves a CO2 column which, in conjunction with prior knowledge on CO2acts as a proxy for scattering effects. The physics‐based method accounts for scattering by retrieving three effective parameters of a scattering layer. Both retrievals are validated on a 19‐month data set using ground‐based at 12 stations of the Total Carbon Column Observing Network (TCCON), showing comparable performance: for the proxy retrieval we find station‐dependent retrieval biases from −0.312% to 0.421% of a standard deviation of 0.22% and a typical precision of 17 ppb. The physics method shows biases between −0.836% and −0.081% with a standard deviation of 0.24% and a precision similar to the proxy method. Complementing this validation we compared both retrievals with simulated methane fields from a global chemistry‐transport model. This identified shortcomings of both retrievals causing biases of up to 1ings and provide a satisfying validation of any methane retrieval from space‐borne SWIR measurements, in our opinion it is essential to further expand the network of TCCON stations.
Key Points
Shortcomings of current methane retrieval algorithms are identified
For a satisfying algorithm validation the TCCON should be expanded
The Orbiting Carbon Observatory-2 (OCO-2), launched on 2 July 2014, is a NASA mission designed to measure the column-averaged CO2 dry air mole fraction, XCO2. Towards that goal, it will collect ...spectra of reflected sunlight in narrow spectral ranges centered at 0.76, 1.6 and 2.0 μm with a resolving power (λ/Δ λ) of 20 000. These spectra will be used in an optimal estimation framework to retrieve XCO2. About 100 000 cloud free soundings of XCO2 each day will allow estimates of net CO2 fluxes on regional to continental scales to be determined. Here, we evaluate the OCO-2 spectrometer performance using pre-launch data acquired during instrument thermal vacuum tests in April 2012. A heliostat and a diffuser plate were used to feed direct sunlight into the OCO-2 instrument and spectra were recorded. These spectra were compared to those collected concurrently from a nearby high-resolution Fourier Transform Spectrometer that was part of the Total Carbon Column Observing Network (TCCON). Using the launch-ready OCO-2 calibration and spectroscopic parameters, we performed total column scaling fits to all spectral bands and compared these to TCCON results. On 20 April, we detected a CO2 plume from the Los Angeles basin at the JPL site with strongly enhanced short-term variability on the order of 1% (3–4 ppm). We also found good (< 0.5 ppm) inter-footprint consistency in retrieved XCO2. The variations in spectral fitting residuals are consistent with signal-to-noise estimates from instrument calibration, while average residuals are systematic and mostly attributable to remaining errors in our knowledge of the CO2 and O2 spectroscopic parameters. A few remaining inconsistencies observed during the tests may be attributable to the specific instrument setup on the ground and will be re-evaluated with in-orbit data.
New observations of the vertically integrated CO2 mixing ratio, ⟨CO2⟩, from ground-based remote sensing show that variations in CO2⟩ are primarily determined by large-scale flux patterns. They ...therefore provide fundamentally different information than observations made within the boundary layer, which reflect the combined influence of large-scale and local fluxes. Observations of both ⟨CO2⟩ and CO2 concentrations in the free troposphere show that large-scale spatial gradients induce synoptic-scale temporal variations in ⟨CO2⟩ in the Northern Hemisphere midlatitudes through horizontal advection. Rather than obscure the signature of surface fluxes on atmospheric CO2, these synoptic-scale variations provide useful information that can be used to reveal the meridional flux distribution. We estimate the meridional gradient in ⟨CO2⟩ from covariations in ⟨CO2⟩ and potential temperature, θ, a dynamical tracer, on synoptic timescales to evaluate surface flux estimates commonly used in carbon cycle models. We find that simulations using Carnegie Ames Stanford Approach (CASA) biospheric fluxes underestimate both the ⟨CO2⟩ seasonal cycle amplitude throughout the Northern Hemisphere midlatitudes and the meridional gradient during the growing season. Simulations using CASA net ecosystem exchange (NEE) with increased and phase-shifted boreal fluxes better fit the observations. Our simulations suggest that climatological mean CASA fluxes underestimate boreal growing season NEE (between 45–65° N) by ~40%. We describe the implications for this large seasonal exchange on inference of the net Northern Hemisphere terrestrial carbon sink.
The Total Carbon Column Observing Network (TCCON) produces precise measurements of the column average dry-air mole fractions of CO2, CO, CH4, N2O and H2O at a variety of sites worldwide. These ...observations rely on spectroscopic parameters that are not known with sufficient accuracy to compute total columns that can be used in combination with in situ measurements. The TCCON must therefore be calibrated to World Meteorological Organization (WMO) in situ trace gas measurement scales. We present a calibration of TCCON data using WMO-scale instrumentation aboard aircraft that measured profiles over four TCCON stations during 2008 and 2009. These calibrations are compared with similar observations made in 2004 and 2006. The results indicate that a single, global calibration factor for each gas accurately captures the TCCON total column data within error.
Inadequate treatment of aerosol scattering can be a significant source of error when retrieving column‐averaged dry‐air mole fractions of CO2 (XCO2) from space‐based measurements of backscattered ...solar shortwave radiation. We have developed a retrieval algorithm, RemoTeC, that retrieves three aerosol parameters (amount, size, and height) simultaneously with XCO2. Here we evaluate the ability of RemoTeC to account for light path modifications by clouds, subvisual cirrus, and aerosols when retrieving XCO2 from Greenhouse Gases Observing Satellite (GOSAT) Thermal and Near‐infrared Sensor for carbon Observation (TANSO)‐Fourier Transform Spectrometer (FTS) measurements. We first evaluate a cloud filter based on measurements from the Cloud and Aerosol Imager and a cirrus filter that uses radiances measured by TANSO‐FTS in the 2 micron spectral region, with strong water absorption. For the cloud‐screened scenes, we then evaluate errors due to aerosols. We find that RemoTeC is well capable of accounting for scattering by aerosols for values of aerosol optical thickness at 750 nm up to 0.25. While no significant correlation of errors is found with albedo, correlations are found with retrieved aerosol parameters. To further improve the XCO2 accuracy, we propose and evaluate a bias correction scheme.
Measurements from 12 ground‐based stations of the Total Carbon Column Observing Network (TCCON) are used as a reference in this study. We show that spatial colocation criteria may be relaxed using additional constraints based on modeled XCO2 gradients, to increase the size and diversity of validation data and provide a more robust evaluation of GOSAT retrievals. Global‐scale validation of satellite data remains challenging and would be improved by increasing TCCON coverage.
Key Points
Errors due to clouds and aerosols are evaluated in full physics XCO2 retrievals
A bias correction is tested to improve regional accuracy of RemoTeC retrievals
Two co‐location methods are evaluated for validation of satellite retrievals
Methane emissions inventories for Southern California's South Coast Air Basin (SoCAB) have underestimated emissions from atmospheric measurements. To provide insight into the sources of the ...discrepancy, we analyze records of atmospheric trace gas total column abundances in the SoCAB starting in the late 1980s to produce annual estimates of the ethane emissions from 1989 to 2015 and methane emissions from 2007 to 2015. The first decade of measurements shows a rapid decline in ethane emissions coincident with decreasing natural gas and crude oil production in the basin. Between 2010 and 2015, however, ethane emissions have grown gradually from about 13 ± 5 to about 23 ± 3 Gg yr−1, despite the steady production of natural gas and oil over that time period. The methane emissions record begins with 1 year of measurements in 2007 and continuous measurements from 2011 to 2016 and shows little trend over time, with an average emission rate of 413 ± 86 Gg yr−1. Since 2012, ethane to methane ratios in the natural gas withdrawn from a storage facility within the SoCAB have been increasing by 0.62 ± 0.05 % yr−1, consistent with the ratios measured in the delivered gas. Our atmospheric measurements also show an increase in these ratios but with a slope of 0.36 ± 0.08 % yr−1, or 58 ± 13 % of the slope calculated from the withdrawn gas. From this, we infer that more than half of the excess methane in the SoCAB between 2012 and 2015 is attributable to losses from the natural gas infrastructure.
The Los Angeles basin is a significant anthropogenic source of major greenhouse gases (CO2 and CH4) and the pollutant CO, contributing significantly to regional and global climate change. We present ...a novel approach for monitoring the spatial and temporal distributions of greenhouse gases in the Los Angeles basin using a high-resolution spectroscopic remote sensing technique. A new Fourier transform spectrometer called CLARS-FTS has been deployed since May, 2010, at Jet Propulsion Laboratory (JPL)'s California Laboratory for Atmospheric Remote Sensing (CLARS) on Mt. Wilson, California, for automated long-term measurements of greenhouse gases. The instrument design and performance of CLARS-FTS are presented. From its mountaintop location at an altitude of 1673 m, the instrument points at a programmed sequence of ground target locations in the Los Angeles basin, recording spectra of reflected near-IR solar radiation. Column-averaged dry-air mole fractions of greenhouse gases (XGHG) including XCO2, XCH4, and XCO are retrieved several times per day for each target. Spectra from a local Spectralon® scattering plate are also recorded to determine background (free tropospheric) column abundances above the site. Comparisons between measurements from LA basin targets and the Spectralon® plate provide estimates of the boundary layer partial column abundances of the measured species. Algorithms are described for transforming the measured interferograms into spectra, and for deriving column abundances from the spectra along with estimates of the measurement precision and accuracy. The CLARS GHG measurements provide a means to infer relative, and possibly absolute, GHG emissions.
Long‐term time series of hydrogen chloride (HCl) and chlorine nitrate (ClONO2) total column abundances has been retrieved from high spectral resolution ground‐based solar absorption spectra recorded ...with infrared Fourier transform spectrometers at nine NDSC (Network for the Detection of Stratospheric Change) sites in both Northern and Southern Hemispheres. The data sets span up to 24 years and most extend until the end of 2001. The time series of Cly (defined here as the sum of the HCl and ClONO2 columns) from the three locations with the longest time‐span records show rapid increases until the early 1990s superimposed on marked day‐to‐day, seasonal and inter‐annual variability. Subsequently, the buildup in Cly slows and reaches a broad plateau after 1996, also characterized by variability. A similar time evolution is also found in the total chlorine concentration at 55 km altitude derived from Halogen Occultation Experiment (HALOE) global observations since 1991. The stabilization of inorganic chlorine observed in both the total columns and at 55 km altitude indicates that the near‐global 1993 organic chlorine (CCly) peak at the Earth's surface has now propagated over a broad altitude range in the upper atmosphere, though the time lag is difficult to quantify precisely from the current data sets, due to variability. We compare the three longest measured time series with two‐dimensional model calculations extending from 1977 to 2010, based on a halocarbon scenario that assumes past measured trends and a realistic extrapolation into the future. The model predicts broad Cly maxima consistent with the long‐term observations, followed by a slow Cly decline reaching 12–14% relative to the peak by 2010. The data reported here confirm the effectiveness of the Montreal Protocol and its Amendments and Adjustments in progressively phasing out the major man‐related perturbations of the stratospheric ozone layer, in particular, the anthropogenic chlorine‐bearing source gases.
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