Radiocarbon in CO2 (14CO2) measurements can aid in discriminating between fast (<1 year) and slower (>5–10 years) cycling of C between the atmosphere and the terrestrial biosphere due to the 14C disequilibrium between atmospheric and terrestrial C. However, 14CO2 in the atmosphere is typically much more strongly impacted by fossil fuel emissions of CO2, and, thus, observations often provide little additional constraints on respiratory flux estimates at regional scales. Here we describe a data set of 14CO2 observations from a tall tower in northern Wisconsin (USA) where fossil fuel influence is far enough removed that during the summer months, the biospheric component of the 14CO2 budget dominates. We find that the terrestrial biosphere is responsible for a significant contribution to 14CO2 that is 2–3 times higher than predicted by the Carnegie-Ames-Stanford approach terrestrial ecosystem model for observations made in 2010. This likely includes a substantial contribution from the North American boreal ecoregion, but transported biospheric emissions from outside the model domain cannot be ruled out. The 14CO2 enhancement also appears somewhat decreased in observations made over subsequent years, suggesting that 2010 may be anomalous. With these caveats acknowledged, we discuss the implications of the observation/model comparison in terms of possible systematic biases in the model versus short-term anomalies in the observations. Going forward, this isotopic signal could be exploited as an important indicator to better constrain both the long-term carbon balance of terrestrial ecosystems and the short-term impact of disturbance-based loss of carbon to the atmosphere.
In this project we have developed atmospheric measurement capabilities and a suite of atmospheric modeling and analysis tools that are well suited for verifying emissions of green- house gases (GHGs) on an urban-through-regional scale. We have for the first time applied the Community Multiscale Air Quality (CMAQ) model to simulate atmospheric CO2 . This will allow for the examination of regional-scale transport and distribution of CO2 along with air pollutants traditionally studied using CMAQ at relatively high spatial and temporal resolution with the goal of leveraging emissions verification efforts for both air quality and climate. We have developed a bias-enhanced Bayesian inference approach that can remedy the well-known problem of transport model errors in atmospheric CO2 inversions. We have tested the approach using data and model outputs from the TransCom3 global CO2 inversion comparison project. We have also performed two prototyping studies on inversion approaches in the generalized convection-diffusion context. One of these studies employed Polynomial Chaos Expansion to accelerate the evaluation of a regional transport model and enable efficient Markov Chain Monte Carlo sampling of the posterior for Bayesian inference. The other approach uses de- terministic inversion of a convection-diffusion-reaction system in the presence of uncertainty. These approaches should, in principle, be applicable to realistic atmospheric problems with moderate adaptation. We outline a regional greenhouse gas source inference system that integrates (1) two ap- proaches of atmospheric dispersion simulation and (2) a class of Bayesian inference and un- certainty quantification algorithms. We use two different and complementary approaches to simulate atmospheric dispersion. Specifically, we use a Eulerian chemical transport model CMAQ and a Lagrangian Particle Dispersion Model - FLEXPART-WRF. These two models share the same WRF assimilated meteorology fields, making it possible to perform a hybrid simulation, in which the Eulerian model (CMAQ) can be used to compute the initial condi- tion needed by the Lagrangian model, while the source-receptor relationships for a large state vector can be efficiently computed using the Lagrangian model in its backward mode. In ad- dition, CMAQ has a complete treatment of atmospheric chemistry of a suite of traditional air pollutants, many of which could help attribute GHGs from different sources. The inference of emissions sources using atmospheric observations is cast as a Bayesian model calibration problem, which is solved using a variety of Bayesian techniques, such as the bias-enhanced Bayesian inference algorithm, which accounts for the intrinsic model deficiency, Polynomial Chaos Expansion to accelerate model evaluation and Markov Chain Monte Carlo sampling, and Karhunen-Lo %60 eve (KL) Expansion to reduce the dimensionality of the state space. We have established an atmospheric measurement site in Livermore, CA and are collect- ing continuous measurements of CO2 , CH4 and other species that are typically co-emitted with these GHGs. Measurements of co-emitted species can assist in attributing the GHGs to different emissions sectors. Automatic calibrations using traceable standards are performed routinely for the gas-phase measurements. We are also collecting standard meteorological data at the Livermore site as well as planetary boundary height measurements using a ceilometer. The location of the measurement site is well suited to sample air transported between the San Francisco Bay area and the California Central Valley.