Assessing fossil fuel CO₂ emissions in California using atmospheric observations and models

Analysis systems incorporating atmospheric observations could provide a powerful tool for validating fossil fuel CO2 (ffCO2) emissions reported for individual regions, provided that fossil fuel sources can be separated from other CO2 sources or sinks and atmospheric transport can be accurately accounted for. We quantified ffCO2 by measuring radiocarbon (14C) in CO2, an accurate fossil-carbon tracer, at nine observation sites in California for three months in 2014–15. There is strong agreement between the measurements and ffCO2 simulated using a high-resolution atmospheric model and a spatiotemporally-resolved fossil fuel flux estimate. Inverse estimates of total in-state ffCO2 emissions are consistent with the California Air Resources Board's reported ffCO2 emissions, providing tentative validation of California's reported ffCO2 emissions in 2014–15. Continuing this prototype analysis system could provide critical independent evaluation of reported ffCO2 emissions and emissions reductions in California, and the system could be expanded to other, more data-poor regions

Roadmap on dynamics of molecules and clusters in the gas phase

This roadmap article highlights recent advances, challenges and future prospects in studies of the dynamics of molecules and clusters in the gas phase. It comprises nineteen contributions by scientists with leading expertise in complementary experimental and theoretical techniques to probe the dynamics on timescales spanning twenty order of magnitudes, from attoseconds to minutes and beyond, and for systems ranging in complexity from the smallest (diatomic) molecules to clusters and nanoparticles. Combining some of these techniques opens up new avenues to unravel hitherto unexplored reaction pathways and mechanisms, and to establish their significance in, e.g. radiotherapy and radiation damage on the nanoscale, astrophysics, astrochemistry and atmospheric science

Eddy covariance fluxes and vertical concentration gradient measurements of NO and NO2 over a ponderosa pine ecosystem: Observational evidence for within-canopy chemical removal of NOx

Exchange of NOx (NO+NO2) between the atmosphere and biosphere is important for air quality, climate change, and ecosystem nutrient dynamics. There are few direct ecosystem-scale measurements of the direction and rate of atmosphere-biosphere exchange of NOx. As a result, a complete description of the processes affecting NOx following emission from soils and/or plants as they transit from within the plant/forest canopy to the free atmosphere remains poorly constrained and debated. Here, we describe measurements of NO and NO2 fluxes and vertical concentration gradients made during the Biosphere Effects on AeRosols and Photochemistry EXperiment 2009. In general, during daytime we observe upward fluxes of NO and NO2 with counter-gradient fluxes of NO. We find that NOx fluxes from the forest canopy are smaller than calculated using observed flux-gradient relationships for conserved tracers and also smaller than measured soil NO emissions. We interpret these differences as primarily due to chemistry converting NOx to higher nitrogen oxides within the forest canopy, which might be part of a mechanistic explanation for the "canopy reduction factor" applied to soil NOx emissions in large-scale models. © 2014 Author(s)