This report describes the design of atmospheric CO2 concentration measurements that, in combination with other measurements and models, would be used to quantify regionally distributed CO2 exchanges from California's terrestrial ecosystems and CO2 emissions from fossil fuel combustion. Using models of net ecosystem CO2 exchange (NEE), fossil fuel CO2 emissions, and regional meteorology, we predict CO2 concentration "signals" in the atmosphere. The predictions of NEE exhibit spatial and temporal variations that are controlled by land cover and climate. Fossil fuel CO2 emissions from metropolitan areas are the strongest localized sources of CO2 while weaker but spatially extensive fossil emissions are present throughout the Central Valley. We subdivide the CO2 sources into four components: NEE inside and outside CA, and fossil fuel CO2 inside and outside CA. Maps of predicted atmospheric CO2 concentration signals from these four sources largely mirror the instantaneous emissions near strong sources but plumes of CO2 enriched or depleted air are predicted to advect far from their sources. We then identify a baseline set of observing stations from existing and possible future sites that could be used to characterize in-state and out-of-state ecosystem and fossil fuel contributions to atmospheric CO2 concentrations. For each of the stations we calculate mean midday concentration signals with standard deviation for each month and source. We also calculate the covariance of the signal due to NEE inside CA with each of the other signals to quantify how much of the signal from NEE inside CA might be readily separable from the other signals. On the basis of these predictions, we identify new observing stations and a measurement protocol that, in combination with existing stations, would provide data to estimate NEE within CA. Although beyond the scope of this project, future work should estimate the uncertainties in estimating California's NEE that would be obtained using atmospheric concentration data from the stations identified herein.