The air-sea transfer of carbon dioxide can be viewed as a dynamical system through which atmospheric and oceanic processes push surface waters away from thermodynamic equilibrium, while diffusive gas transfer pulls them back towards local equilibrium. These push/pull processes drive significant sub-seasonal, seasonal, and interannual variability in air-sea carbon fluxes, the quantification of which is critical both for diagnosing the ocean response to fossil fuel emissions and for attempts to mitigate anthropogenic climate disruption through intentional modification of surface ocean biogeochemistry. In this study, we present a new approach for attributing air-sea carbon fluxes to specific mechanisms. The new framework is first applied to the two-box ocean nutrient and carbon cycle model as an illustrative example. Next, the outputs from a regional eddy-resolving model of the Southern Ocean are analyzed. The roles of multiple physical and biogeochemical processes are identified. Decomposition of the seasonal air-sea carbon flux shows the dominant role of biological carbon pumps that are partially compensated by the transport convergence. Finally, the framework is used to diagnose the response to mesoscale iron and alkalinity release, explicitly quantifying transport feedbacks and eventual impacts on net air-sea carbon flux. Ocean carbon transport have divergent influences between iron and alkalinity release, due to opposing near-surface gradients of dissolved inorganic carbon. More broadly, we suggest that our attribution framework may be a useful analytical technique for monitoring natural ocean carbon fluxes and quantifying the impacts of human intervention on the ocean carbon cycle.