Abstract
South Asian air is among the most polluted in the world, causing premature death of millions and asserting a strong perturbation of the regional climate. A central component is carbon monoxide (CO), which is a key modulator of the oxidizing capacity of the atmosphere and a potent indirect greenhouse gas. While CO concentrations are declining elsewhere, South Asia exhibits an increasing trend for unresolved reasons. In this paper, we use dual-isotope (δ(13)C and δ(18)O) fingerprinting of CO intercepted in the South Asian outflow to constrain the relative contributions from primary and secondary CO sources. Results show that combustion-derived primary sources dominate the wintertime continental CO fingerprint (f(primary) ∼ 79 ± 4%), significantly higher than the global estimate (f(primary) ∼ 55 ± 5%). Satellite-based inventory estimates match isotope-constrained f(primary)-CO, suggesting observational convergence in source characterization and a prospect for model-observation reconciliation. This "ground-truthing" emphasizes the pressing need to mitigate incomplete combustion activities for climate/air quality benefits in South Asia.