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Abstract:
We have performed high-precision measurements of the 18O and position dependent 15N isotopic composition of N2O from Antarctic firn air samples. By comparing these data to simulations carried out with a firn air diffusion model, we have reconstructed the temporal evolution of the N2O isotope signatures since pre-industrial times. The heavy isotope content of atmospheric N2O is presently decreasing for all signatures at rates of about -0.038‰ yr -1 for 1δ15N, -0.046‰ yr -1 for 2δ15N and -0.025‰ yr -1 for δ18O. The total decrease since pre-industrial times is estimated to be about -1.8‰ for 1δ15N at both positions and -2.2‰ for 2δ15N. Isotope budget calculations using these trends and recent stratospheric measurements allow to isotopically characterize the present and the pre-industrial global average N2O source, as well as the additional N2O emissions that have caused the global N2O increase since pre-industrial times. The increased fluxes from the depleted surface sources alone are insufficient to explain the inferred temporal isotope changes. In addition, the global average N2O source signature is calculated to be significantly depleted today relative to the pre-industrial value, in agreement with recent indications from soil emission measurements.
