Stratospheric Incursion as a Source of Enhancement of the Isotopic Ratios of Atmospheric N2O at Western Pacific

Abstract

Abstract We present analyses of nitrogen and oxygen isotopic ratios and site‐preference (SP) values of atmospheric nitrous oxide samples obtained from Taiwan in west Pacific. Air samples were collected during September 2013 to January 2016 from Taipei and during November 2011 to December 2014 from Keelung, located in the northeastern coast of Taiwan. The average values of δ15N, δ18O, and SP are 6.4 ± 0.3 ‰, 44.0 ± 0.4 ‰, and 17.1 ± 1.0 ‰, respectively, at Taipei and 6.4 ± 0.2 ‰, 44.6 ± 0.4 ‰, and 17.9 ± 1.3 ‰, for δ15N, δ18O, and SP respectively, at Keelung, comparable to the average values (6.6 ± 0.2, 44.2 ± 0.2, and 18.1 ± 0.5 ‰, scaled to year 2014) from Hateruma, an open ocean station in western Pacific. Strong temporal variations in the delta values, however, are seen. During a subtropical jet‐strengthening period in October to mid‐December 2014, the δ15N, δ18O and SP values increased at the rate of 0.006 ± 0.002 ‰/day, 0.010 ± 0.002 ‰/day and 0.008 ± 0.002 ‰/day, respectively at Taipei and 0.013 ± 0.005 ‰/day, 0.011 ± 0.005 ‰/day and 0.011 ± 0.027 ‰/day at Keelung. This suggests intrusion of air to the lower troposphere from the stratosphere where δ15N, δ18O and SP values are higher. This is consistent with earlier observations of oxygen isotope anomaly in atmospheric CO2 and elevated 35S in sulfate aerosols, indicating frequent stratospheric intrusions in this region. The observed δ15N and δ18O values, along with the oxygen isotope anomaly in CO2 and multiple sulfur isotopes in sulfate, can be used to constrain local emissions from the surface, improving our knowledge of anthropogenic contribution to the global budget of N2O.

Keywords

• Atmospheric N2O
• δ15N & δ18O
• site preference (SP)
• subtropical jet
• stratospheric intrusion
• potential vorticity (PV)