An intercomparison of total column-averaged nitrous oxide between ground-based FTIR TCCON and NDACC measurements at seven sites and comparisons with the GEOS-Chem model

Minqiang Zhou, Bavo Langerock, Kelley C. Wells, Dylan B. Millet, Corinne Vigouroux, Mahesh Kumar Sha, Christian Hermans, Jean Marc Metzger, Rigel Kivi, Pauli Heikkinen, Dan Smale, David F. Pollard, Nicholas Jones, Nicholas M. Deutscher, Thomas Blumenstock, Matthias Schneider, Mathias Palm, Justus Notholt, James W. Hannigan, Martine De Mazière

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Abstract

Nitrous oxide (N 2 O) is an important greenhouse gas and it can also generate nitric oxide, which depletes ozone in the stratosphere. It is a common target species of ground-based Fourier transform infrared (FTIR) nearinfrared (TCCON) and mid-infrared (NDACC) measurements. Both TCCON and NDACC networks provide a longterm global distribution of atmospheric N 2 O mole fraction. In this study, the dry-air column-averaged mole fractions of N 2 O (XN 2 O) from the TCCON and NDACC measurements are compared against each other at seven sites around the world (Ny-Ålesund, Sodankylä, Bremen, Izaña, Réunion, Wollongong, Lauder) in the time period of 2007–2017. The mean differences in XN 2 O between TCCON and NDACC (NDACC–TCCON) at these sites are between -3:32 and 1.37 ppb (-1:1 %–0.5 %) with standard deviations between 1.69 and 5.01 ppb (0.5 %–1.6 %), which are within the uncertainties of the two datasets. The NDACC N 2 O retrieval has good sensitivity throughout the troposphere and stratosphere, while the TCCON retrieval underestimates a deviation from the a priori in the troposphere and overestimates it in the stratosphere. As a result, the TCCON XN 2 O measurement is strongly affected by its a priori profile. Trends and seasonal cycles of XN 2 O are derived from the TCCON and NDACC measurements and the nearby surface flask sample measurements and compared with the results from GEOS-Chem model a priori and a posteriori simulations. The trends and seasonal cycles from FTIR measurement at Ny-Ålesund and Sodankylä are strongly affected by the polar winter and the polar vortex. The a posteriori N 2 O fluxes in the model are optimized based on surface N 2 O measurements with a 4D-Var inversion method. The XN 2 O trends from the GEOS-Chem a posteriori simulation (0:97-0:02 (1) ppb yr-1) are close to those from the NDACC (0:93- 0:04 ppb yr-1) and the surface flask sample measurements (0:93-0:02 ppb yr-1). The XN 2 O trend from the TCCON measurements is slightly lower (0:81-0:04 ppb yr-1) due to the underestimation of the trend in TCCON a priori simulation. The XN 2 O trends from the GEOS-Chem a priori simulation are about 1.25 ppb yr-1, and our study confirms that the N 2 O fluxes from the a priori inventories are overestimated. The seasonal cycles of XN 2 O from the FTIR measurements and the model simulations are close to each other in the Northern Hemisphere with a maximum in August–October and a minimum in February–April. However, in the Southern Hemisphere, the modeled XN 2 O values show a minimum in February–April while the FTIR XN 2 O retrievals show different patterns. By comparing the partial column-averaged N 2 O from the model and NDACC for three vertical ranges (surface–8, 8–17, 17–50 km), we find that the discrepancy in the XN 2 O seasonal cycle between the model simulations and the FTIR measurements in the Southern Hemisphere is mainly due to their stratospheric differences.

Original languageEnglish (US)
Pages (from-to)1393-1408
Number of pages16
JournalAtmospheric Measurement Techniques
Volume12
Issue number2
DOIs
StatePublished - 2019

Bibliographical note

Funding Information:
Acknowledgements. Minqiang Zhou is supported by the Belgian complementary researchers program. We would like to thank TCCON and NDACC networks for making the data publicly available. The FTIR sites at Réunion are operated by the BIRA-IASB and locally supported by LACy/UMR8105, Université de La Réunion. We would like to thank Nicolas Kumps, Bart Dils and Francis Scolas (BIRA-IASB) for their contributions to the FTIR measurement maintenance and Edward Dlugokencky (NOAA) for sharing the flask sample measurements. Development of the GEOS-Chem N2O simulation was supported by NOAA (grant no. NA13OAR4310086) and the Minnesota Supercomputing Institute. The Lauder FTIR measurements are core funded by NIWA from New Zealand’s Ministry of Business, Innovation and Employment. Wollongong TCCON and NDACC measurements are supported by the Australian Research Council, grants DP160101598, DP140101552, DP110103118, DP0879468 and LE0668470. The Réunion TCCON measurements are supported by Belgian Science Policy through contracts FR/35/IC1 to IC3.

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