First retrievals of peroxyacetyl nitrate (PAN) from ground-based FTIR solar spectra recorded at remote sites, comparison with model and satellite data

Emmanuel Mahieu (1) , Emily V. Fischer (2) , Bruno Franco (3) , Mathias Palm (4) , Tyler Wizenberg (5) , Dan Smale (6) , Lieven Clarisse (3) , Cathy Clerbaux (3, 7) , Pierre-François Coheur (3) , James W. Hannigan (8) , Erik Lutsch (5) , Justus Notholt (4) , Irene Pardo Cantos (1) , Maxime Prignon (1) , Christian Servais (1) , Kimberly Strong (5)

1 Institut d'Astrophysique et de Géophysique [Liège]
2 Department of Atmospheric Science [Fort Collins]
3 SQUARES - Spectroscopy, Quantum Chemistry and Atmospheric Remote Sensing
4 IUP - Institute of Environmental Physics [Bremen]
5 Department of Physics [Toronto]
6 NIWA - National Institute of Water and Atmospheric Research [Lauder]
7 TROPO - LATMOS
8 NCAR - National Center for Atmospheric Research [Boulder]

Peroxyacetyl nitrate (PAN) is the main tropospheric reservoir of NO x (NO þ NO 2). Its lifetime can reach several months in the upper cold troposphere. This enables the long-range transport of NO x radicals, under the form of PAN, far from the regions of emission. The subsequent release of NO x through the PAN thermal decomposition leads to the efficient formation of tropospheric ozone (O 3), with important consequences for tropospheric oxidative capacity and air quality. The chemical properties of PAN have stimulated the progressive development of remote-sensing products by the satellite community, and recent additions open the prospect for the production of decadal and near-global time series. These products will provide new constraints on the distribution and evolution of this key trace gas in the Earth's atmosphere, but they will also require reliable measurements for validation and characterization of performance. We present an approach that has been developed to retrieve PAN total columns from ground-based high-resolution solar absorption Fourier transform infrared (FTIR) spectra. This strategy is applied to observations recorded at remote FTIR stations of the Network for the Detection of Atmospheric Composition Change (NDACC). The resulting data sets are compared with total column time series derived from IASI (Infrared Atmospheric Sounding Interferometer) satellite observations and to a global chemical transport model. The results are discussed in terms of their overall consistency, mutual agreement, and seasonal cycles. Noticeable is the fact that the FTIR data point to substantial deficiencies in the global model simulation over high latitudes, a poorly sampled region, with an underestimation of the PAN columns during spring, at the peak of the seasonal cycle. Finally, we suggest avenues for development that should make it possible to limit intra-or intersite biases and extend the retrieval of PAN to other NDACC stations that are more affected by water vapor interferences.

Mots clés: PAN; Remote-sensing; FTIR technique; NDACC network; Air quality

Domaines: Physique Atmosphérique et Océanique [physics.ao-ph]; Océan, Atmosphère; Sciences de l'environnement

Emmanuel Mahieu, Emily V. Fischer, Bruno Franco, Mathias Palm, Tyler Wizenberg, et al.. First retrievals of peroxyacetyl nitrate (PAN) from ground-based FTIR solar spectra recorded at remote sites, comparison with model and satellite data. Elementa: Science of the Anthropocene, 2021, 9 (1), pp.00027. ⟨10.1525/elementa.2021.00027⟩. ⟨insu-03364109⟩