Radiative forcing from aircraft emissions of NOx: model calculations with CH4 surface flux boundary condition

Pitari, G, Cionni, I, Di Genova, G, Søvde, OA and Lim, L (2017) Radiative forcing from aircraft emissions of NOx: model calculations with CH4 surface flux boundary condition. Meteorologische Zeitschrift, 26 (6). pp. 663-687. ISSN 0941-2948

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Abstract

© 2017 The authors. Two independent chemistry-transport models with troposphere-stratosphere coupling are used to quantify the different components of the radiative forcing (RF) from aircraft emissions of NO x , i.e., the University of L'Aquila climate-chemistry model (ULAQ-CCM) and the University of Oslo chemistry-transport model (Oslo-CTM3). The tropospheric NO x enhancement due to aircraft emissions produces a short-term O 3 increase with a positive RF (+17.3mW/m 2 ) (as an average value of the two models). This is partly compensated by the CH 4 decrease due to the OH enhancement (-9.4mW/m 2 ). The latter is a long-term response calculated using a surface CH 4 flux boundary condition (FBC), with at least 50 years needed for the atmospheric CH 4 to reach steady state. The radiative balance is also affected by the decreasing amount of CO 2 produced at the end of the CH 4 oxidation chain: an average CO 2 accumulation change of -2.2 ppbv/yr is calculated on a 50 year time horizon (-1.6mW/m 2 ). The aviation perturbed amount of CH 4 induces a long-term response of tropospheric O 3 mostly due to less HO 2 and CH 3 O 2 being available for O 3 production, compared with the reference case where a constant CH 4 surface mixing ratio boundary condition is used (MBC) (-3.9mW/m 2 ). The CH 4 decrease induces a long-term response of stratospheric H2O (-1.4mW/m 2 ). The latter finally perturbs HO x and NO x in the stratosphere, with a more efficient NO x cycle for mid-stratospheric O 3 depletion and a decreased O 3 production from HO 2 +NO in the lower stratosphere. This produces a long-term stratospheric O 3 loss, with a negative RF (-1.2mW/m 2 ), compared with the CH 4 MBC case. Other contributions to the net NO x RF are those due to NO 2 absorption of UV-A and aerosol perturbations (the latter calculated only in the ULAQ-CCM). These comprise: increasing sulfate due to more efficient oxidation of SO 2 , increasing inorganic and organic nitrates and the net aerosols indirect effect on warm clouds. According to these model calculations, aviation NO x emissions for 2006 produced globally a net cooling effect of -5.7mW/m 2 (-6.2 and -5.1mW/m 2 , from ULAQ and Oslo models, respectively). When the effects of aviation sulfur emissions are taken into account in the atmospheric NO x balance (via heterogeneous chemistry), the model-average net cooling effects of aviation NO x increases to -6.2mW/m 2 . Our study applies to a sustained and constant aviation NO x emission and for the given background NOy conditions. The perturbation picture, however, may look different if an increasing trend in aviation NO x emissions would be allowed.