A comprehensive study of ozone sensitivity with respect to emissions over Europe with a chemistry‐transport model

[1] A detailed sensitivity analysis of ozone concentrations with respect to anthropogenic and biogenic emissions is performed at European scale in summer 2001 through the use of the chemistry-transport model Polair3D. We estimate the time evolution of the sensitivities and the extent of the sensitive regions. We discriminate the chemical species to which photochemistry is the most sensitive. This work is intended as a preliminary study for inverse modeling of emissions. Local sensitivities are computed using a tangent linear model and an adjoint model of the underlying chemistry-transport model. Global sensitivities are approximated by means of Monte Carlo simulations. It is shown that NO emissions have a prominent impact and that VOC emissions also play an important role. Major emission sources are associated with the highest sensitivities, although a non-negligible sensitivity of the concentrations at observation stations can cover the whole domain. A typical relative sensitivity of ozone concentrations to NO emissions is about 6 μg · m−3, which is low as to compared to the error and the uncertainty in output concentrations.

[1]  Michael E. Chang,et al.  On using inverse methods for resolving emissions with large spatial inhomogeneities , 1997 .

[2]  V. Mallet,et al.  Uncertainty in a chemistry-transport model due to physical parameterizations and numerical approximations: An ensemble approach applied to ozone modeling , 2006 .

[3]  V. Mallet,et al.  Software architecture of an ideal modeling platform in air quality – A first step: Polyphemus , 2005 .

[4]  Robert Vautard,et al.  A comparison of simulated and observed ozone mixing ratios for the summer of 1998 in Western Europe , 2001 .

[5]  Donald J. Wuebbles,et al.  Sensitivity of regional ozone concentrations to temporal distribution of emissions , 2004 .

[6]  F. Kirchner,et al.  A new mechanism for regional atmospheric chemistry modeling , 1997 .

[7]  J. Louis.  A parametric model of vertical eddy fluxes in the atmosphere , 1979 .

[8]  Robert Vet,et al.  A revised parameterization for gaseous dry deposition in air-quality models , 2003 .

[9]  Denis Quélo,et al.  Simulation numérique et assimilation de données variationnelle pour la dispersion atmosphérique de polluants. (Numerical simulation and variational data assimilation for atmospheric dispersion of polluants) , 2004 .

[10]  M. Wesely.  Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models , 1989 .

[11]  I. Troen,et al.  A simple model of the atmospheric boundary layer; sensitivity to surface evaporation , 1986 .

[12]  H. Elbern,et al.  4D-Var Data Assimilation and its Numerical Implications for Case Study Analyses , 2002 .

[13]  Hauke Schmidt,et al.  Adjoint sensitivity of episodic ozone in the Paris area to emissions on the continental scale , 2003 .

[14]  J. Lamarque,et al.  A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2 , 2001 .

[15]  C. N. Hewitt,et al.  Inventorying emissions from nature in Europe , 1999 .

[16]  H. Christopher Frey,et al.  Uncertainties in predicted ozone concentrations due to input uncertainties for the UAM-V photochemical grid model applied to the July 1995 OTAG domain , 2001 .

[17]  Vivien Mallet,et al.  3-D chemistry-transport model Polair: numerical issues, validation and automatic-differentiation strategy , 2004 .

[18]  A case study of emission changes and ozone responses , 1998 .

[19]  Z. Zlatev,et al.  Studying cumulative ozone exposures in Europe during a 7‐year period , 1997 .

[20]  Vivien Mallet,et al.  Development and validation of a fully modular platform for numerical modelling of air pollution: POLAIR , 2004 .

[21]  A. Russell,et al.  Estimation of emission adjustments from the application of four-dimensional data assimilation to photochemical air quality modeling , 2001 .

[22]  Willem Hundsdorfer,et al.  Numerical time integration for air pollution models , 1998 .

[23]  Donald L. Singleton,et al.  Sensitivity of ozone concentrations to VOC and NOx emissions in the Canadian Lower Fraser Valley , 1997 .

[24]  D. Simpson,et al.  Comparison of model results obtained with several european regional air quality models , 1997 .

[25]  S. Hanna,et al.  Monte carlo estimates of uncertainties in predictions by a photochemical grid model (UAM-IV) due to uncertainties in input variables , 1998 .

[26]  Paulette Middleton,et al.  Aggregation and analysis of volatile organic compound emissions for regional modeling , 1990 .

[27]  Laurent Menut,et al.  Adjoint modeling for atmospheric pollution process sensitivity at regional scale , 2003 .

[28]  Vivien Mallet,et al.  Inverse modeling of NOx emissions at regional scale over northern France: Preliminary investigation of the second‐order sensitivity , 2005 .