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Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn

机译：大气化学模型的长期卤代烃趋势和预算受极地测量的限制

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The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114,CFC-115, CCl4 and SF6) are studied by comparing measurements in polarfirn air from two Arctic and three Antarctic sites, and simulation results oftwo numerical models: a 2-D atmospheric chemistry model and a 1-D firndiffusion model. The first one is used to calculate atmosphericconcentrations from emission trends based on industrial inventories; thecalculated concentration trends are used by the second one to produce depthconcentration profiles in the firn. The 2-D atmospheric model is validated inthe boundary layer by comparison with atmospheric station measurements, andvertically for CFC-12 by comparison with balloon and FTIR measurements. Firnair measurements provide constraints on historical atmospheric concentrationsover the last century. Age distributions in the firn are discussed using aGreen function approach. Finally, our results are used as input to aradiative model in order to evaluate the radiative forcing of our targetgases. Multi-species and multi-site firn air studies allow to betterconstrain atmospheric trends. The low concentrations of all studied gases atthe bottom of the firn, and their consistency with our model results confirmthat their natural sources are small. Our results indicate that theemissions, sinks and trends of CFC-11, CFC-12, CFC-113, CFC-115 and SF6are well constrained, whereas it is not the case for CFC-114 and CCl4.Significant emission-dependent changes in the lifetimes of halocarbonsdestroyed in the stratosphere were obtained. Those result from the timeneeded for their transport from the surface where they are emitted to thestratosphere where they are destroyed. Efforts should be made to update andreduce the large uncertainties on CFC lifetimes.
机译：研究了七种卤化气体（CFC-11，CFC-12，CFC-113，CFC-114，CFC-115，CCl 4 和SF 6 ）的预算比较了两个北极和三个南极地点极地空气中的测量结果，以及两个数值模型的模拟结果：一个二维大气化学模型和一个一维扩散模型。第一个用于根据工业清单根据排放趋势计算大气浓度;第二个计算出的浓度趋势将用于生成烧成中的深度浓度曲线。通过与大气站测量结果进行比较，可以在边界层中验证二维大气模型，并且通过与气球和FTIR测量结果进行比较，可以对CFC-12进行垂直验证。 Fiairair的测量结果限制了上个世纪的历史大气浓度。使用格林函数方法讨论了年龄中的年龄分布。最后，我们的结果被用作辐射模型的输入，以评估目标气体的辐射强迫。多物种和多地点的飞行空气研究可以更好地限制大气趋势。炉膛底部所有研究气体的浓度低，并且它们与我们的模型结果一致，证实了它们的天然气源很小。我们的结果表明，CFC-11，CFC-12，CFC-113，CFC-115和SF 6 的排放，下沉和趋势受到了很好的约束，而CFC-114和CFC-11的情况并非如此CCl 4 。获得了在平流层中被破坏的卤代烃寿命中与排放有关的显着变化。这些是由于需要时间将它们从发射表面传送到平流层，然后破坏它们。应努力更新和减少氟氯化碳寿命方面的巨大不确定性。

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