Abstract Atmospheric tracers are effective tools for characterizing dispersion and for testing computational models of atmospheric transport. Atmospheric trace gas measurements are now used widely to infer geographical surface flux distributions. However, robust flux estimates critically rely on well-validated knowledge of atmospheric chemistry, loss processes and transport, without which we are not fully realizing the potential of atmospheric measurements collected on the ground, or from aircraft and satellites. This challenge has taken on renewed importance in the shadow of the Paris Agreement that will likely take advantage of atmospheric trace gas measurements to help improve national and global greenhouse gas emission budgets. We describe a wide range of existing and new potential atmospheric tracers for improving our understanding of atmospheric dispersion. We consider the investigation of atmospheric transport over two scales: 1) short-to-medium length scale (on the order of 1-1000 km) to improve our understanding of convection and boundary layer transport processes, and 2) hemisphere-to-global length scale (on the order of 1,000-10,000 km), where large-scale mixing, cross hemisphere transport and stratosphere-troposphere exchange are important. Although we note the possibility of using “tracers of opportunity,” our primary focus is on deliberate-release tracers, and we explore the use of cyclic perfluorocarbons, hydrofluorocarbons, hydrochlorofluorocarbons, hydrofluoroethers and novel tracers of deuterium-substituted halocarbons. We examine how we might exploit existing instrumentation already deployed at remote global monitoring sites as well as requirements for new instrumentation. To guide the discussion, we provide example scenarios for how experiments might be set up, covering regional to global spatial scales for the evaluation and improvement of atmospheric transport models. However, we stress that appropriate three-dimensional modelling studies and preliminary experiments would need to be carried out to determine the specific details of any real-world experiment.

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用于评估区域至全球尺度大气传输和氧化计算模型的示踪剂

摘要 大气示踪剂是表征扩散和测试大气传输计算模型的有效工具。大气痕量气体测量现在被广泛用于推断地理表面通量分布。然而，可靠的通量估计严重依赖于经过充分验证的大气化学、损失过程和传输知识，如果没有这些知识，我们就不能完全意识到在地面上或从飞机和卫星收集的大气测量的潜力。在《巴黎协定》的阴影下，这一挑战重新变得重要起来，该协定可能会利用大气痕量气体测量来帮助改善国家和全球温室气体排放预算。我们描述了广泛的现有和新的潜在大气示踪剂，以提高我们对大气扩散的理解。我们考虑在两个尺度上对大气传输进行调查：1）短到中长尺度（大约 1-1000 公里）以提高我们对对流和边界层传输过程的理解，以及 2）半球到全球长度尺度（大约 1,000-10,000 公里），其中大规模混合、跨半球运输和平流层-对流层交换很重要。虽然我们注意到使用“机会示踪剂”的可能性，但我们的主要重点是故意释放示踪剂，我们探索使用环状全氟化碳、氢氟碳、氢氯氟碳、氢氟醚和氘取代卤代烃的新型示踪剂。我们研究了如何利用已部署在远程全球监控站点的现有仪器以及对新仪器的要求。为了指导讨论，我们提供了如何设置实验的示例场景，涵盖区域到全球空间尺度，以评估和改进大气传输模型。然而，我们强调需要进行适当的三维建模研究和初步实验，以确定任何真实世界实验的具体细节。涵盖区域到全球空间尺度，用于评估和改进大气传输模型。然而，我们强调需要进行适当的三维建模研究和初步实验，以确定任何真实世界实验的具体细节。涵盖区域到全球空间尺度，用于评估和改进大气传输模型。然而，我们强调需要进行适当的三维建模研究和初步实验，以确定任何真实世界实验的具体细节。