Mao Jingqiu, Carlton Annmarie, Cohen Ronald C, Brune William H, Brown Steven S, Wolfe Glenn M, Jimenez Jose L, Pye Havala O T, Ng Nga Lee, Xu Lu, McNeill V Faye, Tsigaridis Kostas, McDonald Brian C, Warneke Carsten, Guenther Alex, Alvarado Matthew J, de Gouw Joost, Mickley Loretta J, Leibensperger Eric M, Mathur Rohit, Nolte Christopher G, Portmann Robert W, Unger Nadine, Tosca Mika, Horowitz Larry W
Geophysical Institute and Department of Chemistry, University of Alaska Fairbanks, Fairbanks, AK, USA.
Department of Environmental Sciences, Rutgers University, New Brunswick, NJ, USA.
Atmos Chem Phys. 2018;18(4):2615-2651. doi: 10.5194/acp-18-2615-2018. Epub 2018 Feb 22.
Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes) elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS) conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales. This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA) and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and elsewhere. Here we address questions surrounding four key themes: gas-phase chemistry, aerosol chemistry, regional climate and chemistry interactions, and natural and anthropogenic emissions. We expect this review to serve as a guidance for future modeling efforts.
在过去几十年里,美国大气中痕量物种的浓度发生了显著变化,这是对污染控制策略、国内能源政策和经济的转变以及世界其他地区经济发展(以及由此产生的排放变化)的响应。对未来大气进行可靠预测,要求模型不仅要准确描述当前的大气浓度,而且要通过在概念和定量上忠实反映化学、物理和生物过程来做到这一点。只有通过纳入控制排放的过程以及代表活性分子间关键转化的化学机制,模型才能可靠地预测未来政策、能源和气候情景的影响。在密集观测期内,对气相和凝聚相中各种特定化学物质进行并置测量,有助于大气模型正确识别和实施基本及控制机制。2013年夏季开展的东南大气研究(SAS,包括SENEX、SOAS、NOMADSS和SEAC4RS)为大气建模界提供了一个前所未有的机会,使他们能够齐聚一堂,评估、诊断和改进不同时空尺度模型中基本气候和空气质量过程的表示。本文旨在以与SAS观测结果的比较为指导,讨论在评估、诊断和改进空气质量及气候建模方面取得的进展,以此来思考模型中机制和参数化的改进。这项工作主要集中在对对流层中臭氧、二次有机气溶胶(SOA)和其他痕量物种形成至关重要的基本大气过程的模型表示上,最终目标是了解这些物种在东南部及其他地区的辐射影响。在这里,我们探讨围绕四个关键主题的问题:气相化学、气溶胶化学、区域气候与化学相互作用以及自然和人为排放。我们期望这篇综述能为未来的建模工作提供指导。