Fundamental studies of (photo)chemical reactions at atmospheric interfaces: bridging the gap between nano-scale and macroscale atmospheric chemistry

缺乏对气溶胶和云之间相互作用的洞察力，构成了理解气候变化的主要知识鸿沟。由于人们对气溶胶和云之间的相互作用知之甚少，因此重点研究这一主题具有重要意义。因此，我们的研究计划致力于通过选择物理和(生物)分析大气化学方面的基础研究来缩小这一知识差距，重点是金属和有机气溶胶的相互作用。在此提出了两个研究计划。每一项都有可能对我们目前的知识状况作出重大贡献，并填补国家和国际科学组织公认的关于气溶胶-云过程的知识的主要空白。基于我们在汞动力学和动力学以及(生物)有机物理和分析大气化学领域的开创性研究，我们的研究现在将进入下一个复杂水平。第一个研究主题涉及了解汞在雪/空气表面等大气界面上的复杂氧化和还原反应的动力学和机理。我们的目标也是开发新的分析技术，用于空气中各种汞化合物的超微量化学形态，注意到目前没有能力对这种有害的神经毒物和广泛存在的污染物进行详细的化学形态分析。由于缺乏对汞化合物化学结构的了解，科学家无法充分预测大气汞沉积的命运，因为它发生在春季日出期间的极地地区。这项拟议研究的第二个主题是对涉及与雪-空气界面生物气溶胶有关的有机化合物的选定物理和化学过程进行调查。我们的研究将通过相互关联的实验室、现场和数值模拟研究来进行。我们16人组中的11名科学家将在这个多学科的大气化学研究实验室接受全面培训。我们可能会有助于理解污染-气候相互作用领域中与大气相关的关键问题，以及对加拿大的重要性。

The lack of insight involving the interaction between aerosols and clouds constitutes a major knowledge gap in understanding the climate change. Since little is known about the interaction between aerosols and clouds, a research initiative focused on this subject is of major importance. Our research program is thus dedicated to reduce this knowledge gap through selected fundamental studies in physical and (bio)analytical atmospheric chemistry with a focus on interactions of metallic and organic containing aerosols. Two research programs are herein proposed. Each has the potential to contribute significantly to our current state of knowledge and fill in the major gaps in knowledge of aerosol-cloud processes well recognized by the national and international scientific organizations. Building on our pioneering research in the areas of mercury kinetics and dynamics as well as (bio)organic physical and analytical atmospheric chemistry, our research will now move to the next level of complexity. The first research theme involves the understanding of kinetics and mechanism of complex oxidation and reduction reactions of mercury at atmospheric interfaces such as snow/air surfaces. Our aim is also to develop novel analytical techniques for ultra-trace chemical speciation of various mercury compounds in air, noting that there is currently no capability for detailed chemical speciation of this detrimental neurotoxicant and widespread pollutant. The lack of understanding of the chemical structure of mercury compounds precludes scientists to predict the fate of atmospheric mercury depositions adequately, as it occurs in the polar regions during the spring sunrise. The second theme of this proposed research entails the investigation of selected physical and chemical processes involving organic compounds relevant to biological aerosols at snow-air interface. Our research will be performed through interconnected laboratory, field, and numerical modeling studies. 11 scientists in our group of 16 will be fully trained in this multidisciplinary atmospheric chemistry research laboratory. We will potentially contribute to the understanding of key questions of atmospheric relevance in the area of pollution-climate interactions, and of importance to Canada.