Elucidating the Heterogeneous Chemistry of Nitrogen Containing Species Involving Aqueous Droplets, Ice Crystals and Gas-to-Particle Conversion

越来越多的证据表明，涉及云滴、冰粒和气溶胶的非均质过程在全球对流层化学中发挥着重要作用。作为对解开所涉及的许多复杂现象的一项贡献，国际和平研究所建议对与对大气具有重要意义的含氮物种的化学有关的广泛反应进行调查。分子过程的细节将通过三个主要活动进行调查。第一个将涉及解开与对流层中的氮、硝酸和亚硝基硫酸以及氨的氧化物有关的复杂化学物质的贡献。第二阶段的工作将包括热化学测量，这些测量将提供关于反应的能量学的信息，特别是关于络合物的稳定性的信息，这些信息可能对含氮物种的缩合及其气体到颗粒的转化很重要。第三个研究领域将包括对水相团簇和冰状晶体的结构、生长和成核的调查。这项工作的总体目标是提供补充数据，这些数据将有助于通过在模拟计算、大气测量和其他实验室研究的基础上对已提出的特别重要的反应进行调查，在分子一级阐明一些物理和化学现象。方法是研究水化程度不断增加的团簇，这些团簇起到从小团簇区域到宏观粒子状态的桥梁作用。我们实验室的最新进展使我们能够研究整个颗粒大小范围内的变化。

There is increasing evidence that heterogeneous processes involving cloud droplets, ice particles, and aerosols play an important role in global tropspheric chemistry. As a contribution to unraveling the many complex phenomena involved, the PI proposes to undertake investigations of a wide range of reactions pertaining to the chemistry of nitrogen containing species of atmospheric importance. The details of the molecular processes will be investigated through three major activities. The first will involve contribution to unraveling the complex chemistry associated with oxides of nitrogen, nitric acid and nitrosyl sulfuric acid, and ammonia in the troposphere. The second phase of the work will encompass thermochemical measurements which will provide information on the energetics of the reactions, and particularly on the stability of complexes which are likely to be important in the condensation of nitrogen containing species and in their gas-to-particle conversion. The third area of study will comprise investigations of the structure, growth and nucleation of aqueous phase clusters and ice-like crystals. The overall aim of the work is to provide complementary data which will serve to elucidate a number of the physical and chemical phenomena at the molecular level, through an investigation of reactions which have been proposed to be of particular importance on the basis of modeling calculations, atmospheric measurements, and other laboratory studies. The approach is to study clusters of ever increasing degrees of hydration that serve to bridge the regime from the small cluster domain to the macroscopic particle state. Recent advances in out laboratory enable us to investigate transformations over this entire range of particle size.