CAREER: Interplay of Particle Phase State and Thermodynamic Mixing in Secondary Organic Aerosol Formation and Partitioning

森林和人类活动排放的活性气体经过复杂的过程转化为细颗粒物。目前的模型无法预测这种二次粒子的产生和粒子特性，限制了我们评估对区域空气质量和水循环影响的能力。该项目将开发一个详细的第一原理模型，并通过测量对其进行校准，以预测二次细颗粒的产生、其性质及其对对流风暴中冰和云形成的影响。教育部分将开发一个基于网络的交互式计算化学模型，以告知和吸引学生进行大气研究。研究将利用气溶胶和云中气体-颗粒相互作用的主要化学机理和动力学多层模型，明确解决颗粒表面和体积的相敏反应和质量传输。这个新的模式将受到实验室数据的大小分辨的颗粒相和化学成分的二次有机气溶胶（SOA）形成的有机气体。如何形成机制的过渡和SOA的属性变化，因为我们去异戊二烯（生物）萘（人为）有机气体将被调查，以获得分子水平的洞察力。模拟将扩展到对流制度的相对湿度，温度和上升气流速度，涉及冰成核的SOA颗粒的途径，并与最近的实验室测量。

Forests and anthropogenic activities emit reactive gases that convert to fine particles by complex processes. Current models are unable to predict this secondary particle production and the particle properties limiting our ability to assess impacts on regional air quality and water cycle. This project will develop a detailed first principles model and calibrate it with measurements to predict secondary fine particle production, their properties and their impacts on ice and cloud formation in convective storms. The educational component will develop a web based interactive computational chemistry model to inform and attract students to atmospheric research.The research will harness a master chemical mechanism and a kinetic multi-layer model of gas-particle interactions in aerosols and clouds that explicitly resolves the phase sensitive reactions and mass transport at the particle surface and bulk. This new model will be constrained by laboratory data on size resolved particle phase and chemical composition of secondary organic aerosol (SOA) formation from organic gases. How this formation mechanism transitions and the SOA properties change as we go from isoprene (biogenic) to naphthalene (anthropogenic) organic gases will be investigated to gain molecular level insight. The simulations will be extended to convective regimes of relative humidity, temperatures and updraft velocities that involve ice-nucleation pathways for SOA particles and compared to recent laboratory measurements.