权益分类	功能权益	普通用户	{{item.name}}会员
{{category.name}}	{{benefitItem.name}}

Theoretical Study on Surface Structure and Mass Transfer at Atmospheric Aerosols

大气气溶胶表面结构与传质的理论研究

基本信息

批准号：
15550012
负责人：
MORITA Akihiro
金额：
$ 2.11万
依托单位：
National Institute of Natural Sciences Okazaki Research Facilities (2004-2005)Okazaki National Research Institutes (2003)
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2003
资助国家：
日本
起止时间：
2003 至 2005
项目状态：
已结题

项目摘要

This study aims at understanding heterogeneous atmospheric chemistry, particularly surface structure and mass transfer at aerosol surfaces, by molecular simulations and fluid dynamics simulations. A particular focus is put on the previous evaluation of mass accommodation coefficients of gas species into liquid surfaces, important parameters in atmospheric modeling, since it is not straightforward to estimate these coefficients by laboratory experiments alone. To help precisely analyze uptake experiments, we performed computational fluid dynamics simulation of the droplet train flow tube experiments, and quantitatively evaluated the transport in the gas phase at realistic conditions of the flow tube. The simulation suggested that previous experiment of water condensation is actually in accord with molecular dynamics simulation, after careful calibration of the gas-phase diffusion. As the final year of this project, we summarized our studies this year in a review paper of Chemistry Reviews.Another focus of this project is development of theory and simulation methods for interfacial sum frequency generation (SFG) spectroscopy, toward investigating liquid interfaces relevant to atmospheric chemistry. We proposed non-empirical analysis of SFG spectroscopy with the help of ab initio molecular modeling and molucular dynamics simulations. This year we performed revised SFG calculation for water surface, demonstrating significant improvement in accuracy of the calculations. In connection to the SFG calculation, we have extended the charge response kernel theory on the basis of the density functional formalism. Development of flexible and polarizable molecular modeling is a indispensable step for use of general application of SFG simulation. We plan to apply the revised and improved molecular model to SFG analysis of a wide variety of interfaces.

这项研究旨在通过分子模拟和流体动力学模拟来了解非均相大气化学，特别是表面结构和气溶胶表面的质量传递。特别着重于以前对气体进入液体表面的质量容纳系数的评估，这是大气模拟中的重要参数，因为仅通过实验室实验估计这些系数并不直接。为了帮助准确分析吸收实验，我们对液滴串流管实验进行了计算流体力学模拟，并定量地评估了在实际流管条件下气相中的传输。模拟结果表明，经过仔细的气相扩散校正，以前的水冷凝实验实际上与分子动力学模拟是一致的。作为本项目的最后一年，我们在《化学评论》的综述论文中总结了我们今年的研究。本项目的另一个重点是界面和频率产生(SFG)光谱的理论和模拟方法的发展，以研究与大气化学相关的液体界面。通过从头算分子模拟和分子动力学模拟，我们提出了对SFG光谱的非经验分析。今年，我们对水面进行了修正的SFG计算，表明计算的准确性有了显著的提高。结合SFG计算，我们在密度泛函理论的基础上推广了电荷响应核理论。发展灵活的、可极化的分子模拟是SFG模拟广泛应用不可缺少的一步。我们计划将修正和改进的分子模型应用于各种界面的SFG分析。

项目成果

期刊论文数量（67）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Molecular Dynamics Study of Mass Accommodation of Methanol at Liquid-Vapor Intergace of Methanol/Water Binary Solutions od Various Concentrations,

不同浓度甲醇/水二元溶液液-汽界面处甲醇质量调节的分子动力学研究，

DOI：
发表时间：
2003
期刊：
Chem, Phys. Lett 375
影响因子：
0
作者：
Hisako Sato;Akihiro Morita;Kanta Ono;haruyuki Nakano;Noboru Wakabayashi;Akihiko Yamagishi;Akihiro Morita
通讯作者：
Akihiro Morita

Reply to Comment on Mass Accommodation Coefficient of Water : Molecular Dynamics Simulation and Revised Analysis of Droplet Train/Flow Reactor Experiment

回复关于水的质量调节系数的评论：液滴序列/流动反应器实验的分子动力学模拟和修订分析