U.S.-Japan Cooperative Research: Statistical Spectroscopy of Unimolecular Dynamics

该奖项将促进麻省理工学院化学系Robert W. Field教授和日本东京大学土屋Soji教授及其各自研究小组成员之间的合作。科学家们将利用实验和理论方法，从高度激发的小多原子分子（包含两个以上原子的分子）的旋转振动光谱中获得有关单分子（单分子）化学反应的信息，如氰化氢、二氧化硫和乙炔。这种光谱在传统的光谱学意义上本质上是不可解释的。这项合作将探索新的实验方法，以产生大量高质量的、可解释的光谱，以及新的、基于统计的方法，从这些光谱中获取信息。如果成功，这项工作将首次允许从高能量分子的高分辨率光谱中提取有关某些化学过程的详细信息，例如单分子异构化。了解控制分子内能量流动的因素将有机会诊断、设计和影响分子特定部分的激发。这个项目的目的是获得对分子内振动能量再分配的基本理解，在孤立的小多原子分子中，这些分子被化学上有趣的内部旋转振动激励所激励。这些分子足够简单，可以通过最先进的实验和基于超级计算机的理论技术来详细检查。例如，可以用这种方法研究分子激发后HCN向HNC的异构化。两个研究小组将采用互补的实验和理论方法。作为该项目的重要组成部分，Field教授小组的研究生将对东京大学实验室进行大约一个月的工作访问，土屋教授的同事将对麻省理工学院进行类似的访问。

This award will facilitate collaboration between Professor Robert W. Field, Department of Chemistry, Massachusetts Institute of Technology, and Professor Soji Tsuchiya, University of Tokyo, Japan, and members of their respective research groups. The scientists will utilize experimental and theoretical approaches to obtain information about unimolecular (single molecule) chemical reactions from rotation- vibration spectra of highly excited small polyatomic molecules (molecules containing more than two atoms) such as hydrogen cyanide, sulfur dioxide, and acetylene. Such spectra are intrinsically uninterpretable in the traditional spectroscopic sense. This collaboration will explore new experimental ways to generate large quantities of high-quality, interpretable spectra as well as new, statistically based ways to obtain information from these spectra. If successful, the effort will permit, for the first time, the extraction of detailed information about certain chemical processes, such as unimolecular isomerization, from high resolution spectra of highly energized molecules. Knowledge of the factors controlling intramolecular energy flow will lead to opportunities to diagnose, design, and effect excitations localized in specific parts of a molecule. The purpose of this project is to gain a fundamental understanding of intramolecular vibrational energy redistribution in isolated, small polyatomic molecules that are energized with chemically interesting amounts of internal rotation-vibration excitation. These molecules are simple enough that they can be examined in detail by state-of- the-art experimental and supercomputer-based theoretical techniques. For example, the isomerization of HCN to HNC following excitation of the molecule may be studied in this way. Complementary experimental and theoretical approaches in the two research groups will be utilized. As a significant part of this project, graduate students in Professor Field's group will make approximately one-month working visits to the University of Tokyo laboratory, and associates of Professor Tsuchiya will make similar visits to MIT.