Reaction Dynamics in Manybody Chemical Systems---Complexity and Specificity of Chemical Dynamics and its Quantum Effects---

我们研究了许多体化学系统的复杂性和专一性的分子起源，如液相和生物分子中的化学反应动力学。这些体系的反应动力学涉及涨落和集体分子运动。人们已经从实验和理论两个方面研究了如何观测导致特定反应的最重要的运动，这些运动隐藏在许多粒子随机运动的噪声中。这些方法是为了处理势能面的整体性质和势能面上的动力学问题而发展起来的。发展了高度非线性的闪光光解技术，特别是在红外区域，以处理复杂体系的相空间动力学，以及用于在分子尺度和超快时间域检测热流的瞬时分级技术。为了找出为什么特定的过程总是发生在生物分子反应中，我们对细菌视紫红质和DNA分子的反应进行了研究。研究了氢液中化学反应的量子效应对振动弛豫和反应动力学的影响。1999年和2001年在京都举行了两次国际会议和五次国内会议。在这一年(2002年)，我们总结了整个三年活动(1998-2001)的报告，共200多页。该研究项目的成员已被邀请参加许多(100多个)国际会议。在该项目下发表了260多篇论文。我们还邀请了几位著名的外国科学家进行合作。

We have investigated the molecular origin for the complexity and specificity of manybody chemical systems, such as chemical reaction dynamics in liquid phase and biomolecules. The reaction dynamics of those systems involves fluctuations and collective molecular motions. Experimental and theoretical studies have been made how to observe the most important motions leading to the specific reaction, which are imbedded in the noise of many particle random motions.. The methods were developed to deal with global nature of the potential energy surfaces(GPES) and the dynamics on this GPES. Highly nonlinear flash photolysis technique, especially in Infra-red region, was developed to deal with the phase space dynamics of the complex systems and Transient Grading technique for detect heat flow in molecular scale and in ultrafast time domain. Reactions of Bacteria rhodopsin and DNA molecules were examined to find our why the specific process always take place in biomolecular reactions. Quantum effects on vibrational relaxation and reaction dynamics were investigated for chemical reactions in hydrogen liquid.Two international conferences in addition to five domestic conferences were held at Kyoto in 1999 and 2001.In this year (2002) we summarize the report of whole three years activities (1998-2001) which contains more than 200 pages. Members of this research projects have been invited to many (more than 100) international conferences. More than 260 papers were published under this project. We also invited several distinguished foreign scientists to pursue the cooperative works.