A Divide and Conquer Approach to the Response Properties of Biomolecules: Electron Transfer Reactions, Raman Spectroscopy, and Spectroscopic Probes of Chirality

生物分子响应特性的分而治之的方法：电子转移反应、拉曼光谱和手性光谱探针

基本信息

批准号：
9727657
负责人：
David Beratan
金额：
$ 29.3万
依托单位：
University of Pittsburgh
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
1998
资助国家：
美国
起止时间：
1998-03-01 至 2001-10-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=9727657&HistoricalAwards=false
关键词：
Divide Conquer Approach Response Properties

项目摘要

David Beratan is supported by a grant from the Theoretical and Computational Chemistry Program to study response properties of biomolecules including electron transfer reactions and Raman spectroscopic probes of chirality. The goal of the proposed work is to develop a general new tool that will enable the theoretical exploration of biochemical structure-function and reactivity relations by exploiting the local nature of chemical interactions. An ab initio divide-and-conquer method is proposed, tailored to describe the electronic and vibronic response properties of macromolecules. The methods will be developed in such a way that they can be used to: 1) establish a link between 3D structure and electron transfer rates in proteins and DNA; 2) assist in relating molecular structure to chiroptical properties critical for drug discovery and protein structure determination, and 3) expand the structure-property interpretations of proteins available via Raman spectroscopy. The actual implementation of this strategy involves the use of an effective Hamiltonian, and Greens function theory to determine the relevant response function. A quantitative molecular-level description of biological function will arise from a detailed description of macromolecular electronic and vibronic structure. Yet, reliable electronic structure calculations are possible on systems of only modest size. Beratan's research program will enable the theoretical exploration of biochemical structure-function and reactivity relations at the molecular level for macromolecular systems of biological interest.

戴维·贝拉坦（David Beratan）得到了理论和计算化学计划的赠款的支持，该计划将研究生物分子的反应特性，包括电子传递反应和手性的拉曼光谱探针。拟议工作的目的是开发一种一般的新工具，该工具将通过利用化学相互作用的局部性质来实现生化结构功能和反应性关系的理论探索。提出了一种从头静止的划分和诱饵方法，以描述大分子的电子和振动响应特性。这些方法的开发方式可以用于以下方式：1）在蛋白质和DNA中建立3D结构和电子传递速率之间的联系； 2）有助于将分子结构与对药物发现和蛋白质结构确定至关重要的手律特性相关，3）扩大通过拉曼光谱法获得的蛋白质的结构质能解释。该策略的实际实施涉及使用有效的哈密顿量和绿色功能理论来确定相关响应函数。生物学功能的定量分子级描述将来自大分子电子和振动性结构的详细描述。但是，仅在适度大小的系统上进行可靠的电子结构计算。 Beratan的研究计划将对生物学意义的大分子系统的生化结构功能和反应性关系进行理论探索。