Intermolecular Coulombic Decay in Biological Systems and Open-Shell Species

生物系统和开壳物种中的分子间库仑衰变

• 批准号: 221566449
• 负责人: Professor Dr. Andreas Dreuw
• 金额: --
• 依托单位: Chair of Theoretical and Computational Chemistry
• 依托单位国家: 德国
• 项目类别: Research Units
• 财政年份: 2012
• 资助国家: 德国
• 起止时间: 2011-12-31 至 2019-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/221566449?language=en
• 关键词: Intermolecular; Coulombic; Decay; Biological; Systems

The proposed project aims at the development of efficient computational tools for the investigation of ionization and excitation induced ICD in large molecular systems and their application to the initial, photo-induced electron transfer step in photolyases as well as to solvated amino acids and nucleobases. For this objective, we plan to implement excitation and ionization algebraic diagrammatic construction schemes in combination with the complex absorbing potential technique, exploiting modern numerical techniques like local orbitals and spin-component scaling. These programs will then be employed to demonstrate for the first time ICD to be a functional mechanism in the electron generation in DNA photolyases, which initiates repair of photo-damaged DNA. Hand in hand with the experimental groups of Hergenhahn and Winter, ICD in solvated amino acids and nucleobases will be investigated, such as the dependence of ICD efficiency on cluster size, hydrogen bonds of excitation energy, for example. These findings can be expected to have an immediate impact onto the fundamental understanding of low-energy electron generation in nature and hence of radiation-induced damage in biological tissue.

拟议的项目旨在开发有效的计算工具，用于研究大分子系统中电离和激发诱导的ICD，并将其应用于光解酶中的初始光诱导电子转移步骤以及溶剂化氨基酸和核碱基。为了这个目标，我们计划实施激发和电离的代数图解结合复杂的吸收势技术的建设计划，利用现代数值技术，如本地轨道和自旋分量标度。然后，这些程序将首次用于证明ICD是DNA光解酶中电子产生的功能机制，它启动了光损伤DNA的修复。与Hergenhahn和Winter的实验组携手，将研究溶剂化氨基酸和核碱基中的ICD，例如ICD效率对簇大小的依赖性，激发能的氢键。这些发现有望对自然界中低能电子产生的基本认识产生直接影响，从而对生物组织中辐射引起的损伤产生影响。