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，以研究大分子系统中的电离和激发引起的ICD，并将其应用于光溶解酶的初始光诱导的电子传递步骤以及溶剂化的氨基酸和核碱基。为了实现这一目标，我们计划与复杂的吸收潜在技术相结合实施激发和电离代数图构造方案，利用现代数值技术（如本地轨道和自旋组件缩放）。然后，这些程序将被用来首次证明ICD是DNA光析中电子产生的功能机制，该机制启动了光损伤的DNA的修复。将与Hergenhahn和Winter的实验组手动研究，将研究溶剂化氨基酸和核碱基的ICD，例如ICD效率对簇大小的依赖性，例如，激发能的氢键。可以预期，这些发现对自然界中低能电子产生的基本了解以及生物组织中辐射诱导的损伤的基本了解会立即产生影响。