Intermolecular Coulombic Decay in Biological Systems and Open-Shell Species

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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.