Quantum Transport in DNA-based molecular wires: Towards a realistic description of charge transport and dynamics in complex molecular systems

基于 DNA 的分子线中的量子传输：对复杂分子系统中电荷传输和动力学的真实描述

• 批准号: 25002742
• 负责人: Professor Dr. Gianaurelio Cuniberti
• 金额: --
• 依托单位: Abteilung für Theoretische Chemische Biologie
• 依托单位国家: 德国
• 项目类别: Priority Programmes
• 财政年份: 2006
• 资助国家: 德国
• 起止时间: 2005-12-31 至 2015-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/25002742?language=en
• 关键词: Quantum; Transport; DNA; based; molecular

The project main goal is to theoretically investigate the interplay between quantum transport (coherent and incoherent), disorder and stretching effects in DNA-based molecular wires, which are the focus of recent experimental work. The complexity of this issue makes necessary to use both density functional theory and model Hamiltonian approaches. We plan to proceed along the following lines: (i) Perform density-functional-based calculations of short DMA oligomers with different base sequences, in different environments as well as on stretched oligomers, in order to gain information about the electronic structure of the base pairs, their mutual interaction and the coupling with the environment; (ii) Investigate the mechanisms leading to polaron formation and its stability under different conditions (base sequence, environment) by a combined density-functional-based molecular dynamics approach; (iii) Formulate effective tight-binding Hamiltonians to minimally describe the electronic structure of DNA wires with arbitrary lengths, including the effects of an environment, and of internal vibrational degrees of freedom. The Hamiltonian wilt be parametrized by the density functional calculations of points (i) and (ii); (iv) Study nonequilibrium quantum transport in the previous model Hamiltonians. We will use Keldysh Green function techniques to describe the nonequilibrium regime. The use of the mentioned techniques will shed new light on ongoing experiments addressing the influence of disorder, as generated by biologically relevant base pair compositions, DNA-stretching, and structural fluctuations.

该项目的主要目标是从理论上研究基于DNA的分子线中量子传输（相干和非相干），无序和拉伸效应之间的相互作用，这是最近实验工作的重点。这个问题的复杂性使得有必要使用密度泛函理论和模型哈密顿方法。我们计划沿着以下路线进行：（i）对具有不同碱基序列的短DMA低聚物、在不同环境中以及对拉伸低聚物进行基于密度泛函的计算，以便获得关于碱基对的电子结构、它们的相互作用以及与环境的耦合的信息; ㈡研究导致极化子形成的机制及其在不同条件下的稳定性（碱基序列、环境）的分子动力学方法;（iii）制定有效的紧束缚哈密顿量，以最小限度地描述具有任意长度的DNA线的电子结构，包括环境和内部振动自由度的影响。哈密顿量将通过点（i）和（ii）的密度泛函计算参数化;（iv）研究在以前的模型哈密顿量的非平衡量子输运。我们将使用Keldysh绿色函数技术来描述非平衡状态。上述技术的使用将为正在进行的实验提供新的线索，这些实验涉及生物学相关碱基对组成、DNA拉伸和结构波动所产生的紊乱的影响。