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首页> 外文期刊>The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical >What Governs the Charge Transfer in DNA? The Role of DNA Conformation and Environment
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What Governs the Charge Transfer in DNA? The Role of DNA Conformation and Environment

机译：什么控制DNA中的电荷转移？ DNA构象与环境的作用

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摘要

Charge transfer in DNA has received much attention in the last few years due to its role in oxidative damage and repair in DNA and also due to possible applications of DNA in nanoelectronics. Despite intense experimental and theoretical efforts, the mechanism underlying long-range hole transport is still unresolved. This is in particular due to the sensitive dependence of charge transfer on the complex structure and dynamics of DNA and the interaction with the solvent, which could not be addressed adequately in the modeling approaches up to now. In this work, we study the factors governing hole transfer in detail, using a DFT-based fragment-orbital method, which allows to compute the charge transfer parameters along multinanosecond molecular dynamics simulations. Environmental effects are captured using a hybrid quantum mechanics-molecular mechanics (QM/MM) coupling scheme. This methodology allows to analyze several factors responsible for charge transfer in DNA in detail. The fluctuation of counterions, strongly counterbalanced by the surrounding water, leads to large oscillations of onsite energies, which govern the energetics of hole propagation along the DNA strand. In contrast, the electronic couplings depend only on DNA conformation and are not affected by the solvent. In particular, the onsite energies are strongly correlated between neighboring nucleobases, indicating that a conformational-gating type of mechanism may be induced by the collective environmental degrees of freedom.
机译：近年来，DNA中的电荷转移由于其在DNA中的氧化损伤和修复中的作用以及DNA在纳米电子学中的可能应用而备受关注。尽管进行了大量的实验和理论上的努力，但远距离空穴传输的机理仍未得到解决。这尤其是由于电荷转移对DNA的复杂结构和动力学以及与溶剂的相互作用的敏感依赖性，到目前为止，在建模方法中尚不能充分解决这一问题。在这项工作中，我们使用基于DFT的碎片轨道方法详细研究了控制空穴传输的因素，该方法可以沿着多纳秒分子动力学模拟计算电荷传输参数。使用混合量子力学-分子力学（QM / MM）耦合方案捕获环境影响。这种方法可以详细分析导致DNA电荷转移的几种因素。抗衡离子的波动被周围的水强烈地抵消，导致现场能量的大幅振荡，从而控制了空穴沿着DNA链传播的能量。相反，电子偶联仅取决于DNA构象，不受溶剂的影响。特别地，现场能量在相邻核碱基之间强烈相关，表明构象门控类型的机制可能是由集体环境自由度诱导的。

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