Department of Chemistry and Biochemistry, University of Arizona, Tucson, Arizona, USA.
J Phys Chem B. 2010 Apr 8;114(13):4416-23. doi: 10.1021/jp9099094.
We present a DFT/classical molecular dynamics model of DNA charge conductivity. The model involves a temperature-driven, hole-hopping charge transfer and includes the time-dependent nonequilibrium interaction of DNA with its molecular environment. We validate our method against a variety of hole transport experiments. The method predicts a significant hole-transfer slowdown of approximately 35% from dry to wet DNA with and without electric field bias. In addition, in agreement with experiments, it also predicts an insulating behavior of (GC)(N) oligomers for 40 < N < 1000, depending on the experimental setup.
我们提出了一种 DNA 电荷传导的密度泛函理论/经典分子动力学模型。该模型涉及由温度驱动的空穴跳跃电荷转移，并包括 DNA 与其分子环境的时变非平衡相互作用。我们通过各种空穴输运实验验证了我们的方法。该方法预测，在有和没有电场偏压的情况下，干燥和湿润 DNA 的空穴转移速度会分别显著减慢约 35%。此外，与实验结果一致的是，该方法还预测了（GC）（N）寡聚物在 40 < N < 1000 范围内的绝缘行为，这取决于实验设置。
