文献类型：期刊文献

英文题名：Unexpected large charge transfer rate mediated by adenine in twisted DNA structure

作者：Song, Yongshun[1];Gao, Yi[2];Fang, Haiping[1,3]

机构：[1]East China Univ Sci & Technol, Sch Phys, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Adv Res Inst, Phonon Sci Res Ctr Carbon Dioxide, Shanghai 201210, Peoples R China;[3]Zhejiang Univ, Sch Phys, Hangzhou 310027, Peoples R China

年份：2024

卷号：109

期号：6

外文期刊名：PHYSICAL REVIEW E

收录：;EI(收录号：20242716563897);WOS:【SCI-EXPANDED(收录号:WOS:001255333500009)】；

基金：We thank Dr. J. Yang, Dr. C. Wang, and Prof. Y. Shao for their constructive suggestions. Support from the Shanghai Science and Technology Innovation Action Plan (Grant No. 23JC1401400) , the Fundamental Research Funds for the Central Universities of China, the Guanghe Fund (the second phase) , and the Shanghai Supercomputer Center of China are acknowledged.

语种：英文

外文关键词：Biological systems - Charge transfer - Molecular orbitals - Positive ions

摘要：DNA exhibits remarkable charge transfer ability, which is crucial for its biological functions and potential electronic applications. The charge transfer process in DNA is widely recognized as primarily mediated by guanine, while the contribution of other nucleobases is negligible. Using the tight-binding models in conjunction with first-principles calculations, we investigated the charge transfer behavior of homogeneous GC and AT pairs. We found that the charge transfer rate of adenine significantly changes. With overstretching, the charge transfer rate of adenine can even surpass that of guanine, by as much as five orders of magnitude at a twist angle of around 26 degrees. Further analysis reveals that it is attributed to the turnover of the relative coupling strength between homogeneous GC and AT base pairs, which is caused by the symmetry exchange between the two highest occupied molecular orbitals of base pairs occurring at different twist angles. Given the high degree of flexibility of DNA in vivo and in vitro conditions, these findings prompt us to reconsider the mechanism of biological functions concerning the charge transfer in DNA molecules and further open the potential of DNA as a biomaterial for electronic applications.