文献类型：期刊文献

英文题名：Bridge- and Solvent-Mediated Intramolecular Electronic Communications in Ubiquinone-Based Biomolecular Wires

作者：Liu, Xiao-Yuan;Ma, Wei;Zhou, Hao;Cao, Xiao-Ming;Long, Yi-Tao[1]

机构：[1]E China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China; E China Univ Sci & Technol, Dept Chem, Shanghai 200237, Peoples R China

年份：2015

卷号：5

外文期刊名：SCIENTIFIC REPORTS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000355504300001)】；

基金：This research is supported by the National Base Research 973 Program (2013CB733700), the Science Fund for Creative Research Groups (21421004) and National Natural Science Foundation of China (21327807). Y.-T. Long is grateful for funds from the National Science Fund for Distinguished Young Scholars of China (21125522) and Shanghai Pujiang Program (12JC1403500).

语种：英文

摘要：Intramolecular electronic communications of molecular wires play a crucial role for developing molecular devices. In the present work, we describe different degrees of intramolecular electronic communications in the redox processes of three ubiquinone-based biomolecular wires (Bis-CoQ(0)s) evaluated by electrochemistry and Density Functional Theory (DFT) methods in different solvents. We found that the bridges linkers have a significant effect on the electronic communications between the two peripheral ubiquinone moieties and solvents effects are limited and mostly depend on the nature of solvents. The DFT calculations for the first time indicate the intensity of the electronic communications during the redox processes rely on the molecular orbital elements V-L for electron transfer (half of the energy splitting of the LUMO and LUMO+1), which is could be affected by the bridges linkers. The DFT calculations also demonstrates the effect of solvents on the latter two-electron transfer of Bis-CoQ(0)s is more significant than the former two electrons transfer as the observed electrochemical behaviors of three Bis-CoQ(0)s. In addition, the electrochemistry and theoretical calculations reveal the intramolecular electronic communications vary in the four-electron redox processes of three Bis-CoQ(0)s.