A Metallofullerene Electron Donor that Powers an Efficient Spin Flip in a Linear Electron Donor-Acceptor Conjugate

作者：Rudolf Marc; Feng Lai^*; Slanina Zdenek; Akasaka Takeshi; Nagase Shigeru; Gudi Dirk M

来源：Journal of the American Chemical Society, 2013, 135(30): 11165-11174.

DOI：10.1021/ja403763e

The dream target of artificial photosynthesis is the realization of long-lived radical ion pair states that power catalytic centers and, consequently, the production of solar fuels. Notably, magnetic field effects, especially internal magnetic field effects, are rarely employed in this context. Here, we report on a linear Lu3N@I-h-C-80 PDI electron donor acceptor conjugate, in which the presence of the Lu3N duster exerts an appreciable electron nuclear hyperfine coupling on the charge transfer dynamics. As such, a fairly efficient radical ion pair intersystem crossing converts the initially formed singlet radical ion pair state, (1)[(Lu3N@I-h-C-80)(center dot+)-PDI center dot-], to the corresponding triplet radical ion pair state, (3)[(Lu3N@I-h-C-80)(center dot+)-PDI center dot-]. Most notably, the radical ion pair state lifetime of the latter is nearly 1000 times longer than that of the former.

• 出版日期2013-7-31
• 单位华中科技大学; 苏州大学