A Metallofullerene Electron Donor that Powers an Efficient Spin Flip in a Linear Electron Donor鈥揂cceptor Conjugate

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• 作者：Marc Rudolf ; Lai Feng ; Zdenek Slanina ; Takeshi Akasaka ; Shigeru Nagase ; Dirk M. Guldi
• 刊名：The Journal of the American Chemical Society
• 出版年：2013
• 出版时间：July 31, 2013
• 年：2013
• 卷：135
• 期：30
• 页码：11165-11174
• 全文大小：509K
• 年卷期：v.135,no.30(July 31, 2013)
• ISSN：1520-5126

文摘

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-C₈₀鈥揚DI electron donor鈥揳cceptor conjugate, in which the presence of the Lu₃N cluster 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-C₈₀)^鈥?鈥揚DI^{鈥⑩€?/sup>], to the corresponding triplet radical ion pair state, 3[(Lu₃N@I_h-C₈₀)鈥?鈥揚DI鈥⑩€?/sup>]. Most notably, the radical ion pair state lifetime of the latter is nearly 1000 times longer than that of the former.}