Singlet Exciton Fission in Polycrystalline Thin Films of a Slip-Stacked Perylenediimide

被引:316
作者
Eaton, Samuel W. [1 ,2 ]
Shoer, Leah E. [1 ,2 ]
Karlen, Steven D. [1 ,2 ]
Dyar, Scott M. [1 ,2 ]
Margulies, Eric A. [1 ,2 ]
Veldkamp, Brad S. [1 ,2 ]
Ramanan, Charusheela [1 ,2 ]
Hartzler, Daniel A. [3 ]
Savikhin, Sergei [3 ]
Marks, Tobin J. [1 ,2 ]
Wasielewski, Michael R. [1 ,2 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[2] Northwestern Univ, Argonne Northwestern Solar Energy Res ANSER Ctr, Evanston, IL 60208 USA
[3] Purdue Univ, Dept Phys, W Lafayette, IN 47907 USA
基金
美国国家科学基金会;
关键词
PHOTOINDUCED ELECTRON-TRANSFER; EXCIMER-FORMING CRYSTAL; TRIPLET EXCITONS; CHARGE SEPARATION; ENERGY-TRANSFER; MAGNETIC-FIELD; RHODOSPIRILLUM-RUBRUM; PHOTOSYNTHETIC SYSTEM; TETRACENE CRYSTALS; SPIN-RESONANCE;
D O I
10.1021/ja4053174
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The crystal structure of N,N-bis(n-octyl)-2,5,8,11-tetraphenylperylene-3,4:9,10-bis(dicarboximide), 1, obtained by X-ray diffraction reveals that 1 has a nearly planar perylene core and pi-pi stacks at a 3.5 angstrom interplanar distance in well-separated slip-stacked columns. Theory predicts that slip-stacked, pi-pi-stacked structures should enhance interchromophore electronic coupling and thus favor singlet exciton fission. Photoexcitation of vapor-deposited polycrystalline 188 nm thick films of 1 results in a 140 +/- 20% yield of triplet excitons ((3)*1) in tau(SF) = 180 +/- 10 ps. These results illustrate a design strategy for producing perylenediimide and related rylene derivatives that have the optimized interchromophore electronic interactions which promote high-yield singlet exciton fission for potentially enhancing organic solar cell performance and charge separation in systems for artificial photosynthesis.
引用
收藏
页码:14701 / 14712
页数:12
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