Observing the Multiexciton State in Singlet Fission and Ensuing Ultrafast Multielectron Transfer

被引:465
作者
Chan, Wai-Lun [1 ]
Ligges, Manuel [1 ]
Jailaubekov, Askat [1 ]
Kaake, Loren [1 ]
Miaja-Avila, Luis [1 ]
Zhu, X. -Y. [1 ]
机构
[1] Univ Texas Austin, Dept Chem & Biochem, Austin, TX 78712 USA
基金
美国国家科学基金会;
关键词
PENTACENE THIN-FILMS; CARRIER MULTIPLICATION; SEMICONDUCTOR NANOCRYSTALS; QUANTUM COHERENCE; ELECTRON-TRANSFER; TRIPLET EXCITONS; SOLAR-CELLS; GENERATION; DYNAMICS; TEMPERATURE;
D O I
10.1126/science.1213986
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Multiple exciton generation (MEG) refers to the creation of two or more electron-hole pairs from the absorption of one photon. Although MEG holds great promise, it has proven challenging to implement, and questions remain about the underlying photo-physical dynamics in nanocrystalline as well as molecular media. Using the model system of pentacene/fullerene bilayers and femtosecond nonlinear spectroscopies, we directly observed the multiexciton (ME) state ensuing from singlet fission (a molecular manifestation of MEG) in pentacene. The data suggest that the state exists in coherent superposition with the singlet populated by optical excitation. We also found that multiple electron transfer from the ME state to the fullerene occurs on a subpicosecond time scale, which is one order of magnitude faster than that from the triplet exciton state.
引用
收藏
页码:1541 / 1545
页数:5
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