Polaron pair mediated triplet generation in polymer/fullerene blends

被引:80
作者
Dimitrov, Stoichko D. [1 ]
Wheeler, Scot [1 ]
Niedzialek, Dorota [2 ]
Schroeder, Bob C. [1 ]
Utzat, Hendrik [1 ]
Frost, Jarvist M. [2 ]
Yao, Jizhong [2 ]
Gillett, Alexander [1 ]
Tuladhar, Pabitra S. [1 ]
McCulloch, Iain [1 ,3 ]
Nelson, Jenny [2 ]
Durrant, James R. [1 ]
机构
[1] Univ London Imperial Coll Sci Technol & Med, Ctr Plast Elect, Dept Chem, London SW7 2AZ, England
[2] Univ London Imperial Coll Sci Technol & Med, Ctr Plast Elect, Dept Phys, London SW7 2AZ, England
[3] King Abdullah Univ Sci & Technol, SPERC, Phys Sci & Engn Div, Thuwal 239556900, Saudi Arabia
来源
NATURE COMMUNICATIONS | 2015年 / 6卷
基金
英国工程与自然科学研究理事会;
关键词
CHARGE-TRANSFER EXCITONS; GEMINATE RECOMBINATION; ELECTRON-TRANSFER; SOLAR-CELLS; PHOTOCURRENT COLLECTION; STATE; DISSOCIATION; ENERGY; NONGEMINATE; SPIN;
D O I
10.1038/ncomms7501
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
Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields.
引用
收藏
页数:8
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