The entangled triplet pair state in acene and heteroacene materials

被引:195
作者
Yong, Chaw Keong [1 ,2 ]
Musser, Andrew J. [1 ,3 ]
Bayliss, Sam L. [1 ]
Lukman, Steven [1 ]
Tamura, Hiroyuki [4 ]
Bubnova, Olga [1 ]
Hallani, Rawad K. [5 ]
Meneau, Aurelie [1 ]
Resel, Roland [6 ]
Maruyama, Munetaka [7 ]
Hotta, Shu [7 ]
Herz, Laura M. [8 ]
Beljonne, David [9 ]
Anthony, John E. [5 ]
Clark, Jenny [3 ]
Sirringhaus, Henning [1 ]
机构
[1] Univ Cambridge, Cavendish Lab, Optoelect Grp, Madingley Rd,JJ Thomson Ave, Cambridge CB3 0HE, England
[2] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA
[3] Univ Sheffield, Dept Phys & Astron, Hicks Buildling,Hounsfield Rd, Sheffield S3 7RH, S Yorkshire, England
[4] Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan
[5] Univ Kentucky, Dept Chem, Lexington, KY 40506 USA
[6] Graz Univ Technol, Inst Solid State Phys, Petersgasse 16, A-8010 Graz, Austria
[7] Kyoto Inst Technol, Fac Mat Sci & Engn, Sakyo Ku, Kyoto 6068585, Japan
[8] Univ Oxford, Dept Phys, Clarendon Lab, Parks Rd, Oxford OX1 3PU, England
[9] Univ Mons, Lab Chem Novel Mat, Pl Parc 20, B-7000 Mons, Belgium
基金
英国工程与自然科学研究理事会; 美国国家科学基金会;
关键词
SINGLET-EXCITON-FISSION; ELECTRONIC-STRUCTURE; TETRACENE CRYSTALS; CHARGE-TRANSFER; QUANTUM EFFICIENCY; THIN-FILMS; PENTACENE; ANNIHILATION; FLUORESCENCE; DYNAMICS;
D O I
10.1038/ncomms15953
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
Entanglement of states is one of the most surprising and counter-intuitive consequences of quantum mechanics, with potent applications in cryptography and computing. In organic materials, one particularly significant manifestation is the spin-entangled triplet-pair state, which mediates the spin-conserving fission of one spin-0 singlet exciton into two spin-1 triplet excitons. Despite long theoretical and experimental exploration, the nature of the triplet-pair state and inter-triplet interactions have proved elusive. Here we use a range of organic semiconductors that undergo singlet exciton fission to reveal the photophysical properties of entangled triplet-pair states. We find that the triplet pair is bound with respect to free triplets with an energy that is largely material independent (similar to 30 meV). During its lifetime, the component triplets behave cooperatively as a singlet and emit light through a Herzberg-Teller-type mechanism, resulting in vibronically structured photoluminescence. In photovoltaic blends, charge transfer can occur from the bound triplet pairs with >100% photon-to-charge conversion efficiency.
引用
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页数:12
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