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The entangled triplet pair state in acene and heteroacene materials

Author

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  • Chaw Keong Yong

    (Cavendish Laboratory, Optoelectronics Group, University of Cambridge
    University of California)

  • Andrew J. Musser

    (Cavendish Laboratory, Optoelectronics Group, University of Cambridge
    The University of Sheffield)

  • Sam L. Bayliss

    (Cavendish Laboratory, Optoelectronics Group, University of Cambridge)

  • Steven Lukman

    (Cavendish Laboratory, Optoelectronics Group, University of Cambridge)

  • Hiroyuki Tamura

    (The University of Tokyo)

  • Olga Bubnova

    (Cavendish Laboratory, Optoelectronics Group, University of Cambridge)

  • Rawad K. Hallani

    (University of Kentucky)

  • Aurélie Meneau

    (Cavendish Laboratory, Optoelectronics Group, University of Cambridge)

  • Roland Resel

    (Institute of Solid State Physics, Graz University of Technology)

  • Munetaka Maruyama

    (Faculty of Materials Science and Engineering, Kyoto Institute of Technology, Matsugasaki)

  • Shu Hotta

    (Faculty of Materials Science and Engineering, Kyoto Institute of Technology, Matsugasaki)

  • Laura M. Herz

    (Clarendon Laboratory, University of Oxford)

  • David Beljonne

    (Laboratory for Chemistry of Novel Materials, University of Mons)

  • John E. Anthony

    (University of Kentucky)

  • Jenny Clark

    (The University of Sheffield)

  • Henning Sirringhaus

    (Cavendish Laboratory, Optoelectronics Group, University of Cambridge)

Abstract

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 (∼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.

Suggested Citation

  • Chaw Keong Yong & Andrew J. Musser & Sam L. Bayliss & Steven Lukman & Hiroyuki Tamura & Olga Bubnova & Rawad K. Hallani & Aurélie Meneau & Roland Resel & Munetaka Maruyama & Shu Hotta & Laura M. Herz , 2017. "The entangled triplet pair state in acene and heteroacene materials," Nature Communications, Nature, vol. 8(1), pages 1-12, August.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms15953
    DOI: 10.1038/ncomms15953
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    Cited by:

    1. Yongseok Hong & Maximilian Rudolf & Munnyon Kim & Juno Kim & Tim Schembri & Ana-Maria Krause & Kazutaka Shoyama & David Bialas & Merle I. S. Röhr & Taiha Joo & Hyungjun Kim & Dongho Kim & Frank Würthn, 2022. "Steering the multiexciton generation in slip-stacked perylene dye array via exciton coupling," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    2. Nilabja Maity & Woojae Kim & Naitik A. Panjwani & Arup Kundu & Kanad Majumder & Pranav Kasetty & Divji Mishra & Robert Bittl & Jayashree Nagesh & Jyotishman Dasgupta & Andrew J. Musser & Satish Patil, 2022. "Parallel triplet formation pathways in a singlet fission material," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    3. Yanju Luo & Kai Zhang & Zhenming Ding & Ping Chen & Xiaomei Peng & Yihuan Zhao & Kuan Chen & Chuan Li & Xujun Zheng & Yan Huang & Xuemei Pu & Yu Liu & Shi-Jian Su & Xiandeng Hou & Zhiyun Lu, 2022. "Ultra-fast triplet-triplet-annihilation-mediated high-lying reverse intersystem crossing triggered by participation of nπ*-featured excited states," Nature Communications, Nature, vol. 13(1), pages 1-12, December.

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