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Unraveling two distinct polymorph transition mechanisms in one n-type single crystal for dynamic electronics

Author

Listed:
  • Daniel William Davies

    (University of Illinois at Urbana-Champaign)

  • Bumjoon Seo

    (Purdue University
    Seoul National University of Science and Technology)

  • Sang Kyu Park

    (University of Illinois at Urbana-Champaign
    Korea Institute of Science and Technology)

  • Stephen B. Shiring

    (Purdue University)

  • Hyunjoong Chung

    (University of Illinois at Urbana-Champaign)

  • Prapti Kafle

    (University of Illinois at Urbana-Champaign)

  • Dafei Yuan

    (Institute of Chemistry, Chinese Academy of Sciences
    Hunan University)

  • Joseph W. Strzalka

    (Argonne National Laboratory)

  • Ralph Weber

    (Bruker BioSpin Corp.)

  • Xiaozhang Zhu

    (Institute of Chemistry, Chinese Academy of Sciences)

  • Brett M. Savoie

    (Purdue University)

  • Ying Diao

    (University of Illinois at Urbana-Champaign
    Beckman Institute for Advanced Science and Technology)

Abstract

Cooperativity is used by living systems to circumvent energetic and entropic barriers to yield highly efficient molecular processes. Cooperative structural transitions involve the concerted displacement of molecules in a crystalline material, as opposed to typical molecule-by-molecule nucleation and growth mechanisms which often break single crystallinity. Cooperative transitions have acquired much attention for low transition barriers, ultrafast kinetics, and structural reversibility. However, cooperative transitions are rare in molecular crystals and their origin is poorly understood. Crystals of 2-dimensional quinoidal terthiophene (2DQTT-o-B), a high-performance n-type organic semiconductor, demonstrate two distinct thermally activated phase transitions following these mechanisms. Here we show reorientation of the alkyl side chains triggers cooperative behavior, tilting the molecules like dominos. Whereas, nucleation and growth transition is coincident with increasing alkyl chain disorder and driven by forming a biradical state. We establish alkyl chain engineering as integral to rationally controlling these polymorphic behaviors for novel electronic applications.

Suggested Citation

  • Daniel William Davies & Bumjoon Seo & Sang Kyu Park & Stephen B. Shiring & Hyunjoong Chung & Prapti Kafle & Dafei Yuan & Joseph W. Strzalka & Ralph Weber & Xiaozhang Zhu & Brett M. Savoie & Ying Diao, 2023. "Unraveling two distinct polymorph transition mechanisms in one n-type single crystal for dynamic electronics," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36871-9
    DOI: 10.1038/s41467-023-36871-9
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    References listed on IDEAS

    as
    1. Hyunjoong Chung & Dmytro Dudenko & Fengjiao Zhang & Gabriele D’Avino & Christian Ruzié & Audrey Richard & Guillaume Schweicher & Jérôme Cornil & David Beljonne & Yves Geerts & Ying Diao, 2018. "Rotator side chains trigger cooperative transition for shape and function memory effect in organic semiconductors," Nature Communications, Nature, vol. 9(1), pages 1-12, December.
    2. Manas K. Panda & Tomče Runčevski & Subash Chandra Sahoo & Alexei A. Belik & Naba K. Nath & Robert E. Dinnebier & Panče Naumov, 2014. "Colossal positive and negative thermal expansion and thermosalient effect in a pentamorphic organometallic martensite," Nature Communications, Nature, vol. 5(1), pages 1-8, December.
    3. Sheng-Qun Su & Takashi Kamachi & Zi-Shuo Yao & You-Gui Huang & Yoshihito Shiota & Kazunari Yoshizawa & Nobuaki Azuma & Yuji Miyazaki & Motohiro Nakano & Goro Maruta & Sadamu Takeda & Soonchul Kang & S, 2015. "Assembling an alkyl rotor to access abrupt and reversible crystalline deformation of a cobalt(II) complex," Nature Communications, Nature, vol. 6(1), pages 1-7, December.
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