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Title: Intrinsically stretchable and healable semiconducting polymer for organic transistors

Abstract

Developing a molecular design paradigm for conjugated polymers applicable to intrinsically stretchable semiconductors is crucial toward the next generation of wearable electronics. Current molecular design rules for high charge carrier mobility semiconducting polymers are unable to render the fabricated devices simultaneously stretchable and mechanically robust. Here in this paper, we present a new design concept to address the above challenge, while maintaining excellent electronic performance. This concept involves introducing chemical moieties to promote dynamic non-covalent crosslinking of the conjugated polymers. These non-covalent covalent crosslinking moieties are able to undergo an energy dissipation mechanism through breakage of bonds when strain is applied, while retaining its high charge transport ability. As a result, our polymer is able to recover its high mobility performance (>1 cm 2/Vs) even after 100 cycles at 100% applied strain. Furthermore, we observed that the polymer can be efficiently repaired and/or healed with a simple heat and solvent treatment. These improved mechanical properties of our fabricated stretchable semiconductor enabled us to fabricate highly stretchable and high performance wearable organic transistors. This material design concept should illuminate and advance the pathways for future development of fully stretchable and healable skin-inspired wearable electronics.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [1];  [3];  [4];  [1];  [3];  [5];  [6];  [1];  [1]
  1. Stanford Univ., CA (United States). Dept. of Chemical Engineering
  2. Stanford Univ., CA (United States). Dept. of Chemical Engineering; Asahi Kasei Corporation, Fuji (Japan). Corporate Research and Development, Performance Materials Technology Center
  3. Stanford Univ., CA (United States). Dept. of Electrical Engineering
  4. Stanford Univ., CA (United States). Dept. of Chemical Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  5. Stanford Univ., CA (United States). Dept. of of Civil and Environmental Engineering
  6. Stanford Univ., CA (United States). Dept. of Chemical Engineering; Samsung Advanced Inst. of Technology, Yeongtong-gu, Suwon-si (South Korea)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); US Air Force Office of Scientific Research (AFOSR); Ministry of Science and Technology, Taiwan; Swiss National Science Foundation (SNSF)
OSTI Identifier:
1360199
Grant/Contract Number:
AC02-76SF00515; FA9550-15-1-0106; DGE-114747
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 539; Journal Issue: 7629; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Conjugated polymers; Electronic devices

Citation Formats

Oh, Jin Young, Rondeau-Gagné, Simon, Chiu, Yu-Cheng, Chortos, Alex, Lissel, Franziska, Wang, Ging-Ji Nathan, Schroeder, Bob C., Kurosawa, Tadanori, Lopez, Jeffrey, Katsumata, Toru, Xu, Jie, Zhu, Chenxin, Gu, Xiaodan, Bae, Won-Gyu, Kim, Yeongin, Jin, Lihua, Chung, Jong Won, Tok, Jeffrey B. -H., and Bao, Zhenan. Intrinsically stretchable and healable semiconducting polymer for organic transistors. United States: N. p., 2016. Web. doi:10.1038/nature20102.
Oh, Jin Young, Rondeau-Gagné, Simon, Chiu, Yu-Cheng, Chortos, Alex, Lissel, Franziska, Wang, Ging-Ji Nathan, Schroeder, Bob C., Kurosawa, Tadanori, Lopez, Jeffrey, Katsumata, Toru, Xu, Jie, Zhu, Chenxin, Gu, Xiaodan, Bae, Won-Gyu, Kim, Yeongin, Jin, Lihua, Chung, Jong Won, Tok, Jeffrey B. -H., & Bao, Zhenan. Intrinsically stretchable and healable semiconducting polymer for organic transistors. United States. doi:10.1038/nature20102.
Oh, Jin Young, Rondeau-Gagné, Simon, Chiu, Yu-Cheng, Chortos, Alex, Lissel, Franziska, Wang, Ging-Ji Nathan, Schroeder, Bob C., Kurosawa, Tadanori, Lopez, Jeffrey, Katsumata, Toru, Xu, Jie, Zhu, Chenxin, Gu, Xiaodan, Bae, Won-Gyu, Kim, Yeongin, Jin, Lihua, Chung, Jong Won, Tok, Jeffrey B. -H., and Bao, Zhenan. Wed . "Intrinsically stretchable and healable semiconducting polymer for organic transistors". United States. doi:10.1038/nature20102. https://www.osti.gov/servlets/purl/1360199.
@article{osti_1360199,
title = {Intrinsically stretchable and healable semiconducting polymer for organic transistors},
author = {Oh, Jin Young and Rondeau-Gagné, Simon and Chiu, Yu-Cheng and Chortos, Alex and Lissel, Franziska and Wang, Ging-Ji Nathan and Schroeder, Bob C. and Kurosawa, Tadanori and Lopez, Jeffrey and Katsumata, Toru and Xu, Jie and Zhu, Chenxin and Gu, Xiaodan and Bae, Won-Gyu and Kim, Yeongin and Jin, Lihua and Chung, Jong Won and Tok, Jeffrey B. -H. and Bao, Zhenan},
abstractNote = {Developing a molecular design paradigm for conjugated polymers applicable to intrinsically stretchable semiconductors is crucial toward the next generation of wearable electronics. Current molecular design rules for high charge carrier mobility semiconducting polymers are unable to render the fabricated devices simultaneously stretchable and mechanically robust. Here in this paper, we present a new design concept to address the above challenge, while maintaining excellent electronic performance. This concept involves introducing chemical moieties to promote dynamic non-covalent crosslinking of the conjugated polymers. These non-covalent covalent crosslinking moieties are able to undergo an energy dissipation mechanism through breakage of bonds when strain is applied, while retaining its high charge transport ability. As a result, our polymer is able to recover its high mobility performance (>1 cm2/Vs) even after 100 cycles at 100% applied strain. Furthermore, we observed that the polymer can be efficiently repaired and/or healed with a simple heat and solvent treatment. These improved mechanical properties of our fabricated stretchable semiconductor enabled us to fabricate highly stretchable and high performance wearable organic transistors. This material design concept should illuminate and advance the pathways for future development of fully stretchable and healable skin-inspired wearable electronics.},
doi = {10.1038/nature20102},
journal = {Nature (London)},
number = 7629,
volume = 539,
place = {United States},
year = {Wed Nov 16 00:00:00 EST 2016},
month = {Wed Nov 16 00:00:00 EST 2016}
}

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  • Organic semiconductors are emerging as a viable alternative to amorphous silicon in a range of thin-film transistor devices. With the possibility to formulate these p-type materials as inks and subsequently print into patterned devices, organic-based transistors offer significant commercial advantages for manufacture, with initial applications such as low performance displays and simple logic being envisaged. Previous limitations of both air stability and electrical performance are now being overcome with a range of both small molecule and polymer-based solution-processable materials, which achieve charge carrier mobilities in excess of 0.5 cm2 V-1 s-1, a benchmark value for amorphous silicon semiconductors. Polymer semiconductorsmore » based on thienothiophene copolymers have achieved amongst the highest charge carrier mobilities in solution-processed transistor devices. In this Progress Report, we evaluate the advances and limitations of this class of polymer in transistor devices.« less
  • The primary goal of the field concerned with organic semiconductors is to produce devices with performance approaching that of silicon electronics, but with the deformability—flexibility and stretchability—of conventional plastics. However, an inherent competition between deformability and charge transport has long been observed in these materials, and achieving the extreme (or even moderate) deformability implied by the word “plastic” concurrently with high charge transport may be elusive. This competition arises because the properties needed for high carrier mobilities—e.g., rigid chains in π-conjugated polymers and high degrees of crystallinity in the solid state—are antithetical to deformability. On the device scale, this competitionmore » can lead to low-performance yet mechanically robust devices, or high-performance devices that fail catastrophically (e.g., cracking, cohesive failure, and delamination) under strain. There are, however, some observations that contradict the notion of the mutual exclusivity of electronic and mechanical performances. These observations suggest that this problem may not be a fundamental trade-off, but rather an inconvenience that may be negotiated by a logical selection of materials and processing conditions. For example, the selection of the poly(3-alkylthiophene) with a critical side-chain length—poly(3-heptylthiophene) (n = 7)—marries the high deformability of poly(3-octylthiophene) (n = 8) with the high electronic performance (as manifested in photovoltaic efficiency) of poly(3-hexylthiophene) (n = 6). This review explores the relationship between deformability and charge transport in organic semiconductors. The principal conclusions are that reducing the competition between these two parameters is in fact possible, with two demonstrated routes being: (1) incorporation of softer, insulating material into a stiffer, semiconducting material and (2) increasing disorder in a highly ordered film, but not enough to disrupt charge transport pathways. The aim of this review is to provide a bridge between the fields interested in electronic properties and mechanical properties of conjugated polymers. We provide a high-level introduction to some of the important electronic and mechanical properties and measurement techniques for organic electronic devices, demonstrate an apparent competition between good electronic performance and mechanical deformability, and highlight potential strategies for overcoming this undesirable competition. A marriage of these two fields would allow for rational design of materials for applications requiring large-area, low-cost, printable devices that are ultra-flexible or stretchable, such as organic photovoltaic devices and wearable, conformable, or implantable sensors.« less