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Title: Metal–Ligand Based Mechanophores Enhance Both Mechanical Robustness and Electronic Performance of Polymer Semiconductors

Journal Article · · Advanced Functional Materials
ORCiD logo [1];  [2];  [1];  [1];  [1];  [3];  [4];  [5];  [6];  [7];  [8];  [8];  [8];  [9];  [5]; ORCiD logo [1]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); Dresden Univ. of Technology (Germany); Leibniz Inst. of Polymer Research (IPF), Dresden (Germany)
  3. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  4. Stanford Univ., CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Nanjing Univ. (China)
  6. Stanford Univ., CA (United States); Keio Univ., Kanagawa (Japan)
  7. Inst. of High Performance Computing A*STAR, Connexis (Singapore)
  8. Zhejiang Univ., Hangzhou (China)
  9. National Taiwan Univ., Taipei (Taiwan)
+ Show Author Affiliations

The backbone of diketopyrrolopyrrole-thiophene-vinylene-thiophene-based polymer semiconductors (PSCs) is modified with pyridine (Py) or bipyridine ligands to complex Fe(II) metal centers, allowing the metal–ligand complexes to act as mechanophores and dynamically crosslink the polymer chains. Here, mono- and bi-dentate ligands are observed to exhibit different degrees of bond strengths, which subsequently affect the mechanical properties of these Wolf-type-II metallopolymers. The counter ion also plays a crucial role, as it is observed that Py-Fe mechanophores with non-coordinating BPh4– counter ions (Py-FeB) exhibit better thin film ductility with lower elastic modulus, as compared to the coordinating chloro ligands (Py-FeC). Interestingly, besides mechanical robustness, the electrical charge carrier mobility can also be enhanced concurrently when incorporating Py-FeB mechanophores in PSCs. This is a unique observation among stretchable PSCs, especially that most reports to date describe a decreased mobility when the stretchability is improved. Next, it is determined that improvements to both mobility and stretchability are correlated to the solid-state molecular ordering and dynamics of coordination bonds under strain, as elucidated via techniques of grazing-incidence X-ray diffraction and X-ray absorption spectroscopy techniques, respectively. This study provides a viable approach to enhance both the mechanical and the electronic performance of polymer-based soft devices.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
Ministry of Science and Technology of Taiwan; National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1767437
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 11 Vol. 31; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
charge transport
mechanophore
metal‐ligand coordination
polymer semiconductor
stretchable electronics