4.8 Article

Understanding of Face-On Crystallites Transitioning to Edge-On Crystallites in Thiophene-Based Conjugated Polymers

Journal

CHEMISTRY OF MATERIALS
Volume 33, Issue 12, Pages 4541-4550

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.1c00946

Keywords

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Funding

  1. NSF [CBET-1639429]
  2. National Research Foundation of Korea (NRF) - Korea government (MSIT) [2021R1A2C3004420]
  3. National Research Foundation of Korea [PAL-2021, 2021R1A2C3004420] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The orientation of crystallites in semicrystalline conjugated polymer thin films significantly impacts charge transport properties. In this study, a random copolymer RP-3T demonstrated a transition from predominantly face-on to edge-on orientation during annealing. Through detailed analysis, it was found that face-on crystallites disappear at a lower temperature while edge-on crystallites continue to grow, providing insight into the transition process.
The orientation of crystallites (face-on or edge-on, in regard to the plane of the substrate) in semicrystalline conjugated polymer thin films has a significant impact on charge transport properties of such thin films. It has been observed in a number of conjugated polymers where predominantly face-on orientation in the as-cast film can transition to edge-on upon cooling from the melt (melt-annealing). However, why and how do face-on crystallites transition to edge-on during melt-annealing remain unclear. To answer these fundamental questions, we designed and synthesized a random copolymer (RP-3T) by inserting unsubstituted terthiophenes into regioregular poly(3-hexylthiophene)s. RP-3T shows a predominantly face-on orientation in an as-cast film but transitioning to an almost exclusively edge-on orientation upon annealing at 190 degrees C, a temperature below the T-m (194 degrees C). Through a detailed investigation on changes in the microstructure and orientation of crystallites in RP-3T with annealing temperature, we find that face-on crystallites in RP-3T start to disappear at 170 degrees C (notably lower than the T-m), while edge-on crystallites continue to grow as the annealing temperature increases toward the T-m. This finding provides a reasonable explanation for the transition of face-on orientation to edge-on orientation during thermal annealing in RP-3T, in particular, at a temperature below the T-m.

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