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Polymorph-Dependent Multi-Level Supramolecular Self-Assembly and Local Charge Transport of a Conjugated Polymer in Solution and Solid States
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DOI：10.1002/aenm.202402778.png)
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Abstract
En 中文
The polymorphic behavior of conjugated polymers enables tunable optoelectronic properties, but their transport mechanism remains elusive due to the inherent complexity and uncontrollability of polymorphic self-assembly behaviors and electronic processes at various length scales, alongside the ambiguous relationship between solution and solid states. Herein, precise control of multi-level supramolecular self-assembly of a polymorphic conjugated polymer, N-PDPP4T-HD with two distinct semi-crystalline aggregated phases (beta 1 and beta 2) via solvent engineering is demonstrated. beta 1 forms 1D worm-like nanostructures in solution, whereas beta 2 generates 2D nanoscale lamellar configuration, confirmed by experimental observation and molecular dynamic simulation. Such solution-state features are inherited in the solid state (1D nanofibers for beta 1 and 2D granular-like structures for beta 2). X-ray characterizations reveal larger crystalline domains on the nanometer scale, reduced pi-stacking distance on the & Aring;ngstrom scale, and diminished paracrystallinity disorder for solid-state beta 2. Going beyond conventional DC transistor characterizations, contact-free ultrafast terahertz spectroscopy to unveil AC short-range, intrinsic transport properties is employed. Longer charge carrier scattering time and thus intrinsic mobility of beta 2 result in threefold higher short-range photoconductivity than beta 1. This work establishes the solution structure - solid structure - local transport relation in polymorphic conjugated polymers and provides new opportunities for high-performance plastic electronic devices. Two distinct semi-crystalline aggregated phases (beta 1 and beta 2) of polymorphic N-PDPP4T-HD exhibit different dimensionalities in solution: beta 1 forms 1D nanostructures, while beta 2 adopts 2D configuration, as confirmed by experimental observations and molecular dynamic simulations. This solution-state supramolecular self-assembly is inherited in the solid state with structural differences on various scales, significantly affecting local transport characterized by contact-free ultrafast terahertz spectroscopy. image
Keywords:
charge transport
conjugate polymers
polymorphism
supramolecular assembly
terahertz spectroscopy
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