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Closing the loop between microstructure and charge transport in conjugated polymers by combining microscopy and

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Understanding semiconducting polymer charge transport requires bridging molecular and mesoscale structures. This study reveals defects significantly impact charge motion, influencing device performance and offering new design rules for materials science.

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Area of Science:

  • Materials Science
  • Polymer Physics
  • Condensed Matter Physics

Background:

  • Macroscopic properties of materials are influenced by molecular composition and structure across various length scales.
  • Bridging these length scales remains a significant challenge in materials science for accurate property prediction.

Purpose of the Study:

  • To develop and apply a unified experimental-theoretical framework for understanding charge transport in semiconducting polymers.
  • To correlate molecular-level physical modeling with mesoscale structural measurements.
  • To investigate the impact of microstructure on charge transport properties.

Main Methods:

  • Spatially-resolved nanodiffraction in a transmission electron microscope to characterize mesoscale structure.
  • Self-consistent framework of polymer chain statistics to model molecular-level behavior.
  • Multiscale charge transport calculations using experimental data as input.

Main Results:

  • The framework provides a detailed picture of polymer microstructure from molecular to device-relevant scales.
  • Defects play a crucial, often underrepresented, role in charge transport models.
  • Short-range transport is more complex than anticipated, with drift velocity being a minor component.
  • Local transport is sensitive to polymer chain alignment and geometry.
  • Mesoscale features like domains and grain boundaries create inhomogeneous charge distributions, impacting mobility.

Conclusions:

  • The combined multiscale approach offers a flexible pipeline for analyzing functional properties across length scales.
  • Chain stiffness and alignment are identified as beneficial for charge transport, while local homogeneity has no positive effect.
  • The study provides a general strategy for extending the accessible length scales of experimental and theoretical probes.