2025-10-08 ノースカロライナ州立大学（NC State）
＜関連情報＞
- https://news.ncsu.edu/2025/10/engineering-polymer-electronics/
- https://www.cell.com/matter/abstract/S2590-2385(25)00520-X
AI誘導による共役ポリマードーピングのハイスループット調査により、局所的なポリマー秩序とドーパント-ポリマー分離の重要性が明らかになった AI-guided high-throughput investigation of conjugated polymer doping reveals importance of local polymer order and dopant-polymer separation
Jacob P. Mauthe ∙ Ankush Kumar Mishra ∙ Abhradeep Sarkar ∙ … ∙ Raja Ghosh ∙ Baskar Ganapathysubramanian ∙ Aram Amassian
Mattre Published:October 8, 2025
DOI:https://doi.org/10.1016/j.matt.2025.102477
Graphical abstract
Progress and potential
A detailed study of dip-doped pBTTT was conducted using high-throughput methods and quantum chemical calculations across a wide formulation and processing window, allowing materials informatics to reveal that counter ion location outside the lamellae is primarily responsible for highly delocalized polarons exhibiting higher mobility. This work includes the creation of a new materials acceleration platform (MAP) that automated hot casting of conjugated polymers, improving its reproducibility. This MAP conducted closed-loop experimental campaigns guided by Bayesian optimization, enabling a data-driven investigation of the relation between doped conductivity and polymer structural descriptors. It is revealed that polaron delocalization is directly impacted by enhancing the pre-doping order of the polymer, as measured via the 0-0/0-1 peak ratio from UV-vis spectroscopy and lamellar coherence length from grazing incidence wide-angle X-ray scattering. We ascribe the difference in polaron delocalization to location and distance of the dopant anion relative to the polymer backbone using first-principles quantum chemical simulations. Together, dopant location and polymer order in highly doped pBTTT influence polaron delocalization, which accounts for order-of-magnitude variations in charge carrier mobility and conductivity.
Highlights
- Thousand-fold variations in conductivity explained through polaron delocalization
- Polaron delocalization depends on dopant location and polymer order
- AI-guided campaign is used to elucidate process-structure-property relationship
- Robotic experimentation and IR simulation reveal importance of peripheral ions
Summary
Highly conducting polymers are essential for next-generation wearable electronics. However, achieving high conductivity remains an art form owing to complex intermolecular dopant-polymer interactions. In this study, we use AI-guided high-throughput experimentation combined with quantum chemical calculations to explore samples of diverse polymer order and polaron delocalization to reveal hidden correlations between charge transport, polymer order, carrier delocalization, and dopant location in F4TCNQ-doped pBTTT. We find that undoped aggregation benefits polaron delocalization and conductivity after doping, and lamellar stacking order correlates with two orders of magnitude variation in carrier mobility and highly influences polaron delocalization. Using quantum chemical theory, we deduce that increased mobility originates from highly delocalized polarons formed by “peripheral” counterions located at distances (≈1.3–1.8 nm) much greater than those of the lamellar intercalated counterions (≈0.4–0.8 nm). We find that achieving high conductivity (σ > 100 S/cm) in F4TCNQ-doped pBTTT requires processing conditions promoting ordered domains decorated by peripheral counter ions.
