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Abstract Highly crystalline thin films in organic semiconductors are important for applications in high‐performance organic optoelectronics. Here, the effect of grain boundaries on the Hall effect and charge transport properties of organic transistors based on two exemplary benchmark systems is elucidated: (1) solution‐processed blends of 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene (C8‐BTBT) small molecule and indacenodithiophene‐benzothiadiazole (C16IDT‐BT) conjugated polymer, and (2) large‐area vacuum evaporated polycrystalline thin films of rubrene (C42H28). It is discovered that, despite the high field‐effect mobilities of up to 6 cm2V−1s−1and the evidence of a delocalized band‐like charge transport, the Hall effect in polycrystalline organic transistors is systematically and significantly underdeveloped, with the carrier coherence factor α < 1 (i.e., yields an underestimated Hall mobility and an overestimated carrier density). A model based on capacitively charged grain boundaries explaining this unusual behavior is described. This work significantly advances the understanding of magneto‐transport properties of organic semiconductor thin films.
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This content will become publicly available on May 16, 2026
Accelerating ion transport in polycrystalline conductors: On pores and grain boundaries
Polycrystalline ion conductors are widely used as solid electrolytes in energy storage technologies. However, they often exhibit poor ion transport across grain boundaries and pores. This work demonstrates that strategically tuning the mesoscale microstructures, including pore size, pore distribution, and chemical compositions of grain boundaries, can improve ion transport. Using LiTa2PO8as a case study, we have shown that the combination of LiF as a sintering agent with Hf4+implantation improves grain-grain contact, resulting in smaller, evenly distributed pores, reduced chemical contrast, and minimized nonconductive impurities. A suite of techniques has been used to decouple the effects of LiF and Hf4+. Specifically, LiF modifies particle shape and breaks large pores into smaller ones, while Hf4+addresses the chemical mismatches between grains and grain boundaries. Consequently, this approach achieves nearly two orders of magnitude improvement in ion conduction. Tuning mesoscale structures offers a cost-effective method for enhancing ion transport in polycrystalline systems and has notable implications for synthesizing high-performance ionic materials.
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- Award ID(s):
- 1847038
- PAR ID:
- 10596382
- Publisher / Repository:
- AAAS
- Date Published:
- Journal Name:
- Science Advances
- Volume:
- 11
- Issue:
- 20
- ISSN:
- 2375-2548
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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