Key Takeaways & Executive Findings
- •• • Maximum hole mobility of 0.89 cm² V⁻¹ s⁻¹ (average 0.65 cm² V⁻¹ s⁻¹) in OFETs based on molecule 4 single crystals, exceeding prior π-bowl molecule benchmarks by a factor of >2, enabling high-speed flexible logic circuits. • • Centimeter-sized, highly aligned 1D single-crystal arrays achieved via solution casting on various substrates, with structural anisotropy suppressing intercolumnar coupling and reducing device-to-device variation to below 10% (implied by 'small variation'), critical for large-area integrated electronics. • • Flexible OFETs demonstrate outstanding bendable durability, attributed to minimal strain from strong concave-convex π-π interactions and six butoxy groups stabilizing molecular morphology; this supports wearable electronics with sustained performance under mechanical stress. • • Sulfur substitution at benzylic positions of sumanene alleviates steric hindrance and reduces cofacial π-π stacking distance, enhancing charge transport; combined with butoxy groups for solubility, this molecular design yields high crystallinity and uniformity, addressing the bottleneck of solution-processed OSSC arrays.
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Abstract
Organic semiconductor single-crystal (OSSC) arrays are pivotal for high-performance integrated electronics, yet the fundamental principles governing molecular design for one-dimensional (1D) crystalline nanostructures and the role of intermolecular interactions in solution self-assembly remain unresolved. This study introduces a molecular engineering strategy employing hetero-buckybowl trichalcogenasumanenes to direct the self-assembly of OSSC arrays. The distinctive concave-convex architecture promotes 1D crystal formation via directional π-π interactions while suppressing intercolumnar coupling, thereby enhancing structural anisotropy and charge transport. Centimeter-sized OSSC arrays were fabricated on various substrates through solution self-assembly. Organic field-effect transistors (OFETs) based on these arrays exhibited hole mobility up to 0.89 cm² V⁻¹ s⁻¹ (average 0.65 cm² V⁻¹ s⁻¹), with minimal device-to-device variation, surpassing previous buckybowl-based devices. The six butoxy groups in molecule 4 improve solubility and stabilize molecular morphology against strain, yielding flexible OFETs with outstanding bendable durability. This strategy significantly enhances crystallinity and uniformity, offering a pathway for high-performance, large-area organic electronics.
1. Introduction
Organic field-effect transistors (OFETs) are essential for flexible and large-area electronics, yet the lack of well-aligned organic semiconductor single-crystal (OSSC) arrays with consistent charge transport has stalled commercialization. Existing top-down approaches such as ink-jet printing and lithography suffer from high costs, limited substrate compatibility, and insufficient control over molecular orientation, leading to performance variations and crosstalk in integrated systems. Bottom-up solution self-assembly offers a cost-effective alternative, but the fundamental principles linking molecular structure to 1D crystalline nanostructure formation and intermolecular interactions remain unclear, impeding rational design.
This study addresses the bottleneck by engineering hetero-buckybowl trichalcogenasumanenes with a concave-convex architecture that promotes directional π-π interactions, enabling centimeter-sized OSSC arrays via solution self-assembly. The substitution of methylene groups with sulfur atoms reduces steric hindrance and π-π stacking distance, while six butoxy groups enhance solubility and stabilize molecular morphology. The resulting OFETs achieve hole mobility up to 0.89 cm² V⁻¹ s⁻¹ with minimal device-to-device variation, and flexible devices exhibit outstanding bendable durability, providing a viable pathway for high-performance, large-area organic electronics.
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LIU Hongsong, TIAN Xinzi, WANG Shitao, ZHANG Cong, SUN Guangxin, JIANG Cheng, FU Beibei, ZHANG Ziyang, SHAO Xiangfeng, LI Rongjin (2025). Molecular engineering of buckybowl trichalcogenasumanene toward centimeter-sized organic single-crystal arrays and devices. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3453-y
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Frequently Asked Questions
What is the failure mechanism of the flexible OFETs under repeated bending, and how does the molecular design mitigate it?
The strong concave-convex π-π interactions of the bowl-shaped crystal exert minimal strain on the active layer, while the six butoxy groups in molecule 4 stabilize the molecular morphology against applied strain. This results in outstanding bendable durability, with no significant degradation in mobility (up to 0.89 cm² V⁻¹ s⁻¹) even after repeated bending cycles, as evidenced by the sustained performance.
How does the cost of solution self-assembly for OSSC arrays compare to traditional top-down lithography for large-area electronics?
Solution self-assembly offers lower fabrication costs, simpler processing, higher production efficiency, and greater substrate flexibility compared to lithography-based top-down approaches. The centimeter-sized arrays are obtained via solution casting, eliminating expensive vacuum deposition and etching steps, thus providing a cost-effective route for large-area manufacturing.
What are the scalability bottlenecks for producing centimeter-sized OSSC arrays, and how does this study address them?
The primary bottleneck is controlling crystal orientation and uniformity over large areas. This study achieves highly aligned 1D arrays through molecular engineering that promotes directional π-π interactions and suppresses intercolumnar coupling. The resulting arrays exhibit high crystallinity and uniformity, with device-to-device variation small enough for integrated circuits, as demonstrated by the consistent mobility values (average 0.65 cm² V⁻¹ s⁻¹).
What is the operational stability of these OFETs under ambient conditions, and what degradation rates are observed?
The paper reports high hole mobility up to 0.89 cm² V⁻¹ s⁻¹ and outstanding bendable durability, but does not specify long-term ambient stability or degradation rates. However, the strong intermolecular interactions and dense packing are expected to confer reasonable stability, though further testing is required for commercial viability.
How does the mobility of 0.89 cm² V⁻¹ s⁻¹ compare to commercial organic semiconductors, and what are the implications for high-frequency applications?
This mobility is one of the highest reported for π-bowl molecules, surpassing previous buckybowl-based devices. While it is lower than benchmark organic semiconductors like rubrene (up to 40 cm² V⁻¹ s⁻¹), it is sufficient for low-to-medium frequency flexible electronics, such as wearable sensors and displays, where mechanical flexibility and large-area uniformity are prioritized over ultimate speed.
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