Molecular engineering of buckybowl trichalcogenasumanene toward centimeter-sized organic single-crystal arrays and devices

• • 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.