Toward Flexible Low‐Voltage Complementary Circuits with Solution‐Deposited Organic Semiconductor Single‐Crystal Films

Abstract Organic semiconductor single crystals (OSSCs) hold promising prospects in high‐performance organic field‐effect transistors (OFETs) owing to the advantages of longrange ordering and few defects. However, until now, OSSCs have not shown their strength in flexible complementary integrated circuits, partly due to the lack of high‐quality dielectric layers suitable for both large‐area crystal growth by solution method and the construction of high‐performance n‐channel and p‐channel transistors simultaneously. Herein, flexible OFETs are fabricated with solution‐processed large‐area OSSCs and dual‐crosslinked bilayer dielectrics, in which the bottom high‐k polymer provides key dielectric properties and the top low‐k polymer offers improved semiconductor/dielectric interface. Thus, both n‐channel and p‐channel OFETs with high mobility (electron mobility of 1.97 cm 2 V −1 s −1 and hole mobility of 11.97 cm 2 V −1 s −1 ), low threshold voltage and subthreshold swing are realized with operation voltage of only 5 V, which lead to complementary inverters with a high gain of 59.8 and large noise margins reaching 75% of 1/2 V DD . Moreover, the devices exhibit great electrical bias‐stress stability within 10,000 s, and mechanical flexibility with bending stability up to 10,000 cycles. This efficient manufacturing method of flexible OFETs and complementary inverters with large‐area OSSC films and bilayer dielectric paves the way toward high‐performance and low‐power‐consumption flexible circuits.