Interface Collaborative Strategy for High Mobility Organic Single‐Crystal Field‐Effect Transistors with Ideal Current–Voltage Curves

The key roles of electrode/semiconductor and semiconductor/dielectric interfaces play in the ideality of organic field‐effect transistors (OFETs) by traditional device preparation technologies are not yet fully understood, which severely limits progress in the design of molecules, the understanding of transport mechanisms, and the circuit applications of OFETs. Herein, at a quantitative level, the origin of nonideal current–voltage (I–V) curves and possibly overestimated mobility in single‐crystal OFETs is revealed, including contact resistance (Rc), charge trapping, and scattering at interfaces of devices. Impressively, an efficient interface collaborative strategy, which consists of transferred “doped” electrodes with tunable contact “doping” localized regions at the source‐drain contacts and polymer‐modified SiO2 with suitable surface polarity (γsp) is further demonstrated that have great advantages in the construction of ideal high mobility devices. Also, an interesting double‐edged sword effect of γsp of dielectric on the ideality of OFETs is observed. The dielectric with a lower γsp can result in higher mobility, while too low γsp would degrade the device ideality due to significant effect of charge scattering. The findings not only provide new perspectives and strategies to construct ideal OFETs but also offer useful guidance to correctly evaluate organic semiconductor materials. A high‐efficiency “interface collaborative strategy”, comprising of transferring “doped” electrodes and utilizing polymer modified layer on SiO2 with suitable surface polarity (γsp) is demonstrated that have great advantages in constructing ideal single‐crystal OFETs attributed to tunable injection contact without direct chemical bonding and weakened charge scattering effect, providing some useful guidance to correctly evaluate organic semiconductor materials.