High-performance X-ray detectors are usually based on single crystals, due to the long-range ordering and hence outstanding electronic properties. On the other hand, bulk heterojunctions (BHJs) that can effectively enhance photogenerated exciton dissociation are widely used for photodetectors. The benefits of both spur investigation into how to combine these two strategies to enhance X-ray detection. Here, TiO 2 networks are incorporated into PbI 2 crystals to form interpenetrating type II heterojunctions, namely BHJs. These BHJs exhibit long-range ordering in molecular packing similar to that of single crystals. Compared with single crystals, the long-range ordered BHJs facilitate the separation of photogenerated electrons and holes to inhibit recombination, extend the mobility lifetime product by 6.4 times, and consequently improve X-ray sensitivity by 5.8 times. Hence, this work provides a new strategy using gel-grown crystals to fabricate highperformance X-ray detectors as well as a new platform for studying the behavior of X-raygenerated carriers in BHJs with long-range ordering.

Organic single crystals, with regular molecular packing and fewer structural defects, have presented record-high carrier mobility of various organic semiconductor materials, making them ideal charge-transport media for flexible devices. However,...

Ambipolar organic field‐effect transistors (OFETs) are promising candidates for compact organic complementary circuits. High and balanced ambipolar mobilities that facilitate high operation speed and simplifying layout designs, as well as symmetric electrodes that minimize fabrication complexity are critical integrities for state‐of‐art ambipolar OFETs. Organic single crystals with intrinsic ambipolar characteristics are ideal active layer materials because of the high molecular ordering and low density of defects, whereas the generally low electron mobility hindered their further implantation. In this work, the highly crystallized 6,13‐bis(triisopropylsilylethynyl) pentacene single crystals are employed and successfully unveiled the intrinsic high electron mobility by a facile alcohol treatment approach. The resulting ambipolar OFETs showed averaged hole and electron mobilities both higher than 1 cm2 V−1 s−1 by a single type of metal electrode. The presented ambipolar OFETs not only improved the static and dynamic performance of ambipolar OFET‐based complementary inverters and ring oscillators by showing a high voltage gain of 186 and a short stage delay time of 0.7 ms, but they also allowed one logic gate to show two logic functions and potentially benefit the design and functionalities of future OFET‐based complementary circuits as well.