Accurate detection of x-ray radiation is essential for tissue equivalence detection and safety control during medical radiotherapy. Here, a promising radiation detector based on organic 1,8-naphthalimide (C12H7NO2, NTI) single crystals is proposed. NTI single crystals with dimensions of 8 × 2 × 1 mm3 were synthesized by an optimized solvent-cooling method, and the crystal structure was characterized to elucidate the anisotropy mechanism. The coplanar detector made by NTI has a leakage current of less than 0.1 pA at an electric field strength of 1 kV cm−1 and provides excellent detection of 5.49 MeV α-particles (241Am) with a full-energy peak resolution of up to 32.3%. The calculated electron mobility (μe) and electron mobility-lifetime product (μτ)e were 7.9 cm2 V−1s−1 and 1.56 × 10−6 cm2 V−1, respectively. Additionally, the detection limit of the NTI detector was 0.35 µGy s−1 in the electric field strength range of 0.2–1.0 kV cm−1 under a 20 kV x-ray beam with a high sensitivity of 56.2 μC Gy−1cm−2. Consequently, the NTI detector achieves an excellent spatial resolution of 0.8–0.9 lp mm−1 in terms of x-ray imaging capability.
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