Flexible thin-film transistors (TFTs) based on N-doped Ba(Ti,Zr,Mo,Hf,Ta)O3 dielectric and ZnSnO channel show high electrical and UV-sensing performance. The optimal N-doped Ba(Ti,Zr,Mo,Hf,Ta)O3 compositions with low equivalent oxide thicknesses (≈2 nm) and high-entropy (configurational entropy ≈ 1.59 R) are efficiently determined from a wide composition space (library). The film library is patterned to 450 metal–insulator-metal stacks, revealing dielectric constants ≈ 262–322 and loss (tan δ) ≈ 0.01–0.30 for the N-doped Ba(Ti,Zr,Mo,Hf,Ta)O3 at 1 kHz. The library is further integrated to 63 TFTs, and the promising ones exhibit the remarkable parameters: current on/off ratio of 108, threshold voltage (VT) of 0.02 V, saturation field-effect mobility of ≈76 cm2⋅V−1⋅s−1, and subthreshold swing of 0.062 V dec−1. The devices also exhibit desirable long-term stability for up to five months and perform reliably with small or negligible changes in VT and drain-source current under various gate-bias stress and temperature conditions. Furthermore, the TFT-based ultraviolet (253 nm) detector demonstrates impressive sensitivity (≈ 2 × 106) and responsibility (≈ 1171.9 A W−1). There is no substantial degradation in electrical or sensing characteristics under various levels of deformation. Charge transport in constructed energy band diagrams is used to elucidate the observed remarkable performance.
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