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[en] Li-based scintillators are promising candidates for thermal neutron detection due to the presence of 6Li nuclei in the host lattice. In this study, pure and doped lithium iodide (LiI) crystals are grown by using the two-zone vertical Bridgman technique with diameters of ∼1 cm and lengths of ∼4 cm. The crystals were doped with Na, CO3 and Tl activators with the aim to develop a scintillator having enhanced neutron detection efficiency. Among the grown crystals, LiI(Tl) showed the highest luminescence intensity under X-ray excitation. The LiI(Tl) crystal exhibited a broad emission spectrum between 300 and 700 nm peaking at 470 nm. Under γ-ray excitation, The LiI(Tl) crystal showed two decay-time components of 180 ns and 900 ns, respectively. The response of the LiI(Tl) crystal to spallation neutrons and the radiation damage effects were determined at the Korea Multi-purpose Accelerator Complex (KOMAC). A clear neutron capture peak was measured at 3 MeVee under spallation-neutron irradiation.