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It is found that thiocyanate (SCN) is an alternative dopant that greatly stabilizes the p‐type semiconducting properties of CuI. Thiocyanate doping can be achieved by a complete removal of the excess iodine and introduction of thiocyanate via suitable precursors at ambient temperature. A method of removal of iodine from CuI before casting films is described. The electrical and optical properties of thiocyanate‐doped CuI thin films are also discussed.

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