In this work, we prepared the highly efficient yellow light-emitting vacancy-ordered Te4+-doped Rb2ZrCl6 microcrystals (RZCTs) through a hydrothermal method. RZCT with a photoluminescence quantum yield of 34.6% was prepared at Te4+ feeding ratio of 5%. RZCT is used to fabricate high-efficiency white light-emitting diodes, and adjusting the current can realize the transition of cold and warm white light with CIE color coordinates of (0.31, 0.28) and (0.36, 0.37), respectively. It is also applied to non-contact thermometry using photoluminescence lifetime, of which maximum relative and absolute sensitivities were obtained as 0.89% and 4.76 × 10−3 K−1, respectively. The study shows that the lead-free Te4+-doped perovskite microcrystals exist great potential in next-generation solid-state lighting and non-contact optical thermometry.

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