Sb3+ Dopant and Halogen Substitution Triggered Highly Efficient and Tunable Emission in Lead-Free Metal Halide Single Crystals

Jing, YY (Jing, Yuyu)[ 1 ] ; Liu, Y (Liu, Ying)[ 1 ] ; Jiang, XX (Jiang, Xingxing)[ 3 ] ; Molokeev, MS (Molokeev, Maxim S.)[ 4,5,6 ] ; Lin, ZS (Lin, Zheshuai)[ 3,7 ] ; Xia, ZG (Xia, Zhiguo)[ 1,2 ]. CHEMISTRY OF MATERIALS. DOI: 10.1021/acs.chemmater.0c01708

Rational doping and compositional control remain significant challenges in designing luminescent metal halides to achieve highly efficient and tunable emission. Here, the air-stable lead-free Cs2InCl5 center dot H2O crystal with a zero-dimensional structure was investigated as a pristine compound to design new luminescence materials. Sb3+-doping inCs(2)InCl(5)center dot H2O:Sb3+ enabled broadband yellow emission with a photoluminescence quantum yield up to 95.5%. The emission colors can be expanded into the orange-red region by halogen compositional substitution for Cs2InCl5 center dot H2O:Sb3+ (X = Cl/Br/I). The optical characterizations along with the theoretical calculations demonstrate that the characteristic singlet and triplet self-trapped exciton emissions of ns(2)-metal-halide centers account for the tunable luminescence. Moreover, the admirable stability against air and heat pave way for its further applications in white light-emitting diodes and high-resolution fluorescent signs in anticounterfeiting technology. Our achievement in the case of Sb3+-doped Cs2InCl5 center dot H2O represents a successful strategy for developing stable lead-free metal halides with highly efficient emission for versatile optical applications.


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