Rb 4 CuSb 2 Cl 11 and Rb 2 In 0.91(0.2) Sb 0.09 Cl 5 ·H 2 O: Wide Band Gap 0D Metal Halide Semiconductors

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Abstract
Herein, we report the discovery, structural and photophysical characterization of a new zero-dimensional (0D) lead-free all-inorganic halide, Rb4CuSb2Cl11, which adopts a new structure type. Single-crystal X-ray diffraction (SCXRD) shows that the structure consists of isolated, distorted seesaw [SbCl4]- and trigonal planar [CuCl3]2- units, separated by Rb+ cations that provide charge balance. Optoelectronic measurements and density functional theory (DFT) calculations indicate an indirect band gap of 2.89 eV, making it a candidate for wide-bandgap optoelectronic applications. Electrical resistivity was measured at 1.29 × 1010 Ω·cm, and the trap-state density (ntrap) was found to be 7.44 × 1010 cm-3. Attempts to synthesize substitution analogs of Rb4CuSb2Cl11 led to the synthesis of Rb2In0.91(0.2)Sb0.09Cl5·H2O, which was erroneously reported as Rb2SbCl5O in a previous study. Rb2In0.91(0.2)Sb0.09Cl5·H2O adopts a vacancy-ordered perovskite structure and exhibits broad-band yellow emission under UV excitation. The measured photoluminescence quantum yield (PLQY) for Rb2In0.91(0.2)Sb0.09Cl5·H2O is 18.2%. These findings add to the growing class of quaternary metal halides with multiple cation and anion compositions, expanding the chemical phase space for the discovery of new materials with functional properties.
Funding Information
  • Welch Foundation (E-2181)
  • U.S. Department of Energy (DE-SC0020300)
  • National Aeronautics and Space Administration (80NSSC23M73)
  • National Institute of General Medical Sciences (P20GM103640)
  • National Institute of General Medical Sciences (P30GM145423)
  • National Science Foundation (0922269)

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