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Lead free double perovskites (DPs) are promising materials due to their non-toxic and tunable optical properties. In this work, a series of lead-free halide DP single crystals (SCs) and nanocrystals (NCs) (Cs 4 Cu 1-x Ag 2x Sb 2 Cl 12 ) were reported. With alloying strategy, the optical band-gap engineering was realized and the dimension can be controlled between 2D and 3D. The Cu-alloyed SCs exhibit strong absorption from the UV-visible region to the near-infrared range (can even completely cover the bands of NIR-I and NIR-II). In addition, (Cs 4 Cu 1-x Ag 2x Sb 2 Cl 12 ) NCs were synthesized via a top-down approach, which maintains similar optical properties and the dimensional transformation phenomenon to SCs. These results suggest the great potential of Cs 4 Cu 1-x Ag 2x Sb 2 Cl 12  SCs and NCs for photovoltaic and optoelectronic applications.

Band-Gap and Dimensional Engineering in Lead-Free Inorganic Halide Double Perovskite Cs4Cu1-xAg2xSb2Cl12 Single Crystals and Nanocrystals