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We devised a hot-injection synthesis to prepare colloidal double-perovskite Cs 2 NaBiCl 6 nanocrystals (NCs). We also examined the effects of replacing Na + with Ag + cations by preparing and characterizing Cs 2 Na 1- x  Ag  x  BiCl 6 alloy NCs with x ranging from 0 to 1. Whereas Cs 2 NaBiCl 6 NCs were not emissive, Cs 2 Na 1- x  Ag  x  BiCl 6 NCs featured a broad photoluminescence band at ∼690 nm, Stokes-shifted from the respective absorption by ≥1.5 eV. The emission efficiency was maximized for low Ag + amounts, reaching ∼3% for the Cs 2 Na 0.95 Ag 0.05 BiCl 6 composition. Density functional theory calculations coupled with spectroscopic investigations revealed that Cs 2 Na 1- x  Ag  x  BiCl 6 NCs are characterized by a complex photophysics stemming from the interplay of (i) radiative recombination via trapped excitons localized in spatially connected AgCl 6 -BiCl 6 octahedra; (ii) surface traps, located on undercoordinated surface Bi centers, behaving as phonon-assisted nonradiative decay channels; and (iii) a thermal equilibrium between trapping and detrapping processes. These results offer insights into developing double-perovskite NCs with enhanced optoelectronic efficiency.

Compositional Tuning of Carrier Dynamics in Cs2Na1–xAgxBiCl6 Double-Perovskite Nanocrystals

Compositional Tuning of Carrier Dynamics in Cs₂Na_1–xAg_xBiCl₆ Double-Perovskite Nanocrystals