Highly stable hetero-structured green-emitting cesium lead bromide nanocrystals via ligand-mediated phase control.

Green-emissive Cs4PbBr6 shows promise for light-emitting diode devices superior to that of CsPbBr3 NCs owing to their stability and high photoluminescence efficiency. Nevertheless, there is still no consensus regarding the basis of their green emission, which decelerates their advance in light-emitting applications. Herein, a systematic investigation on the concentration of capping ligands (oleylamine and oleic acid), which determines the predominant phase between CsPbBr3 and Cs4PbBr6 for a given Cs to Pb feed ratio, is conducted. This study deduces that oleylamine to oleic acid ratio plays a crucial role in obtaining either green-emissive or non-emissive Cs4PbBr6 NCs. Scrutiny of Cs4PbBr6 microscopic and optical data in addition to their emission quenching study with a hole-withdrawing molecule reveals that the green emission originates from the CsPbBr3 impurity phase. Furthermore, stable green emission is observed for CsPbBr3/Cs4PbBr6 nanocrystals when CsPbBr3 particles are well protected by the Cs4PbBr6 matrix. These CsPbBr3/Cs4PbBr6 films remained highly luminescent even after UV exposure for hours or annealing at ∼150 °C for days in addition to their long-term stability under an ambient atmosphere, which are the desirable properties for various practical applications.