A sandwiched luminescent heterostructure based on lanthanide‐doped Gd2O2S@NaYF4 core/shell nanocrystals

Abstract Lanthanide (Ln3+) oxysulfide nanocrystals (NCs) have great prospect in many advanced technologies; however, they suffer from a low photoluminescence efficiency due to the volatility of sulfur and deleterious surface quenching effect. Herein, we report a novel sandwiched luminescent heterostructure based on Ln3+‐doped Gd2O2S@NaYF4 core/shell NCs with tunable sulfur content in the sandwich layer. By means of Eu3+ as the sensitive structural probes, we unravel the ligand‐mediated structure control of the NCs from Gd2O3: Ln3+@NaYF4 to Gd2O2S: Ln3+@NaYF4 with tailored S2– deficiency. Such a sandwich‐type core/shell heterostructure enables us to achieve efficient and multicolor downshifting and upconversion luminescence (UCL), with up to 208.8 folds of enhancement in UCL intensity as compared to that of their core‐only counterparts. These findings provide a general approach for the controlled synthesis of lanthanide oxysulfide@fluoride heterostructure, which offers a new way for the materials design towards diverse emerging applications.