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Bright Blue Emitting Cu-Doped Cs₂ZnCl₄ Colloidal Nanocrystals.

ABSTRACT: We report here the synthesis of undoped and Cu-doped Cs₂ZnCl₄ nanocrystals (NCs) in which we could tune the concentration of Cu from 0.7 to 7.5%. Cs₂ZnCl₄ has a wide band gap (4.8 eV), and its crystal structure is composed of isolated ZnCl₄ tetrahedra surrounded by Cs⁺ cations. According to our electron paramagnetic resonance analysis, in 0.7 and 2.1% Cu-doped NCs the Cu ions were present in the +1 oxidation state only, while in NCs at higher Cu concentrations we could detect Cu(II) ions (isovalently substituting the Zn(II) ions). The undoped Cs₂ZnCl₄ NCs were non emissive, while the Cu-doped samples had a bright intragap photoluminescence (PL) at ∼2.6 eV mediated by band-edge absorption. Interestingly, the PL quantum yield was maximum (∼55%) for the samples with a low Cu concentration ([Cu] ≤ 2.1%), and it systematically decreased when further increasing the concentration of Cu, reaching 15% for the NCs with the highest doping level ([Cu] = 7.5%). The same (∼2.55 eV) emission band was detected under X-ray excitation. Our density functional theory calculations indicated that the PL emission could be ascribed only to Cu(I) ions: these ions promote the formation of trapped excitons, through which an efficient emission takes place. Overall, these Cu-doped Cs₂ZnCl₄ NCs, with their high photo- and radio-luminescence emission in the blue spectral region that is free from reabsorption, are particularly suitable for applications in ionizing radiation detection.

SUBMITTER: Zhu D

PROVIDER: S-EPMC8016065 | biostudies-literature |

REPOSITORIES: biostudies-literature

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