Enhanced Photoluminescence and Imaging Applications of Sb-Doped CsCdCl and CsCdCl Driven by Structure-Property Relationships.

Ruddlesden-Popper phases CsCdCl and CsCdCl are widely used in experimental research of optoelectronics due to their excellent doping matrix properties, but their optoelectronic mechanisms have not been fully explored. This study uses first-principles calculations and experiments to analyze the differences in point defect crystal growth and optoelectronic properties caused by Sb doping of these two materials. Sb tends to replace the position of Cd in both structures. Additional doping energy levels are introduced in the Sb doping of CsCdCl, and the flat band edge increases the local charge density and improves the electron-hole recombination efficiency. The photoluminescence quantum yield (PLQY) of 0.1% Sb:CsCdCl doping is as high as 79.09%. Molecular dynamics simulations show that the octahedral distortion of [SbCl] in CsCdCl is highly sensitive to temperature, and the Jahn-Teller distortion causes the formation of self-trapped excitons, which is more conducive to the generation of exciton recombination luminescence. In contrast, Sb doping of CsCdCl produces a lower PLQY, which can be explained by the more delocalized charge distribution at its band edges and the lower octahedral structural distortion. Sb:CsCdCl exhibits high-performance X-ray imaging capabilities. This work provides valuable insights and guidance for optimizing Sb-doped Cd-based optoelectronic materials.