Role of Magnetic Coupling in Photoluminescence Kinetics of Mn2+-Doped ZnS Nanoplatelets

Mn2+-doped semiconductor nanocrystals with tuned location and concentration of Mn2+ ions can yield diverse coupling regimes, which can highly influence their optical properties such as emission wavelength and photoluminescence (PL) lifetime. However, investigation on the relationship between the Mn2+ concentration and the optical properties is still challenging because of the complex interactions of Mn2+ ions and the host and between the Mn2+ ions. Here, atomically flat ZnS nanoplatelets (NPLs) with uniform thickness were chosen as matrixes for Mn2+ doping. Using time-resolved (TR) PL spectroscopy and density functional theory (DFT) calculations, a connection between coupling and PL kinetics of Mn2+ ions was established. Moreover, it is found that the Mn2+ ions residing on the surface of a nanostructure produce emissive states and interfere with the change of properties by Mn2+-Mn2+ coupling. In a configuration with suppressed surface contribution to the optical response, we show the underlying physical reasons for double and triple exponential decay by DFT methods. We believe that the presented doping strategy and simulation methodology of the Mn2+-doped ZnS (ZnS:Mn) system is a universal platform to study dopant location- and concentration-dependent properties also in other semiconductors.

Automated summary

Investigation on Mn2+-doped semiconductor nanocrystals with tuned location and concentration of Mn2+ ions has shown that the optical properties, such as emission wavelength and photoluminescence lifetime, are highly influenced by these factors. Atomically flat ZnS nanoplatelets were used as matrixes for Mn2+ doping, revealing a connection between coupling and PL kinetics of Mn2+ ions through time-resolved PL spectroscopy and DFT calculations. It was found that Mn2+ ions residing on the surface of a nanostructure produce emissive states and interfere with the change of properties by Mn2+-Mn2+ coupling, with the physical reasons for double and triple exponential decay being explained by DFT methods.