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Mn2+-doped semiconductor nanocrystals with tuned location and concentrationof Mn2+ ions can yield diverse coupling regimes, which can highly influencetheir 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 thecomplex interactions of Mn2+ ions and the host and between the Mn2+ ions. Here,atomically flat ZnS nanoplatelets (NPLs) with uniform thickness were chosen asmatrixes for Mn2+ doping. Using time-resolved (TR) PL spectroscopy and densityfunctional theory (DFT) calculations, a connection between coupling and PLkinetics of Mn2+ ions was established.  Moreover, it was found that the Mn2+ ions residing on the surface of ananostructure produce emissive states and interfere with the change ofproperties by Mn2+/Mn2+ coupling.  In a configuration with suppressed surface contribution to the opticalresponse we show the underlying physical reasons for double and tripleexponential decay by DFT methods. We believe that the presented doping strategyand simulation methodology of the Mn2+-doped ZnS system is a universal platformto study dopant location- and concentration-dependent properties also in othersemiconductors.

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