The
incorporation of manganese (Mn) ions into Cd(Zn)-chalcogenide
QDs activates strong spin-exchange interactions between the magnetic
ions and intrinsic QD excitons that have been exploited for color
conversion, sunlight harvesting, electron photoemission, and advanced
imaging and sensing. The ability to take full advantage of novel functionalities
enabled by Mn dopants requires accurate control of doping levels over
a wide range of Mn contents. This, however, still represents a considerable
challenge. Specific problems include the difficulty in obtaining high
Mn contents, considerable broadening of QD size dispersion during
the doping procedure, and large batch-to-batch variations in the amount
of incorporated Mn. Here, we show that these problems originate from
the presence of unreacted cadmium (Cd) complexes whose abundance is
linked to uncontrolled impurities participating in the QD synthesis.
After identifying these impurities as secondary phosphines, we modify
the synthesis by introducing controlled amounts of “functional”
secondary phosphine species. This allows us to realize a regime of
nearly ideal QD doping when incorporation of magnetic ions occurs
solely via addition of Mn–Se units without uncontrolled deposition
of Cd–Se species. Using this method, we achieve very high per-dot
Mn contents (>30% of all cations) and thereby realize exceptionally
strong exciton-Mn exchange coupling with g-factors
of ∼600.