Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 130, Issue 32, Pages 10605-10611Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja801249z
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It has been an outstanding problem that a semiconducting host in the bulk form can be doped to a large extent, while the same host in the nanocrystal form is found to resist any appreciable level of doping rather stubbornly, this problem being more acute in the wurtzite form compared to the zinc blende one. In contrast, our results based on the lattice parameter tuning in a ZnxCd1-xS alloy nanocrystal system achieves similar to 7.5% Mn2+ doping in a wurtzite nanocrystal, such a concentration being substantially higher compared to earlier reports even for nanocrystal hosts with the favorable zinc-blende structure. These results prove a consequence of local strains due to a size mismatch between the dopant and the host that can be avoided by optimizing the composition of the alloyed host. Additionally, the present approach opens up a new route to dope such nanocrystals to a macroscopic extent as required for many applications. Photophysical studies show that the quantum efficiency per Mn2+ ion decreases exponentially with the average number of Mn2+ ions per nanocrystal; en route, a high quantum efficiency of similar to 25% is achieved for a range of compositions.
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