4.8 Article

Decoupling and Coupling of the Host-Dopant Interaction by Manipulating Dopant Movement in Core/Shell Quantum Dots

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 11, Issue 15, Pages 5992-5999

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c01861

Keywords

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Funding

  1. Syracuse University
  2. ACS-PRF [59861-DNI5]
  3. NSF [CHE-1944978, CHE-1349892]
  4. NSF MRSEC program [DMR-1719875]
  5. National Institutes of Health [NIH/NIBIB R010EB00315]
  6. National Science Foundation [DMR1708617]
  7. U.S. Department of Energy (DOE)
  8. MRCAT member institutions
  9. DOE Office of Science [DE-AC02-06CH11357]

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Doping through the incorporation of transition metal ions allows for the emergence of new optical, electrical, and magnetic properties in quantum dots (QDs). While dopants can be introduced into QDs through many synthetic methods, the control of dopant location and host-dopant (H-D) coupling through directional dopant movement is still largely unexplored. In this work, we have studied dopant behaviors in Mn:CdS/ZnS core/shell QDs and found that dopant transport behavior is very sensitive to the temperature and microenvironments within the QDs. The migration of Mn toward the alloyed interface of the core/shell QDs, below a temperature boundary (T-b) at similar to 200 degrees C, weakens the H-D interactions. At temperatures higher than the T-b, however, dopant ejection and global alloying of CdS/ZnS QDs can occur, leading to stronger H-D coupling. The behavior of incorporated dopants inside QDs is fundamentally important for understanding doping mechanisms and the host-dopant interaction-dependent properties of doped nanomaterials.

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