TY - JOUR
T1 - Decoupling and Coupling of the Host-Dopant Interaction by Manipulating Dopant Movement in Core/Shell Quantum Dots
AU - Hofman, Elan
AU - Khammang, Alex
AU - Wright, Joshua T.
AU - Li, Zhi Jun
AU - McLaughlin, Peter Francis
AU - Davis, Andrew Hunter
AU - Franck, John Mark
AU - Chakraborty, Arindam
AU - Meulenberg, Robert W.
AU - Zheng, Weiwei
N1 - Funding Information:
W.Z. acknowledges support from a start-up grant from Syracuse University, ACS-PRF #59861-DNI5, and NSF CHE-1944978. Transmission electron microscopy measurements were performed at the Cornell Center for Materials Research (CCMR), which are supported through the NSF MRSEC program (DMR-1719875). The authors appreciate Dr. Boris Dzikovski for the assistance with EPR measurements. This work for ACERT was supported by National Institutes of Health Grant NIH/NIBIB R010EB00315. The work at the University of Maine and Illinois Institute of Technology was supported by National Science Foundation Grant DMR-1708617. Materials Research Collaborative Access Team (MRCAT) operations are supported by the U.S. Department of Energy (DOE) and the MRCAT member institutions. Portions of this research used resources of the Advanced Photon Source, a DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. A. C. acknowledges support from NSF under Grant No. CHE-1349892.
Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/8/6
Y1 - 2020/8/6
N2 - 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 (Tb) at â200 °C, weakens the H-D interactions. At temperatures higher than the Tb, 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.
AB - 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 (Tb) at â200 °C, weakens the H-D interactions. At temperatures higher than the Tb, 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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U2 - 10.1021/acs.jpclett.0c01861
DO - 10.1021/acs.jpclett.0c01861
M3 - Article
C2 - 32633980
AN - SCOPUS:85089612632
SN - 1948-7185
VL - 11
SP - 5992
EP - 5999
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 15
ER -