Volume 54, Issue 45 pp. 13312-13317
Communication

Energy Migration Upconversion in Manganese(II)-Doped Nanoparticles

Dr. Xiyan Li

Dr. Xiyan Li

Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore)

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Xiaowang Liu

Xiaowang Liu

Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore)

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Daniel M. Chevrier

Daniel M. Chevrier

Department of Chemistry, Dalhousie University, Halifax, Nova Scotia, B3H 4J3 (Canada)

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Dr. Xian Qin

Dr. Xian Qin

Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), 3 Research Link, Singapore 117602 (Singapore)

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Dr. Xiaoji Xie

Dr. Xiaoji Xie

Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore)

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Dr. Shuyan Song

Dr. Shuyan Song

State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022 (P. R. China)

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Prof. Hongjie Zhang

Corresponding Author

Prof. Hongjie Zhang

State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022 (P. R. China)

Hongjie Zhang, State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022 (P. R. China)

Peng Zhang, Department of Chemistry, Dalhousie University, Halifax, Nova Scotia, B3H 4J3 (Canada)

Xiaogang Liu, Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore)

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Prof. Peng Zhang

Corresponding Author

Prof. Peng Zhang

Department of Chemistry, Dalhousie University, Halifax, Nova Scotia, B3H 4J3 (Canada)

Hongjie Zhang, State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022 (P. R. China)

Peng Zhang, Department of Chemistry, Dalhousie University, Halifax, Nova Scotia, B3H 4J3 (Canada)

Xiaogang Liu, Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore)

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Prof. Xiaogang Liu

Corresponding Author

Prof. Xiaogang Liu

Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore)

Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), 3 Research Link, Singapore 117602 (Singapore)

Hongjie Zhang, State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022 (P. R. China)

Peng Zhang, Department of Chemistry, Dalhousie University, Halifax, Nova Scotia, B3H 4J3 (Canada)

Xiaogang Liu, Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore)

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First published: 11 September 2015
Citations: 65

Graphical Abstract

On the up: The upconversion emission of Mn2+ ions can be realized in NaGdF4:Yb/Tm@NaGdF4:Mn core–shell nanoparticles by utilizing energy migration through the gadolinium sublattice (see figure). The multiphoton upconversion process can be further enhanced under pulsed laser excitation at high power densities. The ability of the Mn2+-doped nanoparticles to easily undergo oxidization makes them attractive for use in hydrogen peroxide detection.

Abstract

We report the synthesis and characterization of cubic NaGdF4:Yb/Tm@NaGdF4:Mn core–shell structures. By taking advantage of energy transfer through Yb→Tm→Gd→Mn in these core–shell nanoparticles, we have realized upconversion emission of Mn2+ at room temperature in lanthanide tetrafluoride based host lattices. The upconverted Mn2+emission, enabled by trapping the excitation energy through a Gd3+ lattice, was validated by the observation of a decreased lifetime from 941 to 532 μs in the emission of Gd3+ at 310 nm (6P7/28S7/2). This multiphoton upconversion process can be further enhanced under pulsed laser excitation at high power densities. Both experimental and theoretical studies provide evidence for Mn2+ doping in the lanthanide-based host lattice arising from the formation of F vacancies around Mn2+ ions to maintain charge neutrality in the shell layer.

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