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Tuning upconversion through energy migration in core–shell nanoparticles

Nature Materials volume 10, pages 968–973 (2011)Cite this article

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Abstract

Photon upconversion is promising for applications such as biological imaging, data storage or solar cells. Here, we have investigated upconversion processes in a broad range of gadolinium-based nanoparticles of varying composition. We show that by rational design of a core–shell structure with a set of lanthanide ions incorporated into separated layers at precisely defined concentrations, efficient upconversion emission can be realized through gadolinium sublattice-mediated energy migration for a wide range of lanthanide activators without long-lived intermediary energy states. Furthermore, the use of the core–shell structure allows the elimination of deleterious cross-relaxation. This effect enables fine-tuning of upconversion emission through trapping of the migrating energy by the activators. Indeed, the findings described here suggest a general approach to constructing a new class of luminescent materials with tunable upconversion emissions by controlled manipulation of energy transfer within a nanoscopic region.

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Figure 1: Simplified energy level diagrams depicting reported and proposed anti-Stokes processes.
Figure 2: Tuning upconversion through energy migration in core–shell nanoparticles.
Figure 3: Mechanistic investigation of the EMU process in core–shell nanoparticles.
Figure 4: Effect of energy transfer between nanoparticles by means of energy migration.

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Acknowledgements

The bulk of the work was supported by the Singapore Ministry of Education (No. MOE2010T2-1-083), the Singapore-MIT Alliance, and the Agency for Science, Technology and Research (No. IMRE/11-1C0110). Y.H. is grateful to KAUST Global Collaborative Research for the Academic Excellence Alliance (AEA) fund. H.Z. and X.C. acknowledge the financial support from the NSFC (Nos. 10974200 and 51002151) and the 863 programs of MOST (Nos. 2009AA03Z430 and 2011AA03A407). We thank T. Nguyen, Y. Liu and L. Tan for their help in sample characterization.

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Authors and Affiliations

  1. Department of Chemistry, National University of Singapore, 117543, Singapore

    Feng Wang, Renren Deng, Juan Wang & Xiaogang Liu

  2. Advanced Membrane and Porous Materials Center & Imaging and Characterization Core Lab, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia

    Qingxiao Wang & Yu Han

  3. Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China

    Haomiao Zhu & Xueyuan Chen

  4. Institute of Materials Research and Engineering, 3 Research Link, 117602, Singapore

    Xiaogang Liu

  5. Singapore-MIT Alliance, 4 Engineering Drive 3, 117576, Singapore

    Xiaogang Liu

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Contributions

F.W. and X.L. conceived the experiments and wrote the paper. F.W., R.D. and J.W. were primarily responsible for the experiments. Q.W. and Y.H. performed the STEM, EDX and EELS characterizations. H.Z. and X.C. carried out the time-decay measurements. All authors contributed to the analysis of this manuscript.

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Correspondence to Xiaogang Liu.

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Wang, F., Deng, R., Wang, J. et al. Tuning upconversion through energy migration in core–shell nanoparticles. Nature Mater 10, 968–973 (2011). https://doi.org/10.1038/nmat3149

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