Enhancing multiphoton upconversion through energy clustering at sublattice level
Macdonald, Mark A B
Hor, Andy Sum Andy
KAUST DepartmentAdvanced Membranes and Porous Materials Research Center
Physical Sciences and Engineering (PSE) Division
Chemical Science Program
Nanostructured Functional Materials (NFM) laboratory
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AbstractThe applications of lanthanide-doped upconversionnanocrystals in biological imaging, photonics, photovoltaics and therapeutics have fuelled a growing demand for rational control over the emission profiles of the nanocrystals. A common strategy for tuning upconversion luminescence is to control the doping concentration of lanthanide ions. However, the phenomenon of concentration quenching of the excited state at high doping levels poses a significant constraint. Thus, the lanthanide ions have to be stringently kept at relatively low concentrations to minimize luminescence quenching. Here we describe a new class of upconversion nanocrystals adopting an orthorhombic crystallographic structure in which the lanthanide ions are distributed in arrays of tetrad clusters. Importantly, this unique arrangement enables the preservation of excitation energy within the sublattice domain and effectively minimizes the migration of excitation energy to defects, even in stoichiometric compounds with a high Yb 3+ content (calculated as 98 mol%). This allows us to generate an unusual four-photon-promoted violet upconversion emission from Er 3+ with an intensity that is more than eight times higher than previously reported. Our results highlight that the approach to enhancing upconversion through energy clustering at the sublattice level may provide new opportunities for light-triggered biological reactions and photodynamic therapy. © 2014 Macmillan Publishers Limited. All rights reserved.
SponsorsThe bulk of the work was supported by the Institute of Materials Research and Engineering (IMRE/12-8C0101) and the Singapore Ministry of Education (MOE2010-T2-1-083). Y.H. is grateful to KAUST Global Collaborative Research for the Academic Excellence Alliance (AEA) fund and P.Z. acknowledges the financial support from NSERC Canada. The PNC/XSD facilities at the Advanced Photon Source are supported by the US Department of Energy (DOE)-Basic Energy Sciences, a Major Resources Support grant from NSERC, the University of Washington, the Canadian Light Source, and the Advanced Photon Source. Use of the Advanced Photon Source was supported by the US DOE under contract no. DE-AC02-06CH11357. We thank PNC/XSD staff beamline scientist R. Gordon for synchrotron technical support. The authors thank H. Zhu, S. Animesh and R. Chen for technical assistance.
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