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Research Article | Open Access

Volume and surface effects on two-photonic and three-photonic processes in dry co-doped upconversion nanocrystals

Bettina Grauel1Christian Würth1Christian Homann3Lisa Krukewitt1,Elina Andresen1Janina Roik2Sebastian Recknagel2Markus Haase3( )Ute Resch-Genger1( )
Federal Institute for Materials Research and Testing (BAM), Division 1.2 Biophotonics, Richard-Willstaetter-Str. 11, 12489 Berlin, Germany
Federal Institute for Materials Research and Testing (BAM), Division 1.6 Inorganic Reference Materials, Richard-Willstaetter-Str. 11, 12489 Berlin, Germany
Institute of Chemistry of New Materials, Department Biology/Chemistry, University Osnabrueck, Barbarastr. 7, 49076 Osnabrueck, Germany
Present address: Department of Anesthesiology and Intensive Care Medicine, University Medical Center Rostock, Schillingallee 35, 18057 Rostock, Germany
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Abstract

Despite considerable advances in synthesizing high-quality core/shell upconversion (UC) nanocrystals (NC; UCNC) and UCNC photophysics, the application of near-infrared (NIR)-excitable lanthanide-doped UCNC in the life and material sciences is still hampered by the relatively low upconversion luminescence (UCL) of UCNC of small size or thin protecting shell. To obtain deeper insights into energy transfer and surface quenching processes involving Yb3+ and Er3+ ions, we examined energy loss processes in differently sized solid core NaYF4 nanocrystals doped with either Yb3+ (YbNC; 20% Yb3+) or Er3+ (ErNC; 2% Er3+) and co-doped with Yb3+ and Er3+ (YbErNC; 20% Yb3+ and 2% Er3+) without a surface protection shell and coated with a thin and a thick NaYF4 shell in comparison to single and co-doped bulk materials. Luminescence studies at 375 nm excitation demonstrate back-energy transfer (BET) from the 4G11/2 state of Er3+ to the 2F5/2 state of Yb3+, through which the red Er3+ 4F9/2 state is efficiently populated. Excitation power density (P)-dependent steady state and time-resolved photoluminescence measurements at different excitation and emission wavelengths enable to separate surface-related and volume-related effects for two-photonic and three-photonic processes involved in UCL and indicate a different influence of surface passivation on the green and red Er3+ emission. The intensity and lifetime of the latter respond particularly to an increase in volume of the active UCNC core. We provide a three-dimensional random walk model to describe these effects that can be used in the future to predict the UCL behavior of UCNC.

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Nano Research
Pages 2362-2373
Cite this article:
Grauel B, Würth C, Homann C, et al. Volume and surface effects on two-photonic and three-photonic processes in dry co-doped upconversion nanocrystals. Nano Research, 2022, 15(3): 2362-2373. https://doi.org/10.1007/s12274-021-3727-y
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Received: 23 February 2021
Revised: 01 July 2021
Accepted: 03 July 2021
Published: 28 August 2021
© The Author (s) 2021

Copyright: 2021 by the author(s). This article is an open access article distributed under Creative Commons Attribution License (CC BY 4.0), visit https://creativecommons.org/licenses/by/4.0/.

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