Tracking the motion of lanthanide ions within core-shell-shell NaYF4 nanocrystals via resonance energy transfer
- Lanthanide resonance energy transfer (LRET) was used to investigate the motion of dopant ions during the synthesis of core-shell-shell-nanocrystals (NCs) that are frequently used as frequency upconversion materials. Reaction conditions (temperature, solvent) as well as lattice composition and precursors were adapted from a typical hydrothermal synthesis approach used to obtain upconversion nanoparticles (UCNPs). Instead of adding the lanthanide ions Yb3+/Er3+ as the sensitizer/activator couple, Eu3+/Nd3+ as the donor/acceptor were added as the LRET pair to the outer shell (Eu-3) and the core (Nd-3). By tailoring the thickness of the insulation shell ("middle shell"), the expected distance between the donor and the acceptor was increased beyond 2 R-0, a distance for which no LRET is expected. The successful synthesis of core- shell-shell NCs with different thicknesses of the insulation layer was demonstrated by high-resolution transmission electron microscopy measurement. The incorporation of the Eu3+ ions into the NaYF4 lattice wasLanthanide resonance energy transfer (LRET) was used to investigate the motion of dopant ions during the synthesis of core-shell-shell-nanocrystals (NCs) that are frequently used as frequency upconversion materials. Reaction conditions (temperature, solvent) as well as lattice composition and precursors were adapted from a typical hydrothermal synthesis approach used to obtain upconversion nanoparticles (UCNPs). Instead of adding the lanthanide ions Yb3+/Er3+ as the sensitizer/activator couple, Eu3+/Nd3+ as the donor/acceptor were added as the LRET pair to the outer shell (Eu-3) and the core (Nd-3). By tailoring the thickness of the insulation shell ("middle shell"), the expected distance between the donor and the acceptor was increased beyond 2 R-0, a distance for which no LRET is expected. The successful synthesis of core- shell-shell NCs with different thicknesses of the insulation layer was demonstrated by high-resolution transmission electron microscopy measurement. The incorporation of the Eu3+ ions into the NaYF4 lattice was investigated by high-resolution time-resolved luminescence measurements. Two major Eu3+ species (bulk and surface) were found. This was supported by steady-state as well as time-resolved luminescence data. Based on the luminescence decay kinetics, the intermixing of lanthanides during synthesis of core- shell UCNPs was evaluated. The energy transfer between Eu3+ (donor) and Nd3+ (acceptor) ions was exploited to quantify the motion of the dopant ions. This investigation reveals the migration of Ln(3+) ions between different compatiments in core-shell NCs and affects the concept of using core-shell architectures to increase the efficiency of UCNPs. In order to obtain well-separated core and shell structures with different dopants, alternative concepts are needed.…
Author details: | Philipp U. BastianORCiDGND, Selma NacakORCiDGND, Vladimir RoddatisORCiD, Michael Uwe KumkeORCiDGND |
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DOI: | https://doi.org/10.1021/acs.jpcc.0c02588 |
ISSN: | 1932-7447 |
ISSN: | 1932-7455 |
Title of parent work (English): | The journal of physical chemistry : C |
Publisher: | American Chemical Society |
Place of publishing: | Washington, DC |
Publication type: | Article |
Language: | English |
Date of first publication: | 2020/04/24 |
Publication year: | 2020 |
Release date: | 2023/05/23 |
Volume: | 124 |
Issue: | 20 |
Number of pages: | 10 |
First page: | 11229 |
Last Page: | 11238 |
Funding institution: | Helmholtz Recruiting Initiative [I-044-16-01]; Republic of Turkey,; Ministry of National EducationMinistry of National Education - Turkey; [YLSY-2010]; Helmholtz-Graduate School Macromolecular Bioscience; (MacroBio), Helmholtz-Zentrum Geesthach |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC classification: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften |
Peer review: | Referiert |