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Arteaga Cardona, F.* ; Madirov, E.* ; Popescu, R.* ; Wang, D.* ; Busko, D.* ; Ectors, D.* ; Kübel, C.* ; Eggeler, Y.M.* ; Arus, B.A. ; Chmyrov, A. ; Bruns, O.T. ; Richards, B.S.* ; Hudry, D.*

Dramatic impact of materials combinations on the chemical organization of core-shell nanocrystals: Boosting the Tm3+ emission above 1600 nm.

ACS Nano, DOI: 10.1021/acsnano.4c07932 (2024)
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This article represents the first foray into investigating the consequences of various material combinations on the short-wave infrared (SWIR, 1000-2000 nm) performance of Tm-based core-shell nanocrystals (NCs) above 1600 nm. In total, six different material combinations involving two different types of SWIR-emitting core NCs (α-NaTmF4 and LiTmF4) combined with three different protecting shell materials (α-NaYF4, CaF2, and LiYF4) have been synthesized. All corresponding homo- and heterostructured NCs have been meticulously characterized by powder X-ray diffraction and electron microscopy techniques. The latter revealed that out of the six investigated combinations, only one led to the formation of a true core-shell structure with well-segregated core and shell domains. The direct correlation between the downshifting performance and the spatial localization of Tm3+ ions within the final homo- and heterostructured NCs is established. Interestingly, to achieve the best SWIR performance, the formation of an abrupt interface is not a prerequisite, while the existence of a pure (even thin) protective shell is vital. Remarkably, although all homo- and heterostructured NCs have been synthesized under the exact same experimental conditions, Tm3+ SWIR emission is either fully quenched or highly efficient depending on the type of material combination. The most efficient combination (LiTmF4/LiYF4) achieved a high photoluminescence quantum yield of 39% for SWIR emission above 1600 nm (excitation power density in the range 0.5-3 W/cm2) despite significant intermixing. From now on, highly efficient SWIR-emitting probes with an emission above 1600 nm are within reach to unlock the full potential of in vivo SWIR imaging.
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Publication type Article: Journal article
Document type Scientific Article
Keywords Swir Imaging ; Core−shell ; Material Combinations ; Nanocrystals ; Photoluminescence Quantum Yield ; Shortwave Infrared ; Thulium; Up-conversion Luminescence; Core/shell Nanoparticles; Energy Migration; In-vivo; Enhancement
Language english
Publication Year 2024
HGF-reported in Year 2024
ISSN (print) / ISBN 1936-0851
e-ISSN 1936-086X
Journal ACS Nano
Publisher American Chemical Society (ACS)
Publishing Place 1155 16th St, Nw, Washington, Dc 20036 Usa
Reviewing status Peer reviewed
Institute(s) Helmholtz Pioneer Campus (HPC)
POF-Topic(s) 30205 - Bioengineering and Digital Health
Research field(s) Pioneer Campus
PSP Element(s) G-510001-001
Grants Helmholtz Imaging
Helmholtz Association via Research Field Energy - Program Materials and Technologies for the Energy Transition - Topic 1 Photovoltaics
Helmholtz Association via Professorial Recruitment Initiative Funding
Helmholtz Research Infrastructure at Karlsruhe Institute of Technology (KIT)
Karlsruhe Nano Micro Facility (KNMFi)
DOI 10.1021/acsnano.4c07932
WOS ID 001312737400001
Scopus ID 85203794530
PubMed ID 39264287
Erfassungsdatum 2024-10-23
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