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Quantification of the Activator and Sensitizer Ion Distributions in NaYF4:Yb3+, Er3+ Upconverting Nanoparticles Via Depth-Profiling with Tender X-Ray Photoemission

  • The spatial distribution and concentration of lanthanide activator and sensitizer dopant ions are of key importance for the luminescence color and efficiency of upconverting nanoparticles (UCNPs). Quantifying dopant ion distributions and intermixing, and correlating them with synthesis methods require suitable analytical techniques. Here, X-ray photoelectron spectroscopy depth-profiling with tender X-rays (2000–6000 eV), providing probe depths ideally matched to UCNP sizes, is used to measure the depth-dependent concentration ratios of Er3+ to Yb3+, [Er3+]/[Yb3+], in three types of UCNPs prepared using different reagents and synthesis methods. This is combined with data simulations and inductively coupled plasma-optical emission spectroscopy (ICP-OES) measurements of the lanthanide ion concentrations to construct models of the UCNPs’ dopant ion distributions. The UCNP sizes and architectures are chosen to demonstrate the potential of this approach. Core-only UCNPs synthesized withThe spatial distribution and concentration of lanthanide activator and sensitizer dopant ions are of key importance for the luminescence color and efficiency of upconverting nanoparticles (UCNPs). Quantifying dopant ion distributions and intermixing, and correlating them with synthesis methods require suitable analytical techniques. Here, X-ray photoelectron spectroscopy depth-profiling with tender X-rays (2000–6000 eV), providing probe depths ideally matched to UCNP sizes, is used to measure the depth-dependent concentration ratios of Er3+ to Yb3+, [Er3+]/[Yb3+], in three types of UCNPs prepared using different reagents and synthesis methods. This is combined with data simulations and inductively coupled plasma-optical emission spectroscopy (ICP-OES) measurements of the lanthanide ion concentrations to construct models of the UCNPs’ dopant ion distributions. The UCNP sizes and architectures are chosen to demonstrate the potential of this approach. Core-only UCNPs synthesized with XCl3·6H2O precursors (β-phase) exhibit a homogeneous distribution of lanthanide ions, but a slightly surface-enhanced [Er3+]/[Yb3+] is observed for UCNPs prepared with trifluroacetate precursors (α-phase). Examination of Yb-core@Er-shell UCNPs reveals a co-doped, intermixed region between the single-doped core and shell. The impact of these different dopant ion distributions on the UCNP's optical properties is discussed to highlight their importance for UCNP functionality and the design of efficient UCNPs.zeige mehrzeige weniger

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Metadaten
Autor*innen:P.C.J Clark, Elina AndresenORCiD, M. J. Sear, M. Favaro, L. Girardi, R. van de Krol, Ute Resch-GengerORCiD, D.E. Starr
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):Small
Jahr der Erstveröffentlichung:2022
Organisationseinheit der BAM:1 Analytische Chemie; Referenzmaterialien
1 Analytische Chemie; Referenzmaterialien / 1.2 Biophotonik
Veröffentlichende Institution:Bundesanstalt für Materialforschung und -prüfung (BAM)
Verlag:Wiley-VCH-Verlag
Verlagsort:Weinheim, Germany
Aufsatznummer:2107976
Erste Seite:1
Letzte Seite:13
DDC-Klassifikation:Naturwissenschaften und Mathematik / Chemie / Analytische Chemie
Freie Schlagwörter:Coating; Core-shell; Excitation power density; HAXPES; Intermixing; Lanthanide; Method; Nano; Nanomaterial; Photoluminescence; Photophysics; Quantum yield; Shell; Surface; Upconversion nanoparticle; XPS
Themenfelder/Aktivitätsfelder der BAM:Chemie und Prozesstechnik
Material
Material / Nano
DOI:10.1002/smll.202107976
URN:urn:nbn:de:kobv:b43-552075
ISSN:1613-6813
Verfügbarkeit des Dokuments:Datei für die Öffentlichkeit verfügbar ("Open Access")
Lizenz (Deutsch):License LogoCreative Commons - CC BY - Namensnennung 4.0 International
Datum der Freischaltung:07.07.2022
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:07.07.2022
Schriftenreihen ohne Nummerierung:Wissenschaftliche Artikel der BAM
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