The Formation of NaYF4: Er3+, Yb3+ Nanocrystals Studied by In Situ X-ray Scattering: Phase Transition and Size Focusing

P. Tim Prins, Johanna C. van der Bok, Thomas P. van Swieten, Stijn O.M. Hinterding, Andy J. Smith, Andrei V. Petukhov, Andries Meijerink, Freddy T. Rabouw*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

β-NaYF4 nanocrystals are a popular class of optical materials. They can be doped with optically active lanthanide ions and shaped into core-multi-shell geometries with controlled dopant distributions. Here, we follow the synthesis of β-NaYF4 nanocrystals from α-NaYF4 precursor particles using in situ small-angle and wide-angle X-ray scattering and ex situ electron microscopy. We observe an evolution from a unimodal particle size distribution to bimodal, and eventually back to unimodal. The final size distribution is narrower in absolute numbers than the initial distribution. These peculiar growth dynamics happen in large part before the α-to-β phase transformation. We propose that the splitting of the size distribution is caused by variations in the reactivity of α-NaYF4 precursor particles, potentially due to inter-particle differences in stoichiometry. Rate equation modeling confirms that a continuous distribution of reactivities can result in the observed particle growth dynamics.

Original languageEnglish
Article numbere202305086
JournalAngewandte Chemie - International Edition
Volume62
Issue number28
DOIs
Publication statusPublished - 10 Jul 2023

Bibliographical note

Funding Information:
The authors thank Johannes D. Meeldijk for HR‐TEM measurements at the Electron Microscopy Centre Utrecht, Diamond Light Source for providing beamtime (proposal SM21871), the Dutch Research Council (NWO) for funding (Q‐Lumicon 14614, VI.Vidi.203.031), and The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture, and Science of the government of The Netherlands.

Publisher Copyright:
© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Funding

The authors thank Johannes D. Meeldijk for HR‐TEM measurements at the Electron Microscopy Centre Utrecht, Diamond Light Source for providing beamtime (proposal SM21871), the Dutch Research Council (NWO) for funding (Q‐Lumicon 14614, VI.Vidi.203.031), and The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation Programme funded by the Ministry of Education, Culture, and Science of the government of The Netherlands.

FundersFunder number
Electron Microscopy Centre UtrechtSM21871
Dutch Research Council (NWO)14614, VI.Vidi.203.031
Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC)
Ministry of Education, Culture, and Science of the government of The Netherlands

    Keywords

    • Crystal Growth
    • Nanoparticles
    • Phase-Transitions
    • Upconversion
    • X-Ray Scattering

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