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Impact of crystallinity and local disorder on the luminescence properties of solvothermally synthesized LuPO4:Pr3+ nanocrystals

Maji, Sanu Bifal ; Vanetsev, Alexander ; Nagirnyi, Vitali ; Chernenko, Kirill LU ; Feldbach, Eduard ; Kozlova, Jekaterina ; Mändar, Hugo ; Romet, Ivo ; Rähn, Mihkel and Kirm, Marco (2025) In Journal of Materials Chemistry C 13(20). p.10139-10151
Abstract

In this study, we present the solvothermal synthesis of LuPO4:Pr3+ (1%) nanocrystals in a dimethyl sulfoxide-water solvent system. The as-prepared nanocrystals exhibit a relatively high degree of crystallinity, along with significant short-range disorder, particularly in the anionic sublattice, as revealed by XRD and Raman spectroscopy data. Low temperature luminescence spectroscopy under VUV excitation showed that this disorder hinders the energy transfer from the host lattice to the Pr3+ ions, resulting in the absence of the 4f15d1→4f2 emission under high energy excitation. Thermal annealing of as-prepared nanocrystals significantly reduces the degree of local disorders... (More)

In this study, we present the solvothermal synthesis of LuPO4:Pr3+ (1%) nanocrystals in a dimethyl sulfoxide-water solvent system. The as-prepared nanocrystals exhibit a relatively high degree of crystallinity, along with significant short-range disorder, particularly in the anionic sublattice, as revealed by XRD and Raman spectroscopy data. Low temperature luminescence spectroscopy under VUV excitation showed that this disorder hinders the energy transfer from the host lattice to the Pr3+ ions, resulting in the absence of the 4f15d1→4f2 emission under high energy excitation. Thermal annealing of as-prepared nanocrystals significantly reduces the degree of local disorders enhancing UV-C luminescence in the 4.4-5.5 eV range by improving energy transfer processes from the LuPO4 host to Pr3+ ions. Time-integrated luminescence spectra reveal up to a five-fold increase in UV-C emission intensity after annealing. UV-C emissions due to Pr3+ ions in LuPO4 are efficiently excited in the deep intrinsic absorption region at 45 eV, which simulates the energy conversion process for radiotherapy applications. Time-resolved studies identify two types of Pr3+ ions. One group consists of strongly perturbed ions near the nanoparticle surface, influenced by structural imperfections, while the other includes weakly perturbed ions located in the bulk. These results highlight the critical role of local structural imperfections almost undetectable by XRD in energy transfer processes involving the host lattice.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Materials Chemistry C
volume
13
issue
20
pages
13 pages
publisher
Royal Society of Chemistry
external identifiers
  • scopus:105003457548
ISSN
2050-7526
DOI
10.1039/d5tc00391a
language
English
LU publication?
yes
id
c1738781-60ba-4618-b970-5b332911bb2a
date added to LUP
2025-08-12 10:33:26
date last changed
2025-10-14 11:07:01
@article{c1738781-60ba-4618-b970-5b332911bb2a,
  abstract     = {{<p>In this study, we present the solvothermal synthesis of LuPO<sub>4</sub>:Pr<sup>3+</sup> (1%) nanocrystals in a dimethyl sulfoxide-water solvent system. The as-prepared nanocrystals exhibit a relatively high degree of crystallinity, along with significant short-range disorder, particularly in the anionic sublattice, as revealed by XRD and Raman spectroscopy data. Low temperature luminescence spectroscopy under VUV excitation showed that this disorder hinders the energy transfer from the host lattice to the Pr<sup>3+</sup> ions, resulting in the absence of the 4f<sup>1</sup>5d<sup>1</sup>→4f<sup>2</sup> emission under high energy excitation. Thermal annealing of as-prepared nanocrystals significantly reduces the degree of local disorders enhancing UV-C luminescence in the 4.4-5.5 eV range by improving energy transfer processes from the LuPO<sub>4</sub> host to Pr<sup>3+</sup> ions. Time-integrated luminescence spectra reveal up to a five-fold increase in UV-C emission intensity after annealing. UV-C emissions due to Pr<sup>3+</sup> ions in LuPO<sub>4</sub> are efficiently excited in the deep intrinsic absorption region at 45 eV, which simulates the energy conversion process for radiotherapy applications. Time-resolved studies identify two types of Pr<sup>3+</sup> ions. One group consists of strongly perturbed ions near the nanoparticle surface, influenced by structural imperfections, while the other includes weakly perturbed ions located in the bulk. These results highlight the critical role of local structural imperfections almost undetectable by XRD in energy transfer processes involving the host lattice.</p>}},
  author       = {{Maji, Sanu Bifal and Vanetsev, Alexander and Nagirnyi, Vitali and Chernenko, Kirill and Feldbach, Eduard and Kozlova, Jekaterina and Mändar, Hugo and Romet, Ivo and Rähn, Mihkel and Kirm, Marco}},
  issn         = {{2050-7526}},
  language     = {{eng}},
  month        = {{04}},
  number       = {{20}},
  pages        = {{10139--10151}},
  publisher    = {{Royal Society of Chemistry}},
  series       = {{Journal of Materials Chemistry C}},
  title        = {{Impact of crystallinity and local disorder on the luminescence properties of solvothermally synthesized LuPO<sub>4</sub>:Pr<sup>3+</sup> nanocrystals}},
  url          = {{http://dx.doi.org/10.1039/d5tc00391a}},
  doi          = {{10.1039/d5tc00391a}},
  volume       = {{13}},
  year         = {{2025}},
}