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Phase dependent luminescence properties of Pr3+ doped BaLu2F8–BaLuF5 materials

Maji, Sanu Bifal ; Vanetsev, Alexander ; Mändar, Hugo ; Nagirnyi, Vitali ; Chernenko, Kirill LU ; Kozlova, Jekaterina ; Kotlov, Aleksei ; Smortsova, Yevheniia and Kirm, Marco (2025) In Optical Materials 167.
Abstract

This work presents a comparative luminescence study of Pr3+ doped phase-pure BaLuF5 and mixed-phase BaLu2F8 – BaLuF5 materials synthesized via a hydrothermal route. The spectroscopic studies were mainly performed for phase-pure BaLuF5 and two mixed-phase materials, which, according to structural and phase compositional analysis, contained 90 or 70 wt% of orthorhombic BaLu2F8 and 10 or 30 wt% of cubic BaLuF5, respectively. Low-temperature time-integrated photoluminescence measurements under both host excitation at 45 eV and intracenter excitation of Pr3+ ions at 6.75 eV revealed pronounced differences in luminescence between the... (More)

This work presents a comparative luminescence study of Pr3+ doped phase-pure BaLuF5 and mixed-phase BaLu2F8 – BaLuF5 materials synthesized via a hydrothermal route. The spectroscopic studies were mainly performed for phase-pure BaLuF5 and two mixed-phase materials, which, according to structural and phase compositional analysis, contained 90 or 70 wt% of orthorhombic BaLu2F8 and 10 or 30 wt% of cubic BaLuF5, respectively. Low-temperature time-integrated photoluminescence measurements under both host excitation at 45 eV and intracenter excitation of Pr3+ ions at 6.75 eV revealed pronounced differences in luminescence between the two systems. The phase-pure BaLuF5 material exhibited only narrow 4f2→4f2 transitions of Pr3+, because the 4f15d1states are energetically situated above the highest lying 4f2 1S0 level. In contrast, the BaLu2F8 rich mixed-phase material showed multiple intense broad bands in the UV-C spectral region due to the 4f15d1→4f2 transitions, in addition to intense 4f2→4f2 emissions in the visible spectral range, indicating enhanced energy transfer processes influenced by the orthorhombic host matrix. A cascade emission mechanism in Pr3+ starting from the 1S0 level was revealed in both materials by the presence of characteristic emissions at 3.04 eV (1S01I6) and 2.57 eV (3P03H4) appearing in two sequent radiative relaxation stages. Time-integrated excitation spectra highlighted distinct excitation bands associated with different Pr3+ energy levels populated below the fundamental absorption edge. Time-resolved spectroscopy of the 4f15d1→4f2 emissions revealed bi-exponential decay kinetics, distinguishing surface-perturbed and bulk Pr3+ centers, with significantly different lifetimes in each phase. The varying intensity ratio of the 4f15d1→4f2 and 4f2→4f2 emissions demonstrates that, depending on the phase composition, it is possible to control the nature of Pr3+ emissions, enabling the design of multifunctional luminescent nanomaterials for diverse applications of deep UV emissions in phototherapy and optoelectronics.

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Contribution to journal
publication status
published
subject
keywords
Mixed-phase fluorides, Nanoparticle, Pr 4f5d→4f transitions, Pr 4f S→4f transitions, Time-resolved luminescence spectra, UV-C radiation
in
Optical Materials
volume
167
article number
117315
publisher
Elsevier
external identifiers
  • scopus:105010677004
ISSN
0925-3467
DOI
10.1016/j.optmat.2025.117315
language
English
LU publication?
yes
id
a6d615c1-cdb2-40f6-98eb-d472953de479
date added to LUP
2025-10-31 10:24:35
date last changed
2025-10-31 10:25:46
@article{a6d615c1-cdb2-40f6-98eb-d472953de479,
  abstract     = {{<p>This work presents a comparative luminescence study of Pr<sup>3+</sup> doped phase-pure BaLuF<sub>5</sub> and mixed-phase BaLu<sub>2</sub>F<sub>8</sub> – BaLuF<sub>5</sub> materials synthesized via a hydrothermal route. The spectroscopic studies were mainly performed for phase-pure BaLuF<sub>5</sub> and two mixed-phase materials, which, according to structural and phase compositional analysis, contained 90 or 70 wt% of orthorhombic BaLu<sub>2</sub>F<sub>8</sub> and 10 or 30 wt% of cubic BaLuF<sub>5</sub>, respectively. Low-temperature time-integrated photoluminescence measurements under both host excitation at 45 eV and intracenter excitation of Pr<sup>3+</sup> ions at 6.75 eV revealed pronounced differences in luminescence between the two systems. The phase-pure BaLuF<sub>5</sub> material exhibited only narrow 4f<sup>2</sup>→4f<sup>2</sup> transitions of Pr<sup>3+</sup>, because the 4f<sup>1</sup>5d<sup>1</sup>states are energetically situated above the highest lying 4f<sup>2</sup> <sup>1</sup>S<sub>0</sub> level. In contrast, the BaLu<sub>2</sub>F<sub>8</sub> rich mixed-phase material showed multiple intense broad bands in the UV-C spectral region due to the 4f<sup>1</sup>5d<sup>1</sup>→4f<sup>2</sup> transitions, in addition to intense 4f<sup>2</sup>→4f<sup>2</sup> emissions in the visible spectral range, indicating enhanced energy transfer processes influenced by the orthorhombic host matrix. A cascade emission mechanism in Pr<sup>3+</sup> starting from the <sup>1</sup>S<sub>0</sub> level was revealed in both materials by the presence of characteristic emissions at 3.04 eV (<sup>1</sup>S<sub>0</sub>→<sup>1</sup>I<sub>6</sub>) and 2.57 eV (<sup>3</sup>P<sub>0</sub>→<sup>3</sup>H<sub>4</sub>) appearing in two sequent radiative relaxation stages. Time-integrated excitation spectra highlighted distinct excitation bands associated with different Pr<sup>3+</sup> energy levels populated below the fundamental absorption edge. Time-resolved spectroscopy of the 4f<sup>1</sup>5d<sup>1</sup>→4f<sup>2</sup> emissions revealed bi-exponential decay kinetics, distinguishing surface-perturbed and bulk Pr<sup>3+</sup> centers, with significantly different lifetimes in each phase. The varying intensity ratio of the 4f<sup>1</sup>5d<sup>1</sup>→4f<sup>2</sup> and 4f<sup>2</sup>→4f<sup>2</sup> emissions demonstrates that, depending on the phase composition, it is possible to control the nature of Pr<sup>3+</sup> emissions, enabling the design of multifunctional luminescent nanomaterials for diverse applications of deep UV emissions in phototherapy and optoelectronics.</p>}},
  author       = {{Maji, Sanu Bifal and Vanetsev, Alexander and Mändar, Hugo and Nagirnyi, Vitali and Chernenko, Kirill and Kozlova, Jekaterina and Kotlov, Aleksei and Smortsova, Yevheniia and Kirm, Marco}},
  issn         = {{0925-3467}},
  keywords     = {{Mixed-phase fluorides; Nanoparticle; Pr 4f5d→4f transitions; Pr 4f S→4f transitions; Time-resolved luminescence spectra; UV-C radiation}},
  language     = {{eng}},
  publisher    = {{Elsevier}},
  series       = {{Optical Materials}},
  title        = {{Phase dependent luminescence properties of Pr<sup>3+</sup> doped BaLu<sub>2</sub>F<sub>8</sub>–BaLuF<sub>5</sub> materials}},
  url          = {{http://dx.doi.org/10.1016/j.optmat.2025.117315}},
  doi          = {{10.1016/j.optmat.2025.117315}},
  volume       = {{167}},
  year         = {{2025}},
}