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. 2024 Sep 10;9(38):39893-39903.
doi: 10.1021/acsomega.4c05453. eCollection 2024 Sep 24.

Influence of Host Lattice Ions on the Dynamics of Transient Multiband Upconversion in Yb-Er Codoped NaLnF4 and LiLnF4 Microcrystals (Ln: Y, Lu, Gd)

Mingchen Li  1   2 , Maohui Yuan  1 , Wenda Cui  1 , Hanchang Huang  1   2 , Chuan Guo  1   3 , Kai Han  1   2
Affiliations

Influence of Host Lattice Ions on the Dynamics of Transient Multiband Upconversion in Yb-Er Codoped NaLnF4 and LiLnF4 Microcrystals (Ln: Y, Lu, Gd)

Mingchen Li et al. ACS Omega. .

Abstract

Inorganic host matrices provide a tunable luminescence environment for lanthanide ions, allowing for the modulation of upconversion luminescence (UCL) properties. AREF4 (A = alkali metal, RE = rare earth) have a low phonon energy and a high optical damage threshold, making them widely used as the host matrix for UCL materials. However, the impact mechanism of alkali metal ions and lanthanide lattice ions on transient UCL dynamics in AREF4 remains unclear. This study utilized a high-power nanosecond-pulsed laser at 976 nm to excite Yb-Er codoped NaLnF4 and LiLnF4 (Ln: Y, Lu, and Gd) microcrystals (MCs). All samples exhibit multiband emission, and the transient UC dynamics are discussed in detail. Compared with LiLnF4, NaLnF4 has higher UC efficiency and red to green (R/G) ratio. Lanthanide ions (Y, Lu, and Gd) affect the energy transfer (ET) distance in Yb-Er codoped systems, thereby altering UC efficiency and the R/G ratio. The energy level coupling between Gd3+ and Er3+ prolongs the duration of the UC emission. Specifically, the red emission lifetime of NaGdF4 is five times longer than that of NaYF4. Our research contributes to exploring excellent alternative host matrices for NaYF4 in the fields of rapid-response optoelectronic devices, micro-nano lasers, and stimulated emission depletion (STED) microscopy.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
SEM images and crystal structures of the AREF4:Yb/Er MCs.
Figure 2
Figure 2
(a–e) Refined X-ray diffraction (XRD) spectra of AREF4 microcrystals (Rietveld method).
Figure 3
Figure 3
(a–e) Transient UCL spectra of AREF4:Yb/Er MCs within 1 μs after excitation.
Figure 4
Figure 4
(a) UCL spectra of AREF4:Yb/Er (A = Na/Li, RE = Y/Lu/Gd) microcrystals (MCs) in 0–1 μs (the transition energy levels corresponding to different emission peaks are marked above); UCL spectra of AREF4:Yb/Er (A = Na/Li, RE = Y/Lu) MCs in 0–5 μs (b) and 0–20 μs (c); (d) sequence of UC pathways in NaLnF4 and LiLnF4 MCs (A/B: UC pathways; the number after the letter represents the amount of photons that need to be absorbed during the UC process; BET, back energy transfer; CR, cross relaxation).
Figure 5
Figure 5
(a) Energy level structure and ET pathways in Yb–Er codoped systems (colorful dashed arrows, gray dashed arrows, and colorful solid arrows represent UC pathways, nonradiative transitions, and UC emissions, respectively; the mutiphoton UC emission is marked with red dashed boxes); percentage intensity of three-photon (b) and four-photon (c) UC emissions in 0–10 μs.
Figure 6
Figure 6
(a) Transient UCL spectra of AREF4:Yb/Er MCs within 100 μs after excitation. Intensity decay curves of different luminescence components in AREF4:Yb/Er MCs: (b) green emission; (c) red emission (the time scale of NaGdF4 is indicated above the figure in red); (d) three-photon emission; (e) four-photon emission.
Figure 7
Figure 7
(a) UCL spectra of AREF4:Yb/Er MCs in 0–1 ms; (b) percentage intensity of different luminescence components of AREF4:Yb/Er MCs in 0–1 ms.
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