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Timestamp: 2019-04-26 12:32:42+00:00

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Spectroscopic properties of Pr3+ and Er3+ -doped KPb2Br5 crystals were investigated for possible applications in eye-safe lasers as well as Ce3+-doped KPb2Cl5 and Eu2+-doped KPb2Cl5/KPb2Br5 for potential radiation detectors. The studied materials were synthesized through careful purification of starting materials including multi-pass zone-refinement and halogenation. The growth of the purified materials was then carried out through the vertical or horizontal Bridgman technique. Under resonant excitation, infrared (IR) emissions at ~1.5 μm and ~1.6 μm were observed from Er:KPb2Br5 and Pr:KPb2Br5 corresponding to the 4f-4f transitions of 4I13/2→4I15/2 and 3F4,3F3→3H4, respectively. Emission characteristics of the ~1.5 μm Er3+ and ~1.6 μm Pr3+ transitions including IR to visible upconversion emission studies were also discussed. Under xenon lamp excitation, spectroscopic results showed allowed 5d-4f Ce3+ emission centered at ~375 nm in Ce3+-doped KPb2Cl5. Fast photoluminescence decay time of ~30-50 ns was attained from Ce:KPb2Cl5, while X-ray excited emission at ~530 nm appeared to originate from the host KPb2Cl5 crystal. In addition, a commercial Ce:YAP (yttrium aluminum perovskite, YAlO3) crystal was included in this study for comparison. Eu2+ 5d-4f emissions were not observed from Eu2+-doped KPb2Cl5 and KPb2Br5 crystals.
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Fig. 1 Room temperature emission cross-section spectra and schematic energy level diagrams for Pr:KPb2Br5 and Er:KPb2Br5. The inset shows the 4I13/2→4I15/2 Er3+ emission band under 1532 nm pumping.
Fig. 2 Visible emission from Pr: KPb2Br5 via (a) 1550 nm, (b) 474 nm, and (c) 590 nm pulsed laser excitation. (d) Visible emission decay transients from the 1D2 state under 1550 nm and 590 nm excitation and (e) Visible emission decay transients from the 3P0 state under 1550 nm and 590 nm excitation.
Fig. 3 Room temperature emission from Er: KPb2Br5 stimulated by 1532 nm CW laser excitation.
Fig. 4 (a) Room temperature excitation spectra of the upconverted emission from 4I9/2→4I15/2 of Er3+ overlaid with the 300K 4I15/2 →4I13/2 ground state absorption band for Er: KPb2Br5. (b) Room temperature excitation spectra of the upconverted emission from 2H11/2 + 4S3/2→4I15/2 of Er3+ overlaid with the 300 K 4I15/2 →4I13/2 ground state absorption band for Er: KPb2Br5. (c) Room temperature upconverted emission decay transients of the 4I9/2→4I15/2 and 2H11/2 + 4S3/2→4I15/2 from Er: KPb2Br5.
Fig. 5 Schematic energy level diagram of (a) Pr3+ ETU processes (i) 3F3 + 3F3 → 3H5 + 1G4, (ii) 1G4 + 1G4 → 1D2 + 3H5, (iii) 1G4 + 1D2 → 3H5 + 3P1, (iv) 1D2 + 3F2→ 3P0 + 3H4. (b) Er3+ ETU processes (i) 4I13/2 + 4I13/2→ 4I15/2 + 4I9/2 (ii) 4I13/2 + 4I9/2→4I15/2 + 2H11/2,4S3/2.
Fig. 6 The excitation (black dotted line) and emission spectra of Ce:YAP crystal at room temperature. The excitation and emission wavelengths are also indicated. The inset shows a schematic energy-level diagram of tentatively assigned optical excitation and emission transitions of Ce3+ in YAP and KPC.
Fig. 7 The excitation (black dotted line) and emission (black solid line) spectra of Ce3+-doped KPb2Cl5 crystal at room temperature. The emission spectrum of undoped KPb2Cl5 is also shown (dashed line). The top of inset shows the excitation and emission spectra of previous study 1wt.% Ce: KPb2Cl5 crystal. The inset (bottom) shows the transmittance of Ce: KPb2Cl5 (right scale).
Fig. 8 Radioluminescence spectra of undoped KPb2Cl5 and Ce3+ doped KPb2Cl5.
Fig. 9 Transmittance spectra of (a) undoped KPb2Cl5 and Eu2+ doped KPb2Cl5 (b) undoped KPb2Br5 and Eu2+ doped KPb2Br5 crystals at room temperature in the region of 200-800 nm. (c) Absorption spectra of both crystals are also depicted. (d) A schematic diagram of tentative energy level of Eu2+ doped potassium lead halides is also shown.

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