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1. Mid-IR Emission Characteristics of Low-Phonon Erbium doped Ternary Chloride-based Single Crystals

   E. Brown, Z. D. (April 2021, Proc. SPIE 11682, Optical Components and Materials.)

   null (Ed.)

   The mid-infrared fluorescence properties of erbium (Er) doped low-phonon ternary chloride-based crystals (KPb2Cl5,Cs2HfCl6, CsPbCl3, CsCdCl3) have been investigated. All crystals were grown by vertical Bridgman technique. Following optical excitations at 805 nm and 660 nm, all Er3+ doped chlorides exhibited infrared emissions at ~2750, ~3500, and ~4500 nm at room temperature. The mid-infrared emission at 4500 nm originating from the 4I9/2 -> 4I11/2 transition showed long emission lifetime values of ~7.8 ms and ~11.6 ms for Er3+ doped Cs2HfCl6 and CsCdCl3 crystals, respectively. In comparison, Er3+ doped KPb2Cl5 and CsPbCl3 demonstrated shorter lifetimes of ~3 ms and ~1.8 ms, respectively. The temperature dependence of the 4I9/2 decay times was performed for Er3+ doped CsPbCl3 and CsCdCl3 crystals. We observed that the fluorescence lifetimes were nearly independent of the temperature, indicating a negligibly small non-radiative decay rate through multiphonon relaxation, as predicted by the energy gap law for low phonon energy hosts. The room temperature stimulated emission cross-sections for the 4I9/2 -> 4I11/2 transition were determined to be in a range of ~0.14-0.54 x 10-20 cm2 for the studied Er doped chloride crystals. 

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2. Comparative study of rare-earth doped low-phonon fluoride and chloride crystals for mid-IR laser potential

   E. Brown, Z. D. (April 2021, Proceedings SPIE 11723, Laser Technology for Defense and Security XVII)

   A comparative study was performed on the mid-infrared emission properties of trivalent erbium (Er3+) and holmium (Ho3+) doped fluorides (BaF2, NaYF4) and ternary chloride-based crystals (CsCdCl3, KPb2Cl5,). All crystals were grown by vertical Bridgman technique. Following optical excitation at 800 nm, all Er3+ doped fluorides and chlorides exhibited mid-infrared emissions at ~4500 nm at room temperature. The mid-infrared emission at 4500 nm, originating from the 4I9/2 -> 4I11/2 transition, showed long emission lifetime values of ~11.6 ms and ~3.2 ms for Er3+ doped CsCdCl3 and KPb2Cl5 crystals, respectively. In comparison, Er3+ doped and BaF2 and NaYF4 demonstrated rather short lifetimes in the microsecond range of ~47 us and ~205 us, respectively. Temperature dependent decay time measurements were performed for the 4I9/2 excited state for Er3+ doped BaF2, NaYF4, and CsCdCl3 crystals. We noticed that the emission lifetimes of Er3+:CsCdCl3 were nearly independent of the temperature, whereas significant emission quenching of 4I9/2 level was observed for both Er3+ doped fluoride crystals. The temperature dependence of the multiphonon relaxation rate for 4.5 um mid-IR emissions was determined for the studied Er3+ doped fluorides using the well-known energy-gap law. Using ~890 nm excitation, all studied Ho3+ doped fluorides and chlorides exhibited mid-infrared emissions at ~3900 nm originating from the 5I5 -> 5I6 transition. The longest emission lifetime of the 5I5 level was determined to be ~14.55 ms from the Ho3+:CsCdCl3 crystal. The room temperature stimulated emission cross-sections for the Er3+ 4I9/2 -> 4I11/2 and Ho3+ 5I5 -> 5I6 transitions were determined using the Füchtbauer-Landenburg equation. Among the studied crystals, Er3+ doped chlorides are more than two orders of magnitude better in terms of emission lifetimes and sigma-tau product than the fluoride crystals. 

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3. Ho ³⁺ doped low-phonon single crystals and chalcogenide glasses for mid-IR source application

   https://doi.org/10.1364/OME.487911  

   Brown, Ei_Ei; Fleischman, Zackery_D; McKay, Jason; Merkle, Larry; Hommerich, Uwe; Palosz, Witold; Trivedi, Sudhir; Dubinskii, Mark (April 2023, Optical Materials Express)

   A comparative study was conducted to investigate the 3.9 µm mid-IR emission properties of Ho³⁺doped NaYF₄and CsCdCl₃crystals as well as Ho³⁺doped Ga₂Ge₅S₁₃glass. Following optical excitation at ∼890 nm, all the studied materials exhibited broad mid-IR emissions centered at ∼3.9 µm at room temperature. The mid-IR emission at 3.9 µm, originating from the⁵I₅→⁵I₆transition, showed long emission lifetime values of ∼16.5 ms and ∼1.61 ms for Ho³⁺doped CsCdCl₃crystal and Ga₂Ge₅S₁₃glass, respectively. Conversely, the Ho³⁺doped NaYF₄crystal exhibited a relatively short lifetime of ∼120 µs. Temperature dependent decay time measurements were performed for the⁵I₅excited state for all three samples. The results showed that the emission lifetimes of Ho³⁺:CsCdCl₃and Ho³⁺:Ga₂Ge₅S₁₃were nearly temperature independent over the range studied, while significant emission quenching of the⁵I₅level was observed in Ho³⁺:NaYF₄. The temperature dependence of the multi-phonon relaxation rate for 3.9 µm mid-IR emission in Ho³⁺:NaYF₄crystal was determined. The room temperature stimulated emission cross-sections for all three samples were calculated using the Füchtbauer-Landenburg equation. Furthermore, the results of Judd-Ofelt analysis are presented and discussed. 

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4. Crystal growth and characterization of undoped and Dy-doped TlPb2Br5 for infrared lasers and nuclear radiation detection

   Hömmerich, U.; Brown, E.; Kabir, A.; Hart, D.; Trivedi, S.B.; Jin, F.; Chen, H. (September 2017, Journal of crystal growth)

   We report results of the crystal growth and characterization of undoped and Dy-doped TlPb2Br5 for applications in infrared (IR) lasers and nuclear radiation detection. TlPb2Br5 (TPB) was synthesized from commercial starting materials of PbBr2 and TlBr and further purified through a combination of zone-refinement and directional solidification. For doping experiments, 2 wt% of DyBr3 was added to the purified TPB material. Crystal growth of TPB and Dy: TPB was carried out in a two-zone tube furnace by a vertical Bridgman method. Following optical excitation at ~1.36um, the Dy: TPB crystal exhibited efficient mid-IR emission bands centered at 2.87um and 4.35um with room-temperature lifetimes of 9.5 ms and 5.2 ms, respectively. The peak emission cross-sections were determined to be ~0.8x10-20 cm2 and ~0.5x10-20 cm2, respectively, which makes Dy: TPB a promising candidate for mid-IR laser applications. Besides its potential as a solid-state laser host, an undoped TPB crystal was also tested for gamma-ray detection. Using Cs-137 and Am-241 sources resulted in energy resolutions for gamma-rays as good as 1-2% (FWHM) at room-temperature under non-optimized conditions. 

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5. Diffusion doping of cobalt in rod-shape anatase TiO ₂ nanocrystals leads to antiferromagnetism

   https://doi.org/10.1039/D0NA00640H  

   Mia, Shahzahan; Varapragasam, Shelton J.; Baride, Aravind; Balasanthiran, Choumini; Balasubramanian, Balamurugan; Rioux, Robert M.; Hoefelmeyer, James D. (October 2020, Nanoscale Advances)

   null (Ed.)

   Cobalt( ii ) ions were adsorbed to the surface of rod-shape anatase TiO 2 nanocrystals and subsequently heated to promote ion diffusion into the nanocrystal. After removal of any remaining surface bound cobalt, a sample consisting of strictly cobalt-doped TiO 2 was obtained and characterized with powder X-ray diffraction, transmission electron microscopy, UV-visible spectroscopy, fluorescence spectroscopy, X-ray photoelectron spectroscopy, SQUID magnetometry, and inductively-coupled plasma atomic emission spectroscopy. The nanocrystal morphology was unchanged in the process and no new crystal phases were detected. The concentration of cobalt in the doped samples linearly correlates with the initial loading of cobalt( ii ) ions on the nanocrystal surface. Thin films of the cobalt doped TiO 2 nanocrystals were prepared on indium-tin oxide coated glass substrate, and the electrical conductivity increased with the concentration of doped cobalt. Magnetic measurements of the cobalt-doped TiO 2 nanocrystals reveal paramagnetic behavior at room temperature, and antiferromagnetic interactions between Co ions at low temperatures. Antiferromagnetism is atypical for cobalt-doped TiO 2 nanocrystals, and is proposed to arise from interstitial doping that may be favored by the diffusional doping mechanism. 

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