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Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition)

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A special issue of Crystals (ISSN 2073-4352). This special issue belongs to the section "Inorganic Crystalline Materials".

Deadline for manuscript submissions: closed (20 March 2024) | Viewed by 14489

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Prof. Dr. Alessandra Toncelli

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Guest Editor

Department of Physics, University of Pisa, 56126 Pisa, PI, Italy
Interests: photonics; rare-earth luminescence; optical spectroscopy; THz spectroscopy; crystal growth
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Dr. Željka Antić

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Guest Editor

Vinča Institute of Nuclear Sciences, National Institute of the Republic of Serbia, University of Belgrade, Belgrade, Serbia
Interests: luminescence; luminescence thermometry; phosphors; advanced optical materials; sensors
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Due to the success of the first volume of the Special Issue “Optical and Spectroscopic Properties of Rare-Earth Doped Crystals” (https://www.mdpi.com/journal/crystals/special_issues/RE_crystals), it is our pleasure to announce a second volume in this series.

Photonics applications based on rare-earth (RE) doped crystals are developing in many different fields, such as photovoltaics, laser technology, optical data storage, sensing, bioimaging, diagnosis, and therapy. RE-doped inorganic bulk materials have long been known to have luminescence emissions that are spectrally distributed throughout the whole optical range, from the ultraviolet (UV) to the mid-infrared region, with unique features which have made these materials highly important, especially for laser applications. Moreover, at the nanometric size, these materials exhibit peculiar behaviours regarding their efficiency, lifetime, energy transfer processes, interaction with the environment, etc., which have stimulated new research devoted, on the one hand, to the physical understanding of these phenomena and on the other hand, to the development of new applications. This Special Issue focuses on both the study of RE-doped bulk crystals and nanocrystal materials and their possible applications in various field.

We invite researchers to contribute to this Special Issue, “Optical and Spectroscopic Properties of Rare-Earth Doped Crystals (Volume II)”, which is intended to serve as a unique multidisciplinary forum covering all aspects of the science, technology, and applications of RE-doped crystals, from growth techniques with specific attention to the emission features of these materials to their applications.

Potential topics include, but are not limited to:

Synthesis and growth of RE-doped crystals
New host materials for efficient emission
Upconversion efficiency
Characterisation of RE-doped crystals by spectroscopic, microscopic, and other advanced techniques
Analysis of the energy transfer processes
Biomedical and imaging applications
Integrated optics applications
Photovoltaic applications
Sensing applications

Prof. Dr. Alessandra Toncelli
Dr. Željka Antić
Guest Editors

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Published Papers (10 papers)

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Research

12 pages, 2847 KiB

Open AccessArticle

On the Energy Dependence of the PL of RE Ions in LuBO₃:RE (RE = Ce, Eu, Gd, or Tb)

by Franziska Schröder, Sven Reetz and Thomas Jüstel

Crystals 2024, 14(4), 341; https://doi.org/10.3390/cryst14040341 - 3 Apr 2024

Cited by 1 | Viewed by 1057

Abstract

LuBO₃ crystallizes in the calcite type (CaCO₃) structure and is a widely applied inorganic host for luminescent materials and scintillators. Even though many scientific works have been published concerning the optical properties of rare-earth-doped LuBO₃, so far, no study of the emission spectra as function of the excitation energy of such orthoborates has been conducted. Therefore, this work elaborates on the photoluminescence of RE-doped LuBO₃ with RE = Ce³⁺, Eu³⁺, Gd³⁺, or Tb³⁺, while an emphasize is laid on the energy dependence of these four luminescent compounds. The reflection, emission, and excitation spectra were additionally recorded, and the particle size distribution was determined. Calcite type LuBO₃ was successfully obtained, and the characteristic RE luminescence was observed. Furthermore, the Gd³⁺-doped sample showed no scintillation due to its monovalence and a sensitizer is required to transfer the respective energy to the Gd³⁺-activator. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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13 pages, 4987 KiB

Open AccessArticle

Potential of Y₂Sn₂O₇:Eu³⁺, Dy³⁺ Inorganic Nanophosphors in Latent Fingermark Detection

by Layla Brini, Hanen Douiri, Marwa Abid, Alessandra Toncelli, Montasir Qasymeh, Ramzi Maalej and Mohamed Abdelhedi

Crystals 2024, 14(4), 300; https://doi.org/10.3390/cryst14040300 - 24 Mar 2024

Cited by 3 | Viewed by 1070

Abstract

In this work, we investigated the potential of Eu³⁺/Dy³⁺-codoped Y₂Sn₂O₇ fluorescent nanophosphors to visualize latent fingermarks. We prepared these nanophosphors with various doping concentrations by the conventional coprecipitation reaction. The crystal structure, morphology, luminescence properties, and energy transfer mechanisms were studied. The crystalline phase was characterized by X-ray diffraction and crystal structure refinement using the Rietveld method. XRD measurements showed that the samples crystallized in the pure single pyrochlore phase with few more peaks originated from secondary phases and impurities generated during phosphor production, and that Eu³⁺ ions occupied D_3d symmetry sites. The average crystallite size after mechanical grinding was less than 100 nm for all compositions. The optical characterization showed that, when excited under 532 nm, the Eu³⁺/Dy³⁺-codoped Y₂Sn₂O₇ samples’ main intense emission peaks were located at 580–707 nm, corresponding to the ⁵D₀→⁷Fj (j = l, 2, 3, and 4) transitions of europium. In fact, the ⁵D₀→⁷F₂ hypersensitive transition is strongly dependent on the local environment and was quite weak in Eu³⁺:Y₂Sn₂O₇ at low Eu³⁺ doping levels. We found that the presence of Dy³⁺ as a codopant permitted enhancing the emission from this transition. The calculated PL CIE coordinates for the synthesized nanophosphors were very close to those of the reddish-orange region and only slightly dependent on the doping level. Various surfaces, including difficult ones (wood and ceramic), were successfully tested for latent fingerprint development with the prepared Eu³⁺/Dy³⁺-codoped Y₂Sn₂O₇ fluorescent nanophosphor powder. Thanks to the high contrast obtained, fingerprint ridge patterns at all three levels were highlighted: core (level 1) islands, bifurcation, and enclosure (level 2), and even sweat pores (level 3). Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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10 pages, 7630 KiB

Open AccessArticle

Energy Transfer in the

{C a S O}_{4} - D y

Thermoluminescent Dosimeter from the Excited State of the

{S O}_{4}^{2 -}

Anionic Complex to the Impurities

by Turlybek N. Nurakhmetov, Temirulan T. Alibay, Keleshek B. Zhangylyssov, Dulat H. Daurenbekov, Zhussupbek M. Salikhodzha, Raushan K. Shamiyeva, Batsaiy M. Sadykova, Bagila N. Yussupbekova and Doszhan A. Tolekov

Crystals 2023, 13(11), 1596; https://doi.org/10.3390/cryst13111596 - 17 Nov 2023

Cited by 1 | Viewed by 1095

Abstract

The creation of a combined radiative state at 2.95–3.1 eV in the phosphor

{C a S O}_{4} - {D y}_{}^{3 +}

has been investigated using vacuum ultraviolet and thermoactivation spectroscopy methods. It is shown that the combined radiative electronic state [...] Read more.

The creation of a combined radiative state at 2.95–3.1 eV in the phosphor

{C a S O}_{4} - {D y}_{}^{3 +}

has been investigated using vacuum ultraviolet and thermoactivation spectroscopy methods. It is shown that the combined radiative electronic state is formed from the radiative electronic states of the impurity electronic trapping centers

{D y}_{}^{2 +} - {S O}_{4}^{-}

and the intrinsic electronic radiative states

{S O}_{4}^{3 -} - {S O}_{4}^{-}

during the excitation of the anion complex

{S O}_{4}^{2 -}

, as a result of charge transfer from the excited anion complex

O_{}^{2 -} - {D y}_{}^{3 +}

to the impurities and the neighboring anion complex

O^{2 -} - {S O}_{4}^{2 -}

. In the

{C a S O}_{4} - D y

phosphor, the combined radiative electronic state and impurity emission of

{D y}_{}^{3 +}

, 2.16 eV and 2.56 eV are excited by photons with energies of 3.95–4.0 eV and 4.5–4.6 eV. Energy transfer from the matrix to the

{D y}_{}^{3 +}

impurities is revealed upon thermal exposure as a result of the ionization of the electronic capture centers of

{D y}^{2 +}

and

{S O}_{4}^{3 -}

. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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11 pages, 2421 KiB

Open AccessArticle

Erbium-Doped LiYF₄ as a Potential Solid-State Frequency Reference: Eligibility and Spectroscopic Assessment

by Erik Cerrato, Chiara Gionco, Giuseppe Rizzelli Martella, Cecilia Clivati, Roberto Gaudino and Davide Calonico

Crystals 2023, 13(10), 1476; https://doi.org/10.3390/cryst13101476 - 10 Oct 2023

Viewed by 1220

Abstract

Time and frequency metrology is a key enabler for both forefront science and innovation. At the moment, atomic frequency standards (AFSs) are based on atoms either in the vapor phase or trapped in magneto-optical lattices in a vacuum. Finding a solid-state material that contains atoms suitable to be used as a frequency reference would be an important step forward in the simplification of the setup of AFSs. Lanthanide-doped inorganic crystals, such as Er-doped LiYF₄, have been studied for several decades, and their intrashell 4f transitions are usually identified as ultra-narrow. Nevertheless, a systematic characterization of these transitions and their linewidths with a correlation to the dopant’s concentration and isotopic purity at low temperatures is lacking. In this work, we studied Er-doped LiYF₄ as a potential benchmark material for solid-state frequency references. We chose Er as it has a set of transitions in the telecom band. The influence of Er concentrations and isotope purity on the transition linewidth was systematically studied using high-resolution optical spectroscopy at 5 K. The results indicate that the material under study is an interesting potential candidate as a solid-state frequency reference, having transition linewidths as low as 250 MHz at ~1530 nm. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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19 pages, 4853 KiB

Open AccessArticle

Li₄Ln[PS₄]₂Cl: Chloride-Containing Lithium Thiophosphates with Lanthanoid Participation (Ln = Pr, Nd and Sm)

by Pia L. Lange, Sebastian Bette, Sabine Strobel, Robert E. Dinnebier and Thomas Schleid

Crystals 2023, 13(10), 1408; https://doi.org/10.3390/cryst13101408 - 22 Sep 2023

Viewed by 954

Abstract

The synthesis and structural analysis of three new chloride-containing lithium thiophosphates(V) Li₄Ln[PS₄]₂Cl with trivalent lanthanoids (Ln = Pr, Nd and Sm) are presented and discussed. Single crystals of Li₄Sm[PS₄]₂Cl were obtained and used for crystal structure determination by applying X-ray diffraction. The other compounds were found to crystallize isotypically in the monoclinic space group C2/c. Thus, Li₄Sm[PS₄]₂Cl (a = 2089.31(12) pm, b = 1579.69(9) pm, c = 1309.04(8) pm, β = 109.978(3)°, Z = 12) was used as a representative model to further describe the crystal structure in detail since Li₄Pr[PS₄]₂Cl and Li₄Nd[PS₄]₂Cl were confirmed to be isotypic using powder X-ray diffraction measurements (PXRD). In all cases, a trigonal structure in the space group R

\bar{3}

(e.g., a = 1579.67(9) pm, c = 2818.36(16) pm, c/a = 1.784, Z = 18, for Li₄Sm[PS₄]₂Cl) displaying almost identical building units worked initially misleadingly. The structure refinement of Li₄Sm[PS₄]₂Cl revealed bicapped trigonal prisms of sulfur atoms coordinating the two crystallographically distinct (Sm1)³⁺ and (Sm2)³⁺ cations, which are further coordinated by four anionic [PS₄]³⁻ tetrahedra. The compounds also contain chloride anions residing within channel-like pores made of [PS₄]³⁻ units. Eight different sites for Li⁺ cations were identified with various coordination environments (C.N. = 4–6) with respect to chlorine and sulfur. EDXS measurements supported the stoichiometric formula of Li₄Ln[PS₄]₂Cl, and diffuse reflectance spectroscopy revealed optical band gaps of 2.69 eV, 3.52 eV, and 3.49 eV for Li₄Sm[PS₄]₂Cl, Li₄Nd[PS₄]₂Cl, and Li₄Pr[PS₄]₂Cl, respectively. The activation energy for Li⁺-cation mobility in Li₄Sm[PS₄]₂Cl was calculated as E_a(Li⁺) = 0.88 eV using BVEL, which indicates potential as a Li⁺-cation conductor. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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20 pages, 5601 KiB

Open AccessArticle

Up-Conversion Luminescence and Optical Temperature Sensing Behaviour of Y₂O₃:Ho³⁺, Yb³⁺ Phosphors

by Vhahangwele Makumbane, Mubarak Y. A. Yagoub, Zhiguo Xia, Robin E. Kroon and Hendrik C. Swart

Crystals 2023, 13(8), 1288; https://doi.org/10.3390/cryst13081288 - 21 Aug 2023

Cited by 7 | Viewed by 1681

Abstract

The up-conversion (UC) and temperature sensing behaviours of Y₂O₃:Ho³⁺, Yb³⁺ phosphors were investigated. A series of Y₂O₃:Ho³⁺, Yb³⁺ phosphors were synthesized using a solution combustion method. The cubic structure [...] Read more.

\bar{3}

space group was analysed by using X-ray powder diffraction. Scanning electron microscopy was conducted to study the surface morphologies of the UC phosphors. Under 980 nm excitation, the UC emissions of Ho³⁺ from the ⁵S₂ → ⁵I₈, ⁵F₅ → ⁵I₈ and ⁵S₂ → ⁵I₇ transitions were observed, which occurred through UC energy transfer (ET) processes. The Yb³⁺ ion concentration severely affected the UC emission. The sensing behaviour of the phosphor was investigated through the green (⁵F₄, ⁵S₂ → ⁵I₈) to red (⁵F₅ → ⁵I₈) fluorescence intensity ratio (FIR). The maximum absolute and relative sensitivity values of S_A = 0.08 K⁻¹ and S_R = 0.64% K⁻¹ were obtained. The results revealed that the prepared Y₂O₃:Ho³⁺, Yb³⁺ phosphor is suitable for optical sensing at high temperatures. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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11 pages, 3251 KiB

Open AccessArticle

Thirty-Fold Increase in Relative Sensitivity of Dy³⁺ Luminescent Boltzmann Thermometers Using Multiparameter and Multilevel Cascade Temperature Readings

by Željka Antić, Aleksandar Ćirić, Milica Sekulić, Jovana Periša, Bojana Milićević, Abdullah N. Alodhayb, Tahani A. Alrebdi and Miroslav D. Dramićanin

Crystals 2023, 13(6), 884; https://doi.org/10.3390/cryst13060884 - 28 May 2023

Cited by 3 | Viewed by 1564

Abstract

The sensitivity of luminescent Boltzmann thermometers is restricted by the energy difference between the thermally coupled excitement levels of trivalent lanthanides, and their values further decrease with increases in temperature, rendering their use at high temperatures difficult. Here, we demonstrate how to overcome this sensitivity limitation by employing multiparameter and multilevel cascade temperature readings. For this purpose, we synthesized Dy³⁺:Y₂SiO₅, a phosphor whose emission is known to begin quenching at very high temperatures. Its photoluminescence-emission features, later used for thermometry, consisted of two blue emission bands centered around 486 nm and 458 nm, and two bands centered around 430 nm and 398 nm, which were only visible at elevated temperatures. Next, we performed thermometry using the standard luminescence-intensity ratio (LIR) method, which employs the ⁴F_9/2 and ⁴I_15/2 Dy³⁺ levels’ emissions and the multilevel cascade method, which additionally uses the ⁴G_11/2 level and overlapping intensities of ⁴I_13/2, ⁴M_21/2, ⁴K_17/2, and ⁴F_7/2 levels to create two LIRs with a larger energy difference than the standard LIR. This approach yielded a sensitivity that was 3.14 times greater than the standard method. Finally, we simultaneously exploited all the LIRs in the multiparameter temperature readings and found a relative sensitivity that was 30 times greater than that of the standard approach. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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20 pages, 9421 KiB

Open AccessArticle

Three New Lanthanum Oxoantimonate(III) Halides: Synthesis and Crystal Structure of La₅Cl₃[SbO₃]₄, La₂Sb₁₂O₁₉Br₄ and La₂Sb₁₂O₁₉I₄

by Ralf J. C. Locke, Kim-Natalie Bozenhardt, Felix C. Goerigk and Thomas Schleid

Crystals 2023, 13(5), 731; https://doi.org/10.3390/cryst13050731 - 26 Apr 2023

Cited by 1 | Viewed by 1507

Abstract

It was possible to synthesize colorless single crystals of La₅Cl₃[SbO₃]₄ (block-shaped) as well as La₂Sb₁₂O₁₉Br₄ and La₂Sb₁₂O₁₉I₄ (both needle-shaped), representing three new compounds from the system of lanthanum oxoantimonate(III) halides, which have not been described in the literature before. La₅Cl₃[SbO₃]₄ crystallizes in the monoclinic space group P2/c with the lattice parameters a = 895.82(5) pm, b = 564.28(3) pm, c = 1728.19(9) pm, and β = 90.007(2)° for Z = 2. This layered compound contains isolated ψ¹-tetrahedral [SbO₃]^3– units, square hemiprisms [LaO₈]^13–, and antiprisms [LaO₄Cl₄]⁹⁻. La₂Sb₁₂O₁₉Br₄ and La₂Sb₁₂O₁₉I₄ crystallize isotypically in the orthorhombic space group Pnma with a = 3184.69(19) pm, b = 417.78(3) pm, c = 1019.85(6) pm for the bromide and a = 3215.08(19) pm, b = 419.94(3) pm, c = 1062.89(6) pm for the iodide. Instead of isolated [SbO₃]³⁻ anions, semi-tubular features

\begin{matrix} 1 \\ \infty \end{matrix}

{[Sb₁₂O₁₉]²⁻} are present, which consist mainly of [SbO₄]⁵⁻ and few [SbO₃]³⁻ units with stereochemically active electronic lone pairs at their Sb³⁺ centers. Within these so-called “double-halfpipes”, La³⁺ is surrounded by nine oxygen atoms as [LaO₉]^15– polyhedron without any contact with X⁻ anions. Single-crystal Raman measurements were performed for La₅Cl₃[SbO₃]₄ and La₂Sb₁₂O₁₉I₄, and La₅Cl₃[SbO₃]₄ was structurally compared with the isostoichiometric, but not isotypic La₅F₃[SbO₃]₄. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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14 pages, 8080 KiB

Open AccessArticle

Columbite–Tantalite from Northern Scandinavia (Kaustinen, Kolmozero) Pegmatites: An Optical and Spectroscopic Properties

by Miłosz Huber, Daniel Kamiński and Urszula Maciołek

Crystals 2023, 13(4), 612; https://doi.org/10.3390/cryst13040612 - 3 Apr 2023

Cited by 1 | Viewed by 2060

Abstract

LCT (lithium–cesium–tantalum) pegmatites from the Kaustinen and Kolmozero regions contain columbite–tantalite mineralization, which has been presented in this study. Crystal structure, Raman microscopy, and optical property analyses of these minerals were performed. As a result of the structural studies and micro-area analyses, it was determined that these minerals in the pegmatites in question constitute a solid solution with numerous Mn-Fe and Nb-Ta substitutions within a single crystal. The ratio between Mn-Fe and Nb-Ta can change from crystal to crystal, which makes it impossible to find precise stechiometry between these ions. The crystallization conditions of these minerals were also determined by studying the associations of other rock-forming minerals and accessory minerals in the discussed rocks. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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14 pages, 4085 KiB

Open AccessArticle

Luminescence Properties of Y₃F[Si₃O₁₀]:Ln³⁺ (Ln = Eu, Tb, Er) with Thalenite-Type Host Lattice and Crystal Structure of Tm₃F[Si₃O₁₀]

by Marion C. Schäfer, Michael Petter, Ingo Hartenbach, Ralf J. C. Locke, Shuang Zhang, Claudia Wickleder and Thomas Schleid

Crystals 2023, 13(3), 511; https://doi.org/10.3390/cryst13030511 - 16 Mar 2023

Cited by 2 | Viewed by 1401

Abstract

With Tm₃F[Si₃O₁₀], a new representative of the Ln₃F[Si₃O₁₀] series could be synthesized by the reaction of Tm₂O₃, TmF₃ and SiO₂ (molar ratio: 1:1:3), applying an [...] Read more.

With Tm₃F[Si₃O₁₀], a new representative of the Ln₃F[Si₃O₁₀] series could be synthesized by the reaction of Tm₂O₃, TmF₃ and SiO₂ (molar ratio: 1:1:3), applying an excess of CsBr as a fluxing agent in gas-tightly sealed platinum crucibles for eight days at 750 °C, and designed to yield Tm₃F₃[Si₃O₉] or Cs₂TmF[Si₄O₁₀]. Single crystals of Tm₃F[Si₃O₁₀] (monoclinic, P2₁/n; a = 725.04(6), b = 1102.43(9), c = 1032.57(8) pm, β = 97.185(7)°; Z = 4) appear as pale celadon, transparent, air- and water-resistant rhombic plates. According to its thalenite-type structure, Tm₃F[Si₃O₁₀] contains catena-trisilicate anions [Si₃O₁₀]⁸⁻ and triangular [FTm₃]⁸⁺ cations. The three crystallographically different Tm³⁺ cations are coordinated by seven plus one (Tm1) or only seven anions (Tm2 and Tm3) exhibiting a single F⁻ anion for each polyhedron, additional to the majority of O²⁻ anions. Furthermore, the luminescence properties of the isotypic colorless compound Y₃F[Si₃O₁₀] doped with Eu³⁺ (red emission), Tb³⁺ (green emission) and Er³⁺ (yellow and infrared emission), respectively, are reported in presenting their different excitation and emission spectra. Full article

(This article belongs to the Special Issue Optical and Spectroscopic Properties of Rare-Earth-Doped Crystals (2nd Edition))

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