Controlled photoluminescence tuning is important for the optimization and modification of phosphor materials. Herein we report an isostructural solid solution of (CaMg)x(NaSc)1-xSi2O6 (0 < x < 1) in which cation nanosegregation leads to the presence of two dilute Eu(2+) centers. The distinct nanodomains of isostructural (CaMg)Si2O6 and (NaSc)Si2O6 contain a proportional number of Eu(2+) ions with unique, independent spectroscopic signatures. Density functional theory calculations provided a theoretical understanding of the nanosegregation and indicated that the homogeneous solid solution is energetically unstable. It is shown that nanosegregation allows predictive control of color rendering and therefore provides a new method of phosphor development.
The cation substitution-dependent
phase transition was used as
a strategy to discover new solid solution phosphors and to efficiently
tune the luminescence property of divalent europium (Eu2+) in the M3(PO4)2:Eu2+ (M = Ca/Sr/Ba) quasi-binary sets. Several new phosphors including
the greenish-white SrCa2(PO4)2:Eu2+, the yellow Sr2Ca(PO4)2:Eu2+, and the cyan Ba2Ca(PO4)2:Eu2+ were reported, and the drastic red shift
of the emission toward the phase transition point was discussed. Different
behavior of luminescence evolution in response to structural variation
was verified among the three M3(PO4)2:Eu2+ joins. Sr3(PO4)2 and Ba3(PO4)2 form a continuous
isostructural solid solution set in which Eu2+ exhibits
a similar symmetric narrow-band blue emission centered at 416 nm,
whereas Sr2+ substituting Ca2+ in Ca3(PO4)2 induces a composition-dependent phase
transition and the peaking emission gets red shifted to 527 nm approaching
the phase transition point. In the Ca3–x
Ba
x
(PO4)2:Eu2+ set, the validity of crystallochemical design of
phosphor between the phase transition boundary was further verified.
This cation substitution strategy may assist in developing new phosphors
with controllably tuned optical properties based on the phase transition.
The union of structural and spectroscopic modeling can accelerate the discovery and improvement of phosphor materials if guided by an appropriate principle. Herein, we describe the concept of "chemical unit cosubstitution" as one such potential design scheme. We corroborate this strategy experimentally and computationally by applying it to the Ca2(Al(1-x)Mg(x))(Al(1-x)Si(1+x))O7:Eu(2+) solid solution phosphor. The cosubstitution is shown to be restricted to tetrahedral sites, which enables the tuning of luminescent properties. The emission peaks shift from 513 to 538 nm with a decreasing Stokes shift, which has been simulated by a crystal-field model. The correlation between the 5d crystal-field splitting of Eu(2+) ions and the local geometry structure of the substituted sites is also revealed. Moreover, an energy decrease of the electron-phonon coupling effect is explained on the basis of the configurational coordinate model.
Learning from natural mineral structures is an efficient way to develop potential host lattices for applications in phosphor converted (pc)LEDs. A narrow‐band blue‐emitting silicate phosphor, RbNa3(Li3SiO4)4:Eu2+ (RNLSO:Eu2+), was derived from the UCr4C4‐type mineral model. The broad excitation spectrum (320–440 nm) indicates this phosphor can be well matched with the near ultraviolet (n‐UV) LED chip. Owing to the UCr4C4‐type highly condensed and rigid framework, RNLSO:Eu2+ exhibits an extremely small Stokes shift and an unprecedented ultra‐narrow (full‐width at half‐maximum, FWHM=22.4 nm) blue emission band (λem=471 nm) as well as excellent thermal stability (96 %@150 °C of the initial integrated intensity at 25 °C). The color gamut of the as‐fabricated (pc)LEDs is 75 % NTSC for the application in liquid crystal displays from the prototype design of an n‐UV LED chip and the narrow‐band RNLSO:Eu2+ (blue), β‐SiAlON:Eu2+ (green), and K2SiF6:Mn4+ (red) components as RGB emitters.
The Lu2.98Ce0.01Y0.01Al5O12 and Y2.99Ce0.01Al5O12 phosphors were synthesized by solid state reaction at temperature 1623 K and pressure 1.5 × 10(7) Pa in (95% N2 + 5% H2) atmosphere. Under the conditions, the compounds crystallize in the form of isolated euhedral partly faceted microcrystals ∼19 μm in size. The crystal structures of the Lu2.98Ce0.01Y0.01Al5O12 and Y2.99Ce0.01Al5O12 garnets have been obtained by Rietveld analysis. The photoluminescence (PL) and X-ray excited luminescence (XL) spectra obtained at room temperature indicate broad asymmetric bands with maxima near 519 and 540 nm for Y2.99Ce0.01Al5O12 and Lu2.98Ce0.01Y0.01Al5O12, respectively. The light source was fabricated using the powder Lu2.98Ce0.01Y0.01Al5O12 phosphor and commercial blue-emitting n-UV LED chips (λ(ex) = 450 nm). It is found that the CIE chromaticity coordinates are (x = 0.388, y = 0.563) with the warm white light emission correlated color temperature (CCT) of 6400 K and good luminous efficiency of 110 lm/W.
Zero-dimensional (0D) metal halides have drawn increasing attention due to the attractive structure dependent photoluminescence (PL) properties. Here, we report two new 0D organic-inorganic hybrid Sb-based halides, (MTP) 6 SbBr 6 Sb 2 Br 9 •H 2 O (MTP = Methyltriphenylphosphonium, crystal 1) and (MTP) 2 SbBr 5 (crystal 2), featuring a reversible structural phase transformation and tunable orange and red emissions upon dehydration and rehydration of H 2 O molecules. Intriguingly, a subsequent heat treatment further enables the formation of glassy state (MTP) 2 SbBr 5 (glass 3) with near-infrared luminescence, moreover, a sequential reverse phase transformation from glass 3 to crystal 2 and 1 is triggered by acetonitrile and water vapor stepwise. The anti-counterfeiting demo based on the tunable and reversible PL switching is finally achieved and thus the phase structure engineering in 0D metal halides expands their multiple applications in optical fields.Luminescent metal halides are widely used in light-emitting diodes, sensors, scintillators, etc. due to their tunable and controlled emissions, variable lifetimes, and high photoluminescence (PL) quantum efficiency. [1][2][3][4][5][6] In particular, [
CaLa2-x(MoO4)4:Ho(3+)/Yb(3+) phosphors with the doping concentrations of Ho(3+) and Yb(3+) (x = Ho(3+) + Yb(3+), Ho(3+) = 0.05; Yb(3+) = 0.35, 0.40, 0.45 and 0.50) have been successfully synthesized by the microwave sol-gel method. The modulated and averaged crystal structures of CaLa2-x(MoO4)4:Ho(3+)/Yb(3+) molybdates have been found by the Rietveld method, and the upconversion photoluminescence properties have been investigated. The synthesized particles, being formed after the heat-treatment at 900 °C for 16 h, showed a highly crystallized state. Under the excitation at 980 nm, CaLa2-x(MoO4)4:Ho(3+)/Yb(3+) particles exhibited strong 545 and 655 nm emission bands in the green and red regions. When the Yb(3+) : Ho(3+) ratios are 9 : 1 and 10 : 1, the UC intensity of CaLa1.5(MoO4)4:Yb0.45/Ho0.05 and CaLa1.45(MoO4)4:Yb0.50/Ho0.05 particles is the highest for different bands. The CIE coordinates calculated for CaLa2-x(MoO4)4:Ho(3+)/Yb(3+) phosphors are related to the yellow color field. The Raman spectrum of undoped CaLa2(MoO4)4 has revealed about 13 narrow lines. The strongest band observed at 906 cm(-1) was assigned to the ν1 symmetric stretching vibration of MoO4 tetrahedra. The spectra of the samples doped with Ho and Yb, as obtained under the 514.5 nm excitation, were dominated by Ho(3+) luminescence over the wavenumber range of >700 cm(-1) preventing the recording of the Raman spectra.
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