The discovery of highly efficient broadband near infrared (NIR) emission material is urgent and crucial for constructing NIR lighting sources and emerging applications. Herein, a series of NIR emission hexafluorides A2BMF6:Cr3+ (A = Na, K, Rb, Cs; B = Li, Na, K, Cs; M = Al, Ga, Sc, In) peaking at ≈733–801 nm with a full width at half maximum (FWHM) of ≈98–115 nm are synthesized by a general ammonium salt assisted synthesis strategy. Benefiting from the pre‐ammoniation of the trivalent metal sources, the Cr3+ can be more efficiently doped into the A2BMF6 and simultaneously prevent the generation of the competitive phase. Particularly, Na3ScF6:Cr3+ (λem = 774 nm, FWHM ≈ 108 nm) with optimal Cr3+‐doping concentration of 35.96% shows a high internal quantum efficiency of 91.5% and an external quantum efficiency of ≈40.82%. A lighting emitting diode (LED) device with a NIR output power of ≈291.05 mW at 100 mA driven current and high photoelectric conversion efficiency of 20.94% is fabricated. The general synthesis strategy opens up new avenues for the exploration of Cr3+‐doped high efficiency phosphors, and the as‐obtained record NIR output power demonstrates for NIR LED lighting sources applications.
The development of highly efficient and thermally stable broadband near‐infrared (NIR) luminescence materials is a great challenge to advance the next‐generation smart NIR light source. Benefitting from the low phonon energy and relatively weak electron phonon coupling effect of the fluoride, K2NaScF6:Cr3+ phosphor is designed and obtained, which demonstrates a full width at half maximum of 100 nm peaking at ≈765 nm. Upon blue light excitation, the phosphor exhibits a high quantum efficiency of 74% and its emission intensity at 150 °C can keep 89.6% of the initial value at 25 °C. An NIR output power of 159.72 mW (input electric power, 1094 mW) with a high photoelectric conversion efficiency of ≈14.60%, light‐emitting diode (LED) device is presented based on this K2NaScF6:Cr3+ phosphor. Furthermore, applying the high‐power NIR phosphor‐converted LED device as lighting source, clear and quick veins imaging and recognition in fingers, palm, wrist, and arm of the human hand are first realized, suggesting K2NaScF6:Cr3+ phosphor has high promise in practical applications.
A new generation of red phosphors of complex fluoride matrices activated with Mn has gained a broad interest in getting high color quality and low color temperature of solid-state white light-emitting diodes (WLEDs). However, besides their instability toward moisture, the extremely irregular and nonuniform morphologies of these phosphors have limited their practical industry applications. In the present study, a novel type of KScF:Mn red phosphor with highly regular, uniform, and high color purity was obtained successfully through a facile coprecipitation route under mild conditions. The crystal structure was identified with aids of the powder X-ray diffraction, Rietveld refinement, and density functional theory calculations. The prototype crystallizes in the space group Fm3 m with a cubic structure, and the lattice parameters are fitted well to be a = b = c = 8.4859(8) Å and V = 611.074(2) Å. The Mn ions occupy Sc sites and locate at the centers of the distorted ScF octahedrons. A wide band gap of approximately 6.15 eV can provide sufficient space to accommodate impurity energy levels. Unlike most other Mn ion-activated fluoride phosphors, the as-prepared KScF:Mn phosphors demonstrate highly uniform and regular morphologies with shapes transforming from cube to octahedron with increasing Mn ion concentration. Under blue light excitation, the as-prepared KScF:Mn sample exhibits intense sharp-line red fluorescence (the strongest peak located at 631 nm) with high color purity. An excellent recovery in luminescence upon heating and cooling processes implies high stability of KScF:Mn. Furthermore, a warm WLED fabricated with blue GaN chips merged with the mixture of KScF:Mn and the well-known commercial YAG:Ce yellow phosphors exhibits wonderful color quality with lower correlated color temperature (3250 K) and higher color-rendering index ( R = 86.4). These results suggest that the KScF:Mn phosphor possesses stupendous potentiality for practical applications.
Upconversion (UC) luminescence materials doped with rare earth ions are extensively investigated as optical temperature probes by the fluorescence intensity ratio technique. However, most Er 3+ -doped materials are still suffering from low sensing sensitivity. In the present study, we attempt to develop high-sensingsensitivity Er 3+ -doped materials based on the thermally coupled energy levels (TCLs) from Stark sublevels as well as the properties at subzero temperatures, for which there is continuous lack of research. Er 3+ /Yb 3+ codoped Ba 3 Y 4 O 9 (BYO) phosphors were produced via a solid-state reaction. Excited by 980 nm, various output colors, including bright green, yellow, and red, in BYO:Er 3+ /Yb 3+ phosphors as well as the relative emission intensities could be regulated through altering Yb 3+ concentrations. Subsequently, on the basis of all 12 pairs of TCLs especially from Stark sublevels of 2 H 11/2 , 4 S 3/2 , and 4 F 9/2 of Er 3+ ions, multiple temperature-sensing performances are evaluated over a wide range of 73−573 K. The results show that the maximum sensitivity of the 2 H 11/2 and 4 S 3/2(1) levels is approximately 1-fold higher than that of traditional TCLs of 2 H 11/2 / 4 S 3/2 at elevated temperature and the maximum sensitivity based on the 2 H 11/2(1) and 2 H 11/2(2) levels is more than 12 times higher than that of the traditional TCLs of 2 H 11/2 / 4 S 3/2 at subzero temperature. Therefore, it is expected to realize high-sensitivity temperature detection from subzero to elevated temperatures by combining two pairs of different TCLs. In addition, the potential of Er 3+ / Yb 3+ codoped BYO phosphors to be used as an optical heater is studied. The generated temperature can be accurately monitored by BYO:Er 3+ /Yb 3+ phosphors and regulated by adjusting the excitation power, which indicate that BYO:Er 3+ /Yb 3+ phosphors can be used as an optical heating device.
Emotional voice conversion aims at converting speech from one emotion state to another. This paper proposes to model timbre and prosody features using a deep bidirectional long shortterm memory (DBLSTM) for emotional voice conversion. A continuous wavelet transform (CWT) representation of fundamental frequency (F0) and energy contour are used for prosody modeling. Specifically, we use CWT to decompose F0 into a five-scale representation, and decompose energy contour into a ten-scale representation, where each feature scale corresponds to a temporal scale. Both spectrum and prosody (F0 and energy contour) features are simultaneously converted by a sequence to sequence conversion method with DBLSTM model, which captures both frame-wise and long-range relationship between source and target voice. The converted speech signals are evaluated both objectively and subjectively, which confirms the effectiveness of the proposed method.
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