Acta Photonica Sinica, Volume. 52, Issue 2, 0216001(2023)

Preparation and Luminescent Properties of Red-emitting Y6TeO12:Eu3+ Phosphor

Rongqing LI, Weiwei ZHOU, Yue TONG*, Qinghua ZHENG, Zhaocheng LV, Wang ZHAO, Zhengrong XIA, and Fangfang LIU
Author Affiliations
  • School of Electrical Engineering,Huainan Normal University,Huainan 232038,China
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    The industry of white light-emitting diodes, next-generation illumination sources, has become an interesting field for their superior advantages such as energy savings, high efficiency, long operating lifetime as well as environmental friendliness. By far, the most effective white light-emitting diode is a combination of a near-ultraviolet chip and yellow-emitting phosphors. However, this type of phosphor converted white light-emitting diode has some disadvantages, it suffers from the weakness of low color rending index and high correlated color temperature because of the deficiency of red component. Thus, to overcome this problem, a large number of red phosphors, especially the trivalent Eu3+ doped phosphor, have been widely studied. Eu3+ ion is an important red activator in most of the commercial red phosphors, which can provide an efficient and narrow band emission due to characteristic 4f-4f transitions. Especially, Eu3+ ions can be used to prove the point group symmetry of the substituted site in the host. When Eu3+ ions occupy noncentrosymmetric lattice sites, Eu3+ can emit intense red emission, benefiting to improve the overall efficiency of the white light-emitting diodes. So the host can affect the intensity of emission peaks of Eu3+ ion. Tellurate exhibits excellent properties in the optical, physical, and chemical fields. Given the low phonon energy of tellurate, this material can avoid the competitive non-radiative decay for the Eu3+ ions doped. Therefore, tellurate is suitable for hosting matrices used in phosphors. We report herein, the preparation and luminescent properties of red-emitting (Y1-x)6TeO12:xEu3+ phosphor. The (Y1-x)6TeO12:xEu3+ phosphors were prepared through the high-temperature solid-state reaction at 1 200 °C for 20 h. The (Y1-x)6TeO12: xEu3+ phosphors were prepared in this way for seven different concentrations of Eu3+ (x=0.1, 0.2, 0.3, 0.4 and 0.5). The samples (Y1-x)6TeO12:xEu3+ were analyzed in detail by XRD, excitation and emission spectra, concentration quenching, thermal stability, luminescent decay curves, quantum efficiency, and color coordinates. To identify the detailed crystal structure information of (Y1-x)6TeO12:xEu3+ phosphors, the Rietveld refinement was performed using the Generalized Structure and Analysis System. The absence of an impurity phase in the present doping concentration ranges (0.1≤x≤0.5) confirmed that incorporation of Eu3+ ions did not show any notable change in Y6TeO12 phase. The refinement results were clear that the as-obtained (Y1-x)6TeO12:xEu3+ phosphors were of trigonal structure with R3(No.146) space group. Further representative particle distribution and scanning electron microscopy of the (Y0.7)6TeO12:0.3Eu3+ phosphors were carried out and the results indicate that average grain size is 4.61 μm with diameter ranging from 2 μm to 8 μm. The band gap energy Eg of (Y0.7)6TeO12:0.3Eu3+ obtained from diffuse reflectance spectra is 3.25 eV. The excitation and emission spectra of (Y1-x)6TeO12:xEu3+ phosphors show that the prepared phosphor can be excited by ultraviolet light (393 nm) or blue light (464 nm), and exhibits a strong red light emission band at 632 nm corresponding to 5D07F2 electric dipole transition of Eu3+ ions. The intensity ratio R of 5D07F2 to 5D07F1 transition (R=I(5D07F2)/I(5D07F1 )) is a good way to measure the symmetry of Eu3+ sites. The intensity ratio value R is calculated to be 6.338. It is higher than some reported Eu3+-doped phosphors. Usually, with the increase of magnitude of R, the ideal value of the color chromaticity is closer. The dependence of integrated intensity on Eu3+ contents reveals the optimum doping concentration is x=0.3, beyond which concentration quenching was observed. Concentration quenching for the prepared (Y1-x)6TeO12:xEu3+ phosphors confirmed that the electric dipole-electric dipole interaction was responsible for energy transfer, resulting in the concentration quenching. The integrated emission intensity of prepared phosphor (Y0.7)6TeO12:0.3Eu3+ at 150℃ is as high as 76.5% of that at ambient temperature. The thermal activation energy was obtained as 0.196 9 eV, which ensures a good thermal stability. This demonstrates its possible application in solid state lighting or optical thermometry. The decay characteristics of (Y1-x)6TeO12:xEu3+ phosphors were studied to understand the average lifetime of an activator ion in an excited state. The decay curves of the prepared (Y1-x)6TeO12:xEu3+ phosphors were monitored under 393 nm excitation wavelength and 632 nm emission wavelength. At doping concentrations of Eu3+, the luminescence lifetimes are 1 114 μs, 907 μs, 813 μs, 661 μs and 583 μs, respectively. The lifetime decreases with an increase in Eu3+ dopant concentration. This type of observation is results when the distance between the dopant Eu3+ ion decreases and this leads to nonradiative transitions. Based on the datum of emission spectrum of (Y0.7)6TeO12:0.3Eu3+, the chromaticity coordinates are determined to be (0.637 6,0.343 1), close to the National Television System Committee value (0.67,0.33). To further evaluate the potential applications of the (Y0.7)6TeO12:0.3Eu3+ phosphor, the prototype light-emitting diodes fabricated by coating the phosphors on the near-UV chips emit a bright light. The strong emission band (360~440 nm) originates from the near-UV chip and other sharp emission bands attribute to the Eu3+ 4f-4f transitions. The phosphor exhibits favorable luminescent properties, thermal stability of luminescence with good chromaticity coordinate, which have potential application in white light-emitting diodes.

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    Rongqing LI, Weiwei ZHOU, Yue TONG, Qinghua ZHENG, Zhaocheng LV, Wang ZHAO, Zhengrong XIA, Fangfang LIU. Preparation and Luminescent Properties of Red-emitting Y6TeO12:Eu3+ Phosphor[J]. Acta Photonica Sinica, 2023, 52(2): 0216001

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    Paper Information

    Category:

    Received: Aug. 21, 2022

    Accepted: Oct. 14, 2022

    Published Online: Mar. 28, 2023

    The Author Email: TONG Yue (22311264@qq.com)

    DOI:10.3788/gzxb20235202.0216001

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