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REGULAR PAPERS 常规论文

Luminescence properties of -activated perovskite compound synthesized by metal organic decomposition
金属有机分解合成 活化 钙钛矿化合物的发光性能

To cite this article: Yuya Onishi et al 2018 Jpn. J. Appl. Phys. 57082601
引用本文: Yuya Onishi et al 2018 Jpn. J. Appl. Phys. 57082601
View the article online for updates and enhancements.
在线查看文章以获取更新和增强功能。

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by metal organic decomposition
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Yuya Onishi , Toshihiro Nakamura , Hayato Sone , and Sadao Adachi
Yuya Onishi 、Toshihiro Nakamura 、Hayato Sone 和 Sadao Adachi
Division of Electronics and Informatics, Faculty of Science and Technology, Gunma University, Kiryu, Gunma 376-8515, Japan
群马大学科学技术学院电子信息学系, 日本 群马 桐生 376-8515
Department of Electrical and Electronic Engineering, Faculty of Science and Engineering, Hosei University, Koganei, Tokyo 188-8584, Japan
法政大学理工学院电气电子工程系, 日本 东京都小金井 188-8584
*E-mail: nakamura @hosei.ac.jp; adachi@gunma-u.ac.jp
*电子邮件:nakamura @hosei.ac.jp;adachi@gunma-u.ac.jp

Received February 2, 2018; revised March 29, 2018; accepted May 2, 2018; published online July 4, 2018
收稿日期: 2018-02-02;2018 年 3 月 29 日修订;2018年5月2日接受;2018年7月4日在线发布

Abstract 抽象

-activated perovskite ( ) phosphor was synthesized by metal organic decomposition and subsequent calcination at in air. The luminescence properties of the TAP: phosphor were investigated in detail by photoluminescence (PL) spectroscopy and excitation (PLE) spectroscopy, together with PL decay measurements. The PLE spectra and PL decay behaviors of the and emissions showed evidence of resonant energy transfer from the TAG host ( ) to . The temperature dependence of the Eu emission intensity was measured at and analyzed using the conventional quenching model with the addition of the phonon occupation number term, which was promising for gaining the parity-forbidden transition intensity. This study was also focused on a lattice site of the dopant ions substituting whether for the -site or -site in the TAP lattice. The Stark splitting of the to level transitions suggests that the ions are substituted for the A-site with the point symmetry . (C) 2018 The Japan Society of Applied Physics
-活化 钙钛矿( )荧光粉是通过金属有机分解和随后在 空气中煅烧合成的。通过光致发光(PL)光谱和 激发(PLE)光谱以及PL衰减测量,详细研究了TAP: 荧光粉的发光特性。PLE谱和PL衰变行为 表明,TAG主机( )向 . 采用常规淬灭模型测量 并分析了Eu 发射强度的温度依赖性,并添加了声子占用数项,这有望获得奇偶校验禁止 的转变强度。本研究还集中在 掺杂剂离子的晶格位点上,该晶格位点取代了TAP晶格中的 -位点 -位点 能级跃迁的斯塔克分裂表明, 离子被具有点对称性的 A 位点取代。(C) 2018年日本应用物理学会

1. Introduction 1. 引言

Perovskite oxide materials in the form of are a special class of compounds, which have applications in various areas of science and technology, including cheap solar cells, multiferroic materials, energy harvesting devices, photocatalysis, anode materials in solid oxide fuel cells, and so on (see Ref. 1). The perovskite oxide materials also have unique physical properties, such as wide band gaps, high refractive indices, high melting points, small thermal expansion coefficients, and high dielectric permittivities.
钙钛矿氧化物材料 是一类特殊的化合物,在科学技术的各个领域都有应用,包括廉价的太阳能电池、多铁性材料、能量收集装置、光催化、固体氧化物燃料电池中的负极材料等(见参考文献1)。钙钛矿氧化物材料还具有独特的物理性能,如宽带隙、高折射率、高熔点、小热膨胀系数和高介电常数。
A trivalent rare-earth (RE) oxide compound, perovskite (TAP), is a member of the perovskite oxide family crystallizing in the orthorhombic structure with the space group Pnma The optical properties of in TAP, such as optical absorption, emission, and magnetooptical absorption and emission, have been studied by a number of researchers. Furthermore, the TAP crystal has been used as a host material for some non-RE and RE activator ions, such as and ) Photoluminescence (PL) investigation has also been performed on heterostructures with thin films deposited on TAP single-crystalline substrates by pulsed laser deposition.
三价稀土(RE)氧化物化合物 钙钛矿(TAP)是钙钛矿氧化物家族的成员,在与空间群Pmma 的斜方结构中结晶,TAP 的光学特性,如光吸收、发射和磁光吸收和发射,已被许多研究人员研究。 此外,TAP晶体已被用作一些非RE和RE活化离子的主体材料,例如 )还通过脉冲激光沉积对TAP单晶衬底上沉积 薄膜 的异质结构进行了光致发光(PL)研究。
The purpose of this study is to determine in detail the PL properties of -activated TAP phosphor. The ion is known to be an efficient activator in a number of phosphor materials. To the best of our knowledge, only one article has been published on a study of the PL properties of TAP:Eu Recently, Gorbenko et al. have reported the PL properties of -activated -mixed perovskites grown on substrates by liquid phase epitaxy. The aim of their study is to develop scintillating screens for use in microimaging applications. They found that , and films can be used as microimaging detectors. Concerning TAP: , they also reported optical spectra of absorption, PL, PL excitation (PLE), and cathodoluminescence, together with the PL decay characteristic measured by monitoring at Eu emission).
本研究的目的是详细确定 活化TAP荧光粉的PL特性。众所周知,该 离子是许多荧光粉材料中的有效活化剂。据我们所知,只有一篇关于 TAP:Eu 的 PL 特性研究的文章发表 最近,Gorbenko 等人 报道了通过液相外延在衬底上 生长的 活化 混合钙钛矿的 PL 特性。他们研究的目的是开发用于显微成像应用的闪烁屏幕。他们发现 ,胶片可以 用作显微成像探测器。关于TAP: ,他们还报告了吸收、PL、PL激发(PLE)和阴极发光的光谱,以及通过监测Eu 发射测量的PL衰变特性)。
Here, we synthesized pure and -activated TAP phosphors by metal organic decomposition (MOD). The structural and PL properties of the phosphor powders were investigated by X-ray diffraction (XRD) analysis, diffuse reflectance spectroscopy, PL analysis, PLE spectroscopy, and PL decay measurements. The temperature dependence of the PL properties was studied from to in increments. PL decay measurements were performed by monitoring at both (Eu emission) and ( emission). The reason for this is to confirm the efficient energy transfer occurring from the host to in the TAP:Eu system. This study was also focused on a lattice site of the dopant ions substituting whether for the A- or B-site in the TAP lattice.
在这里,我们通过金属有机分解(MOD)合成了纯和 活化的TAP荧光粉。通过X射线衍射(XRD)分析、漫反射光谱、PL分析、PLE光谱和PL衰减测量研究了荧光粉的结构和PL性能。研究了PL性能从 温度依赖性。PL衰减测量是通过监测 (Eu 排放)和 排放)进行的。这样做的原因是为了确认从 主机到 TAP:Eu 系统中发生的有效能量转移。本研究还集中在 掺杂剂离子的晶格位点上,该晶格位点取代了TAP晶格中的A位 点或B位 点。

2. Experimental procedure
2.实验程序

The TAP: Eu phosphor was synthesized by MOD. A mixed solution of , isoamyl acetate, and isopropyl alcohol was supplied from Kojundo Chemical Laboratory (Product No. Al-03-P). (KANTO CHEMICAL, ) was dissolved in deionized water and used as a source of . This solution was then mixed with the above-mentioned solution sufficiently. The MOD solutions were in molar ratios of with was dissolved in an aqueous solution and then mixed with the Tb-Al-O MOD solution sufficiently. The trivalent concentrations in were (pure TAP) and (TAP:Eu ). After prebaking in air at for , the MOD precursor was calcined on an alumina boat in an electric furnace at for in air. The synthesized TAP:Eu sample was ground in an agate mortar and used for various measurements.
TAP:Eu荧 光粉由MOD合成。 由乙酸异戊酯和异丙醇组成的 混合溶液由Kojundo化学实验室(货号.AL-03-P)。 (KANTO CHEMICAL, )溶于去离子水中,用作. 然后将该溶液与上述 溶液充分混合。将MOD溶液的摩尔比 溶解在水 溶液中,然后与Tb-Al-O的MOD溶液充分混合。中的三价 浓度为 (纯TAP)和 (TAP:Eu )。 在空气 预烘烤后,MOD前驱体在氧化铝船上的电炉 中煅烧。合成的TAP:Eu 样品在玛瑙研钵中研磨并用于各种测量。
The structural properties of the synthesized phosphor powders were analyzed by XRD spectroscopy using an X-ray diffractometer (SmartLab, Rigaku) with radiation at . The room-temperature diffuse reflectance spectrum was measured using a spectrometer (JASCO V-570) at .
使用X射线衍射仪(SmartLab,理学)通过XRD光谱分析了合成荧光粉的结构特性, 辐射在 。室温漫反射光谱是使用光谱仪(JASCO V-570)在 .
PL measurements were performed using a single monochromator equipped with a charge-coupled device (Princeton Instruments PIXIS 100B) and a Nd:YAG laser (Teem Photonics STV-01E) at with pulse duration at or a laser (Kimmon IK3302R-E) at
PL测量使用配备电荷耦合器件(Princeton Instruments PIXIS 100B)和Nd:YAG激光器(Teem Photonics STV-01E) 的单色器进行, 脉冲持续时间为或 激光器(Kimmon IK3302R-E)在
Fig. 1. (Color online) XRD patterns for the TAP and TAP: samples. The ASTM card pattern for orthorhmbic TAP (space group = Pnma; #01-088-0154) is shown at the bottom. Crosses and open triangles represent the diffraction peaks obtained from the ASTM card for cubic TAG (ASTM: and corundom-type (ASTM: #00-046-1212), respectively,
图 1.(在线彩)用于TAP和TAP 样品的XRD图谱。正交TAP的ASTM卡型(空间组= Pnma;#01-088-0154)显示在底部。十字和开三角形分别表示从ASTM卡中获得的三次TAG(ASTM: 和corundom型 (ASTM:#00-046-1212))的衍射峰,
as the excitation light source at room temperature or at temperatures from to in step. PLE measurements were performed at using a monochromator (JASCO CT-25C) with a Peltier-device cooled photomultiplier tube (Hamamatsu R375) and a xenon lamp as the excitation light source.
作为激发光源,在室温或温度从 步进到 步进 。PLE测量是在 使用单色器(JASCO CT-25C)和帕尔帖器件冷却光电倍增管(Hamamatsu R375)和 氙灯作为激发光源的情况下进行的。
Room-temperature PL decay measurements were performed by the excitation of the sample using the above-mentioned Nd:YAG laser at and . The decay signal was detected using a Peltier-element-cooled photomultiplier tube (Hamamatsu R375), a multichannel scaler (Stanford Research Systems SR 430), and a preamplifier (Stanford Research Systems SR 445A).
室温PL衰减测量是通过使用上述Nd:YAG激光在和 激发样品进行的。使用帕尔帖元件冷却光电倍增管 (Hamamatsu R375)、多通道缩放器 (Stanford Research Systems SR 430) 和前置放大器 (Stanford Research Systems SR 445A) 检测衰减信号。

3. Results and discussion
3. 结果与讨论

3.1 XRD measurements 3.1 XRD测量

TAP can be synthesized from mole of and mole of via
TAP可以由 摩尔 摩尔合成
with . From Eq. (1), one can expect to obtain other stoichiometric compounds at specific values, namely, garnet (TAG) at at 0.667 , and at , together with the end-point binaries of and . However, only ternary materials of TAP and TAG were synthesized by MOD. The synthesis of and by the MOD or other methods was found to be very difficult or, in principle, impossible.
.从式(1)中,可以预期获得其他特定 值的化学计量化合物,即石 榴石(TAG) 0.667处和 在,以及端点二进制的 。然而,MOD只合成了TAP和TAG的三元材料。 发现MOD或其他方法的合成 非常困难,或者原则上是不可能的。
Figure 1 shows the XRD data measured for the TAP and TAP: Eu samples. The diffraction pattern taken from the American Society for Testing and Materials (ASTM) card for orthorhmbic TAP (space group = Pnma; #01-088-0154) is shown at the bottom of Fig. 1. The XRD data in Fig. 1 suggest that our synthesized TAP and TAP:Eu samples
图 1 显示了 TAP 和 TAP: Eu 样品测量的 XRD 数据。图 1 底部显示了美国材料与试验协会 (ASTM) 卡中正交 TAP(空间组 = Pnma;#01-088-0154)的衍射图。图1中的XRD数据表明,我们合成的TAP和TAP:Eu 样品
Fig. 2. Room-temperature diffuse reflectance spectrum of the TAP:Eu sample.
图 2.TAP:Eu 样品的室温漫反射光谱。
contain small amounts of unavoidable TAG and inclusions. Crosses and open triangles represent the diffraction peaks from cubic TAG (ASTM: #00-056-1461) and corundom-type