CN1560890A - Cerium-doped lutetium-yttrium aluminate submicron imaging phosphor screen and preparation method thereof - Google Patents

Cerium-doped lutetium-yttrium aluminate submicron imaging phosphor screen and preparation method thereof Download PDF

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CN1560890A
CN1560890A CNA2004100164741A CN200410016474A CN1560890A CN 1560890 A CN1560890 A CN 1560890A CN A2004100164741 A CNA2004100164741 A CN A2004100164741A CN 200410016474 A CN200410016474 A CN 200410016474A CN 1560890 A CN1560890 A CN 1560890A
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赵广军
徐军
庞辉勇
介明印
何晓明
周圣明
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Shanghai Institute of Optics and Fine Mechanics of CAS
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Abstract

一种掺铈铝酸镥钇亚微米成像荧光屏及其制备方法,该荧光屏的结构是在晶面方向为(010)、(100)或(001)的Lu1-zYzAlO3衬底上生长一层闪烁薄膜Lu1-x-yCeyYxAlO3而构成,其中0≤x≤0.9999,0.0001≤y≤0.05,0≤z≤1),该荧光屏的制备方法是将晶面方向为(010)、(100)或(001)的Lu1-zYzAlO3 (0≤z≤1)单晶衬底作大面积籽晶,在电阻加热液相外延炉中,在LuzY1-zAlO3单晶的结晶温度下,与含有Lu1-x-yCeyYxAlO3多晶料的助熔剂饱和溶液接触界面上生长一层微米及亚微米量级的Lu1-x-yCeyYxAlO3单晶薄膜。该荧光屏具有高效率和高分辨率的特点。

Figure 200410016474

A cerium-doped lutetium-yttrium aluminate submicron imaging phosphor screen and a preparation method thereof, the structure of the phosphor screen is on a Lu 1-z Y z AlO 3 substrate whose crystal plane direction is (010), (100) or (001) It is formed by growing a layer of scintillation film Lu 1-x-y Ce y Y x AlO 3 , where 0≤x≤0.9999, 0.0001≤y≤0.05, 0≤z≤1), the preparation method of the phosphor screen is to change the direction of the crystal plane Make a large-area seed crystal for (010), (100) or (001) Lu 1-z Y z AlO 3 (0≤z≤1) single crystal substrate, in the resistance heating liquid phase epitaxy furnace, in Lu z At the crystallization temperature of Y 1-z AlO 3 single crystal, a layer of micron and sub-micron Lu 1 is grown on the contact interface with flux saturated solution containing Lu 1-x-y Ce y Y x AlO 3 polycrystalline material -x-y Ce y Y x AlO 3 single crystal thin film. The phosphor screen is characterized by high efficiency and high resolution.

Figure 200410016474

Description

掺铈铝酸镥钇亚微米成像荧光屏及其制备方法Cerium-doped lutetium-yttrium aluminate submicron imaging phosphor screen and preparation method thereof

技术领域technical field

本发明涉及一种X射线亚微米成像荧光屏,特别是一种掺铈铝酸镥钇亚微米成像荧光屏及其制备方法,该荧光屏可以广泛应用于医学、科学研究、工业在线检测、安全检查等射线探测领域中。The invention relates to an X-ray submicron imaging fluorescent screen, in particular to a cerium-doped lutetium yttrium aluminate submicron imaging fluorescent screen and a preparation method thereof. in the detection field.

背景技术Background technique

X射线照相术是一种采用闪烁荧光增强屏(闪烁晶体或者荧光粉)和感光胶片进行X射线探测的方法,是一种传统的X射线成像技术,它在医疗诊断、金属缺陷检查等方面具有广泛的应用。但是,这种传统的X射线照相术具有效率低、费时费力、不能进行实时(real-time)观察等缺点,现在已经逐渐被淘汰。采用电荷耦合器件(CCD)或者非晶硅阵列(a-Si:H)等探测器代替X射线照相术中的感光胶片,并结合计算机控制显示,是今后X成像技术发展的重要趋势之一。与传统的X射线照相术相比,这种新型的X射线成像技术具有探测效率高、数字化程度高、可以实现在线实时检测等优点,在疾病诊断、工业无损检测、天文观察、安全检查等技术领域中有着非常广泛的应用价值。而且,随着高亮度高谐振特性的第三代同步辐射光源的发展,这种新型的X射线成像技术还将会在相衬成像、全息成像以及微层析成像等显微X射线成像领域中发挥重要的作用,而显微X射线成像将要求系统具有微米或者亚微米的分辨率、更广的动态范围、以及更快的时间分辨率等特点。闪烁荧光屏是决定X射线成像系统的空间和时间分辨率的关键因素之一。目前,成像系统中的荧光屏多数都采用微细荧光粉(粒度为1微米)制成的2-3微米厚度的荧光屏,这种荧光屏的分辨率一般也在2-3微米的量级。另外,由于荧光粉的粒度大、密度仅为相应晶态薄膜密度的一半,所以荧光粉荧光屏存在X射线吸收及光转换效率低、荧光响应时间长等缺点。为了提高显微X射线成像的分辨率,现在又发展了厚度仅为微米或者亚微米级的单晶闪烁薄膜(SCF)作为X射线成像系统的荧光屏,这种SCF荧光屏将大大提高了X射线成像的分辨率,理论上,SCF闪烁荧光屏的分辨率可达到可见光的衍射极限(约为0.3微米)。(参见:IEEE Trans.Nucl.Sci.1998年,第45卷第5期,第492页;参见:J.Opt.Sco.Am.A,1998年,第15卷第7期,第1940页)。X-ray radiography is a method of X-ray detection using scintillating fluorescent intensifying screens (scintillation crystals or phosphors) and photosensitive film. It is a traditional X-ray imaging technology. Wide range of applications. However, this traditional X-ray radiography has disadvantages such as low efficiency, time-consuming and labor-intensive, and incapable of real-time observation, etc., and has been gradually eliminated now. Using charge-coupled device (CCD) or amorphous silicon array (a-Si:H) detectors to replace photosensitive film in X-ray radiography, combined with computer-controlled display, is one of the important trends in the development of X-ray imaging technology in the future. Compared with traditional X-ray radiography, this new type of X-ray imaging technology has the advantages of high detection efficiency, high degree of digitalization, and online real-time detection. It has a very wide application value in the field. Moreover, with the development of the third-generation synchrotron radiation light source with high brightness and high resonance characteristics, this new type of X-ray imaging technology will also be used in the field of micro-X-ray imaging such as phase contrast imaging, holographic imaging, and micro-tomography. Microscopic X-ray imaging will require the system to have micron or submicron resolution, wider dynamic range, and faster time resolution. The scintillation phosphor screen is one of the key factors determining the spatial and temporal resolution of an X-ray imaging system. At present, most of the phosphor screens in the imaging system are 2-3 micron thick phosphor screens made of fine phosphor powder (with a particle size of 1 micron), and the resolution of such phosphor screens is generally on the order of 2-3 micron. In addition, due to the large particle size and density of the phosphor powder, which is only half the density of the corresponding crystalline film, the phosphor screen has disadvantages such as low X-ray absorption and light conversion efficiency, and long fluorescence response time. In order to improve the resolution of microscopic X-ray imaging, a single crystal scintillation film (SCF) with a thickness of only microns or submicrons has been developed as a fluorescent screen for X-ray imaging systems. This SCF fluorescent screen will greatly improve X-ray imaging. In theory, the resolution of the SCF scintillation fluorescent screen can reach the diffraction limit of visible light (about 0.3 microns). (See: IEEE Trans.Nucl.Sci.1998, Vol. 45, No. 5, p. 492; see: J.Opt.Sco.Am.A, 1998, Vol. 15, No. 7, p. 1940) .

在先技术中主要有CsI(Tl)、Ce:YAG/YAG和Ce:LuAG/YAG等SCF荧光屏,但是这些荧光屏具有下列缺点:(1)CsI(Tl)和Ce:YAG晶体的有效原子序数以及密度都很小(Zeff分别为54.1和32,密度分别为4.52g/cm3和4.55g/cm3),因此,它们的X射线吸收能力以及射线-光转换效率较低。为了提高其分辨率必须增加薄膜的厚度,根据成像线扩展函数(LSF)知道,厚度的增加将减小荧光屏的分辨率(分辨率近似等于它们的厚度);(2)Ce:LuAG虽然有很大的有效原子序数和高的密度(Zeff=58.9,密度=6.67g/cm3),但其光输出较小(3000Ph/Mev),并且,LuAG和作为衬底的YAG之间晶格失配程度较大,这不利于在衬底上生长高质量的单晶薄膜,这将会严重影响荧光屏的光学性能;(3)另外,CsI(Tl)薄膜容易潮解,其光衰减时间较长(600ns),不适于快速实时显微X射线成像;(4)另外,在先技术中的SCF薄膜的分辨率都相对较小,约为0.7-0.8微米。There are mainly SCF fluorescent screens such as CsI(Tl), Ce:YAG/YAG and Ce:LuAG/YAG in the prior art, but these fluorescent screens have the following disadvantages: (1) CsI(Tl) and Ce: effective atomic number of YAG crystals and The densities are very small (Z eff is 54.1 and 32, and the densities are 4.52 g/cm 3 and 4.55 g/cm 3 ), therefore, their X-ray absorption capacity and ray-to-light conversion efficiency are low. In order to improve its resolution, the thickness of the film must be increased. According to the imaging line spread function (LSF), the increase of the thickness will reduce the resolution of the fluorescent screen (the resolution is approximately equal to their thickness); (2) Although Ce:LuAG has a large Large effective atomic number and high density (Z eff =58.9, density =6.67g/cm 3 ), but its light output is small (3000Ph/Mev), and the lattice between LuAG and YAG as the substrate This is not conducive to the growth of high-quality single crystal thin films on the substrate, which will seriously affect the optical properties of the fluorescent screen; (3) In addition, the CsI(Tl) thin film is easy to deliquescence, and its light decay time is longer ( 600ns), not suitable for fast real-time microscopic X-ray imaging; (4) In addition, the resolution of the SCF films in the prior art is relatively small, about 0.7-0.8 microns.

发明内容Contents of the invention

本发明要解决的技术问题是克服在先技术中SCF荧光屏低密度、低光输出、长衰减时间、低分辨率等的缺点,提供一种掺铈铝酸镥钇亚微米成像荧光屏及其制备方法。该荧光屏应具有高效率和高分辨率的特点。The technical problem to be solved by the present invention is to overcome the disadvantages of low density, low light output, long decay time, and low resolution of the SCF fluorescent screen in the prior art, and provide a submicron imaging fluorescent screen doped with cerium-doped lutetium aluminate and its preparation method . The phosphor screen should be characterized by high efficiency and high resolution.

本发明的技术解决方案如下:Technical solution of the present invention is as follows:

一种掺铈铝酸镥钇亚微米成像荧光屏,该荧光屏的结构是在晶面方向为(010)、(100)或(001)的Lu1-zYzAlO3(0≤z≤1)衬底上生长一层闪烁薄膜Lu1-x-yCeyYxAlO3而构成,即Lu1-x-yCeyYxAlO3/Lu1-zYzAlO3(0≤x≤0.9999,0.0001≤y≤0.05,0≤z≤1)。A cerium-doped lutetium-yttrium aluminate submicron imaging phosphor screen, the structure of the phosphor screen is Lu 1-z Y z AlO 3 (0≤z≤1) in the crystal plane direction of (010), (100) or (001) A layer of scintillation film Lu 1-xy Ce y Y x AlO 3 is grown on the substrate, that is, Lu 1-xy Ce y Y x AlO 3 /Lu 1-z Y z AlO 3 (0≤x≤0.9999, 0.0001≤ y≤0.05, 0≤z≤1).

所述Lu1-zYzAlO3(0≤z≤1)衬底的厚度为5-30微米,所述闪烁薄膜Lu1-x-yCeyYzAlO3的厚度为0.3-10微米。The thickness of the Lu 1-z Y z AlO 3 (0≤z≤1) substrate is 5-30 microns, and the thickness of the scintillation film Lu 1-xy Ce y Y z AlO 3 is 0.3-10 microns.

所述的掺铈铝酸镥钇亚微米成像荧光屏的制备方法,其特征在于该荧光屏是将晶面方向为(010)、(100)或(001)的Lu1-zYzAlO3(0≤z≤1)单晶衬底作大面积籽晶,在电阻加热液相外延炉中,在LuzY1-zAlO3单晶的结晶温度下,与含有Lu1-x-yCeyYxAlO3多晶料的助熔剂饱和溶液接触界面上生长一层微米及亚微米量级的Lu1-x-yCeyYxAlO3单晶薄膜。The preparation method of the cerium-doped lutetium-yttrium aluminate submicron imaging phosphor screen is characterized in that the phosphor screen is Lu 1-z Y z AlO 3 (0 ≤z≤1) single crystal substrate as a large-area seed crystal, in a resistance heating liquid phase epitaxy furnace, at the crystallization temperature of Lu z Y 1-z AlO 3 single crystal, and containing Lu 1-xy Ce y Y x A layer of micron and submicron Lu 1-xy Ce y Y x AlO 3 single crystal film is grown on the contact interface of flux saturated solution of AlO 3 polycrystalline material.

所述的含有Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)多晶料助熔剂饱和溶液的原料配比如下:The raw material ratio of the polycrystalline flux saturated solution containing Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) is as follows:

①助熔剂溶液的组分配比为8-15mol的PbO和1mol B2O3,或10-12molBi2O3和1-3mol的B2O3① The component distribution ratio of the flux solution is 8-15mol of PbO and 1mol of B 2 O 3 , or 10-12mol of Bi 2 O 3 and 1-3mol of B 2 O 3 ;

②Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)多晶与助熔剂的重量百分比为:Lu1-x-yCeyYxAlO3/助熔剂溶液=10wt%-50wt%②The weight percent of Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) polycrystal and flux is: Lu 1-xy Ce y Y x AlO 3 /flux solution=10wt% -50wt%

所述的电阻加热液相外延炉的结构主要包括:The structure of the resistance heating liquid phase epitaxy furnace mainly includes:

炉体,炉体下部是主炉体,炉体上部是退火炉体,在炉体内,中央置有坩埚,坩埚与炉体同轴,主炉体中相对坩埚周围设有侧面发热体,侧面发热体的外围为绝热层,坩埚底下有绝热层和能够调节坩埚高低的底托,退火炉内有上侧发热体,主炉体还设有中测温热电偶,退火炉设有上测温热电偶,从炉体的上顶盖中央向下延伸一旋转提拉杆,该旋转提拉杆的下端为衬底夹具,旋转提拉杆与炉体同轴。Furnace body, the lower part of the furnace body is the main furnace body, and the upper part of the furnace body is the annealing furnace body. In the furnace body, there is a crucible in the center, which is coaxial with the furnace body. The periphery of the body is an insulating layer, and there is an insulating layer under the crucible and a bottom bracket that can adjust the height of the crucible. There is an upper side heating element in the annealing furnace, and the main furnace body is also equipped with a middle temperature measuring thermocouple. Coupled, a rotating lifting rod extends downward from the center of the upper top cover of the furnace body. The lower end of the rotating lifting rod is a substrate holder, and the rotating lifting rod is coaxial with the furnace body.

所述的掺铈铝酸镥钇亚微米成像荧光屏的制备方法包括下列步骤:The preparation method of the cerium-doped lutetium-yttrium aluminate submicron imaging fluorescent screen comprises the following steps:

<1>根据选定的Lu1-x-yCeyYxAlO3多晶与助熔剂的配比称量原料,充分混合均匀后装入电阻加热液相外延炉的坩埚中并装入炉体中;<1> Weigh the raw materials according to the selected ratio of Lu 1-xy Ce y Y x AlO 3 polycrystal and flux, mix well and put them into the crucible of the resistance heating liquid phase epitaxy furnace and put them into the furnace body ;

<2>将晶面方向为(100)或(010)或(001)的Lu1-zYzAlO3(0≤z≤1)的衬底晶片置入衬底夹具内,调整旋转提拉杆,使之处于坩埚的同轴位置上;<2> Put the Lu 1-z Y z AlO 3 (0≤z≤1) substrate wafer with crystal plane direction (100) or (010) or (001) into the substrate holder, and adjust the rotating puller , so that it is on the coaxial position of the crucible;

<3>以100℃/Hr的升温速度升温至1050-1200℃,熔融多晶原料Lu1-x-yCeyYxAlO3与助熔剂PbO-B2O3或Bi2O3-B2O3;使其成为饱和溶液(10),待全部溶解后,在1100-1250℃恒温5小时;<3>Raise the temperature to 1050-1200°C at a heating rate of 100°C/Hr, melt polycrystalline raw material Lu 1-xy Ce y Y x AlO 3 and flux PbO-B2O3 or Bi2O3-B2O3; make it a saturated solution (10 ), after being completely dissolved, keep the temperature at 1100-1250°C for 5 hours;

<4>逐渐下降旋转提拉杆使衬底晶片下降到离饱和助熔剂液面3-5mm处,再在Lu1-x-yCeyYxAlO3结晶温度范围900-1150℃条件下恒温2-4小时;<4> Gradually lower and rotate the lifting rod to lower the substrate wafer to 3-5mm from the saturated flux liquid level, and then keep the crystallization temperature range of 900-1150℃ in Lu 1-xy Ce y Y x AlO 3 for 2-4 Hour;

<5>下降旋转提拉杆使衬底晶片正好接触饱和溶液内,旋转提拉杆以100-400r/min速度旋转,根据所需生长Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)薄膜厚度调节相应的生长时间,一般为3-20分钟,生长时间结束后,立即提起旋转提拉杆,使衬底脱离液面;<5> Lower the rotating lifting rod so that the substrate wafer just touches the saturated solution. The rotating lifting rod rotates at a speed of 100-400r/min. According to the required growth Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) Film thickness adjustment corresponding growth time, generally 3-20 minutes, after the growth time is over, lift the rotating lifting rod immediately to make the substrate out of the liquid surface;

<6>退火,将继续提起旋转提拉杆,使衬底晶片及其沉析在其上的Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)薄膜进入退火炉内的上侧发热体区间,调整上发热体的功率使其温度在900℃恒温30-60分钟后,然后以50℃/hr速度降温至室温,完成Lu1-x-yCeyYxAlO3/Lu1-zYzAlO3(0≤x≤0.9999,0.0001≤y≤0.05,0≤z≤1)闪烁荧光屏的制备。<6> For annealing, continue to lift the rotating lifting rod, so that the substrate wafer and the Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) film deposited on it enter the annealing process. For the upper heating element section in the furnace, adjust the power of the upper heating element to keep the temperature at 900°C for 30-60 minutes, then cool down to room temperature at a rate of 50°C/hr to complete Lu 1-xy Ce y Y x AlO 3 /Lu 1-z Y z AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05, 0≤z≤1) scintillation screen preparation.

所述的步骤<5>下降旋转提拉杆之前,先调整主炉体的侧发热体的发热功率,使中测温热电偶指示为900-1150℃,再恒温1-2h,然后再下降旋转提拉杆(6)。Before step <5> lowering and rotating the lifting rod, first adjust the heating power of the side heating element of the main furnace body so that the temperature measuring thermocouple indicates 900-1150°C, keep the temperature for 1-2 hours, and then lower and rotate to lift Pull rod (6).

本发明的技术效果如下:Technical effect of the present invention is as follows:

本发明与现有技术相比,一方面,由于铈离子掺杂的铝酸镥钇单晶Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)具有重密度(随着x的减小密度从5.4增加到8.6g/cm3)、高有效原子序数、高光输出(随着x增大而增大,12000Ph/Mve和15000Ph/Mve),快衰减(18-30ns)等优点,因此,本发明的荧光屏较在先技术中荧光屏具有更高的X射线吸收系数、更高的分辨率;另一方面,衬底采用与闪烁单晶薄膜组成相同的单晶组成,不存在失配,单晶薄膜质量高,荧光屏的光学性质好。另外,这种荧光屏的发光波长在370nm左右,其衍射极限更小,这样更有利于提高荧光屏的分辨率(一般为亚微米)。Compared with the prior art, the present invention, on the one hand, because the cerium ion-doped lutetium yttrium aluminate single crystal Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) has a heavy density (density increases from 5.4 to 8.6g/cm 3 as x decreases), high effective atomic number, high light output (12000Ph/Mve and 15000Ph/Mve increases as x increases), fast decay (18- 30ns) etc., therefore, the fluorescent screen of the present invention has higher X-ray absorption coefficient and higher resolution than the fluorescent screen in the prior art; , there is no mismatch, the quality of the single crystal film is high, and the optical properties of the phosphor screen are good. In addition, the emission wavelength of this fluorescent screen is about 370nm, and its diffraction limit is smaller, which is more conducive to improving the resolution of the fluorescent screen (generally submicron).

因此,采用本发明的闪烁荧光屏可以广泛应用于各种显微X射线成像应用领域中。Therefore, the scintillation fluorescent screen of the present invention can be widely used in various application fields of micro X-ray imaging.

附图说明Description of drawings

图1是本发明制备Lu1-x-yCeyYxAlO3/Lu1-zYzAlO3(0≤x≤0.9999,0.0001≤y≤0.05,0≤z≤1)闪烁荧光屏所用的电阻加热液相外延炉剖面示意图。Fig. 1 is the resistance heating used for the preparation of Lu 1-xy Ce y Y x AlO 3 /Lu 1-z Y z AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05, 0≤z≤1) scintillation fluorescent screen of the present invention Schematic diagram of the cross-section of the liquid phase epitaxy furnace.

具体实施方式Detailed ways

先请参阅图1,由图可见,本发明制备Lu1-x-yCeyYxAlO3/Lu1-zYzAlO3(0≤x≤0.9999,0.0001≤y≤0.05,0≤z≤1)闪烁荧光屏方法所使用的电阻加热液相外延炉的结构主要包括:Please refer to Figure 1 first, it can be seen from the figure that the present invention prepares Lu 1-xy Ce y Y x AlO 3 /Lu 1-z Y z AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05, 0≤z≤1 ) The structure of the resistance heating liquid phase epitaxy furnace used in the flashing fluorescent screen method mainly includes:

炉体1,炉体1下部是主炉体101,炉体1上部是退火炉体102。在炉体101内,中央置有坩埚9,坩埚9与炉体1同轴,主炉体101中相对坩埚9周围设有侧面发热体2,侧面发热体2的外围为绝热层11,坩埚9底下有绝热层13和能够调节坩埚9高低的底托12,退火炉102内有上侧发热体5,主炉体101还设有中测温热电偶3,退火炉102设有上测温热电偶,从炉体1的上顶盖中央向下延伸有一旋转提拉杆6,该旋转提拉杆6的下端为衬底夹具7,旋转提拉杆6与炉体1同轴。Furnace body 1, the lower part of the furnace body 1 is the main furnace body 101, and the upper part of the furnace body 1 is the annealing furnace body 102. In the furnace body 101, a crucible 9 is placed in the center, and the crucible 9 is coaxial with the furnace body 1. In the main furnace body 101, a side heating element 2 is arranged around the relative crucible 9, and the periphery of the side heating element 2 is an insulating layer 11. The crucible 9 There is a heat insulating layer 13 and a bottom support 12 that can adjust the height of the crucible 9. There is an upper side heating element 5 in the annealing furnace 102. The main furnace body 101 is also equipped with a middle temperature measuring thermocouple 3. The annealing furnace 102 is equipped with an upper temperature measuring thermocouple. Even, a rotating lifting rod 6 extends downward from the center of the upper top cover of the furnace body 1 , the lower end of the rotating lifting rod 6 is a substrate holder 7 , and the rotating lifting rod 6 is coaxial with the furnace body 1 .

坩埚9内置放含Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)多晶料和PbO-B2O3或Bi2O3-B2O3的助溶剂饱和溶液。从炉体顶上伸下有旋转提拉杆6,在旋转提拉杆6的下端有衬底夹具7,在衬底夹具7上置有LuzY1-zAlO3(0≤z≤1)衬底晶片,伸进坩埚9里。旋转提拉杆6与炉体1同中心轴线。在主炉体101的坩埚周围有侧面发热体2,在侧面发热体的外围有绝热层11,在坩埚9的底下有绝热层13以及有能够调节坩埚高低的底托12。在炉体1上部的退火炉102内有上侧发热体5。装置中还有中测温热电耦3,上测温热电耦4等。本发明装置中炉体1内的退火炉102使得生长完毕的荧光屏中的热应力,以防止开裂等。The crucible 9 contains Lu 1-xy Ce y Y x AlO 3 (0 ≤ x ≤ 0.9999, 0.0001 ≤ y ≤ 0.05) polycrystalline material and PbO-B 2 O 3 or Bi 2 O 3 -B 2 O 3 auxiliary solvent saturated solution. Extending down from the top of the furnace body is a rotating lifting rod 6, and at the lower end of the rotating lifting rod 6 there is a substrate holder 7, and a Lu z Y 1-z AlO 3 (0≤z≤1) lining is placed on the substrate holder 7. Bottom wafer stretches into crucible 9 li. The rotating lifting rod 6 is concentric with the furnace body 1 on the central axis. Around the crucible of the main furnace body 101, there is a side heating element 2, an insulating layer 11 is arranged on the periphery of the side heating element, an insulating layer 13 is arranged under the crucible 9 and a base 12 that can adjust the height of the crucible is arranged. Inside the annealing furnace 102 on the upper part of the furnace body 1 is an upper heating element 5 . The device also has a middle temperature measuring thermocouple 3, an upper temperature measuring thermocouple 4, and the like. The annealing furnace 102 in the furnace body 1 in the device of the present invention makes the thermal stress in the grown fluorescent screen to prevent cracking and the like.

本发明制备方法所采用的Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)多晶料助熔剂饱和溶液是由Lu1-x-yCeyYxAlO3多晶料与助熔剂氧化铅(PbO)和三氧化二硼(B2O3)或氧化铋(Bi2O3)和三氧化二硼(B2O3)按下列配比制的:The Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) polycrystalline flux saturated solution used in the preparation method of the present invention is composed of Lu 1-xy Ce y Y x AlO 3 Crystal material and flux lead oxide (PbO) and diboron trioxide (B 2 O 3 ) or bismuth oxide (Bi 2 O3) and diboron trioxide (B 2 O 3 ) are prepared according to the following ratio:

助熔剂PbO与B2O3的摩尔比为PbO∶B2O3=(8-15)mol∶1mol;或采取助熔剂Bi2O3与B2O3,其比例为Bi2O3∶B2O3=(10-12)mol∶(1-3mol);The molar ratio of flux PbO to B 2 O 3 is PbO:B2O3=(8-15)mol:1mol; or take flux Bi 2 O 3 and B 2 O 3 , the ratio is Bi 2 O 3 : B 2 O 3 = (10-12)mol: (1-3mol);

Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)多晶与助熔剂的重量百分比为:Lu1-x-yCeyYxAlO3/助熔剂=10wt%-50wt%The weight percent of Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) polycrystal and flux is: Lu 1-xy Ce y Y x AlO 3 /flux=10wt%- 50wt%

现结合以下具体实施例对本发明作进一步说明。The present invention will be further described in conjunction with following specific examples now.

实施例1:Lu0.9999Ce0.0001AlO3/luAlO3荧光屏Embodiment 1: Lu 0.9999 Ce 0.0001 AlO 3 /luAlO 3 fluorescent screen

所选用的电阻加热液相外延炉如图1所示的装置,主体炉101内的坩埚9为铂金坩埚。按照上述的制备工艺步骤<1>将多晶原料Lu0.9999Ce0.0001AlO3与助溶剂(PbO∶B2O3=10mol∶1mol)按重量百分比为Lu0.9999Ce0.0001AlO3/(PbO+B2O3)=0.20的配比进行称量共1000g,混合均匀后装入φ80×80mm的铂金坩埚9内;按工艺步骤<2>将尺寸为φ30×0.03mm,晶面方向为(010)的LuAlO3衬底8置于夹具7内,并将夹具7装入旋转提拉杆6底端,调整坩埚9与衬底晶片8的位置使其同轴,并且都处于主炉体101的中央;按上述步骤<3>将炉体101升温至1150℃,使原料与助熔剂熔融成饱和溶液10,并在1150℃恒温5小时后,按步骤<4>逐渐下降旋转提拉杆6,使衬底晶片8距饱和液面4mm,再在Lu0.9999Ce0.0001AlO3结晶温度范围的1050℃温度下恒温3小时;按上述工艺步骤<5>下降旋转提拉杆6使衬底晶片8刚好接触饱和溶液10内,并使旋转提拉杆6以300r/min速度旋转,在1050℃温度下恒温生长5分钟后,迅速提离旋转提拉杆6使衬底晶片及其上的单晶脱离液面,至此结晶完成;按上述工艺步骤<6>进行退火,将生长的Lu0.9999Ce0.0001AlO3单晶同衬底晶片8一起提拉至炉体1上方退火炉102的发热体5区间内,在900℃温度下恒温30分钟后,以50℃/Hr速度降温至室温,退火完毕,Lu0.9999Ce0.0001AlO3/luAlO3闪烁荧光屏制备完毕。The selected resistance heating liquid phase epitaxy furnace is as shown in FIG. 1 , and the crucible 9 in the main furnace 101 is a platinum crucible. According to the above-mentioned preparation process step <1>, the polycrystalline raw material Lu 0.9999 Ce 0.0001 AlO 3 and the co-solvent (PbO: B2O3 = 10mol: 1mol) are prepared according to the weight percentage of Lu 0.9999 Ce 0.0001 AlO 3 /(PbO+B2O3) = 0.20 Weigh a total of 1000g according to the proportion, mix it evenly, and put it into a platinum crucible 9 with a diameter of 80×80mm; according to the process step <2>, place 8 LuAlO 3 substrates with a size of 30×0.03mm and a crystal plane direction of (010) in the fixture 7, and put the fixture 7 into the bottom end of the rotating lifting rod 6, adjust the position of the crucible 9 and the substrate wafer 8 to make it coaxial, and both are in the center of the main furnace body 101; Heat the furnace body 101 to 1150°C to melt the raw materials and flux to form a saturated solution 10, and after keeping the temperature at 1150°C for 5 hours, gradually lower and rotate the lifting rod 6 according to step <4>, so that the substrate wafer 8 is 4mm away from the saturated liquid surface , and then keep the temperature at 1050°C in the crystallization temperature range of Lu 0.9999 Ce 0.0001 AlO 3 for 3 hours; lower and rotate the lifting rod 6 according to the above process step <5> to make the substrate wafer 8 just touch the saturated solution 10, and make the rotating lifting rod 6. Rotate at a speed of 300r/min. After growing at a constant temperature of 1050°C for 5 minutes, quickly lift off the rotating lifting rod 6 to remove the substrate wafer and the single crystal on it from the liquid surface, and the crystallization is completed; follow the above process steps <6 >Annealing is carried out, and the grown Lu 0.9999 Ce 0.0001 AlO 3 single crystal is pulled together with the substrate wafer 8 to the heating element 5 section of the annealing furnace 102 above the furnace body 1. The temperature is lowered to room temperature at a rate of ℃/Hr, the annealing is completed, and the Lu 0.9999 Ce 0.0001 AlO 3 /luAlO 3 scintillation phosphor screen is prepared.

这种闪烁荧光屏在显微X射线成像方面具有广泛的应用前景。This kind of scintillation fluorescent screen has broad application prospects in microscopic X-ray imaging.

实施例2:Y0.9999Ce0.0001AlO3/YAlO3荧光屏Example 2: Y 0.9999 Ce 0.0001 AlO 3 /YAlO 3 fluorescent screen

按照上述实施例1中步骤<1>将Y0.9999Ce0.0001AlO3多晶料与助溶剂(Bi2O3∶B2O3=8mol∶2mol)按重量百分比为Y0.9999Ce0.0001AlO3/(Bi2O3+B2O3)=0.40的配比进行称量共1000g,按上述实施例1中步骤<2>,将尺寸为φ20×0.03mm,晶面方向为(001)的YAlO3衬底8置于夹具7内,并将夹具7装入旋转提拉杆6底端,调整坩埚9与衬底晶片8的位置使其同轴,并且都处于主炉体101的中央;按上述实施例1中<3>将炉体101升温至1100℃,使原料与助熔剂熔融成饱和溶液10,并在1100℃恒温5小时后,按上述实施例1中<4>逐渐下降旋转提拉杆6,使衬底晶片8距饱和液面3mm,再在Y0.9999Ce0.0001AlO3结晶温度范围的1000℃温度下恒温3小时,按上述实施例1中<5>下降旋转提拉杆6使衬底晶片8的一端面与饱和溶液10液面接触,并使旋转提拉杆6以200r/min速度旋转,在1000℃温度下恒温生长10分钟后,迅速提离旋转提拉杆6使衬底晶片及其上的单晶脱离液面,至此结晶完成;按上述实施例1的步骤<6>进行退火,即将生长的Y0.9999Ce0.0001AlO3单晶同衬底晶片8一起提拉至炉体1上方退火炉102的发热区内,在900℃温度下恒温1小时后,以50℃/Hr速度降温至室温,退火完毕;完成Y0.9999Ce0.0001AlO3/YAlO3闪烁荧光屏的制备。According to step <1> in the above example 1, Y 0.9999 Ce 0.0001 AlO 3 polycrystalline material and cosolvent (Bi2O3: B2O3 = 8mol: 2mol) are Y 0.9999 Ce 0.0001 AlO 3 /(Bi2O3+B2O3) = 0.40 by weight percentage Weigh a total of 1000g according to the proportion of the above-mentioned embodiment 1, according to the step <2> in the above-mentioned embodiment 1, the YAlO 3 substrate 8 with a size of φ20×0.03mm and a crystal plane direction of (001) is placed in the fixture 7, and the fixture 7 Load the bottom end of the rotating lifting rod 6, adjust the position of the crucible 9 and the substrate wafer 8 to make it coaxial, and both are in the center of the main furnace body 101; according to <3> in the above embodiment 1, the furnace body 101 is heated to 1100°C, melt the raw material and the flux to form a saturated solution 10, and after keeping the temperature at 1100°C for 5 hours, gradually lower and rotate the lifting rod 6 according to <4> in the above-mentioned embodiment 1, so that the substrate wafer 8 is 3mm away from the saturated liquid surface, Then keep the temperature at 1000° C. in the crystallization temperature range of Y 0.9999 Ce 0.0001 AlO 3 for 3 hours, lower and rotate the lifting rod 6 according to <5> in the above-mentioned embodiment 1 to make one end surface of the substrate wafer 8 contact with the liquid surface of the saturated solution 10, And make the rotating lifting rod 6 rotate at a speed of 200r/min, and after growing at a constant temperature at 1000°C for 10 minutes, quickly lift off the rotating lifting rod 6 to remove the substrate wafer and the single crystal on it from the liquid surface, and the crystallization is completed; press Step <6> of the above-mentioned Example 1 is annealed, that is, the grown Y 0.9999 Ce 0.0001 AlO 3 single crystal is pulled together with the substrate wafer 8 into the heating zone of the annealing furnace 102 above the furnace body 1, and kept at a constant temperature of 900°C After 1 hour, the temperature was lowered to room temperature at a rate of 50° C./Hr, and the annealing was completed; the preparation of the Y 0.9999 Ce 0.0001 AlO 3 /YAlO 3 scintillation phosphor screen was completed.

实施例3:Y0.995Ce0.005AlO3/YAlO3荧光屏Example 3: Y 0.995 Ce 0.005 AlO 3 /YAlO 3 fluorescent screen

按照上述实施例2中步骤<1>将Y0.9999Ce0.005AlO3多晶料与助溶剂(Bi2O3∶B2O3=10mol∶1mol)按重量百分比为Y0.995Ce0.005AlO3/(Bi2O3+B2O3)=0.40的配比进行称量共1000g,重复上述实施例2中步骤<2>,<3>,<4>,<5>,<6>。最后完成Y0.995Ce0.005AlO3/YAlO3闪烁荧光屏的制备。According to step <1> in the above example 2, Y 0.9999 Ce 0.005 AlO 3 polycrystalline material and co-solvent (Bi2O3: B2O3 = 10mol: 1mol) are Y 0.995 Ce 0.005 AlO 3 /(Bi2O3+B2O3) = 0.40 by weight percentage Proportioning weighs a total of 1000g, and repeats steps <2>, <3>, <4>, <5>, <6> in the above-mentioned embodiment 2. Finally, the preparation of the Y 0.995 Ce 0.005 AlO 3 /YAlO 3 scintillation phosphor screen is completed.

实施例4:Lu0.697Y0.3Ce0.003AlO3/Lu0.7Y0.3AlO3荧光屏Example 4: Lu 0.697 Y 0.3 Ce 0.003 AlO 3 /Lu 0.7 Y 0.3 AlO 3 fluorescent screen

按照上述实施例2中步骤<1>将Lu0.697Y0.3Ce0.003AlO3多晶料与助溶剂(Bi2O3∶B2O3=8mol∶2mol)按重量百分比为Lu0.697Y0.3Ce0.003AlO3/(Bi2O3+B2O3)=0.50的配比进行称量共1000g,按上述实施例2中步骤<2>,将尺寸为φ20×0.03mm,晶面方向为(100)的Lu0.7Y0.3AlO3衬底8置于夹具7内,并将夹具7装入旋转提拉杆6底端,调整坩埚9与衬底晶片8的位置使其同轴,并且都处于主炉体101的中央;按上述实施例2中<3>将炉体101升温至1150℃,使原料与助熔剂熔融成饱和溶液10,并在1150℃恒温5小时后,按上述实施例2中<4>逐渐下降旋转提拉杆6,使衬底晶片8距饱和液面3mm,再在Lu0.697Y0.3Ce0.003AlO3结晶温度范围的1050℃温度下恒温3小时,按上述实施例2中<5>下降旋转提拉杆6使衬底晶片8的端面与饱和溶液10液面接触,并使旋转提拉杆6以400r/min速度旋转,在1050℃温度下恒温生长5分钟后,迅速提离旋转提拉杆6使衬底晶片及其上的单晶脱离液面,至此结晶完成;按上述实施例2的步骤<6>进行退火,即将生长的Lu0.697Y0.3Ce0.003AlO3单晶同衬底晶片8一起提拉至炉体1上方退火炉102的发热区内,在900℃温度下恒温50分钟后,以50℃/Hr速度降温至室温,退火完毕;完成Lu0.697Y0.3Ce0.003AlO3/Lu0.7Y0.3AlO3闪烁荧光屏的制备。According to step <1> in the above-mentioned embodiment 2, Lu 0.697 Y 0.3 Ce 0.003 AlO 3 polycrystalline material and cosolvent (Bi2O3: B2O3 = 8mol: 2mol) were calculated as Lu 0.697 Y 0.3 Ce 0.003 AlO 3 /(Bi2O3+ B2O3) = 0.50 proportioning to weigh a total of 1000g, according to the step <2> in the above-mentioned embodiment 2, the size is φ20 × 0.03mm, the crystal plane direction is (100) Lu 0.7 Y 0.3 AlO 3 substrate 8 placed in the clamp 7, and the clamp 7 is loaded into the bottom end of the rotating lifting rod 6, and the position of the crucible 9 and the substrate wafer 8 is adjusted to make it coaxial, and they are all located in the center of the main furnace body 101; according to the above-mentioned embodiment 2 <3> Heat the furnace body 101 to 1150°C to melt the raw materials and flux to form a saturated solution 10, and after keeping the temperature at 1150°C for 5 hours, gradually lower and rotate the lifting rod 6 according to <4> in the above-mentioned embodiment 2, so that the substrate Wafer 8 is 3 mm away from the saturated liquid surface, and then kept at a temperature of 1050° C. in the crystallization temperature range of Lu 0.697 Y 0.3 Ce 0.003 AlO 3 for 3 hours, and then lowered and rotated the lifting rod 6 according to <5> in the above-mentioned embodiment 2 to make the substrate wafer 8 The end surface is in contact with the liquid surface of the saturated solution 10, and the rotating lifting rod 6 is rotated at a speed of 400r/min. After growing at a constant temperature at 1050°C for 5 minutes, the rotating lifting rod 6 is quickly lifted away to make the substrate wafer and the single crystal on it From the liquid level, the crystallization is completed; annealing is carried out according to the step <6> of the above-mentioned embodiment 2, that is, the grown Lu 0.697 Y 0.3 Ce 0.003 AlO 3 single crystal is pulled together with the substrate wafer 8 to the annealing furnace 102 above the furnace body 1 In the heat generating area, keep the temperature at 900°C for 50 minutes, then cool down to room temperature at a rate of 50°C/Hr, and the annealing is completed; the preparation of the Lu 0.697 Y 0.3 Ce 0.003 AlO 3 /Lu 0.7 Y 0.3 AlO 3 scintillating phosphor screen is completed.

这种闪烁荧光屏具有较高的分辨率,它可以广泛应用于医学、全息成像、相衬成像等应用领域。The scintillation fluorescent screen has high resolution, and it can be widely used in medical, holographic imaging, phase contrast imaging and other application fields.

Claims (7)

1、一种掺铈铝酸镥钇亚微米成像荧光屏,其特征在于该荧光屏的结构是在晶面方向为(010)、(100)或(001)的Lu1-zYzAlO3(0≤z≤1)衬底及生长在其上的闪烁薄膜(Lu1-x-yCeyYxAlO3,即Lu1-x-yCeyYxAlO3/Lu1-zYzAlO3(0≤x≤0.9999,0.0001≤y≤0.05,0≤z≤1)。1. A cerium-doped lutetium-yttrium aluminate submicron imaging fluorescent screen, characterized in that the structure of the fluorescent screen is (010), (100) or (001) Lu 1-z Y z AlO 3 (0 ≤z≤1) substrate and the scintillation film grown on it (Lu 1-xy Ce y Y x AlO 3 , that is, Lu 1-xy Ce y Y x AlO 3 /Lu 1-z Y z AlO 3 (0≤ x≤0.9999, 0.0001≤y≤0.05, 0≤z≤1). 2、根据权利要求1所述的掺铈铝酸镥钇亚微米成像荧光屏,其特征在于所述Lu1-zYzAlO3(0≤z≤1)衬底的厚度为5-30微米,所述闪烁薄膜的厚度为0.3-10微米。2. The cerium-doped lutetium-yttrium aluminate submicron imaging fluorescent screen according to claim 1, characterized in that the Lu 1-z Y z AlO 3 (0≤z≤1) substrate has a thickness of 5-30 microns, The thickness of the scintillation film is 0.3-10 microns. 3、根据权利要求1所述的掺铈铝酸镥钇亚微米成像荧光屏的制备方法,其特征在于该荧光屏是将晶面方向为(010)、(100)或(001)的Lu1-zYzAlO3(0≤z≤1)单晶衬底作大面积籽晶,在电阻加热液相外延炉中,在LuzY1-zAlO3单晶的结晶温度下,与含有Lu1-x-yCeyYxAlO3多晶料的助熔剂饱和溶液接触界面上生长一层微米及亚微米量级的Lu1-x-yCeyYxAlO3单晶薄膜。3. The method for preparing the cerium-doped lutetium-yttrium aluminate submicron imaging fluorescent screen according to claim 1, characterized in that the fluorescent screen is a Lu 1-z crystal plane whose orientation is (010), (100) or (001). Y z AlO 3 (0≤z≤1) single crystal substrate as a large-area seed crystal, in a resistance heating liquid phase epitaxy furnace, at the crystallization temperature of Lu z Y 1-z AlO 3 single crystal, with Lu 1 A layer of Lu 1- xy Ce y Y x AlO 3 single crystal thin film of micron and submicron scale is grown on the contact interface of flux saturated solution of -xy Ce y Y x AlO 3 polycrystalline material. 4、根据权利要求3所述的掺铈铝酸镥钇亚微米成像荧光屏的制备方法,其特征在于所述的含有Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)多晶料助熔剂饱和溶液的原料配比如下:4. The method for preparing the cerium-doped lutetium-yttrium aluminate submicron imaging phosphor screen according to claim 3, characterized in that the said phosphor screen contains Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y ≤0.05) The raw material ratio of polycrystalline flux saturated solution is as follows: ①助熔剂溶液的组分配比为8-15mol的PbO和1mol B2O3,或10-12mol Bi2O3和1-3mol的B2O3① The component distribution ratio of the flux solution is 8-15mol of PbO and 1mol of B 2 O 3 , or 10-12mol of Bi 2 O 3 and 1-3mol of B 2 O 3 ; ②Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)多晶与助熔剂的重量百分比为:Lu1-x-yCeyYxAlO3/助熔剂溶液=10wt%-50wt%②The weight percent of Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05) polycrystal and flux is: Lu 1-xy Ce y Y x AlO 3 /flux solution=10wt% -50wt% 5、根据权利要求3所述的掺铈铝酸镥钇亚微米成像荧光屏的制备方法,其特征在于所述的电阻加热液相外延炉的结构主要包括:5. The method for preparing cerium-doped lutetium-yttrium aluminate submicron imaging fluorescent screen according to claim 3, characterized in that the structure of the resistance heating liquid phase epitaxy furnace mainly includes: 炉体(1),炉体(1)下部是主炉体(101),炉体(1)上部是退火炉体(102),在炉体(101)内,中央置有坩埚(9),坩埚(9)与炉体(1)同轴,主炉体(101)中相对坩埚(9)周围设有侧面发热体(2),侧面发热体(2)的外围为绝热层(11),坩埚(9)底下有绝热层(13)和能够调节坩埚(9)高低的底托(12),退火炉(102)内有上侧发热体(5),主炉体(101)还设有中测温热电偶(3),退火炉(102)设有上测温热电偶(4),从炉体(1)的上顶盖中央向下延伸一旋转提拉杆(6),该旋转提拉杆(6)的下端为衬底夹具(7),旋转提拉杆(6)与炉体(1)同轴。Body of furnace (1), body of furnace (1) bottom is main furnace body (101), body of furnace (1) top is annealing furnace body (102), and in body of furnace (101), crucible (9) is placed in the center, The crucible (9) is coaxial with the furnace body (1), and the main furnace body (101) is provided with a side heating element (2) around the relative crucible (9), and the periphery of the side heating element (2) is a heat insulating layer (11), There is an insulating layer (13) and a base (12) that can adjust the height of the crucible (9) under the crucible (9). There is an upper side heating element (5) in the annealing furnace (102), and the main furnace body (101) is also equipped with In the temperature measuring thermocouple (3), the annealing furnace (102) is provided with an upper temperature measuring thermocouple (4), and a rotating lifting rod (6) is extended downward from the center of the upper top cover of the furnace body (1). The lower end of the pull rod (6) is a substrate holder (7), and the rotating pull rod (6) is coaxial with the furnace body (1). 6、根据权利要求3所述的掺铈铝酸镥钇亚微米成像荧光屏的制备方法,其特征在于该方法包括下列步骤:6. The method for preparing the cerium-doped lutetium-yttrium aluminate submicron imaging fluorescent screen according to claim 3, characterized in that the method comprises the following steps: <1>根据选定的Lu1-x-yCeyYxAlO3多晶与助熔剂的配比称量原料,充分混合均匀后装入电阻加热液相外延炉的坩埚(9)中并装入炉体(1)中;<1> Weigh the raw materials according to the ratio of the selected Lu 1-xy Ce y Y x AlO 3 polycrystal and flux, mix them well and put them into the crucible (9) of the resistance heating liquid phase epitaxy furnace and put them into In the furnace body (1); <2>将晶面方向为(100)或(010)或(001)的Lu1-zYzAlO3(0≤z≤1)的衬底晶片(8)置入衬底夹具(7)内,调整旋转提拉杆(6),使之处于坩埚(9)的同轴位置上;<2> Put the substrate wafer (8) of Lu 1-z Y z AlO 3 (0≤z≤1) whose crystal plane direction is (100) or (010) or (001) into the substrate holder (7) Inside, adjust the rotating lifting rod (6) so that it is on the coaxial position of the crucible (9); <3>以100℃/Hr的升温速度升温至1050-1200℃,熔融多晶原料Lu1-x-yCeyYxAlO3与助熔剂PbO-B2O3或Bi2O3-B2O3;使其成为饱和溶液(10),待全部溶解后,在1100-1250℃恒温5小时;<3>Raise the temperature to 1050-1200°C at a heating rate of 100°C/Hr, melt polycrystalline raw material Lu 1-xy Ce y Y x AlO 3 and flux PbO-B2O3 or Bi2O3-B2O3; make it a saturated solution (10 ), after being completely dissolved, keep the temperature at 1100-1250°C for 5 hours; <4>逐渐下降旋转提拉杆(6)使衬底晶片(8)下降到离饱和助熔剂液面3-5mm处,再在Lu1-x-yCeyYxAlO3结晶温度范围900-1150℃条件下恒温2-4小时;<4> Gradually lower and rotate the lifting rod (6) to lower the substrate wafer (8) to 3-5mm from the saturated flux liquid level, and then crystallize in the Lu 1-xy Ce y Y x AlO 3 temperature range of 900-1150°C Keep the temperature constant for 2-4 hours; <5>下降旋转提拉杆(6)使衬底晶片(8)正好接触饱和溶液(10)内,旋转提拉杆(6)以100-400r/min速度旋转,根据所需生长Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)薄膜厚度调节相应的生长时间,一般为3-20分钟,生长时间结束后,立即提起旋转提拉杆(6),使衬底(8)脱离液面;<5> Lower the rotating lifting rod (6) so that the substrate wafer (8) just touches the saturated solution (10), and the rotating lifting rod (6) rotates at a speed of 100-400r/min to grow Lu 1-xy Ce as required y Y x AlO 3 (0 ≤ x ≤ 0.9999, 0.0001 ≤ y ≤ 0.05) film thickness to adjust the corresponding growth time, generally 3-20 minutes, after the growth time is over, immediately lift the rotating lifting rod (6) to make the substrate (8) out of the liquid surface; <6>退火,将继续提起旋转提拉杆(6),使衬底晶片(8)及其沉析在其上的Lu1-x-yCeyYxAlO3(0≤x≤0.9999,0.0001≤y≤0.05)薄膜进入退火炉(102)内的上侧发热体(5)区间,调整上发热体(5)的功率使其温度在900℃恒温30-60分钟后,然后以50℃/hr速度降温至室温,完成Lu1-x-yCeyYxAlO3/Lu1-zYzAlO3(0≤x≤0.9999,0.0001≤y≤0.05,0≤z≤1)闪烁荧光屏的制备。<6> Annealing, will continue to lift the rotating lifting rod (6), so that the substrate wafer (8) and the Lu 1-xy Ce y Y x AlO 3 (0≤x≤0.9999, 0.0001≤y) precipitated on it ≤0.05) the film enters the section of the upper heating element (5) in the annealing furnace (102), adjust the power of the upper heating element (5) to keep the temperature at 900°C for 30-60 minutes, and then at a speed of 50°C/hr Cool down to room temperature to complete the preparation of Lu 1-xy Ce y Y x AlO 3 /Lu 1-z Y z AlO 3 (0≤x≤0.9999, 0.0001≤y≤0.05, 0≤z≤1) scintillation phosphor screen. 7、根据权利要求6所述的掺铈铝酸镥钇亚微米成像荧光屏的制备方法,其特征在于所述的步骤<5>下降旋转提拉杆(6)之前,先调整主炉体(101)的侧发热体(2)的发热功率,使中测温热电偶(3)指示为900-1150℃,再恒温1-2h,然后再下降旋转提拉杆(6)。7. The method for preparing cerium-doped lutetium-yttrium aluminate submicron imaging fluorescent screen according to claim 6, characterized in that before step <5>, the main furnace body (101) is adjusted before the lifting rod (6) is lowered and rotated The heating power of the side heating element (2) makes the middle temperature measuring thermocouple (3) indicate 900-1150°C, keep the temperature constant for 1-2h, and then lower and rotate the lifting rod (6).
CNB2004100164741A 2004-02-23 2004-02-23 Cerium doped lutetium yttrium aluminium acid submicron imaging screen and its preparation method Expired - Fee Related CN1314067C (en)

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CN102399555A (en) * 2010-09-15 2012-04-04 海洋王照明科技股份有限公司 Aluminate fluorescent powder and preparation method thereof
US8189633B2 (en) 2005-12-13 2012-05-29 General Electric Company Polycrystalline transparent ceramic articles and method of making same
CN103421505A (en) * 2013-03-25 2013-12-04 上海显恒光电科技股份有限公司 UV single crystal fluorescence thin film grown based on liquid phase epitaxial method

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GB1116667A (en) * 1964-05-28 1968-06-12 Sylvania Electric Prod Cathodo-luminescent screens and phosphors therefor
CN1176253C (en) * 2002-07-26 2004-11-17 中国科学院上海光学精密机械研究所 Composite scintillation crystal material of cerium-doped lutetium aluminate yttrium aluminate and preparation method thereof

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CN1982259B (en) * 2005-12-13 2012-11-14 通用电气公司 Polycrystalline transparent ceramic articles and method of making same
CN102838352A (en) * 2005-12-13 2012-12-26 通用电气公司 Polycrystalline transparent ceramic articles and method of making same
CN102399555A (en) * 2010-09-15 2012-04-04 海洋王照明科技股份有限公司 Aluminate fluorescent powder and preparation method thereof
CN102399555B (en) * 2010-09-15 2013-07-24 海洋王照明科技股份有限公司 Aluminate fluorescent powder and preparation method thereof
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