Lu2SiO5: Ce3+透明薄膜制备及其发光性能研究

doi:10.15541/jim20160034

摘要/Abstract

摘要：

Lu₂SiO₅: Ce³⁺薄膜具有高光产额、快衰减时间、高密度、高空间分辨率等优点, 有望成为X射线探测中的闪烁材料, 但制备高质量的薄膜面临挑战。本工作采用溶胶凝-胶法, 通过对制备过程中水硅比、烧结程序、胶黏剂和固含量等四个因素的系统研究与分析, 结果表明: 在空气湿度为85%, 溶胶水硅比为6.6条件下, 适量添加PEG400, 采用优化后最佳固含量, 从450℃开始进行烧结程序后退火, 可制备出具有透明、平整、无裂痕的高质量Lu₂SiO₅: Ce³⁺闪烁薄膜, 单次旋涂获得的膜厚达到167 nm。实验表明水含量是引起薄膜发白的主要因素; 烧结程序决定了薄膜的有机物分解程度及结晶状况; 溶胶固含量及胶黏剂含量是调控薄膜厚度的重要方法。本工作为Lu₂SiO₅: Ce³⁺闪烁薄膜的实际应用奠定了基础。

关键词: Lu2SiO5: Ce3+薄膜, 水硅比, 烧结程序, 胶黏剂, 固含量, 发光性能

Abstract:

Lu₂SiO₅: Ce³⁺ thin film is a promising material for X-ray detection due to its high light output, short decay time, high density, and high spatial resolution. In present work, Lu₂SiO₅: Ce³⁺thin films were prepared by Sol-Gel method. The optimal experimental conditions were obtained concerning solid content, adhesive content, water content, and annealing progress. Under the conditions with air humidity of 85%, sol’s H₂O-Si ratio of 6.6, appropriate amount of PEG400, optimized solid content, and sintering starting from 450℃, the thin films are prepared crack-free with high transparence and excellent luminescent properties. The thickness of its single layer is 167 nm. It is found that water content is the major factor that causes film foggy, and sintering progress affects the reaction of organics and crystallization. Furthermore, solid content and the adhesive content are the two factors controlling the film thickness. The present study may promote the application of Lu₂SiO₅: Ce³⁺ thin films in detection systems.

Key words: Lu2SiO5: Ce3+ thin film, H2O-Si ratio, sintering process, adhesive, solid content, luminescence properties

中图分类号:

O482

吴霜, 刘波, 陈士伟, 张娟楠, 刘小林, 顾牡, 黄世明, 倪晨, 薛超凡. Lu₂SiO₅: Ce³⁺透明薄膜制备及其发光性能研究[J]. 无机材料学报, 2016, 31(9): 948-954.

WU Shuang, LIU Bo, CHEN Shi-Wei, ZHANG Juan-Nan, LIU Xiao-Lin, GU Mu, HUANG Shi-Ming, NI Chen, XUE Chao-Fan. Preparation and Luminescence Properties of Lu₂SiO₅: Ce³⁺ Thin Film[J]. Journal of Inorganic Materials, 2016, 31(9): 948-954.

图/表 12

表1 制备LSO: Ce薄膜的溶胶基础配比

Table 1 Basic composition of sol for preparing LSO: Ce thin film

C₃H₇O₂/mL	H₂O-Si ratio	Lu(NO₃)₃·6H₂O /g	PEG400/mL	Lu/Ce
10	6.6	2.3451	0.45	0.997/0.003

表2 不同环境湿度与水硅比条件下制备的薄膜情况

Table 2 Situation of thin films prepared at environment of different humidity and H2O-Si ratio

Humidity	H₂O-Si ratio	Situation
85%	15.0	Foggy
85%	10.0	Foggy
85%	6.6	Transparent
70%	15.0	Foggy
70%	10.0	Transparent
70%	6.6	Transparent
65%	15.0	Transparent
65%	10.0	Unable to form film
65%	6.6	Unable to form film

图1 空气湿度为85%, 溶胶中水硅比分别为10(a)与6.6(b)条件下所制备的LSO: Ce薄膜照片

Fig. 1 Pictures of LSO: Ce thin films prepared by sol with H2O-Si ratios of 10 (a) and 6.6 (b) at humidity of 85%

图2 添加PEG时干凝胶DSC曲线

Fig. 2 DSC curve of xerogel added with PEG

图3 (a)从室温开始与(b)从450℃开始进行烧结程序制备的LSO: Ce薄膜的光学显微照片及其(c)光致发光光谱图

Fig. 3 Microscope images of LSO: Ce thin films with sintering process starting from (a) room temperature and (b) 450℃, and (c) their corresponding emission spectra

图4 (a)从室温开始与(b)从450℃开始进行烧结程序制备的LSO: Ce薄膜的XRD图谱

Fig. 4 XRD patterns of LSO: Ce thin films sintered at temperature starting from room temperature (a) and 450℃ (b)

图5 添加适量PEG400溶胶所制备的单层LSO: Ce薄膜透射谱

Fig. 5 Transmission spectrum of single LSO: Ce thin film prepared by the added sol with appropriate amount of PEG400

图6 优化配比的溶胶所制备的LSO: Ce薄膜SEM照片

Fig. 6 SEM image of single LSO: Ce thin film prepared by the sol with optimized proportion

图7 不同固含量的溶胶所制备的LSO: Ce薄膜实物图片

Fig. 7 Pictures of LSO: Ce thin films with different solid contents(a) but with 9 mL C3H7O2, (b) according to Table 1 and (c) but with 11 mL C3H7O2

图8 不同固含量溶胶所制备的薄膜发射光谱

Fig. 8 Emission spectra of LSO: Ce thin films with different solid contents Proportioning in Table 1 but 9 mL C3H7O2 (a), proportioning in Table 1 (b) and proportioning in Table 1 but 11 mL C3H7O2 (c)

图9 不同固含量的溶胶所制备的薄膜AFM图片

Fig. 9 AFM images of LSO: Ce thin films with different solid contents According to Table 1 only (a) and with 9 mL C3H7O2 (b)

图10 LSO: Ce薄膜发射光谱及高斯拟合后的图谱

Fig. 10 Emission spectrum of LSO: Ce thin film and its fitting result

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Lu₂SiO₅: Ce³⁺透明薄膜制备及其发光性能研究

Preparation and Luminescence Properties of Lu₂SiO₅: Ce³⁺ Thin Film

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