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金属学报  2020, Vol. 56 Issue (1): 99-111    DOI: 10.11900/0412.1961.2019.00006
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外延膜的高分辨X射线衍射分析
李长记1,邹敏杰1,2,张磊1(),王元明1(),王甦程1
1. 中国科学院金属研究所沈阳材料科学国家研究中心 沈阳 110016
2. 中国科学技术大学材料科学与工程学院 沈阳 110016
High-Resolution X-Ray Diffraction Analysis of Epitaxial Films
LI Changji1,ZOU Minjie1,2,ZHANG Lei1(),WANG Yuanming1(),WANG Sucheng1
1. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
2. School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China
引用本文:

李长记,邹敏杰,张磊,王元明,王甦程. 外延膜的高分辨X射线衍射分析[J]. 金属学报, 2020, 56(1): 99-111.
Changji LI, Minjie ZOU, Lei ZHANG, Yuanming WANG, Sucheng WANG. High-Resolution X-Ray Diffraction Analysis of Epitaxial Films[J]. Acta Metall Sin, 2020, 56(1): 99-111.

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摘要: 

广泛应用于半导体、铁电和光电材料中的外延结构特征以及应变和缺陷会影响外延膜的物理/化学性能。高分辨X射线衍射是对外延结构进行无损准确表征的关键技术。本文从高分辨X射线衍射与外延结构倒易空间的关系出发,重点阐述高分辨X射线衍射与普通X射线衍射的联系与区别,以强调高分辨X射线衍射特征。以铁电外延膜与衬底结构高分辨X射线衍射为例,系统分析它们的高分辨X射线衍射斑特征,包括共格生长、非共格生长、倾斜生长下衍射斑特征,以及外延膜的尺寸、外延膜的倾斜扭转和外延膜的应变对衍射斑的影响等。结合Si1-xGex(x=0.1)等外延膜结构的具体分析阐述如何通过高分辨X射线衍射谱来获取外延膜结构参数,包括外延膜晶格常数、晶格错配度以及厚度和超晶格等信息。本文还系统介绍了高分辨X射线衍射中的倒易平面图的作法,以及相关的理论和实验方法,并据此获得了PbTiO3外延膜的应力状态、畴结构、相变等结构信息。

关键词 薄膜生长外延膜高分辨X射线衍射倒易空间作图    
Abstract

Epitaxy technique has been widely used for semiconductor, ferroelectric and optical materials in the development of electronic and optoelectronic devices. Epitaxial structures with strain and defects may tune the physical properties or affect the performance of devices. High-resolution X-ray diffraction (HRXRD) has significant advantages over traditional XRD with the features of small divergence, monochromatic incident beam and high resolution detection of the diffracted beam. It is a key technique for accurate characterization of epitaxial structures in non-destructive way. In this paper, the techniques of HRXRD for epitaxial film structure characterization are outlined in terms of the relationship between diffraction and reciprocal space, the difference between high-resolution diffraction and powder diffraction such as the optical system and the geometry mode of scanning etc. Based on the corresponding relationship between the epitaxial film and the matrix structure in the reciprocal space, various factors affecting the shape of the diffraction spots are analyzed, including the state of lattice match in coherence and non-coherence, super lattice and inclined growth. The other effective factors are also demonstrated, such as finite size of film, tilt and strain of epitaxial film etc. Real examples, such as Si1-xGex(x=0.1) etc., are used to explain how to obtain the structure parameters of the epitaxial films by HRXRD spectrum analysis, including lattice constant, lattice mismatch, thickness and superlattice information. To obtain more epitaxy information, reciprocal space map (RSM) analysis can be feasibly used by reconstruction of a series of HRXRD patterns. By combining HRXRD spectrum and RSM, microstructure characterizations of PbTiO3 epitaxy films, such as micro-strain, domain structure, phase transformation can be quantitatively analyzed.

Key wordsfilm growth    epitaxial film    high-resolution X-ray diffraction    reciprocal space mapping
收稿日期: 2019-09-29     
ZTFLH:  TG142  
作者简介: 李长记,男,1987年生,博士
图1  SrTiO3单晶的倒易空间与衍射条件示意图
图2  X射线粉末衍射和高分辨衍射的光路系统示意图
图3  样品与探测器的旋转轴
图4  扫描方式与衍射几何示意图
图5  立方结构外延膜和衬底的(h0l)倒易面
图6  影响衍射斑点宽化的因素
图7  立方Si1-xGex/Si外延膜(Layer)和衬底(Substrate)(004)面和(224)面衍射强度和2θ关系曲线
图8  沿ΔG的强度分布
图9  含有8个周期的(La0.3Sr0.7MnO3/PbTiO3)8/DyScO3超晶格结构(002)衍射强度与2θ关系曲线
图10  Si1-xGex/Si外延结构的低角X射线强度与2θ关系曲线
图11  非对称反射方法测定时角度差Δθ=θL-θS和Δτ=τL-τS的成因
图12  Si1-xGex /Si外延结构的(206)+和(206)-衍射强度与2θ关系曲线
图13  沿LaAlO3衬底[001]方向外延生长的PbTiO3薄膜组成的外延结构(010)倒易空间平面示意图
图14  PbTiO3/LaAlO3外延结构中衬底PbTiO3和外延膜中畴结构的(002)衍射斑的(010)倒易空间平面图的局部图
图15  PbTiO3/SrRuO3/SrTiO3外延结构和新相Pb2O3的(002)衍射斑的(010)倒易空间平面图的局部图
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