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金属学报  2019, Vol. 55 Issue (8): 1019-1033    DOI: 10.11900/0412.1961.2018.00470
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交叉轧制周期对高纯Ta板变形及再结晶梯度的影响
祝佳林1,刘施峰1(),曹宇1,柳亚辉1,邓超1,2,刘庆1,2
1. 重庆大学材料科学与工程学院 重庆 400044
2. 重庆大学电子显微镜中心 重庆 400044
Effect of Cross Rolling Cycle on the Deformed and Recrystallized Gradient in High-Purity Tantalum Plate
Jialin ZHU1,Shifeng LIU1(),Yu CAO1,Yahui LIU1,Chao DENG1,2,Qing LIU1,2
1. College of Materials Science and Engineering, Chongqing University, Chongqing 400044, China
2. Electron Microscopy Center, Chongqing University, Chongqing 400044, China
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摘要: 

采用新的轧制工艺即135°交叉轧制,获得1周期和2周期Ta板。结合XRD、EBSD、显微硬度及TEM等技术,系统研究了1和2周期Ta板不同厚度层晶粒的变形及再结晶行为。结果表明,2周期Ta板沿厚度方向形成了均匀的θ-fiber和γ-fiber混合型织构。此外,2周期Ta板不同厚度层中{111}与{100}晶粒内的储存能分布也更为均匀。通过EBSD和TEM对变形Ta板的微结构进行表征发现,1周期中心层{111}晶粒内出现了许多相互平行的微带及微剪切带,而2周期表面与中心层晶粒发生相对均匀的变形且亚组织呈胞块状。这主要是因为交叉轧制周期的增加显著地提高了位错交互、湮灭和重排的几率,有利于改善晶粒内部组织的均匀性。因此,2周期Ta板退火时表面和中心层再结晶动力学基本保持一致。

关键词 高纯Ta交叉轧制周期储存能微剪切带再结晶    
Abstract

Cross rolling plays an important role in the production of high-quality tantalum (Ta) sputtering targets, which are crucial in achieving thin films for micro-electronic components. However, the effect of the cross rolling cycle on the microstructure homogeneity is always ignored. Therefore, 1 and 2 cycle samples were obtained by a new approach named a 135° cross rolling. The deformation and recrystallization behavior of high-purity Ta plate then was systematically compared between 1 and 2 cross rolling cycles, aiming to elucidate why the increase of cross rolling cycles can effectively ameliorate the microstructure gradient along the thickness direction. XRD results showed that the 2 cycle sample through the thickness consisted of a relatively homogenous {111}<uvw> ([111]//normal direction (ND)) and {100}<uvw> ([100]//ND) fibers while texture distribution was extremely uneven for the 1 cycle sample. The stored energy was quantitatively analyzed by X-ray line profile analysis (XLPA) and it was found that the stored energy across the thickness distributed more homogeneously for the 2 cycle sample. Misorientation characteristics of deformed grains with different rolling cycles were analyzed in detail by visualizing the misorientation angle based on an electron backscatter diffraction dataset. Many well-defined microbands and microshear bands occurred in the {111} grain at the center layer for the 1 cycle sample, while it can be effectively destroyed with the increase of the cross rolling cycle and few peaks occurred in the "point to point" plot. Kernel average misorientation (KAM) and grain reference orientation deviation-hyper (GROD-Hyper) further confirmed their differences. Then, micorband and microshear bands were detailedly characterized by TEM, and the analysis based on relative Schmid factor suggested that the primary slip system activated in the {111} grains led to the formation of microbands in the 1 cycle sample, while multiple slip systems appeared to be activated in the 2 cycle sample and deformation was more uniform. Upon annealing, the remarkably reduced stored energy gap between the {111} and {100} grain as well as the relatively homogeneous deformation microstructure between the surface and center layer for the 2 cycle sample was conductive to synchronous recrystallization together, while the high stored energy as driving force and preferential nucleation sites at the center region led to faster recrystallization for the 1 cycle sample. The recrystallization microstructure was relatively uniform and smaller variation in grain size for the 2 cycle sample through the thickness, which was beneficial to the application of Ta sputtering target. Therefore, the increase of cross rolling cycle can ameliorate the recrystallized kinetics and microstructure of high purity Ta plate.

Key wordshigh-purity tantalum    cross rolling cycle    stored energy    microshear band    recrystallization
收稿日期: 2018-10-12     
ZTFLH:  TG146.4  
基金资助:国家自然科学基金项目(Nos.U51421001 and 51701302)
通讯作者: 刘施峰     E-mail: liusf06@cqu.edu.cn
Corresponding author: Shifeng LIU     E-mail: liusf06@cqu.edu.cn
作者简介: 祝佳林,男,1993年生,博士生

引用本文:

祝佳林,刘施峰,曹宇,柳亚辉,邓超,刘庆. 交叉轧制周期对高纯Ta板变形及再结晶梯度的影响[J]. 金属学报, 2019, 55(8): 1019-1033.
Jialin ZHU, Shifeng LIU, Yu CAO, Yahui LIU, Chao DENG, Qing LIU. Effect of Cross Rolling Cycle on the Deformed and Recrystallized Gradient in High-Purity Tantalum Plate. Acta Metall Sin, 2019, 55(8): 1019-1033.

链接本文:

https://www.ams.org.cn/CN/10.11900/0412.1961.2018.00470      或      https://www.ams.org.cn/CN/Y2019/V55/I8/1019

图1  135°交叉轧制中第1周期和第2周期的工艺示意图
Rolling cycleRolling passEntrance thicknessExit thickness mmRolling gap geometryStrain per passTotal rolling reduction
mmh-1%%
First cycle120.017.22.0114.0014.0
217.214.72.2214.5326.5
314.712.62.3714.2837.0
412.610.82.5614.2846.0
510.89.32.7213.8953.5
69.38.02.9513.9860.0
78.06.93.1513.7565.5
86.96.03.2913.0470.0
Second cycle96.05.33.3111.6773.5
105.34.73.4611.3276.5
114.74.23.5510.6479.0
124.23.83.549.5281.0
133.83.53.367.8982.5
143.53.23.668.5784.0
153.23.03.236.2585.0
163.02.83.456.6787.0
表1  周向轧制的具体参数
图2  1和2周期Ta板沿厚度方向的织构分布图
Rolling cyclePositionDiffraction planeYhkl[21,22,23]vhkl[21,22,23]BrBaEhkl
GPaJ·mol-1
First cycleSurface(200)145.5170.3160.1850.1003.997
(222)387.9310.3620.3180.1405.037
Quarter(200)145.5170.3160.1790.1003.636
(222)387.9310.3620.3020.1404.425
Center(200)145.5170.3160.2180.1006.192
(222)387.9310.3620.4530.14011.469
Second cycleSurface(200)145.5170.3160.1900.1004.306
(222)387.9310.3620.3120.1404.804
Quarter(200)145.5170.3160.1860.1004.058
(222)387.9310.3620.2950.1404.166
Center(200)145.5170.3160.1970.1004.753
(222)387.9310.3620.3260.1405.356
表2  不同厚度层不同取向晶粒内的储存能及用于计算的相关参数
图3  1周期和2周期Ta板表面和中心层的取向成像图
图4  1和2周期Ta板表面和中心层{111}和{100}取向晶粒线扫描相邻点之间的取向差分布图
图5  1和2周期样品表面与中心层{111}与{100}晶粒内部的OIM、GROD-Hyper和KAM分布图
图6  1和2周期Ta板表面与中心层晶粒在1050 ℃退火不同时间的OIMs
图7  1和2周期Ta板在1050 ℃退火120 min后的晶粒尺寸分布图
图8  1和2周期Ta板表面和中心层在1050 ℃退火不同时间后的显微硬度曲线
Texture135°270°405°540°
γ fiber(60°, 55°, 45°)(195°, 55°, 45°)(330°, 55°, 45°)(105°, 55°, 45°)(240°, 55°, 45°)
{111}<011>{111}<341>{111}<211>{111}<314>{111}<011>
(90°, 55°, 45°)(225°, 55°, 45°)(0°, 55°, 45°)(135°, 55°, 45°)(270°, 55°, 45°)
{111}<112>{111}<143>{111}<110>{111}<413>{111}<112>
θ fiber(0°, 0°, 45°)(135°, 0°, 45°)(270°, 0°, 45°)(45°, 0°, 45°)(180°, 0°, 45°)
{001}<110>{001}<100>{001}<110>{001}<010>{001}<110>
(45°, 0°, 45°)(180°, 0°, 45°)(315°, 0°, 45°)(90°, 0°, 45°)(225°, 0°, 45°)
{001}<010>{001}<110>{001}<100>{001}<110>{001}<010>
表3  轧制织构随轧制方向旋转角度的演变
图9  1和2周期Ta板{111}和{100}晶粒内位错形貌的TEM像和SAED花样
Rolling cyclepositionPointEuler angle (φ1, φ, φ2)Maximum (SM)Secondary (SS)? / %
First cycleSurface-{111}P1(358.82, 36.219, 49.918)0.43170.39628.2233
P2(1.6153, 35.251, 47.642)0.42510.39247.6923
P3(3.5297, 35.013, 46.584)0.42190.39546.2811
Surface-{100}P1(97.475, 36.196, 2.1378)0.28360.26775.6064
P2(97.253, 36.315, 3.9174)0.28440.26955.2391
P3(97.851, 36.060, 3.2431)0.28710.26936.1999
Center-{111}P1(203.06, 39.914, 17.290)0.46570.395615.0526
P2(201.92, 40.490, 17.615)0.46630.392615.8052
P3(201.61, 40.022, 18.037)0.46750.395615.3796
Center-{100}P1(277.21, 20.078, 87.222)0.36690.33758.0130
P2(278.54, 20.308, 86.565)0.36900.33449.3766
P3(279.73, 20.075, 85.354)0.37020.33379.8595
Second cycleSurface-{111}P1(178.23, 33.425, 48.046)0.42690.40634.8254
P2(177.25, 32.668, 48.757)0.43050.41134.4599
P3(176.55, 33.356, 48.129)0.42470.40913.6731
Surface-{100}P1(284.72, 32.614, 74.052)0.30130.28415.7085
P2(287.28, 31.133, 72.346)0.30680.29075.2477
P3(285.63, 31.163, 73.580)0.30510.28875.3752
Center-{111}P1(38.471, 44.421, 2.9263)0.40780.37667.6508
P2(38.870, 44.086, 2.0842)0.40730.37906.9481
P3(39.115, 43.609, 1.7601)0.40890.37737.7280
Center-{100}P1(103.58, 34.267, 86.929)0.30670.29314.4343
P2(102.67, 34.886, 88.888)0.30440.28855.2233
P3(102.64, 35.064, 88.995)0.30370.28695.5317
表4  相对Schmid因子(?)及其相关参数
图10  沿图5a1~d1中线L1~L8的?分布图
图11  1和2周期Ta板表面和中心层{111}与{100}取向晶粒的衬度分布图
Rolling cyclePositionGrain orientationQi(gi)QmaxQminHi / (J·mol-1)
First cycleSurface{100}86.5121.513.53.241
{111}76.5109.522.53.793
Center{100}82.5119.518.53.663
{111}63.5125.514.55.586
Second cycleSurface{100}96.5130.523.53.178
{111}93.5128.529.53.535
Center{100}91.5126.520.53.302
{111}87.5126.518.53.611
表5  EBSD半定量评估Ta板表面和中心层{111}和{100}晶粒内的储存能及相关参数
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