以濺鍍法製備(Hf0.5Zr0.5)O2 薄膜於玻璃基板及其結構與鐵電性之研究

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Title:	以濺鍍法製備(Hf0.5Zr0.5)O2 薄膜於玻璃基板及其結構與鐵電性之研究
Other Titles:	Structure and ferroelectric properties of sputtered (Hf0.5Zr0.5)O2 films on glass substrates
Authors:	葉朋祐 YEH, PENG-YU
Contributors:	王昌仁;張晃暐 WANG, CHANG-REN;CHANG, HUANG-WEI 應用物理學系
Keywords:	(Hf0.5Zr0.5)O2;濺鍍法;結構;鐵電性 (Hf0.5Zr0.5)O2;sputtering;structure;ferroelectric
Date:	2019
Issue Date:	2019-12-16T07:03:20Z (UTC)
Abstract:	本研究以射頻磁控濺鍍法於Pt/glass 基板上製備HZO 薄膜，並藉由調整熱處理條件、HZO 薄膜生長條件、Pt 底層狀態等方法研究其結構與鐵電性，冀能獲具良好鐵電性之正交HZO 薄膜，並探討其鐵電相形成區間及鐵電性。首先，通入純Ar 作為工作氣體，在沉積壓力為70 mTorr，濺鍍功率為60 W，沉積10 nm 之HZO 薄膜並進行350 至750 oC 後退火，HZO 薄膜在退火550 oC 時，呈現出較高的正交相(111)/四方相(011)相比率，並可獲高的2Pr 為145 μC/cm2。而在上述的相同條下，沉積時通入20 % O2 將會導致HZO 薄膜在退火溫度為700 oC，才呈現出較多的正交相(111)/四方相(011)比率，與更高的2Pr 為188 μC/cm2。其後，本實驗選用前者(退火 550 oC)樣品進一步調整HZO 沉積壓力、不同Pt 底層狀態及不同O2 含量氣氛下後退火。實驗結果發現，HZO 薄膜在濺鍍功率為60 W時，正交相(111)之形成不穩定。若將HZO 薄膜濺鍍功率由60 W 提高至120 W 時，可以觀察到HZO 薄膜之正交相(111)/四方相(011)繞射峰位置由30.74 o偏移至30.48 o，此可證明改變HZO 薄膜濺鍍功率將有助於非鐵電相轉變為鐵電相。而在HZO 薄膜濺鍍功率為100 W 且在70 mTorr 的工作壓力下沉積10 nm HZO 薄膜，並進行550 oC 退火，其展現出較好的鐵電性，此與正交相(111)的出現有關，殘餘極化量與矯頑電場分別為2Pr = 269 μC/cm2、Ec=12.2 MV/cm。此外，濺鍍功率分別為100 W及120 W 下沉積HZO 薄膜於不同Pt 厚度並進行550 oC 後退火，其HZO 之正交相(111)/四方相(011)相比率並沒有明顯的差異。在不同工作距離下沉積Pt 膜後，在沉積以濺鍍功率為100 W 沉積10 nm HZO膜並在550 oC 下進行退火，其正交相(111)/四方相(011)相比率並沒有明顯的差異，值得注意的是，在11 cm 的工作距離下沉積Pt 膜後，在沉積以濺鍍功率為120 W 沉積10 nm HZO 膜並在550 oC 下進行退火，可呈現出優異的正交相(111)/四方相(011)織構。 In this study, we prepared HZO films on Pt/glass substrate by rf magnetron sputtering and studied the structure and ferroelectric properties of HZO films with modification of possessing parameters of HZO films, including thermal treatment conditions and sputtering parameters and also Pt underlayers with various stress states and thicknesses. Firstly, when pure argon is adopted as a working gas to deposit 10-nm-thick HZO films at pressure of 70 mTorr and sputtering power of 60 W, followed by postannealing at 350 to 750 oC, HZO film annealed at 550 oC exhibited higher volume fraction of o/t-phase and therefore a high 2Pr Value of 145 μC/cm2. In contrast, HZO film at sputtered atmosphere with 20% oxygen leads to large volume fraction of the o/t-phase at higher annealing temperature of 700 oC and a higher 2Pr of 188 μC/cm2. However, the experimental results show that the formation of o/t-phase is unstable for HZO films prepared at60 W through further adjustments of the pressure for HZO, Pt bottom state and O2 content atmospheres during post-annealing for HZO deposition at oxygen free environment. When the sputtering power for HZO deposition is increased from 60 W to 120 W, the shifted diffraction peak of o/t-phase from 30.74 ° to 30.48 ° indicates the formation of larger amount of ferroelectric o phase. Good ferroelectric properties of 2Pr = 269μC/cm2 and Ec = 12.2 MV/cm attained for 10-nm-thick HZO film deposited at 100 W and working pressure of 70 mTorr, then annealed at 550 oC, was related to the induction of o-phase (111). In addition, phase components for HZO films prepared at 120 W is almost same with that at 100 W. Effect of Pt underlayer is also studied. For HZO films at 100 W, the almost unchanged phase components with Pt underlayers, prepared at various distancesbetween target and substrate (3.5-11 cm) is found. Nevertheless, the optimized o(111)/t(011) texture is obtained for HZO film at 120 W and Pt underlayer prepared at distance between target and substrate of 11 cm. The result of this study provides important information for HZO films with good ferroelectric properties on metallic Pt underlayers by sputtering.
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