Low temperature preparation of PbTiO3 ultrathin films deposited by PbO gas phase reaction sputtering

Jiyoon Kim, S. Buhlmann, Moonkyu Park, Yunseok Kim, Yong Kwan Kim
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Abstract

In silicon integrated circuit technology, ferroelectric thin films have been importantly studied since they are the most promising materials for future non-volatile memory devices due to their fast switching speed and long-term retention time. PbTiO3 (PTO) is the one of the most suitable material for non-volatile memory devices, because it has the highest spontaneous polarization (PS) value. The subject of size effect on ferroelecticity has been of highest interest for many years to overcome the limit of memory density. As the ferroelectric film thickness decrease, it is possible to make small domain size of penetrating the film thickness direction. Another issue of ferroelectric thin film is reducing the preparation temperature, because the high temperature during the fabrication might degrade the bottom electrode, and leads to interface reaction between the ferroelectric film and Si substrate. To make thin and smooth PTO films, TiO2 was deposited on the Pt bottom electrode, and PbO gas phase reaction was carried out by static and rotation mode at a temperature as low as 450�??. TiO2 seed layer increase the number of active sites for PTO nucleation and, hence, allows crystallization of perovskite phase. To prepare PTO films below TC (493�??), PbO deposition power and target to substrate distance were controlled. As the temperature decreases, PbO layer was remained on the PTO surface, and it degraded the ferroelectric property of PTO films. However, it is possible to eliminate PbO layer on PTO films by reducing the PbO deposition power and increasing the target to sample distance until 100 mm. Zr buffer layer was inserted between PTO film and Pt bottom electrode to enhance the leakage property, and layer-by-layer preparation method was adopted to exclude the un-reacted TiO2. These methods enhance the switching property of PTO films. In summary, thin and smooth PTO ultra-thin films successfully deposited using the gas phase reaction sputtering below TC, and this method suggest us the possibility for high-density memory device.
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PbO气相反应溅射低温制备PbTiO3超薄膜
在硅集成电路技术中,铁电薄膜由于其快速的开关速度和长期的保持时间而成为未来非易失性存储器件最有前途的材料,因此得到了重要的研究。PbTiO3 (PTO)具有最高的自发极化(PS)值,是最适合用于非易失性存储器件的材料之一。为了克服记忆密度的限制,铁电性的尺寸效应是多年来备受关注的课题。随着铁电薄膜厚度的减小,有可能使穿透薄膜厚度方向的畴尺寸变小。铁电薄膜的另一个问题是降低制备温度,因为制备过程中的高温可能会降解底电极,并导致铁电薄膜与Si衬底之间的界面反应。为了制备薄而光滑的PTO薄膜,在Pt底电极上沉积TiO2,在低至450℃的温度下通过静态和旋转方式进行PbO气相反应。TiO2种子层增加了PTO成核的活性位点数量,从而允许钙钛矿相的结晶。为了制备低于TC(493℃)的PTO薄膜,控制了PbO的沉积功率和靶与衬底的距离。随着温度的降低,PbO层残留在PTO表面,降低了PTO薄膜的铁电性能。然而,通过降低PbO沉积功率和增加靶样距离至100 mm,可以消除PbO膜上的PbO层。在PTO膜与Pt底电极之间插入Zr缓冲层以增强漏损性能,并采用逐层制备方法排除未反应的TiO2。这些方法提高了PTO薄膜的开关性能。综上所述,采用气相反应溅射的方法成功地沉积了薄而光滑的PTO超薄薄膜,为高密度存储器件提供了可能。
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