摘 要

本研究是利用具有快速鍍膜及保持多元系統化學計量比的脈衝雷射鍍膜法( pulsed laser deposition，PLD )來進行0.67Pb(Mg1/3Nb2/3)O3-0.33PbTiO3 (PMN-PT)鐵電薄膜的生長。在判斷靶材與薄膜的相鑑定方面是以X-ray繞射儀來進行，薄膜厚度則是利用X-ray反射法來量測。由實驗的結果發現：在鍍膜溫度為600℃~700℃、氧壓為2x10-1 torr，可以在MgO(100)基板上成長出磊晶結構的薄膜；薄膜磊晶結構的品質則利用Φ- scan加以確認。
實驗中藉由成長不同時間的薄膜，發現薄膜在成長時間超過60分鐘後性質上的差異。薄膜的折射率及消光係數是利用橢圓偏光儀來量測，薄膜的表面粗糙度則是利用原子力顯微鏡掃描所獲得。由實驗亦發現：當薄膜成長時間超過60分鐘，開始出現(110)及焦綠石相等其它非磊晶的結構，這樣的現象亦可由折射率和消光係數的變化及表面粗糙度的大幅增加得到印證。最後，成長La0.5Sr0.5CoO3 (LSCO)為上下電極，順利的量測到薄膜的介電性及鐵電性(極化強度-電場)。

Abstract

The growth of 0.67Pb(Mg1/3Nb2/3)O3-0.33PbTiO3 (PMN-PT) ferrooelectric thin films were prepared by pulsed laser deposition ( PLD ), which has the advantages of high depositing rate and maintaining the stoichiometrical ratio. The phase of target and thin films were identified with X-ray diffractometer, and the thickness of thin films was measured by x-ray reflectivity. Epitaxial 0.67PMN-0.33PT thin films on MgO(100) substrate were obtained by PLD at 600℃~700℃ and 2x10-1 torr (O2). The quality of epitaxial films was confirmed by Φ- scan.
With different depositing time, we developed the differences of the properties by depositing thin films over 60 mintues. The refractive index and extinction coefficient of thin films were measured by spectroscopic ellipsometry, and the roughness of thin films were derived by atomic force microscopy. When the depositing time was over 60 minutes, thin films began to form other orientation of (110) and pyrochlore, and so on. It also proved by the variation of refractive index and extinction coefficient and the increase of roughness. Eventually, the dielectric and ferroelectric(P-E curve) were measured successfully by depositing the top and bottom electrode of LSCO.

參考文獻
[1] S. W. Choi, T. R. Shrout, S. T. Jang, and A. S. Bhalla, "Dielectric and pyroelectric properties in the Pb(Mg1/3 Nb2/3)O3-PbTiO3 system", Ferroelectrics. 100, 29 (1989).
[2] S. L. Swartz, T. R. Shrout, W. A. Schultz, and L. E. Cross, "Dielectric properties of Lead-Magnesium Niobate ceramics", J. Am. Ceram. Soc. 67, 311(1984).
[3] L. F. Francis and D. A. Payne, "Thin layer dielectrics in the Pb[(Mg1/3Nb2/3)1-xTix]O3 system", J. Am. Ceram. Soc. 74, 3000(1991).
[4] 汪健民主編，"陶瓷技術手冊"，中華民國產業科技發展協進會及中
華民國冶金協會出版，pp. 230~231(1994).
[5] 吳朗，"電子陶瓷入門"，全欣，pp.159-161（1992）.
[6] 吳朗，"電子陶瓷─介電陶瓷"，(1994).
[7] 詹國楨審定，朱建國主編，"電子與光電子材料"，新文京，pp.139(1992).
[8] Charles Kittel, "Introduction to Solid State Physics", 7th Ed, John Wiley
and Sons, Inc., New York(1995）.
[9] C. -S. Tu, V. Hugo, Schmidt, and I. G. Siny, "Hypersound anomalies and elastic constants in single-crystal PbMg[sub1/3]Nb[sub2/3]O[sub3] by Brillouin scattering", J. Appl. Phys. 78, 5665 (1995).
[10] L.E. Cross, "Relaxor Ferroelectrics", Ferroelectrics 76, 241 (1987).
[11] L. A. Shebanov, P. P. Kapostins, and J. A. Zvirgzds, "The structure change of PMN in the diffuse phase transition region", Ferroelectrics 56, 1057 (1984).

[12] M. L. Mulvihill, S. E. Park, G. Risch, Z. Li, K. Uchino, and T. R. Shrout, " The role of processing variables in the flux growth of Lead Zinc Niobate-Lead Titanate relaxor ferroelectric single crystals", Jpn. J. Appl.
Phys. 35, 3984 (1996).
[13] S. -E. Paek and T. R. Shrout, "Ultrahigh strain and piezoelectric behavior in relaxor based ferroelectric single crystals", J. Appl. Phys. 82, 1804 (1997).
[14] Y. Yamashita, "Large electromechanical coupling factors in perovskite binary material system", Jpn J. Appl. Phys. 33, 5328 (1994).
[15] C. -S. Tu, F. -C. Chao, C. -H. Yeh, C. -L. Tsai, and V. H. Schmidt, Phys. Rev. B 60, 6348 (1999).
[16] B. Noheda, D. E. Cox, G. Shirane, J. Gao, and Z. -G. Ye, "Phase diagram of the ferroelectric-relaxor (1-x)PbMg(1/3)Nb(2/3)O3-xPbTiO3", Phys. Rev. B 66, 054104（2002）.
[17] M. Lejeune and J. P. Boilot, "Formation mechanism and ceramic process of the ferroelectric perovskite : Pb(Mg1/3Nb2/3)O3 and Pb(Fe1/2Nb1/2)O3", . Ceram.Int. 8, 99(1982).
[18] M. Inada, "Analysis of the formation process of the piezoelectric PMN ceramics", Jpn.Nat1.Tech.Repr. 27, 95(1977).
[19] S. L. Swartz and T. R. Shrout, "Fabrication of perovskite Lead Magnesium Niobate", Mat. Res. Bull. 17, 1245 (1982).
[20] L. F. Francis and D. A. Payne, " Processing, perovskite phase
development, and dielectric properties for sol-gel derived Pb[(Mg1/3Nb2/3)0.9Ti0.1]O3 thin layers", Mater. Res. Soc. Symp. Proc. 200, 173(1990).

[21] K. R. Udayakumar, J. Chen, P. J. Schuele, L. E. Cross, V. Kumar and S. B.
Krupanidhi, " Polarization reversal and high dielectric permittivity in lead magnesium niobate titanate thin films", Appl. Phys. Lett. 60, 1187(1992).
[22] J. Chen, Q. Zhang, and L. E. Cross: Ferroelectric Thin Films III, eds. E. R. Myers, and B. A. Tuttle, S. B. Desu and P. K. Larsen, Mater. Res. Soc. Symp. Proc. 310, 47(1993).
[23] M. C. Jiang, T. Hong, and T. B. Wu, " Deposition and characterization of ferroelectric Pb[(Mg1/3Nb2/3) xTi1- x]O3 thin films by RF magnetron sputtering", Jpn. J. Appl. Phys. 33, 6301(1994).
[24] M. C. Jiang and T. B. Wu, " Effects of electrode composition on RF magnetron sputtering deposition of Pb[(Mg1/3Nb2/3)0.7Ti0.3]O3 films", J. Mater. Res. 9, 1879 (1994).
[25] Y. Takeshima, K. Shiratsuyu, H. Takagi, and K. Tomono, "Preparation of Lead Magnesium Niobate Titanate thin films by chemical vapor deposition", Jpn. J. Appl. Phys. 34, 5083 (1995).
[26] C. Tantigate, J. Lee, and A. Safari, " Processing and properties of Pb(Mg1/3Nb2/3)O3–PbTiO3 thin films by pulsed laser deposition", Appl. Phys. Lett. 66, 1611 (1995).
[27] Apurba Laha, S. Saha, and S. B. Krupanidhi, "Role of La0.5Sr0.5CoO3 template layers on dielectric and electrical properties of pulsed-laser ablated Pb(Nb2/3Mg1/3)O3 - PbTiO3 thin films", Thin Solid Films 424, 274(2003).
[28] K. Y. Chan, W. S. Tsang, C. L. Mak, and K. H. Wong, "Effects of composition of PbTiO3 on optical properties of (1–x)PbMg1/3Nb2/3O3-xPbTiO3 thin films", Physical Review B. 69, 144111 (2004).
[29] 汪健民主編，"材料分析"，中國材料科學學會，pp.83~84(1991).
[30] H. G. Tompkins and W. A. McGahan,"Spectroscopic Ellipsometry and Reflectometry, A User’s Guide", John Wiley and Sons, New York(1999).
[31] J. C. Jans, "Nondestructive analysis by spectroscopic ellipsometry", Philips J. Res. 47, 347(1993).
[32] R. M. A. Azzam and N. M. Bashara, "Ellipsometry and Polarized Light",
North-Holland, Amsterdam, (1977).
[33] D. K. Bowen and B. K. Tanner, Nanotechnology 4, 175 (1993).