在蓝宝石衬底上生长的La_（0.5）Ca_（0.5）MnO_3薄膜的面内取向问题研究
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摘要
自从在La2/3Ca1/3MnO3外延薄膜中发现庞磁电阻效应以来,钙钛矿型锰氧化物R1-xAxMnO3(R=La,Nd,Sm,Pr;A=Ca,Sr,Ba,Pb等)一直倍受人们的关注。钙钛矿型锰氧化物在铁磁居里温度附近表现出较大的磁电阻效应(在几特斯拉磁场下可达106%)。与块材相比,锰氧化物薄膜表现出较大的磁电阻效应。锰氧化物薄膜的微结构受到衬底性质的影响,而锰氧化物薄膜的微结构决定了它的磁性和输运性质。因此,对薄膜结构的研究有助于加深对类钙钛矿锰氧化物所具有的各种奇特物性的理解,也会推动以此类材料为基础的磁电子器件的研制。
过去在蓝宝石衬底上生长的锰氧化物薄膜大多是多晶的。本文使用传统固相反应法制作La0.5Ca0.5MnO3靶材,然后通过脉冲激光沉积法在(0001)取向的蓝宝石衬底上生长了La0.5Ca0.5MnO3薄膜。通过调整薄膜制备条件,得到了具有取向性的薄膜。论文利用常规X射线衍射方法分析了La0.5Ca0.5MnO3薄膜与A12O3衬底之间的面外取向关系,然后利用X射线掠入射衍射方法分析了薄膜与衬底的面内取向关系,最终得到薄膜与衬底之间存在着三组平行关系：(110)f//(0006)s,((?))f//(3030)s,(112)f//(1210)s。但是由于X射线衍射技术的局限性,还需借助其他实验技术进一步确认得到的面内取向关系。实验所得到的数据中也存在着一些暂时无法解释的现象,还需做进一步研究。
Perovskite manganites with the formula R1-xAxMnO3 (R=La, Nd, Sm, Pr; A=Ca, Sr, Ba, Pb) have renewed interest since the colossal magnetoresistance was discovered in the epitaxial film. Perovskite manganites display the bigger magnetoresistive effect nearby the ferromagnetic Curie temperature(reach 106% under several Tesla magnetic field). Compare with the bulk materials, manganite films exhibit a stronger magnetoresistive effect. The microstructure of manganite films rely on the nature of substrate, moreover, the microstructure of manganite films influences strongly its magnetism and the transport property. Therefore, the study of the structure of the film will be helpful to understand a variety of peculiar properties in the perovskite-like manganites, and promote the development of magnetoelectronic devices based on such materials.
In the past, all the reports on the growth of manganite films on the sapphire substrate have indicated that the films are polycrystalline in nature. In this article we used the traditional solid state reaction to manufacture La0.5Ca0.5MnO3 target, then we grew the La0.5Ca0.5MnO3 film through the pulse laser deposition on the (0001) orientation sapphire substrate. Through the adjustment of the experiment condition, we obtained the oriented film. In the article we used the conventional X-ray diffraction method to analyze the out-of-plane orientation relationship between the La0.5Ca0.5MnO3 film and Al2O3 substrate and the glancing incidence X-ray diffraction to analyze the in-plane orientation relationship between the film and the substrate, Finally we discovered three groups of parallel relationship between the film and the substrate:(110)f//(0006)s, (220)f//(3030)s, (112)f //(1210)s. But as a result of the X-ray diffraction technical limitation, we need to confirm the obtained in-plane orientation relationship by other experiment technology. In the experiment we also obtained the phenomena which are unable to be explained temporarily and need further studies.
过去在蓝宝石衬底上生长的锰氧化物薄膜大多是多晶的。本文使用传统固相反应法制作La0.5Ca0.5MnO3靶材,然后通过脉冲激光沉积法在(0001)取向的蓝宝石衬底上生长了La0.5Ca0.5MnO3薄膜。通过调整薄膜制备条件,得到了具有取向性的薄膜。论文利用常规X射线衍射方法分析了La0.5Ca0.5MnO3薄膜与A12O3衬底之间的面外取向关系,然后利用X射线掠入射衍射方法分析了薄膜与衬底的面内取向关系,最终得到薄膜与衬底之间存在着三组平行关系：(110)f//(0006)s,((?))f//(3030)s,(112)f//(1210)s。但是由于X射线衍射技术的局限性,还需借助其他实验技术进一步确认得到的面内取向关系。实验所得到的数据中也存在着一些暂时无法解释的现象,还需做进一步研究。
Perovskite manganites with the formula R1-xAxMnO3 (R=La, Nd, Sm, Pr; A=Ca, Sr, Ba, Pb) have renewed interest since the colossal magnetoresistance was discovered in the epitaxial film. Perovskite manganites display the bigger magnetoresistive effect nearby the ferromagnetic Curie temperature(reach 106% under several Tesla magnetic field). Compare with the bulk materials, manganite films exhibit a stronger magnetoresistive effect. The microstructure of manganite films rely on the nature of substrate, moreover, the microstructure of manganite films influences strongly its magnetism and the transport property. Therefore, the study of the structure of the film will be helpful to understand a variety of peculiar properties in the perovskite-like manganites, and promote the development of magnetoelectronic devices based on such materials.
In the past, all the reports on the growth of manganite films on the sapphire substrate have indicated that the films are polycrystalline in nature. In this article we used the traditional solid state reaction to manufacture La0.5Ca0.5MnO3 target, then we grew the La0.5Ca0.5MnO3 film through the pulse laser deposition on the (0001) orientation sapphire substrate. Through the adjustment of the experiment condition, we obtained the oriented film. In the article we used the conventional X-ray diffraction method to analyze the out-of-plane orientation relationship between the La0.5Ca0.5MnO3 film and Al2O3 substrate and the glancing incidence X-ray diffraction to analyze the in-plane orientation relationship between the film and the substrate, Finally we discovered three groups of parallel relationship between the film and the substrate:(110)f//(0006)s, (220)f//(3030)s, (112)f //(1210)s. But as a result of the X-ray diffraction technical limitation, we need to confirm the obtained in-plane orientation relationship by other experiment technology. In the experiment we also obtained the phenomena which are unable to be explained temporarily and need further studies.
引文
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2. Weidong Yu,Xiaomin Li,Feng Wu et al.Effects of oxygen partial pressure on the resistance switching properties of Lao.7Cao.3Mn03 thin films prepared by pulsed laser deposition method.Proc.of SPIE.2008(6984):698439
3. E.Dagotto,Y.Tokura.Theme Article-Strongly Correlated Electronic Materials:Present and Future.MRS Bull.2008(33):1037
4. C.Zener.Interaction between the d-Shells in the Transition Metals. II. Ferromagnetic Compounds of Manganese with Perovskite Structure.Phys.Rev.1951(82):403
5. W.Boujelben,A.Cheikhrouhou,H.Fuess,R.Madar.Structure, ferromagnetism and magnetotransport properties in the barium-deficient Pr0.7Ba0.2□0.1MnO3 manganite oxides.J.Magn.Magn.Mater.2003(257):319
6. P.G.de Gennes.Calculation of the Electron Binding Energies and X-Ray Energies for the Superheavy Elements 114,126, and 140 Using Relativistic Self-Consistent-Field Atomic Wave Functions.Phys.Rev.1960(118):174
7.陈永虔,谷坤明,唐涛等.掺K+和Ag+的LaMnO3的室温磁电阻效应.磁性材料及器件.2001年6月,9
8. T.Tang,Q.Q.Cao,K.M.Gu,H.Y.Xu,S.Y.Zhang,Y.W.Du.Giant magnetoresistance of the La1-xAgxMnO3 polycrystalline inhomogeneous granular system.Appl.Phys.Lett.2001 (77):723
9. Q.Y.Xu,R.P.Wang, Z.Zhang.Role of Ag in La1-xAgxMnO3 manganite perovskite. Phys.Rev.B.2005(71):092401
10.李润伟,王志宏,陈新,沈保根.钙钛矿型稀土锰氧化物La2/3Ca1/3MnO3中Mn位的Ti替代效应.物理学报.1999(13)：105-110
11.李宝河,鲜于文旭,张健,马廷钧,Magnetic Properties and Colossal Magnetoresistance of Lao.7Sro.3MnO3 Materials Doped with Fe.中国稀土学报.2002(20)：2
12. Maigna A,Martin C et al.Oxygen Vacancy Ordering in the Double-layered Ruddlesden-Popper Cobaltite Sm2BaCo2O7-δ.J Magn.Magn.Mater.2000(211):173
13. A.B.Pippard,Magnetoresistance in Metals.Cambridge University Press,Cambridge,1989
14. N.W.Aschcroft,N.D.Mermin.Solid State Physics.Holt,Reihart and Winsoton,New York,1976
15. P.L.Rossiter.The Electrical Resistivity of Metals and Alloys.Cambridge University Press,Cambridge,1987
16. W.F.Leverton,A.J.Dekker.Hall Coefficient and Resistivity of Thin Films of Antimony Prepared by Distillation.Phys.Rev.1950(80):732-736
17. J.Babiskin.Oscillatory Galvanomagnetic Properties of Bismuth Single Crystals in Longitudinal Magnetic Fields.Phys.Rev.1957(107):981-992
18. Z.Y.Lee,J.J.Qiu,G.Q.Lin et al.Fourth International Sysmposition on Physics of Magnetic Materials,1998,26apl-20
19. W.Thomson.On the thermal effects of fluids in motion.Proc.Roy.Soc.1856(8):546
20. H.C.Van Elst.Galvanomagnetic Effects, Magnetostriction, and Spin-Orbit Interaction in Cu-Ni-Fe and Other Ferromagnetic Nickel Alloys.Physica.1959(25):708
21. T.R.McGuire,R.I.Potter.Anisotropic magnetoresistance in ferromagnetic 3d alloys.IEEE Trans.Magn.1975(11):1018-1038
22. R.P.Hunt.A magnetoresistive readout transducer.IEEE Magn.Mag.1971(7):150-154
23. Baibich M N,Broto J M,Fert A.Giant Magnetoresistance of (001)Fe/(001)Cr Magnetic Superlattices. Phys.Rev.Lett.1988(61):2472-2475
24. P.W. Anderson,H.Hasegawa.Considerations on Double Exchange.Phys.Rev.1955(100):675
25. A. J.Mills,P.B.Littlewwod,B.I.Shraiman.Lattice Effects in the Colossal-Magnetoresistance Manganites.Phys.Rev.Lett.1996(76):1356-1359
26. Achutharaman V S,Kraus P A,Vas'ko V A,et al.Growth of La-Ca-Mn-O films by ozone-assisted molecular beam epitaxy.Appl Phys Lett.1995(67):1019-1021
27. Chahara K-I,Ohno T,Kasai M,et al.Magnetoresistance in magnetic manganese oxide with intrinsic antiferromagnetic spin structure.Appl Phys Lett.1993(63):1990-1992
28. Li K,Qi Z,Li X,et al.Growth, Structural Characteristics and Magnetoresistance in LaCaMnO Thin Films Prepared by dc Magnetron Sputtering.Thin Solid Films.1997(304):386-391
29. Vlakhov E S,Chakalov R A,Chakalova R I,et al.Strong influence of the Mn3+ content on the binding energy of the lattice polarons in manganese perovskites.J Appl Phys.1998(83):2152-2157
30. McCormack M,Jin S,Tiefel T H,et al.Very large magnetoresistance in perovskite-like La-Ca-Mn-O thin films.Appl Phys Lett.1994(64):3045-3047
31. Snyder G J,Hiskes R,DiCarolis S,et al.Intrinsic electrical transport and magnetic properties of Lao.67Cao.33MnO3 and Lao.67Sr0.33MnO3 MOCVD thin films and bulk material.Phys Rev B.1996(53):14434-14444
32. Bae S-Y,Wang S X.Fabrication of Lao.8Na0.2Mn1-xCuxO3 (x=0,0.05) thin films on YSZ substrates via chemical solution deposition.J Mater Res.1998(13):3234-3240
33. H.M.Smith,A.F.Turner.Vacuum deposited thin films using a ruby laser. Appl.Opt.1965(4):147-148
34. D.Dijkkamp,T.Venkatesan,X.D.Wu,S.A.Shareen,N.Jiswari,Y.H.MinLee,W.L.McLean, M.Croft.Preparation of Y-Ba-Cu oxide superconductor thin films using pulsed laser evaporation from high Tc bulk material.Appl.Phys.Lett.1987(51):619-621
35.戢明,宋全胜,曾晓雁.脉冲激光沉积(PLD)薄膜技术的研究现状与展望.真空科学与技术.2003(23)：22-26
36.黄继颇,王连卫,高剑侠.脉冲准分子激光沉积AIN薄膜的研究.中国激光.1999(26)：815-818
37. M.Rusop,K.Uma,T.Soga et al.Post-growth annealing of zinc oxide thin films pulsed laser deposited under enhanced oxygen pressure on quartz and silicon substrates.Materials Science and Engineering B.2006(127):150-153
38. J.Narayau,P.Tiwari,X.Chen et al.Epitaxial growth of TiN films on (100) silicon substrates by laser physical vapor deposition.Appl.Phys.Lett.1992(61):1290-1292
39. R.D.Vispute,V.Talyansky,R.P.Sharma et al.Growth of epitaxial GaN films by pulsed laser deposition.Appl.Phys.Lett.1997(71):102-104
40. Hans-Ulrich Krebs et al.Pulsed Laser Deposition (PLD)-a versatile thin film technique.Solid-State.Phys.2003(43):505-517
41. M.Volmer,A.Weber.Keimbildung in ubersattigen gebilden.Z.Phys.Chem.1926(119):277-301
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