纳米La_（0.8）Sr_（0.2）FeO_3薄膜材料制备及其光电子特性研究
摘要
本文使用自行设计并安装的一套提拉膜设备,利用溶胶-凝胶提拉法制备出了合乎要求的La_(0.8)Sr_(0.2)FeO_3纳米薄膜。与其他方法相比,提拉制膜方法既简便易行又节约能源。测试结果表明,与相同粒径该粉体材料相比,薄膜材料最大光伏响应的波长范围发生明显的蓝移现象,这说明该纳米薄膜材料具有更加独特的表面光伏特性和表面电子结构。
利用柠檬酸法制备的过渡金属复合氧化物La_(0.8)Sr_(0.2)FeO_3,通过改变固相反应条件控制其粒径大小。利用光声光谱和表面光电压谱研究了两种不同粒径nano-La_(0.8)Sr_(0.2)FeO_3的光致电荷跃迁机制和能量转换行为。根据测试结果研究了不同粒径该材料的表面电子结构。同时,利用低真空环境下的表面光电压谱研究了在真空环境下样品的光激发电荷转移行为。分析发现,当粒径小于10 nm时,La_(0.8)Sr_(0.2)FeO_3表现出了更加明显的表面效应,这一现象充分证实了前面所得结论的正确性。
研究结果表明,不同粒径的La_(0.8)Sr_(0.2)FeO_3的表面光电压谱及光声光谱不仅响应曲线的峰型发生变化,其响应范围及响应强度也存在明显的差异,这充分体现了纳米材料的量子尺寸效应和表面效应。场诱导表面光电压谱的结果证实该材料具有p型光伏特征,随着粒径的增大其p型光伏特性增强。
研究结果说明,薄膜的制备可以大大拓宽该材料实际应用领域。
Nano-La_(0.8)Sr_(0.2)FeO_3 thin film was prepared by a dip-coating machinemade by ourselves. Comparing with other methods, this is easier to operate.What's more, this can save energy sources. The result shows that shift toshortwave exists in Surface Photovoltage Spectroscopy (SPS) respondingrange of thin film comparing with SPS of powder with same particle size. Thisshows that inimitable photovoltage characters and structure of surfaceelectrons appeared in this thin film.
The transition metal complex oxide nano-La_(0.8)Sr_(0.2)FeO_3 was synthesizedwith citrate method. The size of the particles is controlled by the conditions ofsolid reaction. The photoexcited transition mechanism, the energy conversionbehaviors and the structure of surface electrons of La_(0.8)Sr_(0.2)FeO_3 withdifferent particle size were studied by SPS and Photo acoustic Spectroscopy(PAS). SPS in vacuum was discussed too. More obvious surface effect willappear when the particle size of La_(0.8)Sr_(0.2)FeO_3 is less than 10 nm. Thisphenomenon proved the correctness of the conclusion mentioned before.
The result shows that the shape of respnding peak changed in SPS andPAS of La_(0.8)Sr_(0.2)FeO_3 with different particle-size. Differences existed in SPSresponding range and intensity which can be explained by quantum effect andsurface effect. The characters of p-type photovoltage in this material isrepresented in electric field induced SPS (EFISPS). The characters of p-typephotovoltage will enhance as the augment of particle size.
The prearation of thin film can enlarge the application field of thismaterial by the studies and findings.
利用柠檬酸法制备的过渡金属复合氧化物La_(0.8)Sr_(0.2)FeO_3,通过改变固相反应条件控制其粒径大小。利用光声光谱和表面光电压谱研究了两种不同粒径nano-La_(0.8)Sr_(0.2)FeO_3的光致电荷跃迁机制和能量转换行为。根据测试结果研究了不同粒径该材料的表面电子结构。同时,利用低真空环境下的表面光电压谱研究了在真空环境下样品的光激发电荷转移行为。分析发现,当粒径小于10 nm时,La_(0.8)Sr_(0.2)FeO_3表现出了更加明显的表面效应,这一现象充分证实了前面所得结论的正确性。
研究结果表明,不同粒径的La_(0.8)Sr_(0.2)FeO_3的表面光电压谱及光声光谱不仅响应曲线的峰型发生变化,其响应范围及响应强度也存在明显的差异,这充分体现了纳米材料的量子尺寸效应和表面效应。场诱导表面光电压谱的结果证实该材料具有p型光伏特征,随着粒径的增大其p型光伏特性增强。
研究结果说明,薄膜的制备可以大大拓宽该材料实际应用领域。
Nano-La_(0.8)Sr_(0.2)FeO_3 thin film was prepared by a dip-coating machinemade by ourselves. Comparing with other methods, this is easier to operate.What's more, this can save energy sources. The result shows that shift toshortwave exists in Surface Photovoltage Spectroscopy (SPS) respondingrange of thin film comparing with SPS of powder with same particle size. Thisshows that inimitable photovoltage characters and structure of surfaceelectrons appeared in this thin film.
The transition metal complex oxide nano-La_(0.8)Sr_(0.2)FeO_3 was synthesizedwith citrate method. The size of the particles is controlled by the conditions ofsolid reaction. The photoexcited transition mechanism, the energy conversionbehaviors and the structure of surface electrons of La_(0.8)Sr_(0.2)FeO_3 withdifferent particle size were studied by SPS and Photo acoustic Spectroscopy(PAS). SPS in vacuum was discussed too. More obvious surface effect willappear when the particle size of La_(0.8)Sr_(0.2)FeO_3 is less than 10 nm. Thisphenomenon proved the correctness of the conclusion mentioned before.
The result shows that the shape of respnding peak changed in SPS andPAS of La_(0.8)Sr_(0.2)FeO_3 with different particle-size. Differences existed in SPSresponding range and intensity which can be explained by quantum effect andsurface effect. The characters of p-type photovoltage in this material isrepresented in electric field induced SPS (EFISPS). The characters of p-typephotovoltage will enhance as the augment of particle size.
The prearation of thin film can enlarge the application field of thismaterial by the studies and findings.
引文
1 陈光华,邓金祥.纳米薄膜技术与应用.北京:化学工业出版社,2004:18-24
2 A. L. Kholkin, R. Martins, H. Aguas, et al. Metal–ferroelectric thin film devices. Journal of Non-Crystalline Solids,2002,299:1311-1315
3 Tomita Katsuhiko, Takamuro Daisuke, Samada Kazuaki. Electron emission type infrared imaging sensor using ferroelectric thin plate. Sensors and Actuator A,2002,98:147-152
4 K. Ueda, H. Tabata, T. Kawai. Ferromagnetism in LaFeO_3-LaCrO_3 Superlattices. Science,1998,280:1064-1066
5 A. Scholl, J. St?hr, J. Lüning, et al. Observation of Antiferromagnetic Domains in Epitaxial Thin Films. Science,2000,287:1014-1016
6 陈敬中.现代晶体化学–理论与方法.北京:高等教育出版社,2001:407-408
7 T. Takagahara. Localization and energy transfer of quasi-two-dime-nsional excitons in GaAs-AlAs quantum-well heterostructures. Phys.Rev.B,1985,31:6552
8 R. Kubo. The theory about the nano-materials. J. Phys. Soc. Jpn.,1962,17:975-980
9 M. Achermann, M. A. Petruska. Energy-transfer pumping of semiconductor nanocrystals using an epitaxial quantum well. Nature,2004,429:642-646
10 郑伟涛.薄膜材料与薄膜技术.北京:化学工业出版社,2004:11-25
11 韩喜江.铁氧体薄膜吸波材料的研究进展.中国材料科技与设备,2005,2(2):17
12 王强.溶胶-凝胶法制备 La 掺杂钛酸铋薄膜和多层膜及其铁电性质研究.[苏州大学硕士学位论文].2005:13-20
13 Wen-Tsang Liu, Jyh-Fu Lee, Jenn-Ming Wu. X-ray absorption spectroscopic study of barium ferrite thin films synthesized by sol-sel method. Materials Chemistry and Physics,2001,69:89-94
14 Jae-Gwang Lee, Hi Min Lee, Chul Sung Kim, et al. Magnetic properties of CoFe_2O_4 powders and thin films grown by a sol-sel method. J. Magnetism and Magnetic Materials,1998,177-181:900-902
15 M. Paranthaman, T. G. Chirayil. Fabrication of Long Lengths of YBCO Coated Conductors using a Continuous Reel-to-Reel Dip-Coating Unit. Applied Super Conductivity,2001,11(1):3146-3149
16 何作鹏.溶胶-凝胶提拉法制备 MgxNi1-xO 薄膜与表征.半导体学报,2002, 26(4):721-725
17 K. Daoudi, B. Canut, Blanchi, et al.Tin doped in dium oxide thin films deposited by sol-sel dip-coating technique. Materials Science and Engineering,2002,21:313-317
18 P. J. Kelly, R. D. Arnell. Magnetron sputtering: a review of recent developments and applications. Vacuum,2000(56):159-172
19 尹洪禹,吴作良,谢文利,杨森.超高真空射频磁控溅射镀膜机(双室三靶)及其应用.真空技术与应用,2000,3:25-28
20 I. Safi. A novel reactive magnetron sputtering technique for producing insulating oxides of metal alloys and other compound thin films. Surface and Coatings Technology,2000,135:48-59
21 Yuan-Bin Chen, Cheng-Liang Huang. Properties of MgTiO3 thin films prepared by RF magnetron sputtering for microwave application. Journal of Crystal Growth,2005,282:482-489
22 F. Huisken, B. Kohn. Structured films of light-emitting silicon nanoparticles produced by cluster beam deposition. Applied Physics Letters,1999, 74(25):3776-3778
23 J. F. Tong, H. L. Hsiao, H. L. Hwang. Adjustable emissions from silicon-rich oxide films prepared by plasma-enhanced chemical-vapor deposition. Applied Physics Letters,1999,74(16):2316-2318
24 N. Taylor, H. Kim, P. Desjardins, et al. Greene. Si(011)16×2 gas-source molecular beam epitaxy: Growth kinetics. Applied Physics Letters,2000, 76(20):2853-2855
25 Byungha Shin, P. John Leonard, W. James McCamy, et al. Comparison of morphology evolution of Ge(001) homoepitaxial films grown by pulsed laser deposition and molecular-beam epitaxy. Applied Physics Letters,2005, 87(181916):1-3
26 J. H. Sch?n, M. Dorget, F. C. Beuran, et al. Field-Induced Superconductivity in a Spin-Ladder Cuprate. Science,2001,293:2430-2432
27 W. Wich, M. Mundschau, C. P. Flynn. Interfacial defects in thin refractory metal films imaged by low-energy electron microscopy. Applied Physics Letters,1999, 74(18):2626-2628
28 S. D. Sartale, G. D. Bagde, C. D. Lokhande, et al. Room temperature synthesis of nanocrystalline ferrite(MFe2O4,M=Cu,Co,Ni)thin films using novel electrochemical route. Applied Surface Science,2001,284:113-119
29 Yutaka Adachi, Dong Su, Paul Muralt, et al. Ferroelectric and piezoelectric properties of lanthanoid-substituted Bi4Ti3O12 thin films grown on (111) Pt and (100) IrO2 electrodes. Applied Physics Letters,2005,86(172904):1-3
30 J. Bruce Hinds, Nitin Chopra, Terry Rantell, et al. Aligned Multiwalled Carbon Nanotube Membranes. Science,2004,303: 62-65
31 Sang-In Cho, Soon-Gil Yoon. Improvement of discharge capacity of LiCoO2 thin-film cathodes deposited in trench structure by liquid-delivery metalorganic chemical vapor deposition. Applied Physics Letters,2003,82(19):3345-3347
32 Kyung-Won Park, Kwang-Soon Ahn, Jong-Ho Choi, et al. PtRu–WO3 nanostructured alloy electrode for use in thin-film fuel cells. Applied Physics Letters, 2003,82(7):1090-1092
33 I. H. Weller, U. Koch, M. Gutierrez Ber, et al. Effect of an attractive potential on the interparticle structure of Ionic micelles at high salt concentration. Phys. Chem.,1984,88:649
34 N. Yamazof, Y. Teraora. Oxidation catalysis of pervoskites ralationship to bulk structure and composition (Valence, defect, et al). Catalysis Today,1990,8:175-199
35 J. B. Torrance, P. Lacorre, C. Asavaroengchai, et al. Simple and pervoskite oxides of transition-metals: why some are metallic, while most are insulatin. J. Solid State Chemistry,1991,90:168-172
36 傅希贤,杨秋华.钙钛矿型氧化物 LaFeO3 光催化活性的研究.化学工业与工程, 1999,16(6):316-319
37 杨秋华,傅希贤,王俊珍,等.La1-xSrxFeO3 光催化降解水溶性染料.应用化学, 2000,17(6):585-588
38 周永溶.半导体材料.北京:北京理工大学出版社,1992:81
39 范志新.电子薄膜材料最佳掺杂含量的理论研究.[河北工业大学博士学位论文].2002:7-10
40 殷庆瑞,王通,钱梦騄.光声光热技术及其应用.北京:科学出版社,1999:19-36
41 P. M. Ajayan, M. Terrones, A. de la Guardia, et al. Nanotubes in a Flash-Ignition and Reconstruction. Science,2002,296:705
42 H. X. Chen, G. Diebold. Chemical Generation of Acoustic Waves: A Giant Photoacoustic Effect. Science,1995,270:963-966
43 T. Sun, J. Diebold. Generation of ultrasonic waves from a layered photoacoustic source. Nature,1992,355:806-808
44 I. G. Calasso, W. Craig, G. J. Diebold. Photoacoustic Point Source. Phys. Rev. Lett.,2000,86:3550-3553
45 K. Leeor, S. Yoram. Surface photovoltage phenomena: theory, experiment, and applications. Surf. Sci. Rep.,1999,37:1-206
46 A. Rosencwaig, A. Gersho. Theory of the photoacoustic effect with solids. J. Appl. Phys,1976,47(1):64-69
47 K. Ueda, H. Tabata, T. Kawai. Ferromagnetism in LaFeO3-LaCrO3 Superlattices. Science,1998,280:1064-1066
48 罗森威格.光声学和光声谱学.王耀俊,张淑仪译.北京:科学出版社,1986:50-100
49 李葵英.纳米晶铁酸盐系列光电气敏特性的研究.[吉林大学理学博士学位论文]. 1999:24-27 64-66 80-81
50 谢腾峰.功能材料的光伏特性及光伏气敏特性.[吉林大学理学硕士学位论文]. 1998:20-50
51 张杰.光电诱导表面与界面电荷转移特性研究.[吉林大学理学博士学位论文]. 1996:5-36
52 F. Q. Wu, B. K. Xu, X. Li, et al. The impurity research of La1-xSrxFeO3. Chem. J. Chin. Univ.,1994,6:803-806
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58 L. Gushony, J. Haart, G. Blasse, et al. The Transiton properties of Fe2O3. J. Electrochem. Soc: Electrochem. Sci. Tech.,1985,132a(12):2933
59 吴自勤,王兵.薄膜生长.北京:科学出版社,2001:67-84
2 A. L. Kholkin, R. Martins, H. Aguas, et al. Metal–ferroelectric thin film devices. Journal of Non-Crystalline Solids,2002,299:1311-1315
3 Tomita Katsuhiko, Takamuro Daisuke, Samada Kazuaki. Electron emission type infrared imaging sensor using ferroelectric thin plate. Sensors and Actuator A,2002,98:147-152
4 K. Ueda, H. Tabata, T. Kawai. Ferromagnetism in LaFeO_3-LaCrO_3 Superlattices. Science,1998,280:1064-1066
5 A. Scholl, J. St?hr, J. Lüning, et al. Observation of Antiferromagnetic Domains in Epitaxial Thin Films. Science,2000,287:1014-1016
6 陈敬中.现代晶体化学–理论与方法.北京:高等教育出版社,2001:407-408
7 T. Takagahara. Localization and energy transfer of quasi-two-dime-nsional excitons in GaAs-AlAs quantum-well heterostructures. Phys.Rev.B,1985,31:6552
8 R. Kubo. The theory about the nano-materials. J. Phys. Soc. Jpn.,1962,17:975-980
9 M. Achermann, M. A. Petruska. Energy-transfer pumping of semiconductor nanocrystals using an epitaxial quantum well. Nature,2004,429:642-646
10 郑伟涛.薄膜材料与薄膜技术.北京:化学工业出版社,2004:11-25
11 韩喜江.铁氧体薄膜吸波材料的研究进展.中国材料科技与设备,2005,2(2):17
12 王强.溶胶-凝胶法制备 La 掺杂钛酸铋薄膜和多层膜及其铁电性质研究.[苏州大学硕士学位论文].2005:13-20
13 Wen-Tsang Liu, Jyh-Fu Lee, Jenn-Ming Wu. X-ray absorption spectroscopic study of barium ferrite thin films synthesized by sol-sel method. Materials Chemistry and Physics,2001,69:89-94
14 Jae-Gwang Lee, Hi Min Lee, Chul Sung Kim, et al. Magnetic properties of CoFe_2O_4 powders and thin films grown by a sol-sel method. J. Magnetism and Magnetic Materials,1998,177-181:900-902
15 M. Paranthaman, T. G. Chirayil. Fabrication of Long Lengths of YBCO Coated Conductors using a Continuous Reel-to-Reel Dip-Coating Unit. Applied Super Conductivity,2001,11(1):3146-3149
16 何作鹏.溶胶-凝胶提拉法制备 MgxNi1-xO 薄膜与表征.半导体学报,2002, 26(4):721-725
17 K. Daoudi, B. Canut, Blanchi, et al.Tin doped in dium oxide thin films deposited by sol-sel dip-coating technique. Materials Science and Engineering,2002,21:313-317
18 P. J. Kelly, R. D. Arnell. Magnetron sputtering: a review of recent developments and applications. Vacuum,2000(56):159-172
19 尹洪禹,吴作良,谢文利,杨森.超高真空射频磁控溅射镀膜机(双室三靶)及其应用.真空技术与应用,2000,3:25-28
20 I. Safi. A novel reactive magnetron sputtering technique for producing insulating oxides of metal alloys and other compound thin films. Surface and Coatings Technology,2000,135:48-59
21 Yuan-Bin Chen, Cheng-Liang Huang. Properties of MgTiO3 thin films prepared by RF magnetron sputtering for microwave application. Journal of Crystal Growth,2005,282:482-489
22 F. Huisken, B. Kohn. Structured films of light-emitting silicon nanoparticles produced by cluster beam deposition. Applied Physics Letters,1999, 74(25):3776-3778
23 J. F. Tong, H. L. Hsiao, H. L. Hwang. Adjustable emissions from silicon-rich oxide films prepared by plasma-enhanced chemical-vapor deposition. Applied Physics Letters,1999,74(16):2316-2318
24 N. Taylor, H. Kim, P. Desjardins, et al. Greene. Si(011)16×2 gas-source molecular beam epitaxy: Growth kinetics. Applied Physics Letters,2000, 76(20):2853-2855
25 Byungha Shin, P. John Leonard, W. James McCamy, et al. Comparison of morphology evolution of Ge(001) homoepitaxial films grown by pulsed laser deposition and molecular-beam epitaxy. Applied Physics Letters,2005, 87(181916):1-3
26 J. H. Sch?n, M. Dorget, F. C. Beuran, et al. Field-Induced Superconductivity in a Spin-Ladder Cuprate. Science,2001,293:2430-2432
27 W. Wich, M. Mundschau, C. P. Flynn. Interfacial defects in thin refractory metal films imaged by low-energy electron microscopy. Applied Physics Letters,1999, 74(18):2626-2628
28 S. D. Sartale, G. D. Bagde, C. D. Lokhande, et al. Room temperature synthesis of nanocrystalline ferrite(MFe2O4,M=Cu,Co,Ni)thin films using novel electrochemical route. Applied Surface Science,2001,284:113-119
29 Yutaka Adachi, Dong Su, Paul Muralt, et al. Ferroelectric and piezoelectric properties of lanthanoid-substituted Bi4Ti3O12 thin films grown on (111) Pt and (100) IrO2 electrodes. Applied Physics Letters,2005,86(172904):1-3
30 J. Bruce Hinds, Nitin Chopra, Terry Rantell, et al. Aligned Multiwalled Carbon Nanotube Membranes. Science,2004,303: 62-65
31 Sang-In Cho, Soon-Gil Yoon. Improvement of discharge capacity of LiCoO2 thin-film cathodes deposited in trench structure by liquid-delivery metalorganic chemical vapor deposition. Applied Physics Letters,2003,82(19):3345-3347
32 Kyung-Won Park, Kwang-Soon Ahn, Jong-Ho Choi, et al. PtRu–WO3 nanostructured alloy electrode for use in thin-film fuel cells. Applied Physics Letters, 2003,82(7):1090-1092
33 I. H. Weller, U. Koch, M. Gutierrez Ber, et al. Effect of an attractive potential on the interparticle structure of Ionic micelles at high salt concentration. Phys. Chem.,1984,88:649
34 N. Yamazof, Y. Teraora. Oxidation catalysis of pervoskites ralationship to bulk structure and composition (Valence, defect, et al). Catalysis Today,1990,8:175-199
35 J. B. Torrance, P. Lacorre, C. Asavaroengchai, et al. Simple and pervoskite oxides of transition-metals: why some are metallic, while most are insulatin. J. Solid State Chemistry,1991,90:168-172
36 傅希贤,杨秋华.钙钛矿型氧化物 LaFeO3 光催化活性的研究.化学工业与工程, 1999,16(6):316-319
37 杨秋华,傅希贤,王俊珍,等.La1-xSrxFeO3 光催化降解水溶性染料.应用化学, 2000,17(6):585-588
38 周永溶.半导体材料.北京:北京理工大学出版社,1992:81
39 范志新.电子薄膜材料最佳掺杂含量的理论研究.[河北工业大学博士学位论文].2002:7-10
40 殷庆瑞,王通,钱梦騄.光声光热技术及其应用.北京:科学出版社,1999:19-36
41 P. M. Ajayan, M. Terrones, A. de la Guardia, et al. Nanotubes in a Flash-Ignition and Reconstruction. Science,2002,296:705
42 H. X. Chen, G. Diebold. Chemical Generation of Acoustic Waves: A Giant Photoacoustic Effect. Science,1995,270:963-966
43 T. Sun, J. Diebold. Generation of ultrasonic waves from a layered photoacoustic source. Nature,1992,355:806-808
44 I. G. Calasso, W. Craig, G. J. Diebold. Photoacoustic Point Source. Phys. Rev. Lett.,2000,86:3550-3553
45 K. Leeor, S. Yoram. Surface photovoltage phenomena: theory, experiment, and applications. Surf. Sci. Rep.,1999,37:1-206
46 A. Rosencwaig, A. Gersho. Theory of the photoacoustic effect with solids. J. Appl. Phys,1976,47(1):64-69
47 K. Ueda, H. Tabata, T. Kawai. Ferromagnetism in LaFeO3-LaCrO3 Superlattices. Science,1998,280:1064-1066
48 罗森威格.光声学和光声谱学.王耀俊,张淑仪译.北京:科学出版社,1986:50-100
49 李葵英.纳米晶铁酸盐系列光电气敏特性的研究.[吉林大学理学博士学位论文]. 1999:24-27 64-66 80-81
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51 张杰.光电诱导表面与界面电荷转移特性研究.[吉林大学理学博士学位论文]. 1996:5-36
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