Evolution of microstructures and optical properties of gadolinium oxide with oxygen flow rate and annealing temperature
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摘要
In this study, the effects of oxygen flow rate and annealing temperature on Gd_2 O_3 structures and optical properties were systematically analyzed. Gd_2 O_3 films were deposited on both quartz and ZnS substrates by magnetron sputtering and then annealed under vacuum at 700, 800 and 900℃, Restructure and phase transformation from cubic to monoclinic occur at different temperatures depending on the oxygen flow rate. The optical band gap, which is more sensitive to the annealing temperature than oxygen flow rate changes from 5.32 to 5.65 eV. The refractive index is approximately 1.75 at 550 nm and is adjustable by the oxygen flow rate. The transmittance of the ZnS substrate with Gd_2 O_3 film exceeds 80% and reaches82% at the 7.5-9.5 μm range. When ZnS is coated on both sides, the transmittance is increased to approximately 90%. Our results indicate that Gd_2 O_3 films are promising new candidates for anti-reflective coatings in the infrared region.
In this study, the effects of oxygen flow rate and annealing temperature on Gd_2 O_3 structures and optical properties were systematically analyzed. Gd_2 O_3 films were deposited on both quartz and ZnS substrates by magnetron sputtering and then annealed under vacuum at 700, 800 and 900℃, Restructure and phase transformation from cubic to monoclinic occur at different temperatures depending on the oxygen flow rate. The optical band gap, which is more sensitive to the annealing temperature than oxygen flow rate changes from 5.32 to 5.65 eV. The refractive index is approximately 1.75 at 550 nm and is adjustable by the oxygen flow rate. The transmittance of the ZnS substrate with Gd_2 O_3 film exceeds 80% and reaches82% at the 7.5-9.5 μm range. When ZnS is coated on both sides, the transmittance is increased to approximately 90%. Our results indicate that Gd_2 O_3 films are promising new candidates for anti-reflective coatings in the infrared region.
In this study, the effects of oxygen flow rate and annealing temperature on Gd_2 O_3 structures and optical properties were systematically analyzed. Gd_2 O_3 films were deposited on both quartz and ZnS substrates by magnetron sputtering and then annealed under vacuum at 700, 800 and 900℃, Restructure and phase transformation from cubic to monoclinic occur at different temperatures depending on the oxygen flow rate. The optical band gap, which is more sensitive to the annealing temperature than oxygen flow rate changes from 5.32 to 5.65 eV. The refractive index is approximately 1.75 at 550 nm and is adjustable by the oxygen flow rate. The transmittance of the ZnS substrate with Gd_2 O_3 film exceeds 80% and reaches82% at the 7.5-9.5 μm range. When ZnS is coated on both sides, the transmittance is increased to approximately 90%. Our results indicate that Gd_2 O_3 films are promising new candidates for anti-reflective coatings in the infrared region.
引文
1. Zinkevich M. Thermodynamics of rare earth sesquioxides. Prog Mater Sci.2007;52:597.
2. Adachi GY, Imanaka N. The binary rare earth oxides. Chem Rev. 1998;98:1479.
3. Pavunny S, Scott J, Katiyar R. Lanthanum gadolinium oxide:a new electronic device material for CMOS logic and memory devices. Materials. 2014;7:2669.
4. Xu K, Ranjith R, Laha A, Parala H, Milanov AP, Fischer RA, et al. Atomic layer deposition of Gd_2O_3 and Dy_2O_3:a study of the ALD characteristics and structural and electrical properties. Chem Mater. 2012;24:651.
5. Seppala S, Niinist(o|¨)J, Blanquart T, Kaipio M, Mizohata K, Raisanen J, et al.Heteroleptic cydopentadienyl amidinate precursors for atomic layer deposition(ALD)of Y, Pr, Gd, and Dy oxide thin films. Chem Mater. 2016;28:5440.
6. Liu KC, Tsai JR, Li CS, Chine PH, Chen JN, Feng WS. Characteristics of transparent ZnO-based thin-film transistors with high-k dielectric Gd_2O_3 gate insulators fabricated at room temperature. Jpn J Appl Phys. 2010;49:04DF21.
7. Katherine DB, Haruo K, Katsuhiko Y, Teruhisa H, Harumi Y. Evidence for enhanced oxygen surface exchange reaction in nano structured Gd_2O_3-doped CeO_2 films. Nanotechnology. 2015;26:215401.
8. Mishra M, Kuppusami P, Ramya S, Ganesan V, Singh A, Thirumurugesan R, et al.Microstructure and optical properties of Gd_2O_3 thin films prepared by pulsed laser deposition. Surf Coating Technol. 2015;262:56.
9. Joseph A, Tetzlaff D, Schmidt J, Bottger R, Wietler TF, Osten HJ. Formation and properties of high-dose nitrogen implanted epitaxially grown Gd_2O_3 on silicon.J Appl Phys.2016;120:144103.
10. Shekhter P, Schwendt D, Amouyal Y, Wietler TF, Osten HJ, Eizenberg M. Straininduced phase variation and dielectric constant enhancement of epitaxial Gd_2O_3.J Appl Phys. 2016;120:014101.
11. Feijoo PC, Pampillán MA, Andres ES. Optimization of gadolinium oxide growth deposited on Si by high pressure sputtering.J Vac Sci Technol B. 2013:31:01A103.
12.Peddigari M, Bharti GP, Khare A, Dobbidi P. Optical and dielectric studies on radio frequency sputtered Gd_2O_3 doped K_(0.5)Na_(0.5)NbO_3 thin films for nonlinear photonic and microwave tunable device applications. J Alloys Compd.2016;682:634.
13. Adyani SM, Ghorbani M. A comparative study of physicochemical and photocatalytic properties of visible light responsive Fe, Gd and P single and tri-doped TiO_2 nanomaterials.J Rare Earths. 2018;36(1):72.
14.Jiang XL, Yu L, Yao C, Zhang FQ, Zhang J, Li CJ. Synthesis and characterization of Gd_2O_3 hollow microspheres using a template-directed method. Materials.2016;9:323.
15. Zelenakova A, Hrubovcak P, Kapusta O, Zelenak V, Franco V. Large magnetocaloric effect in fine Gd_2O_3 nanoparticles embedded in porous silica matrix.Appl Phys Lett. 2016;109:5.
16. Sahoo NK, Thakur S, Senthilkumar M, Bhattacharyya D, Das NC. Reactive electron beam evaporation of gadolinium oxide optical thin films for ultraviolet and deep ultraviolet laser wavelengths. Thin Solid Films. 2003;440:155.
17. Sahoo NK,Thakur S, Tokas RB. Growth-dependent refractive index nonlinearity and mean microstructural properties of codeposited composite gadolinia silica films. Appl Opt. 2006;45(14):3243.
18. Yashina EV. Preparation and properties of polycrystalline ZnS for IR applications. Inorg Mater. 2003;39(7):663.
19. Zhang GF, Zheng X. Optical transmittance of antireflective diamond-like coatings on ZnS substrates. Surf Coating Technol.1996;82(1-2):110-113.
20. Li YP, Wang N, Che XS, Chen HB, Liu ZT. Infrared transmissive and rain-erosion resistant performances of GeC/GaP double-layer thin films on ZnS substrates.Appl Surf Sci. 2013:264:538-544.
21. He Q, Guo HB, Wei JJ, Askari SJ, Wang HB, Zhang SY, et al. Deposition of HfO2thin films on ZnS substrates. Thin Solid Films. 2008;516(15):4695-4699.
22. Moghadam RZ, Ahmadvand H, Jannesari M. Design and fabrication of multilayers infrared antireflection coating consisting of ZnS and Ge on ZnS substrate.Infrared Phys Technol. 2016;75:18-21.
23. Strijckmans K, Leroy WP, De Gryse R, Depla D. Modeling reactive magnetron sputtering:fixing the parameter set. Surf Coating Technol. 2012;206:3666.
24. Parreira NMG, Polcar T, Cavaleiro A. Study of the cathode potential in a sputtering discharge by pulsing the reactive gas:case of a W target in an Ar-O_2atmosphere, plasma. Process Polym. 2007;4:62.
25. Lei P, Zhu JQ, Zhu YK, Jiang CZ, Yin XB. Yttrium oxide thin films prepared under different oxygen-content atmospheres:microstructure and optical properties.Appl Phy A-Mate. 2012;108:621.
26. Lei P, Leroy W, Dai B, Zhu JQ, Chen XC, Han J, et al. Study on reactive sputtering of yttrium oxide:process and thin film properties. Surf Coating Technol.2015;276:39.
27. Sarkar BJ, Deb AK, Chakrabarti PK. XRD, HRTEM, Raman and magnetic studies on chemically prepared nanocrystalline Fe-doped gadolinium oxide(Gd_(1.90)Fe_(0.10)O_3-delta)annealed in vacuum. RSC Adv. 2016;6:6395.
28. Hazarika S, Paul N, Mohanta D. Rapid hydrothermal route to synthesize cubicphase gadolinium oxide nanorods. Bull Mater Sci. 2014;37:789.
29. Zou HY, Wang YX, Gao F, Sheng Y, Zheng KY, Zhou XQ. Facile synthesis and luminescence properties of Gd_2O_3:Eu microrods from thermal transformation of Gd(Eu)tartrate complexes. J Alloys Compd. 2015;622:143.
30. Cheraghali R, Aghazadeh M. A simple and facile electrochemical route to synthesis of metal hydroxides and oxides ultrafine nanopartides(M=La, Gd,Ni and Co). Anal Bioanal Chem. 2016;8(1):64.
31. a Lonappan D, Chandra Shekar NV, Sahu PC, Kumarasamy BV,Bandyopadhyay AK, Rajagopalan M. Cubic to hexagonal structural transformation in Gd_2O_3 at high pressure. Phil Mag Lett. 2008;88:473;b Ghosh K, Das S, Fissel A, Osten HJ, Laha A. Long-term stability of epitaxial(Nd_(1-x)Gd_x)_2O_3 thin films grown on Si(001)for future CMOS devices. IEEE Trans Electron Dev. 2016;63:2852.
32. Cheng XH, Xu DP, Song ZR, He DW, Yu YH, Zhao QT, et al. Characterization of gadolinium oxide film by pulse laser deposition. Appl Surf Sci. 2009;256:921.
33. Jeon S, Hwang H. Effect of hygroscopic nature on the electrical characteristics of lanthanide oxides(Pr_2O_3, Sm_2O_3, Gd_2O_3, and Dy_2O_3).J Appl Phys. 2003;93:6393.
34. Manjunatha P, Kumar Thilipan G Arun. Band gap and morphology of magnetron sputtered Gd_2O_3 thin films. Int J Mater Res. 2013; 1(4):452.
35. Zatsepin DA, Boukhvalov DW, Zatsepin AF, Kuznetsova Yu A, Mashkovtsev MA,Rychkov VN, et al. Electronic structure, charge transfer, and intrinsic luminescence of gadolinium oxide nanoparticles:experiment and theory. Appl Surf Sci. 2018;436:697.
36. Hua CY, Chen LX, Li CM, Wang M, Gao JC, Liu JL, et al. Effects of oxygen-to-argon ratio on crystalline structure and properties of Y_2O_3 anti-reflection films for freestanding CVD diamond. J Alloys Compd. 2017;693:468.
2. Adachi GY, Imanaka N. The binary rare earth oxides. Chem Rev. 1998;98:1479.
3. Pavunny S, Scott J, Katiyar R. Lanthanum gadolinium oxide:a new electronic device material for CMOS logic and memory devices. Materials. 2014;7:2669.
4. Xu K, Ranjith R, Laha A, Parala H, Milanov AP, Fischer RA, et al. Atomic layer deposition of Gd_2O_3 and Dy_2O_3:a study of the ALD characteristics and structural and electrical properties. Chem Mater. 2012;24:651.
5. Seppala S, Niinist(o|¨)J, Blanquart T, Kaipio M, Mizohata K, Raisanen J, et al.Heteroleptic cydopentadienyl amidinate precursors for atomic layer deposition(ALD)of Y, Pr, Gd, and Dy oxide thin films. Chem Mater. 2016;28:5440.
6. Liu KC, Tsai JR, Li CS, Chine PH, Chen JN, Feng WS. Characteristics of transparent ZnO-based thin-film transistors with high-k dielectric Gd_2O_3 gate insulators fabricated at room temperature. Jpn J Appl Phys. 2010;49:04DF21.
7. Katherine DB, Haruo K, Katsuhiko Y, Teruhisa H, Harumi Y. Evidence for enhanced oxygen surface exchange reaction in nano structured Gd_2O_3-doped CeO_2 films. Nanotechnology. 2015;26:215401.
8. Mishra M, Kuppusami P, Ramya S, Ganesan V, Singh A, Thirumurugesan R, et al.Microstructure and optical properties of Gd_2O_3 thin films prepared by pulsed laser deposition. Surf Coating Technol. 2015;262:56.
9. Joseph A, Tetzlaff D, Schmidt J, Bottger R, Wietler TF, Osten HJ. Formation and properties of high-dose nitrogen implanted epitaxially grown Gd_2O_3 on silicon.J Appl Phys.2016;120:144103.
10. Shekhter P, Schwendt D, Amouyal Y, Wietler TF, Osten HJ, Eizenberg M. Straininduced phase variation and dielectric constant enhancement of epitaxial Gd_2O_3.J Appl Phys. 2016;120:014101.
11. Feijoo PC, Pampillán MA, Andres ES. Optimization of gadolinium oxide growth deposited on Si by high pressure sputtering.J Vac Sci Technol B. 2013:31:01A103.
12.Peddigari M, Bharti GP, Khare A, Dobbidi P. Optical and dielectric studies on radio frequency sputtered Gd_2O_3 doped K_(0.5)Na_(0.5)NbO_3 thin films for nonlinear photonic and microwave tunable device applications. J Alloys Compd.2016;682:634.
13. Adyani SM, Ghorbani M. A comparative study of physicochemical and photocatalytic properties of visible light responsive Fe, Gd and P single and tri-doped TiO_2 nanomaterials.J Rare Earths. 2018;36(1):72.
14.Jiang XL, Yu L, Yao C, Zhang FQ, Zhang J, Li CJ. Synthesis and characterization of Gd_2O_3 hollow microspheres using a template-directed method. Materials.2016;9:323.
15. Zelenakova A, Hrubovcak P, Kapusta O, Zelenak V, Franco V. Large magnetocaloric effect in fine Gd_2O_3 nanoparticles embedded in porous silica matrix.Appl Phys Lett. 2016;109:5.
16. Sahoo NK, Thakur S, Senthilkumar M, Bhattacharyya D, Das NC. Reactive electron beam evaporation of gadolinium oxide optical thin films for ultraviolet and deep ultraviolet laser wavelengths. Thin Solid Films. 2003;440:155.
17. Sahoo NK,Thakur S, Tokas RB. Growth-dependent refractive index nonlinearity and mean microstructural properties of codeposited composite gadolinia silica films. Appl Opt. 2006;45(14):3243.
18. Yashina EV. Preparation and properties of polycrystalline ZnS for IR applications. Inorg Mater. 2003;39(7):663.
19. Zhang GF, Zheng X. Optical transmittance of antireflective diamond-like coatings on ZnS substrates. Surf Coating Technol.1996;82(1-2):110-113.
20. Li YP, Wang N, Che XS, Chen HB, Liu ZT. Infrared transmissive and rain-erosion resistant performances of GeC/GaP double-layer thin films on ZnS substrates.Appl Surf Sci. 2013:264:538-544.
21. He Q, Guo HB, Wei JJ, Askari SJ, Wang HB, Zhang SY, et al. Deposition of HfO2thin films on ZnS substrates. Thin Solid Films. 2008;516(15):4695-4699.
22. Moghadam RZ, Ahmadvand H, Jannesari M. Design and fabrication of multilayers infrared antireflection coating consisting of ZnS and Ge on ZnS substrate.Infrared Phys Technol. 2016;75:18-21.
23. Strijckmans K, Leroy WP, De Gryse R, Depla D. Modeling reactive magnetron sputtering:fixing the parameter set. Surf Coating Technol. 2012;206:3666.
24. Parreira NMG, Polcar T, Cavaleiro A. Study of the cathode potential in a sputtering discharge by pulsing the reactive gas:case of a W target in an Ar-O_2atmosphere, plasma. Process Polym. 2007;4:62.
25. Lei P, Zhu JQ, Zhu YK, Jiang CZ, Yin XB. Yttrium oxide thin films prepared under different oxygen-content atmospheres:microstructure and optical properties.Appl Phy A-Mate. 2012;108:621.
26. Lei P, Leroy W, Dai B, Zhu JQ, Chen XC, Han J, et al. Study on reactive sputtering of yttrium oxide:process and thin film properties. Surf Coating Technol.2015;276:39.
27. Sarkar BJ, Deb AK, Chakrabarti PK. XRD, HRTEM, Raman and magnetic studies on chemically prepared nanocrystalline Fe-doped gadolinium oxide(Gd_(1.90)Fe_(0.10)O_3-delta)annealed in vacuum. RSC Adv. 2016;6:6395.
28. Hazarika S, Paul N, Mohanta D. Rapid hydrothermal route to synthesize cubicphase gadolinium oxide nanorods. Bull Mater Sci. 2014;37:789.
29. Zou HY, Wang YX, Gao F, Sheng Y, Zheng KY, Zhou XQ. Facile synthesis and luminescence properties of Gd_2O_3:Eu microrods from thermal transformation of Gd(Eu)tartrate complexes. J Alloys Compd. 2015;622:143.
30. Cheraghali R, Aghazadeh M. A simple and facile electrochemical route to synthesis of metal hydroxides and oxides ultrafine nanopartides(M=La, Gd,Ni and Co). Anal Bioanal Chem. 2016;8(1):64.
31. a Lonappan D, Chandra Shekar NV, Sahu PC, Kumarasamy BV,Bandyopadhyay AK, Rajagopalan M. Cubic to hexagonal structural transformation in Gd_2O_3 at high pressure. Phil Mag Lett. 2008;88:473;b Ghosh K, Das S, Fissel A, Osten HJ, Laha A. Long-term stability of epitaxial(Nd_(1-x)Gd_x)_2O_3 thin films grown on Si(001)for future CMOS devices. IEEE Trans Electron Dev. 2016;63:2852.
32. Cheng XH, Xu DP, Song ZR, He DW, Yu YH, Zhao QT, et al. Characterization of gadolinium oxide film by pulse laser deposition. Appl Surf Sci. 2009;256:921.
33. Jeon S, Hwang H. Effect of hygroscopic nature on the electrical characteristics of lanthanide oxides(Pr_2O_3, Sm_2O_3, Gd_2O_3, and Dy_2O_3).J Appl Phys. 2003;93:6393.
34. Manjunatha P, Kumar Thilipan G Arun. Band gap and morphology of magnetron sputtered Gd_2O_3 thin films. Int J Mater Res. 2013; 1(4):452.
35. Zatsepin DA, Boukhvalov DW, Zatsepin AF, Kuznetsova Yu A, Mashkovtsev MA,Rychkov VN, et al. Electronic structure, charge transfer, and intrinsic luminescence of gadolinium oxide nanoparticles:experiment and theory. Appl Surf Sci. 2018;436:697.
36. Hua CY, Chen LX, Li CM, Wang M, Gao JC, Liu JL, et al. Effects of oxygen-to-argon ratio on crystalline structure and properties of Y_2O_3 anti-reflection films for freestanding CVD diamond. J Alloys Compd. 2017;693:468.