Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique

Abdelouahab Gahtar; Said Benramache; Boubaker Benhaoua; Foued Chabane

doi:10.1088/1674-4926/34/7/073002

J. Semicond. > 2013, Volume 34 > Issue 7 > 073002

SEMICONDUCTOR MATERIALS

Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique

Abdelouahab Gahtar¹, Said Benramache^{1, 2,}, Boubaker Benhaoua¹ and Foued Chabane³

+ Author Affiliations

Corresponding author: Said Benramache, Email:saidzno2006@gmail.com

DOI: 10.1088/1674-4926/34/7/073002

Abstract: Transparent conductive Al doped ZnO thin films were deposited by ultrasonic spray technique. Conditions of preparation have been optimized to get good quality. A set of aluminum (Al) doped ZnO (between 0 and 5 wt%) thin films were grown on glass substrate at 350℃. Nanocrystalline films with a hexagonal wurtzite structure show a strong (002) preferred orientation. The maximum value of grain size G=32.05 nm is attained of Al doped ZnO film with 3 wt%. All the films have low absorbance in the visible region, thus the films are transparent in the visible region; the band gap energy increased from 3.10 to 3.26 eV when Al concentration increased from 0 to 3 wt%. The electrical conductivity of the films increased from 7.5 to 15.2 (Ω·cm)^-1. So the best results are achieved in Al doped ZnO film with 3 wt%.

Key words: ZnO:Al, thin films, TCO, ultrasonic spray technique

References

[1]	Zhang Y, Wu C, Zheng Y, et al. Synthesis and efficient field emission characteristics of patterned ZnO nanowires. Journal of Semiconductors, 2012, 33(2):023001 doi: 10.1088/1674-4926/33/2/023001
[2]	Zhu X, Wu H, Wang S, et al. Optical and electrical properties of N-doped ZnO and fabrication of thin-film transistors. Journal of Semiconductors, 2009, 30(3):033001 doi: 10.1088/1674-4926/30/3/033001
[3]	Zhang H, Liu H, Lei C, et al. Low-temperature deposition of transparent conducting Mn-W co-doped ZnO thin films. Journal of Semiconductors, 2010, 31(8):083005 doi: 10.1088/1674-4926/31/8/083005
[4]	Ji Z, Mao Q, Ke W. Effects of oxygen partial pressure on resistive switching characteristics of ZnO thin films by DC reactive magnetron sputtering. Solid State Commun, 2010, 150(8):1919
[5]	Zuo C, Wen J, Zhong C. First-principles study of the electronic structures and optical properties of C-F-Be doped wurtzite ZnO. Journal of Semiconductors, 2012, 33(7):072001 doi: 10.1088/1674-4926/33/7/072001
[6]	Kumar P S, Raj A D, Mangalaraj D, et al. Growth of hierarchical based ZnO micro/nanostructured films and their tunable wettability behavior. Appl Surf Sci, 2011, 257(20):6678
[7]	Ye Z, Yuan G, Li B, et al. Fabrication and characteristics of ZnO thin films with Al/Si (100) substrates. Mater Chem Phys, 2005, 93(2):170
[8]	Zhang H, Yang S, Liu H, et al. Preparation and characterization of transparent conducting ZnO:W films by DC magnetron sputtering. Journal of Semiconductors, 2011, 32(4):043002 doi: 10.1088/1674-4926/32/4/043002
[9]	El Manouni A, Manjon F J, Perales M, et al. Effect of thermal annealing on ZnO:Al thin films grown by spray pyrolysis. Superlattices and Microstructures, 2007, 42(2):134
[10]	Rozati S M, Akesteh S. Characterization of ZnO:Al thin films obtained by spray pyrolysis technique. Materials Characterization, 2007, 58(4):319 doi: 10.1016/j.matchar.2006.05.012
[11]	Saleem M, Siddiqi S A, Atiq S, et al. Carriers-mediated ferromagnetic enhancement in Al-doped ZnMnO dilute magnetic semiconductors. Materials Characterization, 2011, 62(12):1102
[12]	Ma Q B, Ye Z Z, He H P, et al. Preparation and characterization of transparent conductive ZnO:Ga films by DC reactive magnetron sputtering. Materials Characterization, 2008, 59(2):124 doi: 10.1016/j.matchar.2006.11.020
[13]	Benramache S, Benhaoua B, Chabane F. Effect of substrate temperature on the stability of transparent conducting cobalt doped ZnO thin films. Journal of Semiconductors, 2012, 33(9):093001 doi: 10.1088/1674-4926/33/9/093001
[14]	Duclére J R, Novotny M, Meaney A, et al. Properties of Li-, P-and N-doped ZnO thin films prepared by pulsed laser deposition. Superlattices and Microstructures, 2005, 38(3):397
[15]	Hafdallah A, Yanineb F, Aida M S, et al. In doped ZnO thin films. Journal of Alloys and Compounds, 2011, 509(18):7267
[16]	Benramache S, Benhaoua B, Chabane F, et al. Influence of growth time on crystalline structure, conductivity and optical properties of ZnO thin films. Journal of Semiconductors, 2013, 34(2):023001 doi: 10.1088/1674-4926/34/2/023001
[17]	Venkatachalam S, Iida Y, Kanno Y. Preparation and characterization of Al doped ZnO thin films by PLD. Superlattices and Microstructures, 2008, 44(2):127
[18]	Zhu H, Hüpkes J, Bunte E, et al. Reactive sputtering of ZnO:Al thin films from rotatable dual metallic targets. Appl Surf Sci, 2012, 259(4):582
[19]	Zhu H, Hüpkes J, Bunte E, et al. Study of ZnO:Al films for silicon thin film solar cells. Appl Surf Sci, 2012, 261:268 doi: 10.1016/j.apsusc.2012.07.159
[20]	Benramache S, Benhaoua B. Influence of substrate temperature and Cobalt concentration on structural and optical properties of ZnO thin films prepared by ultrasonic spray technique. Superlattices and Microstructures, 2012, 52(4):807 doi: 10.1016/j.spmi.2012.06.005
[21]	Benramache S, Benhaoua B. Influence of annealing temperature on structural and optical properties of ZnO:In thin films prepared by ultrasonic spray technique. Superlattices and Microstructures, 2012, 52(6):1062 doi: 10.1016/j.spmi.2012.08.006
[22]	Romero R, Ibanez R L, Dalchiele E A, et al. Compositional and physico-optical characterization of 0-5% Al-doped zinc oxide films prepared by chemical spray pyrolysis. J Phys D:Appl Phys, 2010, 43(9):095303 doi: 10.1088/0022-3727/43/9/095303
[23]	Mekhnache M, Drici A, Hamideche L S, et al. Properties of ZnO thin films deposited on (glass, ITO and ZnO:Al) substrates. Superlattices and Microstructures, 2011, 49(3):510
[24]	Mosbah A, Aida M S. Influence of deposition temperature on structural, optical and electrical properties of sputtered Al doped ZnO thin films. Journal of Alloys and Compounds, 2012, 515(1):149
[25]	Rahmane S, Djouadi M A, Aida M S, et al. Power and pressure effects upon magnetron sputtered aluminum doped ZnO films properties. Thin Solid Films, 2010, 519(1):5 doi: 10.1016/j.tsf.2010.06.063
[26]	Zhang C. High-quality oriented ZnO films grown by sol-gel process assisted with ZnO. Journal of Physics and Chemistry of Solids, 2010, 71(2):364

Fig. 1. The absorbance spectra of ZnO:Al samples as a function of doping level

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Fig. 2. The typical variation of absorbance A as a function of photon energy of undoped ZnO film. The inset shows the drawn of lnA as a function of photon energy ($hv$) to deduce the Urbach energy

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Fig. 3. Optical band gap energy of undoped and Al doped ZnO thin films as a function of aluminum doping

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Fig. 4. Variation of the Urbach energy and the refractive index of Al doped ZnO films as a function of doping level

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Fig. 5. Electrical conductivity $\sigma$ of undoped and Al doped ZnO thin films as a function of aluminum doping

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Fig. 6. X-ray diffraction patterns of Al doped ZnO thin films at different concentrations

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Fig. 7. The variation of the grain size and the FWHM of undoped and Al doped ZnO thin films

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Table 1. Intensity, Bragg angle 2θ, the full width at half-maximum FWHM, the grain size G, band gap energy $E_{\rm g}$ and electrical conductivity $\sigma$ for ZnO thin films were measured as a function of spraying time

[1]	Zhang Y, Wu C, Zheng Y, et al. Synthesis and efficient field emission characteristics of patterned ZnO nanowires. Journal of Semiconductors, 2012, 33(2):023001 doi: 10.1088/1674-4926/33/2/023001
[2]	Zhu X, Wu H, Wang S, et al. Optical and electrical properties of N-doped ZnO and fabrication of thin-film transistors. Journal of Semiconductors, 2009, 30(3):033001 doi: 10.1088/1674-4926/30/3/033001
[3]	Zhang H, Liu H, Lei C, et al. Low-temperature deposition of transparent conducting Mn-W co-doped ZnO thin films. Journal of Semiconductors, 2010, 31(8):083005 doi: 10.1088/1674-4926/31/8/083005
[4]	Ji Z, Mao Q, Ke W. Effects of oxygen partial pressure on resistive switching characteristics of ZnO thin films by DC reactive magnetron sputtering. Solid State Commun, 2010, 150(8):1919
[5]	Zuo C, Wen J, Zhong C. First-principles study of the electronic structures and optical properties of C-F-Be doped wurtzite ZnO. Journal of Semiconductors, 2012, 33(7):072001 doi: 10.1088/1674-4926/33/7/072001
[6]	Kumar P S, Raj A D, Mangalaraj D, et al. Growth of hierarchical based ZnO micro/nanostructured films and their tunable wettability behavior. Appl Surf Sci, 2011, 257(20):6678
[7]	Ye Z, Yuan G, Li B, et al. Fabrication and characteristics of ZnO thin films with Al/Si (100) substrates. Mater Chem Phys, 2005, 93(2):170
[8]	Zhang H, Yang S, Liu H, et al. Preparation and characterization of transparent conducting ZnO:W films by DC magnetron sputtering. Journal of Semiconductors, 2011, 32(4):043002 doi: 10.1088/1674-4926/32/4/043002
[9]	El Manouni A, Manjon F J, Perales M, et al. Effect of thermal annealing on ZnO:Al thin films grown by spray pyrolysis. Superlattices and Microstructures, 2007, 42(2):134
[10]	Rozati S M, Akesteh S. Characterization of ZnO:Al thin films obtained by spray pyrolysis technique. Materials Characterization, 2007, 58(4):319 doi: 10.1016/j.matchar.2006.05.012
[11]	Saleem M, Siddiqi S A, Atiq S, et al. Carriers-mediated ferromagnetic enhancement in Al-doped ZnMnO dilute magnetic semiconductors. Materials Characterization, 2011, 62(12):1102
[12]	Ma Q B, Ye Z Z, He H P, et al. Preparation and characterization of transparent conductive ZnO:Ga films by DC reactive magnetron sputtering. Materials Characterization, 2008, 59(2):124 doi: 10.1016/j.matchar.2006.11.020
[13]	Benramache S, Benhaoua B, Chabane F. Effect of substrate temperature on the stability of transparent conducting cobalt doped ZnO thin films. Journal of Semiconductors, 2012, 33(9):093001 doi: 10.1088/1674-4926/33/9/093001
[14]	Duclére J R, Novotny M, Meaney A, et al. Properties of Li-, P-and N-doped ZnO thin films prepared by pulsed laser deposition. Superlattices and Microstructures, 2005, 38(3):397
[15]	Hafdallah A, Yanineb F, Aida M S, et al. In doped ZnO thin films. Journal of Alloys and Compounds, 2011, 509(18):7267
[16]	Benramache S, Benhaoua B, Chabane F, et al. Influence of growth time on crystalline structure, conductivity and optical properties of ZnO thin films. Journal of Semiconductors, 2013, 34(2):023001 doi: 10.1088/1674-4926/34/2/023001
[17]	Venkatachalam S, Iida Y, Kanno Y. Preparation and characterization of Al doped ZnO thin films by PLD. Superlattices and Microstructures, 2008, 44(2):127
[18]	Zhu H, Hüpkes J, Bunte E, et al. Reactive sputtering of ZnO:Al thin films from rotatable dual metallic targets. Appl Surf Sci, 2012, 259(4):582
[19]	Zhu H, Hüpkes J, Bunte E, et al. Study of ZnO:Al films for silicon thin film solar cells. Appl Surf Sci, 2012, 261:268 doi: 10.1016/j.apsusc.2012.07.159
[20]	Benramache S, Benhaoua B. Influence of substrate temperature and Cobalt concentration on structural and optical properties of ZnO thin films prepared by ultrasonic spray technique. Superlattices and Microstructures, 2012, 52(4):807 doi: 10.1016/j.spmi.2012.06.005
[21]	Benramache S, Benhaoua B. Influence of annealing temperature on structural and optical properties of ZnO:In thin films prepared by ultrasonic spray technique. Superlattices and Microstructures, 2012, 52(6):1062 doi: 10.1016/j.spmi.2012.08.006
[22]	Romero R, Ibanez R L, Dalchiele E A, et al. Compositional and physico-optical characterization of 0-5% Al-doped zinc oxide films prepared by chemical spray pyrolysis. J Phys D:Appl Phys, 2010, 43(9):095303 doi: 10.1088/0022-3727/43/9/095303
[23]	Mekhnache M, Drici A, Hamideche L S, et al. Properties of ZnO thin films deposited on (glass, ITO and ZnO:Al) substrates. Superlattices and Microstructures, 2011, 49(3):510
[24]	Mosbah A, Aida M S. Influence of deposition temperature on structural, optical and electrical properties of sputtered Al doped ZnO thin films. Journal of Alloys and Compounds, 2012, 515(1):149
[25]	Rahmane S, Djouadi M A, Aida M S, et al. Power and pressure effects upon magnetron sputtered aluminum doped ZnO films properties. Thin Solid Films, 2010, 519(1):5 doi: 10.1016/j.tsf.2010.06.063
[26]	Zhang C. High-quality oriented ZnO films grown by sol-gel process assisted with ZnO. Journal of Physics and Chemistry of Solids, 2010, 71(2):364

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Received: 10 October 2012 Revised: 24 February 2013 Online: Published: 01 July 2013

Article Navigation > Journal of Semiconductors > 2013 > 34(7): 073002

Abdelouahab Gahtar, Said Benramache, Boubaker Benhaoua, Foued Chabane. Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique[J]. Journal of Semiconductors, 2013, 34(7): 073002. doi: 10.1088/1674-4926/34/7/073002 ****A Gahtar, S Benramache, B Benhaoua, F Chabane. Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique[J]. J. Semicond., 2013, 34(7): 073002. doi: 10.1088/1674-4926/34/7/073002.

Citation:

A Gahtar, S Benramache, B Benhaoua, F Chabane. Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique[J]. J. Semicond., 2013, 34(7): 073002. doi: 10.1088/1674-4926/34/7/073002.

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Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique

DOI: 10.1088/1674-4926/34/7/073002

1.
VTRS Laboratory, Institute of Technology, University of El-oued 39000, Algeria
2.
Material Sciences Department, Faculty of Science, University of Biskra 07000, Algeria
3.
Mechanics Department, Faculty of Technology, University of Biskra, Biskra 07000, Algeria

More Information

Corresponding author: Said Benramache, Email:saidzno2006@gmail.com
Received Date: 2012-10-10
Revised Date: 2013-02-24
Published Date: 2013-07-01

Abstract

Abstract

Transparent conductive Al doped ZnO thin films were deposited by ultrasonic spray technique. Conditions of preparation have been optimized to get good quality. A set of aluminum (Al) doped ZnO (between 0 and 5 wt%) thin films were grown on glass substrate at 350℃. Nanocrystalline films with a hexagonal wurtzite structure show a strong (002) preferred orientation. The maximum value of grain size G=32.05 nm is attained of Al doped ZnO film with 3 wt%. All the films have low absorbance in the visible region, thus the films are transparent in the visible region; the band gap energy increased from 3.10 to 3.26 eV when Al concentration increased from 0 to 3 wt%. The electrical conductivity of the films increased from 7.5 to 15.2 (Ω·cm)^-1. So the best results are achieved in Al doped ZnO film with 3 wt%.
- ZnO:Al,
- thin films,
- TCO,
- ultrasonic spray technique

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References(26)

References

[1]	Zhang Y, Wu C, Zheng Y, et al. Synthesis and efficient field emission characteristics of patterned ZnO nanowires. Journal of Semiconductors, 2012, 33(2):023001 doi: 10.1088/1674-4926/33/2/023001
[2]	Zhu X, Wu H, Wang S, et al. Optical and electrical properties of N-doped ZnO and fabrication of thin-film transistors. Journal of Semiconductors, 2009, 30(3):033001 doi: 10.1088/1674-4926/30/3/033001
[3]	Zhang H, Liu H, Lei C, et al. Low-temperature deposition of transparent conducting Mn-W co-doped ZnO thin films. Journal of Semiconductors, 2010, 31(8):083005 doi: 10.1088/1674-4926/31/8/083005
[4]	Ji Z, Mao Q, Ke W. Effects of oxygen partial pressure on resistive switching characteristics of ZnO thin films by DC reactive magnetron sputtering. Solid State Commun, 2010, 150(8):1919
[5]	Zuo C, Wen J, Zhong C. First-principles study of the electronic structures and optical properties of C-F-Be doped wurtzite ZnO. Journal of Semiconductors, 2012, 33(7):072001 doi: 10.1088/1674-4926/33/7/072001
[6]	Kumar P S, Raj A D, Mangalaraj D, et al. Growth of hierarchical based ZnO micro/nanostructured films and their tunable wettability behavior. Appl Surf Sci, 2011, 257(20):6678
[7]	Ye Z, Yuan G, Li B, et al. Fabrication and characteristics of ZnO thin films with Al/Si (100) substrates. Mater Chem Phys, 2005, 93(2):170
[8]	Zhang H, Yang S, Liu H, et al. Preparation and characterization of transparent conducting ZnO:W films by DC magnetron sputtering. Journal of Semiconductors, 2011, 32(4):043002 doi: 10.1088/1674-4926/32/4/043002
[9]	El Manouni A, Manjon F J, Perales M, et al. Effect of thermal annealing on ZnO:Al thin films grown by spray pyrolysis. Superlattices and Microstructures, 2007, 42(2):134
[10]	Rozati S M, Akesteh S. Characterization of ZnO:Al thin films obtained by spray pyrolysis technique. Materials Characterization, 2007, 58(4):319 doi: 10.1016/j.matchar.2006.05.012
[11]	Saleem M, Siddiqi S A, Atiq S, et al. Carriers-mediated ferromagnetic enhancement in Al-doped ZnMnO dilute magnetic semiconductors. Materials Characterization, 2011, 62(12):1102
[12]	Ma Q B, Ye Z Z, He H P, et al. Preparation and characterization of transparent conductive ZnO:Ga films by DC reactive magnetron sputtering. Materials Characterization, 2008, 59(2):124 doi: 10.1016/j.matchar.2006.11.020
[13]	Benramache S, Benhaoua B, Chabane F. Effect of substrate temperature on the stability of transparent conducting cobalt doped ZnO thin films. Journal of Semiconductors, 2012, 33(9):093001 doi: 10.1088/1674-4926/33/9/093001
[14]	Duclére J R, Novotny M, Meaney A, et al. Properties of Li-, P-and N-doped ZnO thin films prepared by pulsed laser deposition. Superlattices and Microstructures, 2005, 38(3):397
[15]	Hafdallah A, Yanineb F, Aida M S, et al. In doped ZnO thin films. Journal of Alloys and Compounds, 2011, 509(18):7267
[16]	Benramache S, Benhaoua B, Chabane F, et al. Influence of growth time on crystalline structure, conductivity and optical properties of ZnO thin films. Journal of Semiconductors, 2013, 34(2):023001 doi: 10.1088/1674-4926/34/2/023001
[17]	Venkatachalam S, Iida Y, Kanno Y. Preparation and characterization of Al doped ZnO thin films by PLD. Superlattices and Microstructures, 2008, 44(2):127
[18]	Zhu H, Hüpkes J, Bunte E, et al. Reactive sputtering of ZnO:Al thin films from rotatable dual metallic targets. Appl Surf Sci, 2012, 259(4):582
[19]	Zhu H, Hüpkes J, Bunte E, et al. Study of ZnO:Al films for silicon thin film solar cells. Appl Surf Sci, 2012, 261:268 doi: 10.1016/j.apsusc.2012.07.159
[20]	Benramache S, Benhaoua B. Influence of substrate temperature and Cobalt concentration on structural and optical properties of ZnO thin films prepared by ultrasonic spray technique. Superlattices and Microstructures, 2012, 52(4):807 doi: 10.1016/j.spmi.2012.06.005
[21]	Benramache S, Benhaoua B. Influence of annealing temperature on structural and optical properties of ZnO:In thin films prepared by ultrasonic spray technique. Superlattices and Microstructures, 2012, 52(6):1062 doi: 10.1016/j.spmi.2012.08.006
[22]	Romero R, Ibanez R L, Dalchiele E A, et al. Compositional and physico-optical characterization of 0-5% Al-doped zinc oxide films prepared by chemical spray pyrolysis. J Phys D:Appl Phys, 2010, 43(9):095303 doi: 10.1088/0022-3727/43/9/095303
[23]	Mekhnache M, Drici A, Hamideche L S, et al. Properties of ZnO thin films deposited on (glass, ITO and ZnO:Al) substrates. Superlattices and Microstructures, 2011, 49(3):510
[24]	Mosbah A, Aida M S. Influence of deposition temperature on structural, optical and electrical properties of sputtered Al doped ZnO thin films. Journal of Alloys and Compounds, 2012, 515(1):149
[25]	Rahmane S, Djouadi M A, Aida M S, et al. Power and pressure effects upon magnetron sputtered aluminum doped ZnO films properties. Thin Solid Films, 2010, 519(1):5 doi: 10.1016/j.tsf.2010.06.063
[26]	Zhang C. High-quality oriented ZnO films grown by sol-gel process assisted with ZnO. Journal of Physics and Chemistry of Solids, 2010, 71(2):364

Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique

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Preparation of transparent conducting ZnO:Al films on glass substrates by ultrasonic spray technique

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