Abstract
Due to its direct band gap and high absorption coefficient, Cupric Oxide (CuO) is widely used as an absorbent material for solar cells, yet most of the available deposition methods are expensive and complex. For this reason, this paper is concerned with the elaboration of CuO thin films using the simple and inexpensive modified successive ionic layer adsorption and reaction method, i.e., modified SILAR method. To that end, glass slide substrates and an aqueous solution of hydrated copper chloride (CuCl\(_{2}\)·2H\(_{2}\)O) complexed with aqueous ammonia (NH\( _{3} \)) (25–28%) were used, then the growth conditions were carefully evaluated to reduce the presence of the remaining phases other than CuO. The elaborated thin films are studied from four perspectives: (1) structural decomposition, (2) morphological decomposition, (3) chemical decomposition and (4) optical properties. It is found that the deposited films are polycrystalline and crystallized in a pure CuO monoclinic structure without any other secondary phase. Raman and X-ray photoelectron spectroscopy confirmed the pure phase obtained and the scanning electron microscopy images showed that the resulting films were dense, smooth and homogeneous. The energy dispersive X-ray spectrum and the elemental mapping scan corroborate the uniform distribution of Cu and O elements on the film surface. Furthermore, UV–visible spectra exhibited a negative correlation between optical transmission and deposition cycles—if the deposition cycles increased, optical transmission decreased similarly the optical band gap. As well as the refractive index and Urbach energy were determined. As a result, the synthesis technique is very simple and low cost, CuO thin films could be appropriate for solar cells applications.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Akaltun, Y.: Effect of thickness on the structural and optical properties of CuO thin films grown by successive ionic layer adsorption and reaction. Thin Solid Films 594(Part A), 30–34 (2015). https://doi.org/10.1016/j.tsf.2015.10.003
Akaltun, Y., Çayir, T.: Fabrication and characterization of NiO thin films prepared by SILAR method. J. Alloys Compd. 625, 144–148 (2015). https://doi.org/10.1016/j.jallcom.2014.10.194
Akaltun, Y., Yıldırım, M.A., Ateşş, A., Yıldırım, M.: Zinc concentration effect on structural, optical and electrical properties of Cd\(_{1-x}\)Zn\(_{x}\)Se thin films. Mater. Res. Bull. 47(11), 3390–3396 (2012). https://doi.org/10.1016/j.materresbull.2012.07.018
Al-Ghamdi, A.A., Khedr, M., Ansari, M.S., Hasan, P., Abdel-wahab, M., Farghali, A.: RF sputtered CuO thin films: structural, optical and photo-catalytic behavior. Phys. E Low-dimens. Syst. Nanostruct. 81(Supplement C), 83–90 (2016). https://doi.org/10.1016/j.physe.2016.03.004
Alkhayatt, A.H.O., Jaafer, M.D., Al Alak, H.H.A., Ali, A.H.: Characterization of CuO/n-Si pn junction synthesized by successive ionic layer adsorption and reaction method. Opt. Quantum Electron. 51(7), 233 (2019). https://doi.org/10.1007/s11082-019-1951-4
Anitha, M., Saravanakumar, K., Anitha, N., Amalraj, L.: Influence of fluorine doped CdO thin films by an simplified spray pyrolysis technique using nebulizer. Opt. Quantum Electron. 51(6), 187 (2019). https://doi.org/10.1007/s11082-019-1901-1
Baturay, S., Tombak, A., Kaya, D., Ocak, Y.S., Tokus, M., Aydemir, M., Kilicoglu, T.: Modification of electrical and optical properties of CuO thin films by Ni doping. J. Sol–Gel Sci. Technol. 78(2), 422–429 (2016). https://doi.org/10.1007/s10971-015-3953-4
Bayansal, F., Şahin, B., Yüksel, M., Biyikli, N., Çetinkara, H., Güder, H.: Influence of coumarin as an additive on CuO nanostructures prepared by successive ionic layer adsorption and reaction (SILAR) method. J. Alloys Compd. 566, 78–82 (2013). https://doi.org/10.1016/j.jallcom.2013.03.018
Bayansal, F., Yüksel, M., Sahin, B.: Facile fabrication and characterization of Sn\(_{x}\)Cu\(_{1-x}\)O composite films by the SILAR method on glass substrates. J. Alloys Compd. 664(Supplement C), 38–44 (2016). https://doi.org/10.1016/j.jallcom.2015.12.174
Boudjema, B., Daira, R., Kabir, A., Djebien, R.: Physico-chemical properties of CuO thin films deposited by spray pyrolysis. In: Material Engineering and Smart Materials, volume 895 of Materials Science Forum, pp. 33–36. Trans Tech Publications (2017). https://doi.org/10.4028/www.scientific.net/MSF.895.33
Cavusoglu, H., Aydin, R.: Complexing agent triethanolamine mediated synthesis of nanocrystalline CuO thin films at room temperature via SILAR technique. Superlattices Microstruct. 128, 37–47 (2019). https://doi.org/10.1016/j.spmi.2019.01.011
ÇAYR TAŞDEMIRCİ T: Synthesis of copper-doped nickel oxide thin films: structural and optical studies. Chem. Phys. Lett. 738:136884 (2020). https://doi.org/10.1016/j.cplett.2019.136884
Chaki, I., EI Hat, A., Mzerd, A., Belayachi, A., Regragui, M., Ajjammouri, T., Sekkat, Z., Abd-Lefdil, M.: Physical properties of Gd doped ZnO thin films grown by spray pyrolysis. In: Proceedings of 2015 IEEE International Renewable and Sustainable Energy Conference, IRSEC 2015 (2016). https://doi.org/10.1109/IRSEC.2015.7455054
Chand, P., Gaur, A., Kumar, A., Gaur, U.K.: Structural and optical study of Li doped CuO thin films on Si (100) substrate deposited by pulsed laser deposition. Appl. Surf. Sci. 307, 280–286 (2014). https://doi.org/10.1016/j.apsusc.2014.04.027
Chtouki, T., Taboukhat, S., Kavak, H., Zawadzka, A., Erguig, H., Elidrissi, B., Sahraoui, B.: Characterization and third harmonic generation calculations of undoped and doped spin-coated multilayered CuO thin films. J. Phys. Chem. Solids 124, 60–66 (2019). https://doi.org/10.1016/j.jpcs.2018.08.035
Daoudi, O., Qachaou, Y., Raidou, A., Nouneh, K., Lharch, M., Fahoume, M.: Study of the physical properties of CuO thin films grown by modified SILAR method for solar cells applications. Superlattices Microstruct. 127, 93–99 (2019). https://doi.org/10.1016/j.spmi.2018.03.006
Debbichi, L., Marco de Lucas, M.C., Pierson, J.F., KrÃger, P.: Vibrational properties of CuO and Cu\(_{4}\)O\(_{3}\) from first-principles calculations, and Raman and infrared spectroscopy. J. Phys. Chem. C 116(18), 10232–10237 (2012). https://doi.org/10.1021/jp303096m
Dhineshbabu, N.R., Rajendran, V., Nithyavathy, N., Vetumperumal, R.: Study of structural and optical properties of cupric oxide nanoparticles. Appl. Nanosci. 6(6), 933–939 (2016). https://doi.org/10.1007/s13204-015-0499-2
Du, Y., Gao, X., Zhang, X., Meng, X.: Characterization of the microstructure and the optical and electrical properties of the direct-current magnetron sputtered CuO films at different substrate temperatures. Phys. B Condens. Matter 546, 28–32 (2018). https://doi.org/10.1016/j.physb.2018.07.013
Gaikwad, M., Suryawanshi, M., Maldar, P., Dongale, T., Moholkar, A.: Nanostructured zinc oxide photoelectrodes by green routes M-SILAR and electrodeposition for dye sensitized solar cell. Opt. Mater. 78, 325–334 (2018). https://doi.org/10.1016/j.optmat.2018.02.040
Gao, C., Shen, H., Sun, L., Shen, Z.: Chemical bath deposition of Bi\(_{2}\)S\(_{3}\) films by a novel deposition system. Appl. Surf. Sci. 257(17), 7529–7533 (2011). https://doi.org/10.1016/j.apsusc.2011.03.080
Gençylmaz, O., Taşköprü, T.: Effect of pH on the synthesis of CuO films by SILAR method. J. Alloys Compd. 695(Supplement C), 1205–1212 (2017). https://doi.org/10.1016/j.jallcom.2016.10.247
Guillén, C., Herrero, J.: Single-phase Cu\(_{2}\)O and CuO thin films obtained by low-temperature oxidation processes. J. Alloys Compd. 737, 718–724 (2018). https://doi.org/10.1016/j.jallcom.2017.12.174
Hu, X., Gao, F., Xiang, Y., Wu, H., Zheng, X., Jiang, J., Li, J., Yang, H., Liu, S.: Influence of oxygen pressure on the structural and electrical properties of CuO thin films prepared by pulsed laser deposition. Mater. Lett. 176, 282–284 (2016). https://doi.org/10.1016/j.matlet.2016.04.055
Jagadeesan, V., Subramaniam, V.: Impact of molarity on structural, optical, morphological and electrical properties of copper oxide thin films prepared by cost effective jet nebulizer spray pyrolysis technique. J. Mater. Sci. Mater. Electron. 30(2), 1571–1578 (2019). https://doi.org/10.1007/s10854-018-0428-8
Jan, T., Iqbal, J., Farooq, U., Gul, A., Abbasi, R., Ahmad, I., Malik, M.: Structural, Raman and optical characteristics of Sn doped CuO nanostructures: a novel anticancer agent. Ceram. Int. 41(10, Part A), 13074–13079 (2015). https://doi.org/10.1016/j.ceramint.2015.06.080
Jellal, I., Ahmoum, H., Khaaissa, Y., Nouneh, K., Boughrara, M., Fahoume, M., Chopra, S., Naja, J.: Experimental and ab-initio investigation of the microstructure and optoelectronic properties of FCMâ CVD-prepared Al-doped ZnO thin films. Appl. Phys. A 125(9), 650 (2019). https://doi.org/10.1007/s00339-019-2947-4
Jiang, T., Wang, Y., Meng, D., Wu, X., Wang, J., Chen, J.: Controllable fabrication of CuO nanostructure by hydrothermal method and its properties. Appl. Surf. Sci. 311(Supplement C), 602–608 (2014). https://doi.org/10.1016/j.apsusc.2014.05.116
Kaur, N., Sharma, S.K., Kim, D.Y., Singh, N.: Highly transparent and lower resistivity of yttrium doped ZnO thin films grown on quartz glass by sol-gel method. Phys. B Condens. Matter 500, 179–185 (2016). https://doi.org/10.1016/j.physb.2016.08.005
Koh, T., O’Hara, E., Gordon, M.: Growth of nanostructured CuO thin films via microplasma-assisted, reactive chemical vapor deposition at high pressures. J. Cryst. Growth 363, 69–75 (2013). https://doi.org/10.1016/j.jcrysgro.2012.10.005
Ma, Q., Lv, X., Wang, Y., Chen, J.: Optical and photocatalytic properties of Mn doped flower-like ZnO hierarchical structures. Opt. Mater. 60, 86–93 (2016). https://doi.org/10.1016/j.optmat.2016.07.014
Moumen, A., Hartiti, B., Thevenin, P., Siadat, M.: Synthesis and characterization of CuO thin films grown by chemical spray pyrolysis. Opt. Quantum Electron. 49(2), 70 (2017). https://doi.org/10.1007/s11082-017-0910-1
Moumen, A., Hartiti, B., Comini, E., Khalidi, Z.E., Arachchige, H.M.M., Fadili, S., Thevenin, P.: Preparation and characterization of nanostructured CuO thin films using spray pyrolysis technique. Superlattices Microstruct. 127, 2–10 (2019). https://doi.org/10.1016/j.spmi.2018.06.061
Naveena, D., Logu, T., Dhanabal, R., Sethuraman, K., Bose, A.C.: Comparative study of effective photoabsorber CuO thin films prepared via different precursors using chemical spray pyrolysis for solar cell application. J. Mater. Sci. Mater. Electron. 30(1), 561–572 (2019). https://doi.org/10.1007/s10854-018-0322-4
Nesa, M., Sharmin, M., Hossain, K.S., Bhuiyan, A.: Structural, morphological, optical and electrical properties of spray deposited zinc doped copper oxide thin films. J. Mater. Sci. Mater. Electron. 28(17), 12523–12534 (2017). https://doi.org/10.1007/s10854-017-7075-3
Ozaslan, D., Erken, O., Gunes, M., Gumus, C.: The effect of annealing temperature on the physical properties of Cu\(_{2}\)O thin film deposited by SILAR method. Phys. B Condens. Matter 580, 411922 (2020). https://doi.org/10.1016/j.physb.2019.411922
Padrón, K., Juárez-Pérez, E.J., Forcade, F., Snyders, R., Noirfalise, X., Laza, C., Jiménez, J., Vigil, E.: Nanostructured CuO films deposited on fluorine doped tin oxide conducting glass with a facile technology. Thin Solid Films 660, 386–390 (2018). https://doi.org/10.1016/j.tsf.2018.06.035
Patil, A.S., Lohar, G.M., Fulari, V.J.: Structural, morphological, optical and photoelectrochemical cell properties of copper oxide using modified SILAR method. J. Mater. Sci. Mater. Electron. 27(9), 9550–9557 (2016). https://doi.org/10.1007/s10854-016-5007-2
Prabhu, R.R., Saritha, A., Shijeesh, M., Jayaraj, M.: Fabrication of p-CuO/n-ZnO heterojunction diode via sol-gel spin coating technique. J. Mater. Sci. Eng. B 220, 82–90, ISSN 0921-5107 (2017). https://doi.org/10.1016/j.mseb.2017.03.008
Raidou, A., Benmalek, F., Sall, T., Aggour, M., Qachaou, A., Laanab, L., Fahoume, M.: Characterization of ZnO thin films grown by SILAR method. Open Access Libr. J. 1, 1–9 (2014). https://doi.org/10.4236/oalib.1100588
Sahu, K., Choudhary, S., Khan, S.A., Pandey, A., Mohapatra, S.: Thermal evolution of morphological, structural, optical and photocatalytic properties of CuO thin films. Nano-Struct. Nano-Objects 17, 92–102 (2019). https://doi.org/10.1016/j.nanoso.2018.12.005
Shabu, R., Raj, A.M.E., Sanjeeviraja, C., Ravidhas, C.: Assessment of CuO thin films for its suitablity as window absorbing layer in solar cell fabrications. Mater. Res. Bull. 68, 1–8 (2015). https://doi.org/10.1016/j.materresbull.2015.03.016
Shinde, S.K., Dubal, D.P., Ghodake, G.S., Kim, D.Y., Fulari, V.J.: Morphological tuning of CuO nanostructures by simple preparative parameters in SILAR method and their consequent effect on supercapacitors. Nano-Struct. Nano-Objects 6, 5–13 (2016). https://doi.org/10.1016/j.nanoso.2016.01.004
Sultana, J., Paul, S., Karmakar, A., Yi, R., Dalapati, G.K., Chattopadhyay, S.: Chemical bath deposited (CBD) CuO thin films on n-silicon substrate for electronic and optical applications: impact of growth time. Appl. Surf. Sci. 418(Part A), 380–387 (2017). https://doi.org/10.1016/j.apsusc.2016.12.139
Sultana, J., Paul, S., Saha, R., Sikdar, S., Karmakar, A., Chattopadhyay, S.: Optical and electronic properties of chemical bath deposited p-CuO and n-ZnO nanowires on silicon substrates: p-CuO/n-ZnO nanowires solar cells with high open-circuit voltage and short-circuit current. Thin Solid Films 699, 137861, ISSN 0040-6090 (2020). https://doi.org/10.1016/j.tsf.2020.137861
Wang, M., Kim, E.J., Kim, S., Chung, J.S., Yoo, I.-K., Shin, E.W., Hahn, S.H., Park, C.: Optical and structural properties of sol–gel prepared MgZnO alloy thin films. Thin Solid Films 516(6), 1124–1129 (2008). https://doi.org/10.1016/j.tsf.2007.05.039
Wang, Y., Jiang, T., Meng, D., Yang, J., Li, Y., Ma, Q., Han, J.: Fabrication of nanostructured CuO films by electrodeposition and their photocatalytic properties. Appl. Surf. Sci. 317(Supplement C), 414–421 (2014). https://doi.org/10.1016/j.apsusc.2014.08.144
Wang, C., Yang, F., Cao, Y., He, X., Tang, Y., Li, Y.: Cupric oxide nanowires on three-dimensional copper foam for application in click reaction. RSC Adv. 7, 9567–9572 (2017). https://doi.org/10.1039/C7RA00014F
Xu, J.F., Ji, W., Shen, Z.X., Li, W.S., Tang, S.H., Ye, X.R., Jia, D.Z., Xin, X.Q.: Raman spectra of CuO nanocrystals. J. Raman Spectrosc. 30(5), 413–415 (1999). https://doi.org/10.1002/(SICI)1097-4555(199905)30:5<413::AID-JRS387>3.0.CO;2-N
Xu, L., Zheng, G., Pei, S., Wang, J.: Investigation of optical bandgap variation and photoluminescence behavior in nanocrystalline CuO thin films. Optik 158, 382–390 (2018). https://doi.org/10.1016/j.ijleo.2017.12.138
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Daoudi, O., Elmadani, A., Lharch, M. et al. A new efficient synthesis of CuO thin films using modified SILAR method. Opt Quant Electron 52, 413 (2020). https://doi.org/10.1007/s11082-020-02530-2
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11082-020-02530-2