Skip to main content

Advertisement

SpringerLink
Log in

Secondary phases and their influence on optical and electrical properties of electrodeposited Cu2FeSnS4 films

  • Published:
Applied Physics A Aims and scope Submit manuscript

Abstract

Cu–Fe–Sn–S have been electrodeposited on indium tin oxide coated glass (ITO/glass) substrates, varying only the deposition time, followed by sulfurization in argon atmosphere at a temperature of 500 °C. X-ray diffraction patterns confirmed the formation of polycrystalline CFTS and other secondary phases. The Raman spectroscopy results confirm the formation of stannite phase, by the existence of the most intense peak at 330 cm−1 corresponding to A-symmetry vibrational mode, while the SnS2 surface phase reduces upon increasing deposition time. The inferred bandgaps by specular transmission are in 1.4–1.7 eV range, influenced by the detected orthorhombic Cu4SnS4 and rhodostannite secondary phases. The electrical measurements confirm the p-type nature of the films, while density of free carriers is relatively high (~ 1019 cm−3), leading to extremely low resistivity in the Ω cm range.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

References

  1. Best Research-Cell Efficiency Chart. https://www.nrel.gov/pv/cell-efficiency.html. Accessed 30 Jun 2021

  2. A. Domínguez, R. Geyer, Photovoltaic waste assessment of major photovoltaic installations in the United States of America. Renew. Energy 133, 1188–1200 (2019)

    Article  Google Scholar 

  3. S.A. Vanalakar, G.L. Agwane, M.G. Gang, P.S. Patil, J.H. Kim, J.Y. Kim, A mild hydrothermal route to synthesis of CZTS nanoparticle inks for solar cell applications. Phys. Status Solidi. C 12, 500–503 (2015)

    Article  ADS  Google Scholar 

  4. S. Giraldo, Z. Jehl, M. Placidi, V. Izquierdo-Roca, A. Pérez-Rodríguez, E. Saucedo, Progress and Perspectives of Thin Film Kesterite Photovoltaic Technology: A Critical Review. Adv. Mater. 31, 1806692 (2019)

    Article  Google Scholar 

  5. X. Meng, H. Deng, J. Tao, H. Cao, X. Li, L. Sun, P. Yang, J. Chu, Heating rate tuning in structure, morphology and electricity properties of Cu2FeSnS4 thin films prepared by sulfurization of metallic precursors. J. Alloys Compd. 680, 446–451 (2016)

    Article  Google Scholar 

  6. C. Yan, C. Huang, J. Yang, F. Liu, J. Liu, Y. Lai, J. Li, Y. Liu, Synthesis and characterizations of quaternary Cu2FeSnS4 nanocrystals. Chem. Commun. 48, 2603 (2012)

    Article  Google Scholar 

  7. C. Nefzi, M. Souli, M. Luisa Dotor Castilla, J.M. García, N. Kamoun-Turki, CFTS-3/In2S3/SnO2F heterojunction structure as eco-friendly photocatalytic candidate for removing organic pollutants. Arab. J. Chem. 13, 6366–6378 (2020)

    Article  Google Scholar 

  8. C. Nefzi, M. Souli, Y. Cuminal, N. Kamoun-Turki, Effect of sulfur concentration on structural, optical and electrical properties of Cu2FeSnS4 thin films for solar cells and photocatalysis applications. Superlattices Microstruct. 124, 17–29 (2018)

    Article  ADS  Google Scholar 

  9. H. Oueslati, M. Ben Rabeh, M. Kanzari, Growth and Characterization of the Evaporated Quaternary Absorber Cu2FeSnS4 for Solar Cell Applications. J. Electron. Mater. 47, 3577–3584 (2018)

    Article  ADS  Google Scholar 

  10. S.J. da Silveira, S. Silvestri, E.M. de Moraes Flores, E. Luiz Foletto, A Novel application of Cu2FeSnS4 particles prepared by solvothermal route as solar Photo-Fenton catalyst. Mater. Lett. 228, 160–163 (2018)

    Article  Google Scholar 

  11. R.R. Prabhakar, N. Huu Loc, M.H. Kumar, P.P. Boix, S. Juan, R.A. John, S.K. Batabyal, L.H. Wong, Facile Water-based Spray Pyrolysis of Earth-Abundant Cu2FeSnS4 Thin Films as an Efficient Counter Electrode in Dye-Sensitized Solar Cells. ACS Appl. Mater. Interfaces 6, 17661–17667 (2014)

    Article  Google Scholar 

  12. L. Ai, J. Jiang, Self-sacrificial templating synthesis of porous quaternary Cu–Fe–Sn–S semiconductor nanotubes via microwave irradiation. Nanotechnology 23, 495601 (2012)

    Article  ADS  Google Scholar 

  13. X. Fontané, V. Izquierdo-Roca, E. Saucedo, S. Schorr, V.O. Yukhymchuk, V.M. Ya, A. Pérez-Rodríguez, J.R. Morante, Vibrational properties of stannite and kesterite type compounds: Raman scattering analysis of Cu2(Fe, Zn) SnS4. J. Alloys Compd. 539, 190–194 (2012)

    Article  Google Scholar 

  14. J. Zhou, S. Yu, X. Guo, L. Wu, H. Li, Preparation and characterization of Cu2FeSnS4 thin films for solar cells via a co-electrodeposition method. Curr. Appl. Phys. 19, 67–71 (2019)

    Article  ADS  Google Scholar 

  15. S. Chatterjee, A.J. Pal, A solution approach to p-type Cu2FeSnS4 thin-films and pn-junction solar cells: Role of electron selective materials on their performance. Sol. Energy Mater. Sol. Cells 160, 233–240 (2017)

    Article  Google Scholar 

  16. H. Kirou, H. Atourki, K. Abouabassi, A. Soltani, A. Almaggoussi, A. Elfanaoui, K. Bouabid, M. Nya, A. Ihla, Effects of Na2SO4 on the optical and structural properties of Cu2ZnSnS4 thin films synthesized using co-electrodeposition technique. Opt. Mater. 201, 219–226 (2018)

    Google Scholar 

  17. X. Miao, R. Chen, W. Cheng, Synthesis and characterization of Cu2FeSnS4 thin films prepared by electrochemical deposition. Mater. Lett. 193, 183–186 (2017)

    Article  Google Scholar 

  18. O. El Khouja, A.C. Galca, K. Nouneh, M.Y. Zaki, M. Ebn Touhami, M. Taibi, E. Matei, C.C. Negrila, M. Enculescu, L. Pintilie, Structural, morphological and optical properties of Cu–Fe–Sn–S thin films prepared by electrodeposition at fixed applied potential. Thin Solid Films 721, 138547 (2021)

    Article  ADS  Google Scholar 

  19. D.R. Gabe, The role of hydrogen in metal electrodeposition processes. J. Appl. Electrochem. 27, 908–915 (1997)

    Article  Google Scholar 

  20. J.J. Scragg, Copper Zinc Tin Sulfide Thin Films for Photovoltaics (Springer, Berlin Heidelberg, Berlin, Heidelberg, 2011), p. 10

    Book  Google Scholar 

  21. J. Trajic, M. Romcevic, M. Petrovic, M. Gilic, P. Balaz, A. Zorkovska, N. Romcevi, Optical properties of the mechanochemically synthesized Cu2FeSnS4 (stannite) nanocrystals: Raman study. Opt. Mater. 75, 314–318 (2018)

    Article  ADS  Google Scholar 

  22. S.M. Yu, K.-S. Lim, D.-W. Shin, T.-S. Oh, J.-B. Yoo, Effect of the intermediate sulfide layer on the Cu2ZnSnS4-based solar cells. J. Mater. Sci. Mater. Electron. 28, 5696–5702 (2017)

    Article  Google Scholar 

  23. B. Unveroglu, G. Zangari, Towards phase pure kesterite CZTS films via Cu-Zn-Sn electrodeposition followed by sulfurization. Electrochim. Acta 219, 664–672 (2016)

    Article  Google Scholar 

  24. M. Guc, S. Levcenko, I.V. Bodnar, V.I. Roca, X. Fontane, L.V. Volkova, E. Arushanov, A.P. Rodriguez, Polarized Raman scattering study of kesterite type Cu2ZnSnS4 single crystals. Sci Rep 6, 19414 (2016)

    Article  ADS  Google Scholar 

  25. T. Raadik, M. Grossberg, J. Krustok, M. Kauk-Kuusik, A. Crovetto, R. Bolt Ettlinger, O. Hansen, J. Schou, Temperature dependent photoreflectance study of Cu2SnS3 thin films produced by pulsed laser deposition. Appl. Phys. Lett. 110, 261105 (2017)

    Article  ADS  Google Scholar 

  26. L. Sun, J. Ma, N. Yao, Z. Huang, J. Chu, Copper content dependence of electrical properties and Raman spectra of Se-deficient Cu(In, Ga)Se2 thin films for solar cells. J. Mater. Sci. Mater. Electron. 27, 9124–9130 (2016)

    Article  Google Scholar 

  27. N.X. Ca, N.Q. Bau, T.L. Phan, V.T.K. Lien, N.T.T. Lieu, N.X. Nghira, Temperature-dependent photoluminescent and Raman studies on type-II CdS/ZnSe core/shell and CdS/CdZnS-ZnCdSe/ZnSe core/intermediate/shell nanoparticles. J. Alloys Compd. 697, 401–408 (2017)

    Article  Google Scholar 

  28. M.O. Semenenko, I.S. Babichuk, O. Kyriienko, I.V. Bodnar, R. Caballero, M. Leon, RF Electromagnetic Field Treatment of Tetragonal Kesterite CZTSSe Light Absorbers. Nanoscale Res. Lett. 12, 408 (2017)

    Article  ADS  Google Scholar 

  29. A. Ghosh, A. Biswas, R. Thangavel, G. Udayabhanu, Photo-electrochemical properties and electronic band structure of kesterite copper chalcogenide Cu2–II–Sn–S4 (II = Fe Co, Ni) thin films. RSC Adv. 6, 96025–96034 (2016)

    Article  ADS  Google Scholar 

  30. M. Himmrich, H. Haeuseler, Far infrared studies on stannite and wurtzstannite type compounds. Spectrochim. Acta Part Mol. Spectrosc. 47, 933–942 (1991)

    Article  ADS  Google Scholar 

  31. M. Benchikri, O. Zaberca, D.R. El Ouatib, B, Oftinger F, Balocchi A, Chane-Ching J.Y, A high temperature route to the formation of highly pure quaternary chalcogenide particles. Mater. Lett. 68, 340–343 (2012)

    Article  Google Scholar 

  32. F. López-Vergara, A. Galdámez, V. Manríquez, G. González, Crystal structure and Raman scattering characterization of Cu2Fe1-xCoxSnS4 chalcogenide compounds. Solid State Sci. 49, 54–60 (2015)

    Article  ADS  Google Scholar 

  33. D.B. Khadka, J. Kim, Structural, optical and electrical properties of Cu2FeSnX4 (X=S, Se) thin films prepared by chemical spray pyrolysis. J. Alloys Compd. 638, 103–108 (2015)

    Article  Google Scholar 

  34. Y. Guo, W. Cheng, J. Jiang, S. Zuo, F. Shi, J. Chu, The structural, morphological and optical–electrical characteristic of Cu2XSnS4 (X: Cu, Mg) thin films fabricated by novel ultrasonic co-spray pyrolysis. Mater. Lett. 172, 68–71 (2016)

    Article  Google Scholar 

  35. U. Chalapathi, Y. Jayasree, S. Uthanna, V. Sundara Raja, Effect of annealing temperature on the properties of spray deposited Cu2SnS3 thin films: Properties of spray deposited Cu2SnS3 thin films. Phys. Status Solidi A 210, 2384–2390 (2013)

    Article  ADS  Google Scholar 

  36. F. Liu, K. Sun, W. Li, C. Yan, H. Cui, L. Jiang, X. Hao, M.A. Green, Enhancing the Cu2ZnSnS 4 solar cell efficiency by back contact modification: Inserting a thin TiB 2 intermediate layer at Cu2ZnSnS4 /Mo interface. Appl. Phys. Lett. 104, 051105 (2014)

    Article  ADS  Google Scholar 

  37. C. Song, S. Wang, W. Dong, X. Fang, J. Shao, J. Zhu, X. Pan, Hydrothermal synthesis of iron pyrite (FeS2) as efficient counter electrodes for dye-sensitized solar cells. Sol. Energy 133, 429–436 (2016)

    Article  ADS  Google Scholar 

  38. C. Rincón, M. Quintero, E. Moreno, Ch. Power, E. Quintero, J.A. Henao, M.A. Macías, G.E. Delgado, R. Tovar, M. Morocoim, X-ray diffraction, Raman spectrum and magnetic susceptibility of the magnetic semiconductor Cu2FeSnS4. Solid State Commun. 151, 947–951 (2011)

    Article  ADS  Google Scholar 

  39. M. Guc, F. Oliva, A. Fairbrother, T. Jawhari, X. Alcobe, M. Placidi, A. Pérez-Rodríguez, E. Saucedo, V. Izquierdo-Roca, Cu-Sn-S system: Vibrational properties and coexistence of the Cu2SnS3, Cu3SnS4 and Cu4SnS4 compounds. Scr. Mater. 186, 180–184 (2020)

    Article  Google Scholar 

  40. H. Toura, Y.K. Khattak, R, Baig F, Soucase BM, Ebn Touhami M, Back contact effect on electrodeposited CZTS kesterite thin films experimental and numerical investigation. Sol. Energy 194, 932–938 (2019)

    Article  ADS  Google Scholar 

  41. J. Caetano de Souza, A. Ferreira da Silva, H. Vargas, Optical fundamental band-gap energy of semiconductors by photoacoustic spectroscopy. J. Phys. IV 04, 129–132 (1994)

    Google Scholar 

  42. P.R. Ghediya, T.K. Chaudhuri, Dip-coated Cu2CoSnS4 thin films from molecular ink for solar photovoltaics. Mater. Res. Express 5, 085509 (2018)

    Article  ADS  Google Scholar 

  43. S. Chen, A. Walsh, Y. Luo, J.-H. Yang, X.G. Gong, S.-H. Wei, Wurtzite-derived polytypes of kesterite and stannite quaternary chalcogenide semiconductors. Phys. Rev. B 82, 195203 (2010)

    Article  ADS  Google Scholar 

  44. Y. Zhang, X. Sun, P. Zhang, X. Yuan, F. Huang, W. Zhang, Structural properties and quasiparticle band structures of Cu-based quaternary semiconductors for photovoltaic applications. J. Appl. Phys. 111, 063709 (2012)

    Article  ADS  Google Scholar 

  45. S. Chen, X.G. Gong, A. Walsh, S.-H. Wei, Electronic structure and stability of quaternary chalcogenide semiconductors derived from cation cross-substitution of II-VI and I-III-VI2 compounds. Phys. Rev. B 79, 165211 (2009)

    Article  ADS  Google Scholar 

  46. K.-L. Huang, C.-H. Huang, W.-T. Lin, Y.-S. Fu, T.-F. Guo, Solvothermal synthesis and tunable bandgap of Cu2(Zn1−xCox) SnS4 and Cu2(Fe1−xCox) SnS4 nanocrystals. J. Alloys Compd. 646, 1015–1022 (2015)

    Article  Google Scholar 

  47. D.B. Khadka, J. Kim, Structural Transition and Band Gap Tuning of Cu2(Zn, Fe)SnS4 Chalcogenide for Photovoltaic Application. J. Phys. Chem. C 118, 14227–14237 (2014)

    Article  Google Scholar 

  48. S.B. Zhang, S.-H. Wei, Reconstruction and energetics of the polar (112) and (1 ¯ 1 ¯2 ¯) versus the nonpolar (220) surfaces of CuInSe 2. Phys. Rev. B 65, 081402 (2002)

    Article  ADS  Google Scholar 

  49. M.K. Gonce, E. Aslan, F. Ozel, I. Hatay Patir, Dye-Sensitized Cu2XSnS4 (X=Zn, Ni, Fe Co, and Mn) Nanofibers for Efficient Photocatalytic Hydrogen Evolution. Chemsuschem 9, 600–605 (2016)

    Article  Google Scholar 

  50. M.Y. Zaki, K. Nouneh, M. Ebn Touhami, R.A. Belakhmima, A.C. Galca, L. Pintilie, M. Enculescu, M. Baibarac, M. Taibi, Effect of mixing complexing agents on the properties of electrodeposited CZTS thin films. Opt. Mater. 83, 252–256 (2018)

    Article  ADS  Google Scholar 

  51. M. Beraich, M. Taibi, A. Guenbour, A. Zarrouk, M. Boudalia, A. Bellaouchou, M. Tabyaou, Z. Sekkat, M. Fahoume, Synthesis and characterization of Cu2CoSnS4 thin film via electrodeposition technique for solar cells. J Mater. Sci. Mater. Electron. 30, 12487–12492 (2019)

    Article  Google Scholar 

  52. F. Ghiyasi, M.R. Fadavieslam, M. Ardyanian, Facile deposition and study of substrate temperature effect on the structural and physical properties of Cu2FeSnS4 (CFTS) thin films. J. Mater. Sci. Mater. Electron. 31, 2398–2405 (2020)

    Article  Google Scholar 

  53. F. Ozel, Earth-abundant quaternary semiconductor Cu2MnSnS4 (M = Fe Co, Ni and Mn) nanofibers: Fabrication, characterization and band gap arrangement. J. Alloys Compd. 657, 157–162 (2016)

    Article  Google Scholar 

  54. J. Tao, L. Chen, H. Cao, C. Zhang, J. Liu, Y. Zhang, L. Huang, J. Jiang, P. Yang, J. Chu, Co-electrodeposited Cu2ZnSnS4 thin-film solar cells with over 7% efficiency fabricated via fine-tuning of the Zn content in absorber layers. J. Mater. Chem. A 4, 3798–3805 (2016)

    Article  Google Scholar 

  55. S.A. Bashkirov, U.S. Hekkel, M.S. Tivanov, A.M. Saad, Cu2ZnSnS4 thin films by sulfurization in melted sulfur. Mater. Lett. 220, 126–128 (2018)

    Article  Google Scholar 

  56. J. Tao, J. Liu, L. Chen, H. Cao, X. Meng, Y. Zhang, C. Zhang, L. Sun, P. Yang, J. Chu, 7.1% efficient co-electroplated Cu2ZnSnS4 thin film solar cells with sputtered CdS buffer layers. Green Chem. 18, 550–557 (2016)

    Article  Google Scholar 

  57. H. Ehira, K. Jimbo, H. Katagiri, Impact of Na-Addition Effect into CZTS Thin Film Solar Cells (Penang, Malaysia, 2017), p. 050004

    Google Scholar 

  58. O.P. Singh, Fast switching response of Na-doped CZTS photodetector from visible to NIR range. Sol Energy Mater. 157, 28–34 (2016)

    Article  Google Scholar 

  59. B. Liu, J. Guo, R. Hao, L. Wang, K. Gu, S. Sun, A. Aierken, Effect of Na doping on the performance and the band alignment of CZTS/CdS thin film solar cell. Sol. Energy 201, 219–226 (2020)

    Article  ADS  Google Scholar 

  60. W. Li, X. Yan, A.G. Aberle, S. Venkataraj, Effect of sodium diffusion on the properties of CIGS solar absorbers prepared using elemental Se in a two-step process. Sci. Rep. 9, 2637 (2019)

    Article  ADS  Google Scholar 

  61. K.S. Gour, Na incorporated improved properties of Cu2ZnSnS4 (CZTS) thin film by DC sputtering. Vacuum 154, 148–153 (2018)

    Article  ADS  Google Scholar 

  62. M. Marzougi, Effect of Na doping on structural and optical properties in Cu2ZnSnS4 thin films synthesized by thermal evaporation method. Thin Solid Films 672, 41–46 (2019)

    Article  ADS  Google Scholar 

  63. Hedstrljm J, Bodegbd M, Kylner A ZnO/CdS/Cu(In, Ga)Se, thin film solar cells with improved performance. Appl. Phys. Lett 62:6.

  64. H. Hou, H. Guan, L. Li, Synthesis of Cu2FeSnS4 thin films with stannite and wurtzite structure directly on glass substrates via the solvothermal method. J. Mater. Sci. Mater. Electron. 28, 7745–7748 (2017)

    Article  Google Scholar 

Download references

Acknowledgements

O.E.K. acknowledges the receipt of the OEA grant AF-15/20-01 from the Abdus Salam International Centre for Theoretical Physics, Trieste, Italy. All authors acknowledge the funding from Moroccan Ministry of Higher Education and Research and Centre National pour la Recherche Scientifique et Technique in the framework of PPR/37/2015 project, and from Romanian Ministry of Research, Innovation and Digitalization trough the Core Program PN19-03 (contract no. 21 N/ 08.02.2019) and PN-III-P4-ID-PCE-2020-0827 (Contract no. PCE74 09/02/2021) project.

Author information

Authors and Affiliations

  1. Laboratory of Materials and Subatomic Physics, Faculty of Sciences, Ibn Tofail University, Campus Universitaire, 14000, Kenitra, Morocco

    Outman El Khouja, Mohamed Yassine Zaki, Abdelali Talbi & Khalid Nouneh

  2. Laboratory of Multifunctional Materials and Structures, National Institute of Materials Physics, Atomistilor 405A, 077125, Magurele, Romania

    Outman El Khouja, Aurelian Catalin Galca, Mohamed Yassine Zaki, Elena Matei, Monica Enculescu & Lucian Pintilie

  3. Laboratory of Advanced Materials and Processes Engineering, Faculty of Sciences, Ibn Tofail University, Campus Universitaire, 14000, Kenitra, Morocco

    Outman El Khouja & Mohamed Ebn Touhami

  4. Key Laboratory of Electromagnetic Processing of Materials (Ministry of Education), Northeastern University, Shenyang, 110819, China

    Hassan Ahmoum

  5. LPCMIO, Materials Science Center, École Normale Supérieure, Mohammed V University, Rabat, Morocco

    M’hamed Taibi

Authors
  1. Outman El Khouja
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Aurelian Catalin Galca
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Mohamed Yassine Zaki
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Abdelali Talbi
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Hassan Ahmoum
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Khalid Nouneh
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Mohamed Ebn Touhami
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. M’hamed Taibi
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Elena Matei
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Monica Enculescu
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Lucian Pintilie
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Aurelian Catalin Galca or Khalid Nouneh.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

El Khouja, O., Galca, A.C., Zaki, M.Y. et al. Secondary phases and their influence on optical and electrical properties of electrodeposited Cu2FeSnS4 films. Appl. Phys. A 127, 887 (2021). https://doi.org/10.1007/s00339-021-05038-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s00339-021-05038-y

Keywords

Search

Navigation