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Effect of Annealing Process on Structural and Optical Properties of Cu3SnS4 Thin Films Obtained by SILAR Technique

Year 2024, , 199 - 208, 01.03.2024
https://doi.org/10.21597/jist.1364232

Abstract

Cu3SnS4 thin films were deposited on glass substrates using successive ionic layer adsorption and reaction (SILAR) method at room temperature and annealed at different temperatures in the nitrogene atmosphere to investigate the effects of the post-deposition annealing process on the structural and optical properties of the films. Structural, surface morphological, and optical properties of films were analysed using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDAX), Raman spectroscopy, and optical absorption measurements. XRD results revealed that the films consisted of a tetragonal Cu3SnS4 phase before annealing, and increasing annealing temperature caused the improvement of crystal structure and the formation of Cu4SnS4, Cu2S and CuS secondary phases. SEM images showed that the films were composed of nanometer-sized randomly shaped particles. EDAX measurements revealed the existence of Cu, Sn and S elements and also showed that the amounts of Sn and S elements decreased with increasing annealing temperature. Raman spectra confirmed the formation of the Cu3SnS4 phase and secondary phases of Cu4SnS4, Cu2S and CuS at high annealing temperatures. From optical absorption measurements, it was determined that the films had direct transitions and the band gap energies decreased from 1.62 eV to 1.47 eV with increasing annealing temperature.

References

  • Aihara, N., Araki, H., Takeuchi, A., Jimbo, K., Katagiri, H. (2013). Fabrication of Cu2SnS3 thin films by sulfurization of evaporated Cu-Sn precursors for solar cells. Physica Status Solidi C, 10, 1086–1092.
  • Alias, M. F. A., Naji, I. S., Taher, B. Y., Al-Douri A. A. J. (2016). Synthesis Cu2SnS3 and Cu3SnS4, nanopowder and studying the composition, structural and morphological properties. Journal of Non-oxide Glasses, 8, 93–97.
  • Avellaneda, D., Paul, A., Shaji, S., Krishnan, B. (2022). Synthesis of Cu2SnS3, Cu3SnS4, and Cu4SnS4 thin films by sulfurization of SnS-Cu layers at a selected temperature and /or Cu layers thickness. Journal of Solid State Chemistry, 306, 122711.
  • Chalapathi, U., Kishore Kumar, Y. B., Uthanna, S., Sundara Raja, V. (2014). Investigations on Cu3SnS4 thin films prepared by spray pyrolysis. Thin Solid Films, 556, 61–67.
  • Chen, X., Wang, X., An, C., Liu, J, Qian, Y. (2003). Preparation and characterization of ternary Cu–Sn–E (E=S, Se) semiconductor nanocrystallites via a solvothermal element reaction route. Journal of Crystal Growth, 256, 368–376.
  • Chen, S. L., Tao, J., Shu, h. B., Tao, h. J., Tang, Y. X., Shen, Y. Z., Wang, T., Pan, l. (2017). Efficient electron transfer kuramite Cu3SnS4 nanosheet thin film towards platinum-free cathode in dye-sensitized solar cells. Journal of Power Sources, 341, 60–67.
  • Fernandes, P. A., Salome, P. M. P., Cunha, A. F. (2010). A study of ternary Cu2SnS3 and Cu3SnS4 thin films prepared by sulfurizing stacked metal precursors. Journal of Physics D: Applied Physics, 43, 215403.
  • Guan, H., Shen, H., Gao, C., He, X. (2013). Structural and optical properties of Cu2SnS3 and Cu3SnS4 thin films by successive ionic layer adsorption and reaction. Journal of Materials Science: Materials in Electronics, 24, 1490–1494.
  • Julien, C. M., Massot, M., Poinsignon, C. (2004). Lattice vibrations of manganese oxides Part I. Periodic structures. Spectrochimica Acta Part A, 60, 689–700.
  • Maheskumar, V., Selvaraju, T., Vidhya, B. (2018). Influence of solvent in solvothermal synthesis of Cu3SnS4: Morphology and band gap dependant electrocatalytic hydrogen evolution reaction and photocatalytic dye degradation. International Journal of Hydrogen Energy, 43, 22861–22873.
  • Nair, M. T. S., Lopez-Mata, C., GomezDaza, O., Nair, P. K. (2003). Copper tin sulfide semiconductor thin films produced by heating SnS–CuS layers deposited from chemical bath. Semiconductor Science and Technology, 18, 755–759.
  • Naji, I. S., Alias, M. F. A., Taher, B. Y., Al-Douri, A. A. J. (2018). Structural and electrical properties of Cu2SnS3 and Cu3SnS4 thin films prepared by CBD technique. Chalcogenide Letters, 15(2), 83–89. Pahtan, H. M., & Lokhande, C. D. (2004). Deposition of metal chalcogenide thin films by successive ionic layer adsorption and reaction (SILAR) method. Bulletin of Materials Science, 27(2), 85–111.
  • Reddy, V. R. M., Pallavolu M. R., Guddeti, P. R., Gedi, S., Reddy, K. K. Y. B., Pejjai, B., Kim, W. K., Kotte, T. R. R., Park, C. (2019). Review on Cu2SnS3, Cu3SnS4, and Cu4SnS4 thin films and their photovoltaic performance. Journal of Industrial and Engineering Chemistry, 76, 39–74.
  • Robles, V., Trigo, J. F., Guillen, C., Herrero, J. (2015). Copper tin sulfide (CTS) absorber thin films obtained by co-evaporation: Influence of the ratio Cu/Sn. Journal of Alloys and Compounds, 642, 40–44.
  • Su, Z., Sun, K., Han, Z., Liu, F., Lai, Y., Li, J., Liu, Y. (2012). Fabrication of ternary Cu–Sn–S sulfides by a modified successive ionic layer adsorption and reaction (SILAR) method. Journal of Materials Chemistry, 22, 16346–16352.
  • Thripuranthaka, M., Neha, S., Tilak, D., Swapnil, V., Satish, S. B., Musthafa, O. T., Mukul, K., Satishchandra, Ogale. (2018). A Combined Experimental and Computational Study of Gas Sensing by Cu3SnS4 Nanoparticulate Film: High Selectivity, Stability, and Reversibility for Room Temperature H2S Sensing. Advanced Materials Interfaces, 5, 1701492.
  • Tipcompor, N., Thongtem, S., Thongtem, T. (2015). Effect of microwave radiation on the morphology of tetragonal Cu3SnS4 synthesized by refluxing method. Superlattices and Microstructures, 85, 488–496.
  • Yang, Y., Ying, P., Wang, J., Liu, X., Du, Z., Chao, Y., Cui, J. (2017). Enhancing the thermoelectric performance of Cu3SnS4-based solid solutions through coordination of the Seebeck coefficient and carrier concentration. Journal of Materials Chemistry A, 5, 18808–18815.
  • Wang, J., Bo, T., Shao, B., Zhang, Y., Jia, L., Tan, X., Zhou, W., Yu, Z. (2021). Effect of S vacancy in Cu3SnS4 on high selectivity and activity of photocatalytic CO2 reduction. Applied Catalysis B: Environmental, 297, 120498.

Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal ve Optik Özellikleri Üzerine Etkisi

Year 2024, , 199 - 208, 01.03.2024
https://doi.org/10.21597/jist.1364232

Abstract

Cu3SnS4 ince filmler, sıralı iyonik tabaka adsorpsiyonu ve reaksiyonu (SILAR) tekniği kullanılarak cam altlıklar üzerine oda sıcaklığında büyütüldü ve azot atmosferinde farklı sıcaklıklarda tavlanarak büyütme sonrası tavlama işleminin filmlerin yapısal ve optik özellikleri üzerindeki etkileri incelendi. Filmlerin yapısal, yüzey morfolojik ve optik özellikleri X-ışını kırınımı (XRD), taramalı elektron mikroskobu (SEM), enerji dağılımlı X-ışını analizi (EDAX), Raman spektroskopisi ve optik soğurma ölçümleri kullanılarak incelendi. XRD sonuçları, filmlerin tavlama öncesinde tetragonal Cu3SnS4 fazından oluştuğunu, tavlama sıcaklığının arttırılmasının kristal yapının iyileşmesine ve Cu4SnS4, Cu2S ve CuS ikincil fazlarının oluşmasına neden olduğunu ortaya çıkardı. SEM görüntüleri, filmlerin nanometre boyutunda rastgele şekilli parçacıklardan oluştuğunu gösterdi. EDAX ölçümleri Cu, Sn ve S elementlerinin varlığını ve ayrıca tavlama sıcaklığının artmasıyla Sn ve S elementlerinin miktarlarının azaldığını ortaya koydu. Raman spektrumları Cu3SnS4 fazının ve yüksek tavlama sıcaklıklarında Cu4SnS4, Cu2S ve CuS ikincil fazlarının oluşumunu doğruladı. Optik soğurma ölçümlerinden filmlerin direkt geçişlere sahip olduğu ve artan tavlama sıcaklığıyla yasak enerji aralığı değerinin 1.62 eV'dan 1.47 eV'a azaldığı belirlendi.

References

  • Aihara, N., Araki, H., Takeuchi, A., Jimbo, K., Katagiri, H. (2013). Fabrication of Cu2SnS3 thin films by sulfurization of evaporated Cu-Sn precursors for solar cells. Physica Status Solidi C, 10, 1086–1092.
  • Alias, M. F. A., Naji, I. S., Taher, B. Y., Al-Douri A. A. J. (2016). Synthesis Cu2SnS3 and Cu3SnS4, nanopowder and studying the composition, structural and morphological properties. Journal of Non-oxide Glasses, 8, 93–97.
  • Avellaneda, D., Paul, A., Shaji, S., Krishnan, B. (2022). Synthesis of Cu2SnS3, Cu3SnS4, and Cu4SnS4 thin films by sulfurization of SnS-Cu layers at a selected temperature and /or Cu layers thickness. Journal of Solid State Chemistry, 306, 122711.
  • Chalapathi, U., Kishore Kumar, Y. B., Uthanna, S., Sundara Raja, V. (2014). Investigations on Cu3SnS4 thin films prepared by spray pyrolysis. Thin Solid Films, 556, 61–67.
  • Chen, X., Wang, X., An, C., Liu, J, Qian, Y. (2003). Preparation and characterization of ternary Cu–Sn–E (E=S, Se) semiconductor nanocrystallites via a solvothermal element reaction route. Journal of Crystal Growth, 256, 368–376.
  • Chen, S. L., Tao, J., Shu, h. B., Tao, h. J., Tang, Y. X., Shen, Y. Z., Wang, T., Pan, l. (2017). Efficient electron transfer kuramite Cu3SnS4 nanosheet thin film towards platinum-free cathode in dye-sensitized solar cells. Journal of Power Sources, 341, 60–67.
  • Fernandes, P. A., Salome, P. M. P., Cunha, A. F. (2010). A study of ternary Cu2SnS3 and Cu3SnS4 thin films prepared by sulfurizing stacked metal precursors. Journal of Physics D: Applied Physics, 43, 215403.
  • Guan, H., Shen, H., Gao, C., He, X. (2013). Structural and optical properties of Cu2SnS3 and Cu3SnS4 thin films by successive ionic layer adsorption and reaction. Journal of Materials Science: Materials in Electronics, 24, 1490–1494.
  • Julien, C. M., Massot, M., Poinsignon, C. (2004). Lattice vibrations of manganese oxides Part I. Periodic structures. Spectrochimica Acta Part A, 60, 689–700.
  • Maheskumar, V., Selvaraju, T., Vidhya, B. (2018). Influence of solvent in solvothermal synthesis of Cu3SnS4: Morphology and band gap dependant electrocatalytic hydrogen evolution reaction and photocatalytic dye degradation. International Journal of Hydrogen Energy, 43, 22861–22873.
  • Nair, M. T. S., Lopez-Mata, C., GomezDaza, O., Nair, P. K. (2003). Copper tin sulfide semiconductor thin films produced by heating SnS–CuS layers deposited from chemical bath. Semiconductor Science and Technology, 18, 755–759.
  • Naji, I. S., Alias, M. F. A., Taher, B. Y., Al-Douri, A. A. J. (2018). Structural and electrical properties of Cu2SnS3 and Cu3SnS4 thin films prepared by CBD technique. Chalcogenide Letters, 15(2), 83–89. Pahtan, H. M., & Lokhande, C. D. (2004). Deposition of metal chalcogenide thin films by successive ionic layer adsorption and reaction (SILAR) method. Bulletin of Materials Science, 27(2), 85–111.
  • Reddy, V. R. M., Pallavolu M. R., Guddeti, P. R., Gedi, S., Reddy, K. K. Y. B., Pejjai, B., Kim, W. K., Kotte, T. R. R., Park, C. (2019). Review on Cu2SnS3, Cu3SnS4, and Cu4SnS4 thin films and their photovoltaic performance. Journal of Industrial and Engineering Chemistry, 76, 39–74.
  • Robles, V., Trigo, J. F., Guillen, C., Herrero, J. (2015). Copper tin sulfide (CTS) absorber thin films obtained by co-evaporation: Influence of the ratio Cu/Sn. Journal of Alloys and Compounds, 642, 40–44.
  • Su, Z., Sun, K., Han, Z., Liu, F., Lai, Y., Li, J., Liu, Y. (2012). Fabrication of ternary Cu–Sn–S sulfides by a modified successive ionic layer adsorption and reaction (SILAR) method. Journal of Materials Chemistry, 22, 16346–16352.
  • Thripuranthaka, M., Neha, S., Tilak, D., Swapnil, V., Satish, S. B., Musthafa, O. T., Mukul, K., Satishchandra, Ogale. (2018). A Combined Experimental and Computational Study of Gas Sensing by Cu3SnS4 Nanoparticulate Film: High Selectivity, Stability, and Reversibility for Room Temperature H2S Sensing. Advanced Materials Interfaces, 5, 1701492.
  • Tipcompor, N., Thongtem, S., Thongtem, T. (2015). Effect of microwave radiation on the morphology of tetragonal Cu3SnS4 synthesized by refluxing method. Superlattices and Microstructures, 85, 488–496.
  • Yang, Y., Ying, P., Wang, J., Liu, X., Du, Z., Chao, Y., Cui, J. (2017). Enhancing the thermoelectric performance of Cu3SnS4-based solid solutions through coordination of the Seebeck coefficient and carrier concentration. Journal of Materials Chemistry A, 5, 18808–18815.
  • Wang, J., Bo, T., Shao, B., Zhang, Y., Jia, L., Tan, X., Zhou, W., Yu, Z. (2021). Effect of S vacancy in Cu3SnS4 on high selectivity and activity of photocatalytic CO2 reduction. Applied Catalysis B: Environmental, 297, 120498.
There are 19 citations in total.

Details

Primary Language Turkish
Subjects Structural Properties of Condensed Matter, Surface Properties of Condensed Matter
Journal Section Fizik / Physics
Authors

Aykut Astam 0000-0002-4321-3626

Cemal Çetin This is me 0000-0003-0293-0095

Early Pub Date February 20, 2024
Publication Date March 1, 2024
Submission Date September 22, 2023
Acceptance Date October 13, 2023
Published in Issue Year 2024

Cite

APA Astam, A., & Çetin, C. (2024). Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal ve Optik Özellikleri Üzerine Etkisi. Journal of the Institute of Science and Technology, 14(1), 199-208. https://doi.org/10.21597/jist.1364232
AMA Astam A, Çetin C. Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal ve Optik Özellikleri Üzerine Etkisi. Iğdır Üniv. Fen Bil Enst. Der. March 2024;14(1):199-208. doi:10.21597/jist.1364232
Chicago Astam, Aykut, and Cemal Çetin. “Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal Ve Optik Özellikleri Üzerine Etkisi”. Journal of the Institute of Science and Technology 14, no. 1 (March 2024): 199-208. https://doi.org/10.21597/jist.1364232.
EndNote Astam A, Çetin C (March 1, 2024) Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal ve Optik Özellikleri Üzerine Etkisi. Journal of the Institute of Science and Technology 14 1 199–208.
IEEE A. Astam and C. Çetin, “Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal ve Optik Özellikleri Üzerine Etkisi”, Iğdır Üniv. Fen Bil Enst. Der., vol. 14, no. 1, pp. 199–208, 2024, doi: 10.21597/jist.1364232.
ISNAD Astam, Aykut - Çetin, Cemal. “Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal Ve Optik Özellikleri Üzerine Etkisi”. Journal of the Institute of Science and Technology 14/1 (March 2024), 199-208. https://doi.org/10.21597/jist.1364232.
JAMA Astam A, Çetin C. Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal ve Optik Özellikleri Üzerine Etkisi. Iğdır Üniv. Fen Bil Enst. Der. 2024;14:199–208.
MLA Astam, Aykut and Cemal Çetin. “Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal Ve Optik Özellikleri Üzerine Etkisi”. Journal of the Institute of Science and Technology, vol. 14, no. 1, 2024, pp. 199-08, doi:10.21597/jist.1364232.
Vancouver Astam A, Çetin C. Tavlama İşleminin SILAR Tekniğiyle Elde Edilen Cu3SnS4 İnce Filmlerin Yapısal ve Optik Özellikleri Üzerine Etkisi. Iğdır Üniv. Fen Bil Enst. Der. 2024;14(1):199-208.