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Effect of copper content and sulfurization process on optical, structural and electrical properties of ultrasonic spray pyrolysed Cu2ZnSnS4 thin films

Effect of copper content and sulfurization process on optical, structural and electrical properties of ultrasonic spray pyrolysed Cu2ZnSnS4 thin films
Effect of copper content and sulfurization process on optical, structural and electrical properties of ultrasonic spray pyrolysed Cu2ZnSnS4 thin films
This paper reports the effect of copper content and of the sulfurization process (using elemental sulfur vapor) on the growth, structure, elemental composition, and on the optical and electrical properties of Cu2ZnSnS4 (CZTS) thin films deposited on glass substrates using ultrasonic Spray Pyrolysis. For this purpose, a series of aqueous solutions consisting of copper (II) and tin (IV) chlorides, zinc (II) acetate and thiourea with different copper concentrations (x = Cu/(Zn + Sn) = 0.8, 1, 1.2 and 1.4 while Zn/Sn = 1) were prepared. X-ray diffraction, Raman spectroscopy, scanning electronic microscopy, atomic force microscopy, energy dispersive X-ray spectroscopy, ultraviolet–visible–near infrared absorbance spectroscopy and sheet resistance analyses were used to follow the evolution of the investigated properties. The results outlined a Kesterite type CZTS phase and a secondary copper sulfide (Cu2-xS) phase, and their ratio strongly depends on the copper salt concentration and heat-treatment atmosphere. No traces of secondary phases of zinc or tin sulfides are found while high purity CZTS was obtained with the post-sulfurized film at x = 1.2. It was found that the application of additional sulfurization enhances the grain growth to reach 300 nm in size and induces significant improvement of both CZTS crystallinity and electrical conductivity. The optical band gap ranges between 1.44 and 1.57 eV depending on the composition and the sulfur deficiency is strongly reduced leading to Cu-poorer and Zn-richer compounds, as compared to those annealed in nitrogen atmosphere.
0254-0584
96-104
Kermadi, S.
944e0919-8213-4c96-ac0f-bbe7e7fae051
Sali, S.
d8ad6bd1-e4b8-4221-b5fa-601d5286d6ff
Ait Ameur, F.
89dbf04c-7c7b-4d6b-92e5-ddc4e0b29a8b
Zougar, L.
f0d0b4c3-2ead-4a89-bae2-ff781a8f46f3
Boumaour, M.
e55a2da2-f4bb-4f40-b84b-9a9604a2c183
Toumiat, A.
b58ac0d9-07c2-45c3-b87a-9ffcc6b278ac
Melnik, N.N.
fb075503-e134-475f-8d46-c29dbf0ea3e6
Hewak, D.W.
87c80070-c101-4f7a-914f-4cc3131e3db0
Duta, A.
81a8dfc4-af6f-4c02-bbd1-7c540b717acb
Kermadi, S.
944e0919-8213-4c96-ac0f-bbe7e7fae051
Sali, S.
d8ad6bd1-e4b8-4221-b5fa-601d5286d6ff
Ait Ameur, F.
89dbf04c-7c7b-4d6b-92e5-ddc4e0b29a8b
Zougar, L.
f0d0b4c3-2ead-4a89-bae2-ff781a8f46f3
Boumaour, M.
e55a2da2-f4bb-4f40-b84b-9a9604a2c183
Toumiat, A.
b58ac0d9-07c2-45c3-b87a-9ffcc6b278ac
Melnik, N.N.
fb075503-e134-475f-8d46-c29dbf0ea3e6
Hewak, D.W.
87c80070-c101-4f7a-914f-4cc3131e3db0
Duta, A.
81a8dfc4-af6f-4c02-bbd1-7c540b717acb

Kermadi, S., Sali, S., Ait Ameur, F., Zougar, L., Boumaour, M., Toumiat, A., Melnik, N.N., Hewak, D.W. and Duta, A. (2016) Effect of copper content and sulfurization process on optical, structural and electrical properties of ultrasonic spray pyrolysed Cu2ZnSnS4 thin films. Materials Chemistry and Physics, 169, 96-104. (doi:10.1016/j.matchemphys.2015.11.035).

Record type: Article

Abstract

This paper reports the effect of copper content and of the sulfurization process (using elemental sulfur vapor) on the growth, structure, elemental composition, and on the optical and electrical properties of Cu2ZnSnS4 (CZTS) thin films deposited on glass substrates using ultrasonic Spray Pyrolysis. For this purpose, a series of aqueous solutions consisting of copper (II) and tin (IV) chlorides, zinc (II) acetate and thiourea with different copper concentrations (x = Cu/(Zn + Sn) = 0.8, 1, 1.2 and 1.4 while Zn/Sn = 1) were prepared. X-ray diffraction, Raman spectroscopy, scanning electronic microscopy, atomic force microscopy, energy dispersive X-ray spectroscopy, ultraviolet–visible–near infrared absorbance spectroscopy and sheet resistance analyses were used to follow the evolution of the investigated properties. The results outlined a Kesterite type CZTS phase and a secondary copper sulfide (Cu2-xS) phase, and their ratio strongly depends on the copper salt concentration and heat-treatment atmosphere. No traces of secondary phases of zinc or tin sulfides are found while high purity CZTS was obtained with the post-sulfurized film at x = 1.2. It was found that the application of additional sulfurization enhances the grain growth to reach 300 nm in size and induces significant improvement of both CZTS crystallinity and electrical conductivity. The optical band gap ranges between 1.44 and 1.57 eV depending on the composition and the sulfur deficiency is strongly reduced leading to Cu-poorer and Zn-richer compounds, as compared to those annealed in nitrogen atmosphere.

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More information

Accepted/In Press date: 21 November 2015
e-pub ahead of print date: 27 November 2015
Published date: 1 February 2016
Organisations: Optoelectronics Research Centre

Identifiers

Local EPrints ID: 390347
URI: http://eprints.soton.ac.uk/id/eprint/390347
ISSN: 0254-0584
PURE UUID: 6b229b63-458e-4ab4-9aac-18c7ac18532c
ORCID for D.W. Hewak: ORCID iD orcid.org/0000-0002-2093-5773

Catalogue record

Date deposited: 24 Mar 2016 12:08
Last modified: 17 Dec 2019 02:00

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