SEMICONDUCTOR PHYSICS

Spray pyrolysis of tin selenide thin-film semiconductors:the effect of selenium concentration on the properties of the thin films

M. R. Fadavieslam and M. M. Bagheri-Mohagheghi

+ Author Affiliations

 Corresponding author: M. R. Fadavieslam, Email:m.r.fadavieslam@du.ac.ir

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Abstract: Thin films of tin selenide (SnxSey) with an atomic ratio of $r=\left[\frac{y}{x}\right]=0.5$, 1 and 1.5 were prepared on a glass substrate at T=470℃ using a spray pyrolysis technique. The initial materials for the preparation of the thin films were an alcoholic solution consisting of tin chloride (SnCl4· 5H2O) and selenide acide (H2SeO3). The prepared thin films were characterized by X-ray diffraction (XRD), scanning electron microscopy, scanning tunneling microscopy, scanning helium ion microscopy, and UV-vis spectroscopy. The photoconductivity and thermoelectric effects of the SnxSey thin films were then studied. The SnxSey thin films had a polycrystalline structure with an almost uniform surface and cluster type growth. The increasing atomic ratio of r in the films, the optical gap, photosensitivity and Seebeck coefficient were changed from 1.6 to 1.37 eV, 0.01 to 0.31 and -26.2 to -42.7 mV/K (at T=350 K), respectively. In addition, the XRD patterns indicated intensity peaks in r=1 that corresponded to the increase in the SnSe and SnSe2 phases.

Key words: thin filmtin selenidespray pyrolysisoptical band gap



[1]
Pejova B, Grozdanov I. Chemical synthesis, structural and optical properties of quantum sized semiconducting tin (Ⅱ) selenide in thin film form. Thin Solid Films, 2007, 515:5203 doi: 10.1016/j.tsf.2006.11.016
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[3]
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[4]
Popescu M A. Non-crystalline chalcogenides, solid state science and technology library. Vol. 8. Kluwer Academic Publishers, 2000
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Ohlidal I, Franta D, Frumar M, et al. Influence of composition, exposure and thermal annealing of optical properties of As-S chalcogenide thin films. Adv Mater, 2004, 6:139 doi: 10.1080/00150190802381985
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Petkov P, Vassilev V, Petkova T, et al. Optical properties of ternary chalcogenide thin films with SnTe. Adv Mater, 2005, 7:1965 http://citeseerx.ist.psu.edu/viewdoc/download?doi=10.1.1.539.1268&rep=rep1&type=pdf
[8]
Platikanova D, Arsova D, Skordeva E, et al. Photo-and thermo-induced changes in As2S1.5Se1.5Gex. J Optoelectron Adv Mater, 2004, 7:337 https://es.scribd.com/document/62391273/Datasheet
[9]
Hegedus J, Kohary K, Kugler S. Light-induced volume changes in glassy selnium Ⅱ. Kinetics of volume expansion. J Optoelectron Adv Mater, 2004, 7:2231 https://hungary.pure.elsevier.com/en/publications/light-induced-volume-changes-in-glassy-selenium-ii-kinetics-of-vo
[10]
Boolchand P. Intermediate phases, reversibility windows, stress-free and non-aging networks, and strong liquids. Chalcogenide Lett, 2006, 3:29 http://www.wenkuxiazai.com/doc/3a2e9377a417866fb84a8e03.html
[11]
Lezal D, Zavadil J, Prochazka M. Sulfide, selenide and telluride glassy systems for optoelectronic applications. J Optoelectron Adv Mater, 2005, 7:2281 http://citeseerx.ist.psu.edu/viewdoc/bookmark?doi=10.1.1.519.7458&site=connotea
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[13]
Trunov M L. Photo-induced plasticity in amorphous chalcogenides:an overview of mechanisms and applications. J Optoelectron Adv Mater, 2004, 7:2235 http://citeseerx.ist.psu.edu/viewdoc/summary?doi=10.1.1.517.5063
[14]
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Bicer M, Sisman I. Electrodeposition and growth mechanism of SnSe thin films. Appl Surf Sci, 2011, 257:2944 doi: 10.1016/j.apsusc.2010.10.096
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Boscher N D, Carmalt C J, Palgrave R G, et al. Atmospheric pressure chemical vapour deposition of SnSe and SnSe2 thin films on glass. Thin Solid Films, 2008, 516:4750 doi: 10.1016/j.tsf.2007.08.100
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Indirajith R, Srinivasan T P, Ramamurthi K, et al. Synthesis, deposition and characterization of tin selenide thin films by thermal evaporation technique. Current Appl Phys, 2010, 10:1402 doi: 10.1016/j.cap.2010.05.002
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Amalrajb L, Jayachandranc M, Sanjeeviraja C. Preparation and characterization of tin diselenide thin film by spray pyrolysis technique. Materials Research Bulletin, 2004, 39:2193 doi: 10.1016/j.materresbull.2004.08.006
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Padiyan D P, Marikani A, Murali K R. Electrical and photoelectrical properties of vacuum deposited SnSe thin films. Cryst Res Technol, 2000, 35:949 doi: 10.1002/(ISSN)1521-4079
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Chandra G H, Kumar J N, Rao N M, et al. Preparation and characterization of flash evaporated tin selenide thin films. J Cryst Growth, 2007, 306:68 doi: 10.1016/j.jcrysgro.2007.05.004
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Singh J P, Bedi R K. Tin selenide films grown by hot wall epitaxy. J Appl Phys, 1990, 68:2776 doi: 10.1063/1.346455
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John K J, Pradeep B, Mathai E. Tin selenide (SnSe) thin films prepared by reactive evaporation. J Mater Sci, 1994, 29:1994 doi: 10.1007/BF00368929
[25]
Zainal Z, Ali A J, Kassim A, et al. Electrodeposition of tin selenide thin film semiconductor:effect of the electrolytes concentration on the film properties. Solar Energy Materials & Solar Cells, 2003, 79:125
[26]
Qiao Z, Shang W, Wang C. Fabrication of Sn-Se compounds on a gold electrode by electrochemical atomic layer epitaxy. J Electroanal Chem, 2005, 576:171 doi: 10.1016/j.jelechem.2004.10.015
[27]
Bagheri-Mohagheghi M M, Shokooh-Saremi M. Investigations on the physical properties of the SnO2-ZnO transparent conducting binary-binary system deposited by spray pyrolysis technique. Thin Solid Films, 2003, 441:238 doi: 10.1016/S0040-6090(03)00948-9
[28]
Sánchez-González J, Diaz-Parralejo A, Ortiz A L, et al. Determination of optical properties in nanostructured thin films using the Swanepoel method. Appl Surf Sci, 2006, 252:6013 doi: 10.1016/j.apsusc.2005.11.009
[29]
Bindu K, Nair P K. Semiconducting tin selenide thin films prepared by heating Se-Sn layers. Semicond Sci Technol, 2004, 19:1348 doi: 10.1088/0268-1242/19/12/003
[30]
Nolas G S, Sharp J, Goldsmid H J. Thermoelectrics:basic principles and new materials developments. Berlin:Springer, 2001
[31]
Li L, Fang L, Chen X M, et al. Influence of oxygen argon ratio on the structural, electrical, optical and thermoelectrical properties of Al-doped ZnO thin films. Physica E, 2008, 41:169 doi: 10.1016/j.physe.2008.07.001
Fig. 1.  The basic set-up for spray deposition.

Fig. 2.  The basic set-up for thermoelectric power measurement.

Fig. 3.  The X-ray diffraction patterns of Sn$_{x}$Se$_{y}$ thin films prepared at (a) $r =$ 0.5, (b) $r =$ 1 and (c) $r =$ 1.5.

Fig. 4.  SEM image of an Sn$_{x}$Se$_{y}$ thin film prepared at $r =$ 0.5.

Fig. 5.  (a) 3D and (b) 2D STM images of an Sn$_{x}$Se$_{y}$ thin film prepared at $r =$ 0.5.

Fig. 6.  SHIM image of an Sn$_{x}$Se$_{y}$ thin film prepared at $r = 0.5$.

Fig. 7.  Variation in (a) absorbance, and (b) transmittance versus the wavelength of the Sn$_{x}$Se$_{y}$ thin films with various ratios of [$y/x$].

Fig. 8.  Plots of ($\alpha h\nu )$$^{2}$ versus $h \nu$ for the Sn$_{x}$Se$_{y}$ thin films with various ratios of [$y/x$].

Fig. 9.  Variations in $S=(R_1$$R_{\rm d}$)/$R_{\rm d}$ versus time for the Sn$_{x}$Se$_{y}$ thin films with various ratios of [$y/x$].

Fig. 10.  The variation in the photosensitivity and electrical resistivity of the Sn$_{x}$Se$_{y}$ thin films with various ratios of [$y/x$].

Fig. 11.  The variation in the thermoelectric–EMF versus the temperature difference of the Sn$_{x}$Se$_{y}$ thin films with various ratios of [$y/x$].

Fig. 12.  The variation in the resistance versus the temperature of the Sn$_{x}$Se$_{y}$ thin films prepared at (a) $r =$ 0.5, (b) $r =$ 1 and (c) $r =$ 1.5.

Table 1.   The spray deposition parameters for the preparation of Sn$_{x}$Se$_{y}$ films.

Table 2.   The optical, photoconductivity and thermo-power measurement results of the Sn$_{x}$Se$_{y}$ thin films.

[1]
Pejova B, Grozdanov I. Chemical synthesis, structural and optical properties of quantum sized semiconducting tin (Ⅱ) selenide in thin film form. Thin Solid Films, 2007, 515:5203 doi: 10.1016/j.tsf.2006.11.016
[2]
Singh J, Shimakawa K. Advances in amorphous semiconductors. In:Sharma D D, Cotliar G, Tokura Y, ed. Advances in Condensed Matter Series. Vol. 5. Taylor and Francis, 2003 doi: 10.1088/0268-1242/17/4/310
[3]
Kolobov A V. Photo-induced metastability in amorph semic. Wiley-VCH, 2003 http://www.wiley.com/WileyCDA/WileyTitle/productCd-3527608664.html
[4]
Popescu M A. Non-crystalline chalcogenides, solid state science and technology library. Vol. 8. Kluwer Academic Publishers, 2000
[5]
Semiconducting chalcogenide glass I, glass formation, structure, and stimulated transformations in chalcogenide glasses. In: Willardson R K, Weber E R, ed. Semiconductors and Semimetals, Treatise, vol. 78, 2004
[6]
Ohlidal I, Franta D, Frumar M, et al. Influence of composition, exposure and thermal annealing of optical properties of As-S chalcogenide thin films. Adv Mater, 2004, 6:139 doi: 10.1080/00150190802381985
[7]
Petkov P, Vassilev V, Petkova T, et al. Optical properties of ternary chalcogenide thin films with SnTe. Adv Mater, 2005, 7:1965 http://citeseerx.ist.psu.edu/viewdoc/download?doi=10.1.1.539.1268&rep=rep1&type=pdf
[8]
Platikanova D, Arsova D, Skordeva E, et al. Photo-and thermo-induced changes in As2S1.5Se1.5Gex. J Optoelectron Adv Mater, 2004, 7:337 https://es.scribd.com/document/62391273/Datasheet
[9]
Hegedus J, Kohary K, Kugler S. Light-induced volume changes in glassy selnium Ⅱ. Kinetics of volume expansion. J Optoelectron Adv Mater, 2004, 7:2231 https://hungary.pure.elsevier.com/en/publications/light-induced-volume-changes-in-glassy-selenium-ii-kinetics-of-vo
[10]
Boolchand P. Intermediate phases, reversibility windows, stress-free and non-aging networks, and strong liquids. Chalcogenide Lett, 2006, 3:29 http://www.wenkuxiazai.com/doc/3a2e9377a417866fb84a8e03.html
[11]
Lezal D, Zavadil J, Prochazka M. Sulfide, selenide and telluride glassy systems for optoelectronic applications. J Optoelectron Adv Mater, 2005, 7:2281 http://citeseerx.ist.psu.edu/viewdoc/bookmark?doi=10.1.1.519.7458&site=connotea
[12]
Strand D. Ovonics:from science to products. J Optoelectron Adv Mater, 2005, 7:1679 http://citeseerx.ist.psu.edu/viewdoc/summary?doi=10.1.1.497.4884
[13]
Trunov M L. Photo-induced plasticity in amorphous chalcogenides:an overview of mechanisms and applications. J Optoelectron Adv Mater, 2004, 7:2235 http://citeseerx.ist.psu.edu/viewdoc/summary?doi=10.1.1.517.5063
[14]
Savastru D, Miclos S, Savastru R. Focusing system based on chalcogenide microlenses attached to optical fibers. J Optoelectron Adv Mater, 2004, 7:1909 doi: 10.3103%2FS1060992X08040024.pdf
[15]
Andriesh A. Chalcogenide glasses as multifunctional photonic materials, chalcogenide glasses as multifunctional photonic materials. J Optoelectron Adv Mater, 2006, 7:2931 http://citeseerx.ist.psu.edu/viewdoc/summary?doi=10.1.1.547.6266
[16]
Bicer M, Sisman I. Electrodeposition and growth mechanism of SnSe thin films. Appl Surf Sci, 2011, 257:2944 doi: 10.1016/j.apsusc.2010.10.096
[17]
Boscher N D, Carmalt C J, Palgrave R G, et al. Atmospheric pressure chemical vapour deposition of SnSe and SnSe2 thin films on glass. Thin Solid Films, 2008, 516:4750 doi: 10.1016/j.tsf.2007.08.100
[18]
Subramanian B, Sanjeeviraja C, Jayachandran M. Brush plating of tin (Ⅱ) selenide thin films. J Cryst Growth, 2002, 234:421 doi: 10.1016/S0022-0248(01)01697-9
[19]
Indirajith R, Srinivasan T P, Ramamurthi K, et al. Synthesis, deposition and characterization of tin selenide thin films by thermal evaporation technique. Current Appl Phys, 2010, 10:1402 doi: 10.1016/j.cap.2010.05.002
[20]
Amalrajb L, Jayachandranc M, Sanjeeviraja C. Preparation and characterization of tin diselenide thin film by spray pyrolysis technique. Materials Research Bulletin, 2004, 39:2193 doi: 10.1016/j.materresbull.2004.08.006
[21]
Padiyan D P, Marikani A, Murali K R. Electrical and photoelectrical properties of vacuum deposited SnSe thin films. Cryst Res Technol, 2000, 35:949 doi: 10.1002/(ISSN)1521-4079
[22]
Chandra G H, Kumar J N, Rao N M, et al. Preparation and characterization of flash evaporated tin selenide thin films. J Cryst Growth, 2007, 306:68 doi: 10.1016/j.jcrysgro.2007.05.004
[23]
Singh J P, Bedi R K. Tin selenide films grown by hot wall epitaxy. J Appl Phys, 1990, 68:2776 doi: 10.1063/1.346455
[24]
John K J, Pradeep B, Mathai E. Tin selenide (SnSe) thin films prepared by reactive evaporation. J Mater Sci, 1994, 29:1994 doi: 10.1007/BF00368929
[25]
Zainal Z, Ali A J, Kassim A, et al. Electrodeposition of tin selenide thin film semiconductor:effect of the electrolytes concentration on the film properties. Solar Energy Materials & Solar Cells, 2003, 79:125
[26]
Qiao Z, Shang W, Wang C. Fabrication of Sn-Se compounds on a gold electrode by electrochemical atomic layer epitaxy. J Electroanal Chem, 2005, 576:171 doi: 10.1016/j.jelechem.2004.10.015
[27]
Bagheri-Mohagheghi M M, Shokooh-Saremi M. Investigations on the physical properties of the SnO2-ZnO transparent conducting binary-binary system deposited by spray pyrolysis technique. Thin Solid Films, 2003, 441:238 doi: 10.1016/S0040-6090(03)00948-9
[28]
Sánchez-González J, Diaz-Parralejo A, Ortiz A L, et al. Determination of optical properties in nanostructured thin films using the Swanepoel method. Appl Surf Sci, 2006, 252:6013 doi: 10.1016/j.apsusc.2005.11.009
[29]
Bindu K, Nair P K. Semiconducting tin selenide thin films prepared by heating Se-Sn layers. Semicond Sci Technol, 2004, 19:1348 doi: 10.1088/0268-1242/19/12/003
[30]
Nolas G S, Sharp J, Goldsmid H J. Thermoelectrics:basic principles and new materials developments. Berlin:Springer, 2001
[31]
Li L, Fang L, Chen X M, et al. Influence of oxygen argon ratio on the structural, electrical, optical and thermoelectrical properties of Al-doped ZnO thin films. Physica E, 2008, 41:169 doi: 10.1016/j.physe.2008.07.001
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    Received: 03 December 2012 Revised: Online: Published: 01 August 2013

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      M. R. Fadavieslam, M. M. Bagheri-Mohagheghi. Spray pyrolysis of tin selenide thin-film semiconductors:the effect of selenium concentration on the properties of the thin films[J]. Journal of Semiconductors, 2013, 34(8): 082001. doi: 10.1088/1674-4926/34/8/082001 M. R. Fadavieslam, M. M. Bagheri-Mohagheghi. Spray pyrolysis of tin selenide thin-film semiconductors:the effect of selenium concentration on the properties of the thin films[J]. J. Semicond., 2013, 34(8): 082001. doi: 10.1088/1674-4926/34/8/082001.Export: BibTex EndNote
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      M. R. Fadavieslam, M. M. Bagheri-Mohagheghi. Spray pyrolysis of tin selenide thin-film semiconductors:the effect of selenium concentration on the properties of the thin films[J]. Journal of Semiconductors, 2013, 34(8): 082001. doi: 10.1088/1674-4926/34/8/082001

      M. R. Fadavieslam, M. M. Bagheri-Mohagheghi. Spray pyrolysis of tin selenide thin-film semiconductors:the effect of selenium concentration on the properties of the thin films[J]. J. Semicond., 2013, 34(8): 082001. doi: 10.1088/1674-4926/34/8/082001.
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      Spray pyrolysis of tin selenide thin-film semiconductors:the effect of selenium concentration on the properties of the thin films

      doi: 10.1088/1674-4926/34/8/082001
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      • Corresponding author: M. R. Fadavieslam, Email:m.r.fadavieslam@du.ac.ir
      • Received Date: 2012-12-03
      • Published Date: 2013-08-01

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