Skip to main content
SpringerLink
Log in

PbS x Se1−x thin films from the thermal decomposition of lead(II) dodecylxanthate and bis(N,N-diethyl-N′-naphthoylselenoureato)lead(II) precursors

  • Electronic materials
  • Published:
Journal of Materials Science Aims and scope Submit manuscript

Abstract

Thin films of PbS x Se(1−x) (0 ≤ x ≤ 1) have been deposited by spin coating of bis(dodecylxanthato)lead(II) (1) and/or bis(N,N-diethyl-N′-naphthoylselenoureato)lead(II) (2) complexes onto glass substrates followed by heating. The mole fraction of the selenium precursor in the coating mixture was varied from 0 to 1 by mixing the S and Se precursors. The as-prepared thin films were then heated at temperatures ranging from 250 to 400 °C. Powder X-ray diffraction showed all films were of the halite structure with preferred orientation along (200) plane. The PbS films showed a closely packed network of nanorods, each comprised of smaller nanoparticles. The nanorods were about 500 nm in length and 25 nm in width; the adhered particles had ca. 30 nm sides. The PbSe nanoparticles were also cubic. The alloys showed an intermediate morphology between the rods and cubes depending on the precursor ratio in the coating mixture. The band gaps estimated from Tauc plots for the films heated at 250 °C for 30 min were 1.03 and 0.79 eV for PbS and PbSe, respectively. The alloyed PbS x Se(1−x) thin films exhibited band gaps between those of PbS and PbSe. The band gaps and lattice parameters of the alloys varied in a Vegardian manner and could be closely correlated with the composition of the precursor mixture.

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

Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
Figure 6
Figure 7
Figure 8
Fig. 9

Similar content being viewed by others

References

  1. Lewis EA, McNaughter PD, Yin Z, Chen Y, Brent R, Saah SA, Raftery J, Awudza JAM, Malik MA, O’Brien P, Haigh S (2015) In situ synthesis of PbS nanocrystals in polymer thin films from lead(II) xanthate and dithiocarbamate complexes: evidence for size and morphology control. Chem Mater 27:2127–2136. https://doi.org/10.1021/cm504765z

    Article  Google Scholar 

  2. Dowland S, Lutz T, Ward A, King SP, Sudlow A, Hill MS, Molloy KC, Haque SA (2011) Direct growth of metal sulfide nanoparticle networks in solid-state polymer films for hybrid inorganic–organic solar cells. Adv Mater 23:2739–2744

    Article  Google Scholar 

  3. Brent JR, McNaughter PD, O’Brien P (2017) Precursor determined lateral size control of monolayer MoS2 nanosheets from a series of alkylammonium thiomolybdates: a reversal of trend between growth media. Chem Commun 53:6428–6431. https://doi.org/10.1039/c7cc01641g

    Article  Google Scholar 

  4. McNaughter PD, Bear JC, Mayes AG, Parkin IP, O’Brien P (2017) The in situ synthesis of PbS nanocrystals from lead(II) n-octylxanthate within a 1,3-diisopropenylbenzene–bisphenol: a dimethacrylate sulfur copolymer. R Soc Open Sci 4:170383. https://doi.org/10.1098/rsos.170383

    Article  Google Scholar 

  5. Al-Shakban RM, Matthews PD, Deogratias G, McNaughter PD, Raftery J, Vitorica-Yrezabal I, Mubofu EI, O’Brien P (2017) Novel xanthate complexes for the size-controlled synthesis of copper sulfide nanorods. Inorg Chem 56(15):9247–9254. https://doi.org/10.1021/acs.inorgchem.7b01288

    Article  Google Scholar 

  6. Akhtar J, Malik MA, O’Brien P, Wijayantha KGU, Dharmadasa R, Samantha JOH, Graham MG, Spencer BF, Stubbs SK, Flavell WR, Binks DJ, Sirotti F, Kazzie ME, Silly M (2010) A greener route to photoelectrochemically active PbS nanoparticles. J Mater Chem 20:2336–2344

    Article  Google Scholar 

  7. Zhao N, Osedach TP, Chang L-Y, Geyer SM, Wanger D, Binda MT, Arango AC, Bawendi MG, Bulovic V (2010) Colloidal PbS quantum dot solar cells with high fill factor. J Am Chem Soc 102:1–9

    Google Scholar 

  8. Lin S, Zhang X, Shi X, Wei J, Lu D, Zhang Y, Kou H, Wang N (2011) Nanoscale semiconductor Pb1−x Sn x Se (x = 0.2) thin films synthesized by electrochemical atomic layer deposition. Appl Surf Sci 257:5803–5807

    Article  Google Scholar 

  9. Ma W, Luther JM, Zheng H, Wu Y, Alivisatos AP (2009) Photovoltaic devices employing ternary PbS x Se1−x nanocrystals. Nano Lett 9:1699–1703

    Article  Google Scholar 

  10. Akhtar J, Afzaal M, Banski M, Podhorodecki A, Syperek M, Misiewicz J, Bangert U, Hardman SJO, Graham DM, Flavell WR, Binks DJ, Gardonio S, O’Brien P (2011) Controlled synthesis of tuned bandgap nanodimensional alloys of PbS x Se1− x . J Am Chem Soc 133:5602–5609

    Article  Google Scholar 

  11. Nam M, Kim S, Kang M, Kim S, Lee K (2012) Efficiency enhancement in organic solar cells by configuring hybrid interfaces with narrow bandgap PbSSe nanocrystals. Org Electron 13:1546–1552

    Article  Google Scholar 

  12. Matthews PD, McNaughter PD, Lewis DJ, O’Brien P (2017) Shining a light on transition metal chalcogenides for sustainable photovoltaics. Chem Sci 8:4177–4187. https://doi.org/10.1039/c7sc00642j

    Article  Google Scholar 

  13. Lifshitz E, Brumer M, Kigel A, Sashchiuk A, Bashouti M, Sirota M, Galun E, Burshtein Z, Quang AQL, Ledoux-Rak I, Zyss J (2006) Air-stable PbSe/PbS and PbSe/PbSe x S1−x core–shell nanocrystal quantum dots and their applications. J Phys Chem B 110:25356–25365

    Article  Google Scholar 

  14. Shao G, Chen G, Zuo J, Gong M, Yang Q (2014) Organometallic synthesis, structure determination, shape evolution, and formation mechanism of hexapod-like ternary PbSe x S1–x nanostructures with tunable compositions. Langmuir 30:7811–7822

    Article  Google Scholar 

  15. Onicha AC, Petchsang N, Kosel TH, Kuno M (2012) Controlled synthesis of compositionally tunable ternary PbSe x S1–x as well as binary PbSe and PbS nanowires. ACS Nano 6:2833–2843

    Article  Google Scholar 

  16. Midgett AG, Luther JM, Stewart JT, Smith DK, Padilha LA, Klimov VI, Nozik AJ, Beard MC (2013) Size and composition dependent multiple exciton generation efficiency in PbS, PbSe, and PbS x Se1–x alloyed quantum dots. Nano Lett 13:3078–3085

    Article  Google Scholar 

  17. Kumar R, Jain G, Saini R, Agarwal R (2010) Compositional effects on properties of PbS1−x Se x thin films. Chalcogenide Lett 7:233–240

    Google Scholar 

  18. Nasir EM, Abas NK, Alatya SJ (2013) Influence of sulfur on structural and electrical properties of PbS x Se1−x films. Int J Thin Film Sci Technol 2:133–142

    Article  Google Scholar 

  19. Zhang W-M, Sun Z-X, Hao W, Su D-W, Vaughan DJ (2011) Synthesis of size tuneable cadmium sulfide nanoparticles from a single source precursor using ammonia as the solvent. Mater Res Bull 46:2266–2270

    Article  Google Scholar 

  20. Akhtar J, Akhtar M, Malik MA, O’Brien P, Raftery J (2012) A single-source precursor route to unusual PbSe nanostructures by a solution–liquid–solid method. J Am Chem Soc 134:2485–2487

    Article  Google Scholar 

  21. McNaughter PD, Saah SA, Akhtar M, Abdulwahab K, Malik MA, Raftery J, Awudza JAM, O’Brien P (2016) The effect of alkyl chain length on the structure of lead(II) xanthates and their decomposition to PbS in melt reactions. Dalton Trans 45:16345–16353. https://doi.org/10.1039/c6dt02859d

    Article  Google Scholar 

  22. Akhtar J, Afzaal M, Vincent MA, Burton NA, Raftery J, Hillier IH, O’Brien P (2011) Understanding the decomposition pathways of mixed sulfur/selenium lead phosphinato complexes explaining the formation of lead selenide. J Phys Chem C 115:16904–16909

    Article  Google Scholar 

  23. Monshi A, Foroughi MR, Monshi MR (2012) Modified Scherrer equation to estimate more accurately nano-crystallite size using XRD. World J Nano Sci Eng 2:154–160

    Article  Google Scholar 

  24. Thomson JW, Wang X, Huch L, Faulkner D, Petrov S, Ozin GA (2012) Discovery and evaluation of a single source selenium sulfide precursor for the synthesis of alloy PbS x Se1−x nanocrystals. J Mater Chem 22:5984–5989

    Article  Google Scholar 

  25. Cui R, Gu Y-P, Zhang Z-L, Xie Z-E, Tiana Z-Q, Pang D-W (2012) Controllable synthesis of PbSe nanocubes in aqueous phase using a quasi-biosystem. J Mater Chem 22:3713–3716

    Article  Google Scholar 

  26. Afonicheva PF, Matyushkin LB (2016) Growth characteristics of nanostructured lead sulfide films prepared by chemical bath deposition. In: IEEE 8-10

  27. Vankhade D, Kothari A, Chaudhuri TK (2016) Direct-coated photoconducting nanocrystalline PbS thin films with tunable band gap. J Electron Mater 45:2789–2795

    Article  Google Scholar 

  28. Rajasshree C, Balu AR, Nagarethinam VS (2014) Substrate temperature effect on the physical properties of spray deposited lead sulfide thin films suitable for solar control coatings. Int J Chem Tech Res 6:347–360

    Google Scholar 

  29. Begum A, Hussain A, Rahman A (2012) Effect of deposition temperature on the structural and optical properties of chemically prepared nanocrystalline lead selenide thin films. Beilstein J Nanotechnol 3:438–443

    Article  Google Scholar 

  30. Obaid AS, Mahdi MA, Hassan Z, Bououdina M (2012) Characterization of nanocrystalline PbS thin films prepared using microwave-assisted chemical bath deposition. Mater Sci Semicond Process 15:564–571

    Article  Google Scholar 

  31. Uhuegbu CC (2011) Limiting and realistic efficiencies of multi-junction solar cells. Can J Sci Ind Res 2:230–241

    Google Scholar 

  32. Barote MA, Yadav AA, Chavan TV, Masumdar EU (2011) Characterization and photoelectrochemical properties of chemical bath deposited n-PbS thin films. Dig J Nanomater Biostruct 6:979–990

    Google Scholar 

  33. Zamana S, Asim MM, Siddique SS, Mahmood SK (2010) Effect of deposition parameters and annealing on the morphology and optical properties of PbS thin films. Key Eng Mater 442:144–151

    Article  Google Scholar 

  34. Mulik RN, Pawar SG, More PD, Pawar SA, Patil VB (2010) Nanocrystalline PbS thin films: synthesis, microstructural and optoelectronic properties. Arch Appl Sci Res 2:1–6

    Google Scholar 

  35. Abbas NK, Al-Fawade EM, Alatya SJ (2013) Band gap engineering in lead sulfur selenide (PbS1−x Se x ) thin films synthesized by chemical bath deposition method. J Mater Sci Eng A 3:82–92

    Google Scholar 

  36. El-Shazly EAA, Zedan IT, El-Rahman KFA (2011) Determination and analysis of optical constants for thermally evaporated PbSe thin films. Vacuum 86:318–323

    Article  Google Scholar 

  37. Kale RB, Sartale SD, Ganesan V, Lokhande CD, Lin Y-F, Lu S-Y (2006) Room temperature chemical synthesis of lead selenide thin films with preferred orientation. Appl Surf Sci 253:930–936

    Article  Google Scholar 

  38. Korkosz RJ, Chasapis TC, Lo S-H, Doak JW, Kim YJ, Wu C-I, Hatzikraniotis E, Hogan TP, Seidman DN, Wolverton C, Dravid VP, Kanatzidis MG (2014) High ZT in p-type (PbTe)1–2x(PbSe)x(PbS)x thermoelectric materials. J Am Chem Soc 136:3225–3237

    Article  Google Scholar 

  39. Lach-Hab M, Papaconstantopoulos DA, Mehl MJ (2002) Electronic structure calculations of lead chalcogenides PbS, PbSe, PbTe. J Phys Chem Solids 63:833–841

    Article  Google Scholar 

  40. Kacimi S, Zaoui A, Abbar B, Bouhauf B (2008) Ab initio study of cubic PbS x Se1−x alloys. J Alloy Compd 462:135–141

    Article  Google Scholar 

Download references

Acknowledgements

The authors thank the Leverhulme Royal Society Africa Awards and the Royal Society DFID Africa Capacity Building Schemes for their financial support. We also thank Engineering and Physical Sciences Research Council (EPSRC) for funding of instruments under Grant Number (EP/K039547/1) used for characterization of the compounds. POB and PDM would also like to acknowledge funding from EPRSC Grant Number (EP/K010298/1). POB would like to thank Dr. David J. Lewis for his invaluable and unwavering assistance in editing this paper.

Author information

Authors and Affiliations

  1. Department of Chemistry, Kwame Nkrumah University of Science and Technology, Kumasi, Ghana

    Selina A. Saah & Johannes A. M. Awudza

  2. The School of Chemistry, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK

    Paul D. McNaughter & Paul O’Brien

  3. The School of Materials, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK

    Mohammed A. Malik & Paul O’Brien

  4. Department of Chemistry, University of Zululand, Private Bag X1001, KwaDlangezwa, 3886, South Africa

    Neerish Revaprasadu

Authors
  1. Selina A. Saah
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Paul D. McNaughter
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Mohammed A. Malik
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Johannes A. M. Awudza
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Neerish Revaprasadu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Paul O’Brien
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Paul O’Brien.

Ethics declarations

Conflict of interest

The authors declare that they have no conflict of interest.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 408 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Saah, S.A., McNaughter, P.D., Malik, M.A. et al. PbS x Se1−x thin films from the thermal decomposition of lead(II) dodecylxanthate and bis(N,N-diethyl-N′-naphthoylselenoureato)lead(II) precursors. J Mater Sci 53, 4283–4293 (2018). https://doi.org/10.1007/s10853-017-1836-5

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10853-017-1836-5

Keywords

Search

Navigation