Scalable and Universal Route for the Deposition of Binary, Ternary, and Quaternary Metal Sulfide Materials from Molecular Precursors.

Ghulam Murtaza,Sai P Venkateswaran,Laila Almanqur,Emmanuel Usman Onche,Usama Zulfiqar,Yasser T Alharbi,Suliman Alderhami,Abdulaziz M Alanazi,Mousa Hossin,David J Lewis

doi:10.1021/acsaem.9b02359

Ghulam Murtaza, Sai P Venkateswaran + Show 8 more

Open Access

https://doi.org/10.1021/acsaem.9b02359

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Abstract

A range of binary, ternary (CFS), and quaternary (CZTS) metal sulfide materials have been successfully deposited onto the glass substrates by air-spray deposition of metal diethyldithiocarbamate molecular precursors followed by pyrolysis (18 examples). The as-deposited materials were characterized by powder X-ray diffraction (p-XRD), Raman spectroscopy, secondary electron microscopy (SEM), and energy-dispersive X-ray (EDX) spectroscopy, which in all cases showed that the materials were polycrystalline with the expected elemental stoichiometry. In the case of the higher sulfides, EDX spectroscopy mapping demonstrated the spatial homogeneity of the elemental distributions at the microscale. By using this simple and inexpensive method, we could potentially fabricate thin films of any given main group or transition metal chalcogenide material over large areas, theoretically on substrates with complex topologies.

Highlights

Metal chalcogenides constitute an important family of medium to narrow band gap semiconductors
All precursors were subject to thermogravimetric analysis (TGA) to investigate the decomposition of the metal dithiocarbamate complexes to the corresponding metal sulfides and in order to find suitable processing temperatures to convert the air sprayed precursors to metal sulfides (Figure S1)
TGA of diethyl dithiocarbamato mixtures two or three precursors in tandem, we could potentially complexes of cadmium, indium, copper, zinc, nickel, lead, and access the higher ternary and quaternary transition metal and iron show single-step decompositions in the temperature range main group sulfides

Summary

■ INTRODUCTION

Metal chalcogenides constitute an important family of medium to narrow band gap semiconductors. TGA of diethyl dithiocarbamato mixtures two or three precursors in tandem, we could potentially complexes of cadmium, indium, copper, zinc, nickel, lead, and access the higher ternary and quaternary transition metal and iron show single-step decompositions in the temperature range main group sulfides The morphologies of the metal sulfide films deposited by the air-spray annealing method were investigated by SEM (Figure 1). The solution was sprayed onto the preheated glass substrates These samples were loaded into a quartz tube and heated in a furnace at temperature 450 °C under argon for 1 h to allow for complete decomposition of metal dithiocarbamate complexes into their respective metal sulfides. Energy-dispersive X-ray (EDX) spectroscopy of the CuFeS2 film deposited onto glass substrate by air-spray annealing show that the chalcopyrite materials are sulfur rich and copper deficient (Table 1). EDX spectrum mapping of Cu, Zn, Sn, and S emission lines in the as-deposited CZTS demonstrate that the constituent elements are uniformly distributed throughout the film at the microscale (Figure 8)

■ CONCLUSIONS

■ ACKNOWLEDGMENTS

■ REFERENCES

Growth and Characterization of Tin Sulphide Nanostructured Thin