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Density functional theory (DFT) study of the gas-phase decomposition of the Cd[(iPr)2PSSe]2 single-source precursor for the CVD of binary and ternary cadmium chalcogenides

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Abstract

The chemistry of group II–VI semiconductors has spurred considerable interest in decomposition reaction mechanisms and has been exploited for various technological applications. In this work, computational chemistry was employed to investigate the possible gas-phase decomposition pathways of the mixed Cd[(iPr)2PSSe]2 single-source precursor for the chemical vapour deposition of cadmium chalcogenides as thin films. The geometries of the species involved were optimised by employing density functional theory at the MO6/LACVP* level. The results indicate that the steps that lead to CdS formation on the singlet potential energy surface are favoured kinetically over those that lead to CdSe and ternary CdSe x S1−x formation. On the doublet PES, the steps that lead to CdSe formation are favoured kinetically over those that lead to CdS and CdSexS1−x formation. However, thermodynamically, the steps that lead to ternary CdSe x S1−x formation are more favourable than those that lead to CdSe and CdS formation on both the singlet and the doublet PESs. Density functional theory calculations revealed that the first steps exhibit huge activation barriers, meaning that the thermodynamically favourable process takes a very long time to initiate.

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Acknowledgments

The authors are very grateful to the National Council for Tertiary Education (NTCE), Ghana, for a research grant under the Teaching and Learning Innovation Fund (TALIF-KNUSTR/3/005/2005). We are also grateful to the Computational Quantum Chemistry Laboratory at the Department of Chemistry, Kwame Nkrumah University of Science and Technology (KNUST), Kumasi, Ghana, for the use of their facilities for this work.

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

    Francis Opoku, Noah Kyame Asare-Donkor & Anthony A. Adimado

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  1. Francis Opoku
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  2. Noah Kyame Asare-Donkor
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  3. Anthony A. Adimado
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Correspondence to Noah Kyame Asare-Donkor.

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Opoku, F., Asare-Donkor, N.K. & Adimado, A.A. Density functional theory (DFT) study of the gas-phase decomposition of the Cd[(iPr)2PSSe]2 single-source precursor for the CVD of binary and ternary cadmium chalcogenides. J Mol Model 20, 2484 (2014). https://doi.org/10.1007/s00894-014-2484-1

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