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Towards a comprehensive understanding of the Si(100)-2×1 surface termination through hydrogen passivation using methylamine and methanol: a theoretical approach

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Abstract

Using density functional theory, we explored the termination process of Si (100)-2 × 1 reconstructed surface mechanistically through the dehydrogenation of small molecules, considering methyl amine and methanol as terminating reagents. At first, both the terminating reagents form two types of adduct through adsorption on the Si (100)-2 × 1 surface, one in chemisorption mode and the other via physisorption, from which the dehydrogenation process is initiated. By analyzing the activation barriers, it was observed that termination of the Si-surface through the dehydrogenation is kinetically almost equally feasible using either reagent. We further examined in detail the mechanism for each termination process by analyzing geometrical parameters and natural population analysis charges. From bonding evaluation, it is evident that hydrogen abstraction from adsorbates on the Si-surface is asymmetric in nature, where one hydrogen is abstracted as hydride by the electrophilic surface Si and the other hydrogen is abstracted as proton by the neucleophilic surface Si. Moreover, it was also observed that hydride transfer from adsorbate to the Si-surface occurs first followed by proton transfer. Overall, our theoretical interpretation provides a mechanistic understanding of the Si (100)-2 × 1 reconstructed surface termination by amine and alcohol that will further motivate researchers to design different types of decorated semiconductor devices.

Surface termination process of Si(100)-2×1 through formation of non-polar Si–H bonds via dehydrogenation of methylamine and methanol as terminating reagents

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Acknowledgments

T.D. and T.A. are thankful to Council of Scientific and Industrial Research (CSIR) and S.S. is thankful to the University Grants Commission (UGC) for providing them with research fellowships.

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Authors and Affiliations

  1. School of Mathematical & Computational Sciences, Indian Association for the Cultivation of Science, Jadavpur, Kolkata, 700032, India

    Tanay Debnath, Tamalika Ash, Subhendu Sarkar & Abhijit Kr. Das

Authors
  1. Tanay Debnath
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  2. Tamalika Ash
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  3. Subhendu Sarkar
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  4. Abhijit Kr. Das
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Corresponding author

Correspondence to Abhijit Kr. Das.

Additional information

Dedicated to Prof. Pratim K. Chattaraj on the happy occasion of his 60th birthday.

This paper belongs to Topical Collection International Conference on Systems and Processes in Physics, Chemistry and Biology (ICSPPCB-2018) in honor of Professor Pratim K. Chattaraj on his sixtieth birthday

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Debnath, T., Ash, T., Sarkar, S. et al. Towards a comprehensive understanding of the Si(100)-2×1 surface termination through hydrogen passivation using methylamine and methanol: a theoretical approach. J Mol Model 24, 286 (2018). https://doi.org/10.1007/s00894-018-3809-2

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  • DOI: https://doi.org/10.1007/s00894-018-3809-2

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