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Lithiation of Silicon Nanoclusters

Andreas Pedersen*, Michael Bieri, and Mathieu Luisier

Laurent Pizzagalli

  • Integrated Systems Laboratory, Department of Electrical Engineering and Information Technology, ETH Zurich, Gloriastrasse 35, 8092 Zurich, Switzerland

  • Institut P′, CNRS UPR 3346, Université de Poitiers, SP2MI, BP 30179, Boulevard Marie et Pierre Curie, 86962 Futuroscope Chasseneuil Cedex, France

  • *andped10@gmail.com
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Phys. Rev. Applied 7, 054012 – Published 16 May, 2017

DOI: https://doi.org/10.1103/PhysRevApplied.7.054012

Abstract

In this paper, we investigate the lithiation of pristine amorphous silicon nanoclusters with diameters from 0.8 to 1.4 nm using first-principles molecular dynamics. It is found that this process occurs in two stages. In the first one, Li atoms accumulate at the surface of the nanocluster. A transfer of electrons from Li to the Si atoms takes place, which is accompanied by moderate structural changes. At a given Li coverage threshold that is related to the nanoparticle size, it becomes energetically favorable for any additional Li atoms to penetrate into the nanoparticle. Our results suggest that the driving force for this transition is the increasing electrostatic repulsion between positively charged surface Li ions. Beyond the threshold a second lithiation stage starts where the nanocluster is progressively filled with Li atoms. This leads to significant structural changes, but no sign of fracture is observed during the first lithiation cycle, suggesting that the amorphous silicon cluster remains intact at this size.

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Phys. Rev. Applied 7, 054012– Published 16 May, 2017
  • Received 19 January 2017

© 2017 American Physical Society

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