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Femtosecond-laser-induced bond breaking and structural modifications in silicon, TiO\(_2\), and defective graphene: an ab initio molecular dynamics study

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Abstract

By exciting or heating electrons, ultrashort laser pulses have a direct influence on bond strengths in two- and three-dimensional solids. Here, we present results of ab initio molecular dynamics simulations performed using our in-house Code for Highly-excIted Valence Electron Systems (CHIVES) for three systems, which each shows a distinctly different structural response to a femtosecond laser pulse. In solid silicon, we show that ultrafast laser-induced bond breaking leads to nonthermal melting, a process which occurs in three stages, involving subsequently superdiffusive, fractionally diffusive, and normally diffusive atomic motions. For TiO\(_2\), we find that the A\(_{1g}\) phonon is coherently excited. At room temperature, we demonstrate that these oscillations are strongly coupled to other phonon modes. In graphene with a single Stone–Wales defect, we study the in-plane and out-of-plane laser-induced atomic motions and find bond breaking, which destroys the structure, when the electrons are heated to at least 31,000 K.

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Acknowledgments

Figure 5 was drawn using the package from [48]. The authors thank DFG, project GA465/15-1, for funding.

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Authors and Affiliations

  1. Theoretical Physics and Center for Interdisciplinary Nanostructure Science and Technology (CINSAT), Universität Kassel, Heinrich Plett-Str. 40, 34132 , Kassel, Germany

    Eeuwe S. Zijlstra, Tobias Zier, Bernd Bauerhenne, Sergej Krylow, Philipp M. Geiger & Martin E. Garcia

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  1. Eeuwe S. Zijlstra
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  2. Tobias Zier
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  3. Bernd Bauerhenne
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Correspondence to Martin E. Garcia.

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Zijlstra, E.S., Zier, T., Bauerhenne, B. et al. Femtosecond-laser-induced bond breaking and structural modifications in silicon, TiO\(_2\), and defective graphene: an ab initio molecular dynamics study. Appl. Phys. A 114, 1–9 (2014). https://doi.org/10.1007/s00339-013-8080-x

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  • DOI: https://doi.org/10.1007/s00339-013-8080-x

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