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On surface pre-melting of metallic nanoparticles: molecular dynamics study

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Abstract

Employing the isothermal molecular dynamics and the embedded atom method, we simulated melting of metallic nanoparticles (Au, Ag, Cu, Ni, and Pb ones). In more detail, the results for Au and Ag nanoparticles are presented and discussed. At first, we analyzed the behavior of the temperature dependences for the potential (cohesive) term into the specific (per atom) internal energy and for the degree of crystallinity in the course of heating nanoparticles. We have found that the results obtained for nanoparticles of about 4 and 8 nm in size (containing 2093 and 20,113 atoms, respectively) demonstrate the continuous melting. Employing the dependence of the specific potential energy on the distance to the nanoparticle center of mass and the common neighbor analysis, we showed that the continuous melting occurs via the surface pre-melting mechanism. Then, we evaluated the self-diffusion coefficient in the surface disordered layers of Au and Ag nanoparticles and found that our results agree in order of magnitude (10−9 m2/s) with the values of the self-diffusion coefficient for the bulk Au and Ag melts at the corresponding bulk melting temperatures. Finally, combining in our molecular dynamics experiments continuous heating Au nanoparticles with annealing them at some constant selected temperatures, we have shown that the liquid nucleation and growth mechanism should be most adequate to the melting behavior of metallic nanoparticles.

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Data availability

The main simulation results were obtained employing open access program LAMMPS. The authors are not able now to share their own additional software for processing MD results (evaluation of the self-diffusion coefficient) freely as it is a proprietary of their organization (Tver State University). However, after the paper is published, the authors will be ready to provide the trial software to interested readers and to discuss with them our approach for determination of the atomic mobility in MD experiments. In addition, it is proposed to make the toolkit available on the GitHub website after the developed software is registered.

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Funding

Our study was performed in Tver State University and supported by the Russian Science Foundation grant No. 23-22-00414, https://rscf.ru/en/project/23-22-00414/.

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Authors and Affiliations

  1. Tver State University, Zhelyabova 33, Tver, 170100, Russia

    V. M. Samsonov, I. V. Talyzin, S. A. Vasilyev, V. V. Puytov & A. A. Romanov

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  1. V. M. Samsonov
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  2. I. V. Talyzin
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  3. S. A. Vasilyev
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  4. V. V. Puytov
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  5. A. A. Romanov
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Contributions

All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by Vladimir Samsonov, Igor Talyzin, Sergey Vasilyev, Vladimir Puytov, and Aleksander Romanov. The first draft of the manuscript was written by Vladimir Samsonov and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Samsonov, V.M., Talyzin, I.V., Vasilyev, S.A. et al. On surface pre-melting of metallic nanoparticles: molecular dynamics study. J Nanopart Res 25, 105 (2023). https://doi.org/10.1007/s11051-023-05743-0

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