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Plasmon-driven sub-picosecond breathing of metal nanoparticles

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Abstract

We present the first real-time atomistic simulation on the quantum dynamics of icosahedral silver nanoparticles under strong laser pulses, using time dependent density functional theory (TDDFT) molecular dynamics. We identify the emergence of sub-picosecond breathing-like radial oscillations starting immediately after laser pulse excitation, with increasing amplitude as the field intensity increases. The ultrafast dynamic response of nanoparticles to laser excitation points to a new mechanism other than equilibrium electron–phonon scattering previously assumed, which takes a much longer timescale. A sharp weakening of all bonds during laser excitation is observed, thanks to plasmon damping into excited electrons in anti-bonding states. This sudden weakening of bonds leads to a uniform expansion of the nanoparticles and launches coherent breathing oscillations.

Graphical abstract: Plasmon-driven sub-picosecond breathing of metal nanoparticles

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Publication details

The article was received on 23 Jun 2017, accepted on 28 Jul 2017 and first published on 03 Aug 2017


Article type: Paper
DOI: 10.1039/C7NR04536K
Citation: Nanoscale, 2017, Advance Article
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    Plasmon-driven sub-picosecond breathing of metal nanoparticles

    F. P. Bonafé, B. Aradi, M. Guan, O. A. Douglas-Gallardo, C. Lian, S. Meng, T. Frauenheim and C. G. Sánchez, Nanoscale, 2017, Advance Article , DOI: 10.1039/C7NR04536K

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