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Dynamics of optically-excited plasmonic nanoparticles are presentlyunderstood as a series of sequential scattering events, involvingthermalization processes after pulsed optical excitation. One important step isthe initiation of nanoparticle breathing oscillations. According to establishedexperiments and models, these are caused by the statistical heat transfer fromthermalized electrons to the lattice. An additional contribution by hotelectron pressure has to be included to account for phase mismatches that arisefrom the lack of experimental data on the breathing onset. We used opticaltransient-absorption spectroscopy and time-resolved single-particlex-ray-diffractive imaging to access the excited electron system and lattice.The time-resolved single-particle imaging data provided structural informationdirectly on the onset of the breathing oscillation and confirmed the need foran additional excitation mechanism to thermal expansion, while the observedphase-dependence of the combined structural and optical data contrastedprevious studies. Therefore, we developed a new model that reproduces all ourexperimental observations without using fit parameters. We identifiedoptically-induced electron density gradients as the main driving source.

Time-resolved single-particle x-ray scattering reveals electron-density as coherent plasmonic-nanoparticle-oscillation source