  Dynamics of optically-excited plasmonic nanoparticles are presently
understood as a series of sequential scattering events, involving
thermalization processes after pulsed optical excitation. One important step is
the initiation of nanoparticle breathing oscillations. According to established
experiments and models, these are caused by the statistical heat transfer from
thermalized electrons to the lattice. An additional contribution by hot
electron pressure has to be included to account for phase mismatches that arise
from the lack of experimental data on the breathing onset. We used optical
transient-absorption spectroscopy and time-resolved single-particle
x-ray-diffractive imaging to access the excited electron system and lattice.
The time-resolved single-particle imaging data provided structural information
directly on the onset of the breathing oscillation and confirmed the need for
an additional excitation mechanism to thermal expansion, while the observed
phase-dependence of the combined structural and optical data contrasted
previous studies. Therefore, we developed a new model that reproduces all our
experimental observations without using fit parameters. We identified
optically-induced electron density gradients as the main driving source.
