Nanoscale subparticle imaging of vibrational dynamics using dark-field ultrafast transmission electron microscopy

An understanding of nanoscale energy transport and acoustic response is important for applications of nanomaterials but hinges on a complete characterization of their structural dynamics. The precise determination of the structural dynamics within nanoparticles, however, is still challenging and requires high spatiotemporal resolution and detection sensitivity. Here we present a centred dark-field imaging approach based on ultrafast transmission electron microscopy that is capable of directly mapping the picosecond-scale evolution of intrananoparticle vibration with a spatial resolution down to 3 nm. Using this approach, we investigated the photo-induced vibrational dynamics in individual gold heterodimers composed of a nanoprism and a nanosphere. We observed not only the retardation of in-plane vibrations in the nanoprisms, which we attribute to thermal and vibrational energy transferred from adjacent nanospheres mediated by surfactants, but also the existence of a complex multimodal oscillation and its spatial variation within individual nanoprisms. This work represents an advance in real-space mapping of vibrational dynamics on the subnanoparticle level with a high detection sensitivity.