Atomic-Scale Dynamics at Solid-Liquid Nanointerfaces Induced by Electron-Beam Irradiation

We report electron-beam induced dynamics at PbS-Pb solid-liquid interfaces. We fabricated PbS-Pb solid-liquid nanointerfaces by heating PbS nanocrystals under vacuum to observe the entire process of structural evolution at the atomic scale. We investigated the dynamics using time-resolved high-angle annular dark-field imaging. Electron-beam irradiation caused layer-by-layer dissolution of PbS at the interface, resulting in the formation of the Pb nanodroplet. Ordered liquid layers were observed adjacent to the interface even under continuous electron-beam irradiation and followed the movement of the interface. Instantaneous epitaxial growth of PbS was observed as a reverse process of the dissolution. The resultant Pb nanodroplet provides indisputable evidence for selective sputtering of sulfur atoms via electron-beam irradiation. This paper demonstrates atomic resolution in situ observations of selective and complete sputtering. The observed dynamics can be explained by the intermittent phase transition via nonequilibrium states of the solid-liquid nanointerface triggered by selective sputtering.