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 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.