Unhindered Brownian Motion of Individual Nanoparticles in Liquid-Phase Scanning Transmission Electron Microscopy

Liquid-phase transmission electron microscopy (LPTEM) offers label-free imaging of nanoparticle (NP) processes in liquid with sub-nanometer spatial and millisecond temporal resolution. However, LPTEM studies have reported only on NPs moving orders of magnitude slower than expected from bulk aqueous liquid conditions, likely due to strong interactions with the LPTEM liquid-enclosing membranes. We demonstrate how scanning transmission electron microscope (STEM) imaging can be used to measure the motion of individual NPs and agglomerates, which are not hindered by such interactions. Only at low electron flux do we find that individual NPs exhibit Brownian motion consistent with optical control experiments and theoretical predictions for unhindered passive diffusive motion in bulk liquids. For increasing electron flux, we find increasingly faster than passive motion that still appears effectively Brownian. We discuss the possible origins of this beam-sample interaction. This establishes conditions for the use of STEM as a reliable tool for imaging nanoscale hydrodynamics in situ TEM.