AbstractThe nuclear disaster at the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March 2011 caused partial meltdowns of three reactors. During the meltdowns, a type of condensed particle, a caesium-rich micro-particle (CsMP), formed inside the reactors via unknown processes. Here we report the chemical and physical processes of CsMP formation inside the reactors during the meltdowns based on atomic-resolution electron microscopy of CsMPs discovered near the FDNPP. All of the CsMPs (with sizes of 2.0–3.4 μm) comprise SiO₂ glass matrices and ~10-nm-sized Zn–Fe-oxide nanoparticles associated with a wide range of Cs concentrations (1.1–19 wt% Cs as Cs₂O). Trace amounts of U are also associated with the Zn–Fe oxides. The nano-texture in the CsMPs records multiple reaction-process steps during meltdown in the severe FDNPP accident: Melted fuel (molten core)-concrete interactions (MCCIs), incorporating various airborne fission product nanoparticles, including CsOH and CsCl, proceeded via SiO₂ condensation over aggregates of Zn-Fe oxide nanoparticles originating from the failure of the reactor pressure vessels. Still, CsMPs provide a mechanism by which volatile and low-volatility radionuclides such as U can reach the environment and should be considered in the migration model of Cs and radionuclides in the current environment surrounding the FDNPP.