The atomic structure of the sample was observed using the aberration-corrected Nion UltraSTEM 100 at the Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences User Facility operated at 60 kV, and the same instrument at the University of Vienna. In a standard treatment, the sample was baked in vacuum at 160°C for 8 hours before insertion into the microscope column. The vacuum level at the sample volume during the experiments was <3 × 10−9 mbar. The convergence semiangle of electron probe is 30 mrad, and the collection semiangle of the electron energy loss spectrum is 48 mrad. The medium angle annular dark field (MAADF) collection semiangle range is 54 to 200 mrad. Electron current was kept in between 50 and 60 pA during all of the imaging. To estimate the doses of the spot irradiation manipulation experiments, we used a model of the expected probe intensity profile as described in (2, 22).

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