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There is increasing attention to chemical applications of transmissionelectron microscopy, which is often plagued by radiation damage. The damage inorganic matter predominantly occurs via ionization (radiolysis). Althoughradiolysis is highly important, previous studies on radiolysis have largelybeen descriptive and qualitative, lacking in such fundamental information asthe product structure, the influence of the energy of the electrons, and thereaction kinetics. We need a chemically well-defined system to obtain suchdata, and have chosen as a model a variable-temperature and variable-voltage(VT/VV) study of the dimerization of a van der Waals dimer [60]fullerene (C60)to C120 in a carbon nanotube (CNT) as studied for individual reaction events atatomic resolution. We report here the identification of five reaction pathwaysthat serve as mechanistic models of radiolysis damage. Two of them occur via aradical cation of the specimen generated by specimen ionization, and threeinvolve singlet or triplet excited states of the specimen, as initiated byelectron excitation of the CNT followed by energy transfer to the specimen. Thepathways were distinguished by the pre-exponential factor and the Arrheniusactivation energy. The prototypal reaction path is the radical cation reactionthat we saw at <200 K, but, at >350 K, the excited-state reactions dominate.The results illustrate the importance of VT/VV kinetic analysis in the studiesof radiation damage, and show that chemical ionization and electron excitationare inseparable but different mechanisms of radiation damage, which has so farbeen classified loosely under the single term "ionization."

proceedings of the national academy of sciences of the united states of america

Ionization and electron excitation of fullerene molecules in a carbon  nanotube. A variable temperature/voltage transmission electron microscopic  study