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Excited state modulation of C70 dimerization in a carbon nanotube under a variable electron acceleration voltage

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Title
Excited state modulation of C70 dimerization in a carbon nanotube under a variable electron acceleration voltage
Author(s)
Dongxin Liu; Dominik Lungerich; Takayuki Nakamuro; Koji Harano; Eiichi Nakamura
Publication Date
2022-09
Journal
Micron, v.160
Publisher
Elsevier Ltd
Abstract
Cinematographic recording of chemical reactions with transmission electron microscopy provides information unavailable by any other analytical methods. Studies have thus far remained mostly phenomenological, lacking information on the reactive species involved. To gain insight into the nature of the reactive species, we need to obtain kinetic information under various temperatures and variable acceleration voltages, i.e., electronic energy supply. We studied the mechanism of [2 + 2] dimerization of [70] fullerene in a carbon nanotube as an example. We describe herein a statistical analysis of individual reaction events of the dimerization that revealed dose-dependent first-order kinetics and voltage-dependent crossover from a singlet to a triplet mechanism, as highlighted by the pre-exponential factor (the frequency of excitation) that is a million times larger for the singlet reaction than for the triplet one. Comparison with the results of a recent study of [60] fullerene dimerization lets us propose that electron-impact excitation of the carbon nanotube is the first step, followed by energy transfer to fullerene molecules and their dimerization via an excited state. The results show that a variable-voltage kinetic study is indispensable for discussing the mechanism of chemical transformations under electron microscopic observation.
URI
https://pr.ibs.re.kr/handle/8788114/11996
DOI
10.1016/j.micron.2022.103316
ISSN
0968-4328
Appears in Collections:
Center for Nanomedicine (나노의학 연구단) > 1. Journal Papers (저널논문)
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