Building Carbon Bridges on and between Fullerenes in Helium Nanodroplets

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• 作者：Serge A. Krasnokutski ; Martin Kuhn ; Alexander Kaiser ; Andreas Mauracher ; Michael Renzler ; Diethard K. Bohme ; Paul Scheier
• 刊名：The Journal of Physical Chemistry Letters
• 出版年：2016
• 出版时间：April 21, 2016
• 年：2016
• 卷：7
• 期：8
• 页码：1440-1445
• 全文大小：434K
• 年卷期：0
• ISSN：1948-7185

文摘

We report the observation of sequential encounters of fullerenes with C atoms in an extremely cold environment. Experiments were performed with helium droplets at 0.37 K doped with C₆₀ molecules and C atoms derived from a novel, pure source of C atoms. Very high-resolution mass spectra revealed the formation of carbenes of the type C₆₀(C:)_n with n up to 6. Bridge-type bonding of the C adatoms to form the known dumbbell C₆₀═C═C₆₀ also was observed. Density functional theory calculations were performed that elucidated the carbene character of the C₆₀(C:)_n species and their structures. Mass spectra taken in the presence of water impurities and in separate experiments with added H₂ also revealed the formation of the adducts C₆₀C_n(H₂O)_n and C₆₀C_n(H₂)_n probably by H–OH and H–H bond insertion, respectively, and nonreactivity for the dumbell. So C adatoms that form carbenes C₆₀(C:)_n can endow pristine C₆₀ with a higher chemical reactivity.