Conformational analysis of single perfluoroalkyl chains by single-molecule real-time transmission electron microscopic imaging

Koji Harano, Shinya Takenaga, Satoshi Okada, Yoshiko Niimi, Naohiko Yoshikai, Hiroyuki Isobe, Kazu Suenaga, Hiromichi Kataura, Masanori Koshino, Eiichi Nakamura

Research output: Contribution to journalArticlepeer-review

15 Citations (Scopus)

Abstract

Whereas a statistical average of molecular ensembles has been the conventional source of information on molecular structures, atomic resolution movies of single organic molecules obtained by single-molecule real-time transmission electron microscopy have recently emerged as a new tool to study the time evolution of the structures of individual molecules. The present work describes a proof-of-principle study of the determination of the conformation of each C-C bond in single perfluoroalkyl fullerene molecules encapsulated in a single-walled carbon nanotube (CNT) as well as those attached to the outer surface of a carbon nanohorn (CNH). Analysis of 82 individual molecules in CNTs under a 120 kV electron beam indicated that 6% of the CF2-CF 2 bonds and about 20% of the CH2-CH2 bonds in the corresponding hydrocarbon analogue are in the gauche conformation. This comparison qualitatively matches the known conformational data based on time- and molecular-average as determined for ensembles. The transmission electron microscopy images also showed that the molecules entered the CNTs predominantly in one orientation. The molecules attached on a CNH surface moved more freely and exhibited more diverse conformation than those in a CNT, suggesting the potential applicability of this method for the determination of the dynamic shape of flexible molecules and of detailed conformations. We observed little sign of any decomposition of the specimen molecules, at least up to 10 7 e·nm-2 (electrons/nm2) at 120 kV acceleration voltage. Decomposition of CNHs under irradiation with a 300 kV electron beam was suppressed by cooling to 77 K, suggesting that the decomposition is a chemical process. Several lines of evidence suggest that the graphitic substrate and the attached molecules are very cold.

Original languageEnglish
Pages (from-to)466-473
Number of pages8
JournalJournal of the American Chemical Society
Volume136
Issue number1
DOIs
Publication statusPublished - 2014 Jan 8

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Fingerprint Dive into the research topics of 'Conformational analysis of single perfluoroalkyl chains by single-molecule real-time transmission electron microscopic imaging'. Together they form a unique fingerprint.

Cite this