Low-energy vibrations in Sc2@C84 and Tm@C82 metallofullerenes with different carbon cages

M. Krause, M. Hulman, H. Kuzmany*, P. Kuran, L. Dunsch, T. J.S. Dennis, M. Inakuma, H. Shinohara

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

40 Citations (Scopus)

Abstract

Raman scattering and infrared absorption is reported for various empty and filled fullerene isomers in the low-energy range below 600 cm-1 to clarify the influence of different carbon cage structures on the bonding strength between encapsulated metal ion and fullerene cage and to check the potential of vibrational spectroscopy for isomer identification. The spectra of three isomers of Tm@C82 and three isomers of Sc2@C84 were measured at room temperature. The results are compared to the response of the most abundant isomers of empty C84 as well as to data for C82 and C60. The vibrational structure of the higher empty fullerene cages C82 and C84 resembles a downshifted and split C60 spectrum. Moreover the spectra of the two C84 isomers exhibited only small differences due to the very similar molecular structure, i.e. identical hexagon indices and direct neighbourhood in the Stone-Wales conversion map. Larger differences of the low-energy cage modes were found for the Tm@C82 isomers and in particular for the Sc2@C84 isomers. This goes along with an increasing difference in hexagon indices and a larger distance on the Stone-Wales conversion map. Due to the charge transfer from the endohedral metal to the fullerene the low- energy cage modes are shifted in the same direction as the modes of C60 during the exohedral doping process with alkali metals. New lines induced by the endohedral scandium and thulium ions with almost complementary Raman and infrared intensities were found for Sc2@C84 below 200, around 250 and 260 cm-1 and for Tm@C82 at 116 to 118 cm-1 and at 42 cm-1. These vibrations were further identified as M-C(2n) stretching and M-C(2n) deformation modes. Only a minor influence of the cage isomerism on these modes was observed. This is consistent with a simple ionic picture for the interaction between carbon cage and encapsulated metal ion. It is the amount of metal to fullerene charge transfer and the distance of the oppositely charge centres which determine the carbon cage-metal ion bond strength. (C) 2000 Elsevier Science B.V.

Original languageEnglish
Pages (from-to)325-340
Number of pages16
JournalJournal of Molecular Structure
Volume521
Issue number1-3
DOIs
Publication statusPublished - 28 Mar 2000
Externally publishedYes

Keywords

  • Carbon cage isomerism
  • Endohedral metallofullerenes
  • Fullerenes
  • IR spectra
  • Low-energy vibrations
  • Metal-to- fullerene charge transfer
  • Metal-to-fullerene bond
  • Raman spectra

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