Structural aspects of two-dimensional polymers: Li4C60, Na4C60 and tetragonal C60. Raman spectroscopy and X-ray diffraction

We present an analysis of three different two-dimensional polymers, tetragonal C₆₀, Li₄C₆₀, and Na₄C₆₀. Based on X-ray diffraction and Raman spectroscopy, we conclude that Li₄C₆₀ forms a tetragonal structure with intermolecular bonds formed by 2+2 cycloaddition, in the same way as for tetragonal C₆₀. Na₄C₆₀, on the other hand, forms a monoclinic structure with single C–C bonds between the molecules. Our Raman spectroscopy results can be interpreted in two ways: either the charge transfer to the C₆₀ molecules is the same in both doped compounds with four electrons/molecule or the electron charge transfer is smaller from the Li ions than from the Na ions.