• lone pair of excess electron;
  • spin evolution;
  • cage-like single molecular solvated dielectron;
  • vertical electron detachment energy;
  • container of excess electrons


For unusual e2@C60F60 (Ih, D6h, and D5d) cage structures with two excess electrons, it is reported that not only the lone pair in singlet state but also two single excess electrons in triplet state can be encapsulated inside the C60F60 cages to form single molecular solvated dielectrons. The interesting relationship between the shape of the cage and the spin state of the system has revealed that ground states are singlet state for spherical shaped e2@C60F60 (Ih) and triplet states for short capsular shaped e2@C60F60 (D6h) and long capsular shaped e2@C60F60 (D5d), which shows a spin evolution from the singlet to triplet state with the deformation of the cage from spherical to capsular shape. For these excess electron systems, the three ground state structures have large vertical electron detachment energies (VDEs (I) of 1.720–2.283 eV and VDEs (II) of 3.959–5.288 eV), which shows their stabilities and suggests that the large C60F60 cage is the efficient container of excess electrons. © 2011 Wiley Periodicals, Inc. J Comput Chem, 2011