X-ray observation of a helium atom and placing a nitrogen atom inside He@C60 and He@C70

Single crystal X-ray analysis has been used as a powerful method to determine the structure of molecules. However, crystallographic data containing helium has not been reported, owing to the difficulty in embedding helium into crystalline materials. Here we report the X-ray diffraction study of He@C60 and the clear observation of a single helium atom inside C60. In addition, the close packing of a helium atom and a nitrogen atom inside fullerenes is realized using two stepwise insertion techniques, that is, molecular surgery to synthesize the fullerenes encapsulating a helium atom, followed by nitrogen radio-frequency plasma methods to generate the fullerenes encapsulating both helium and nitrogen atoms. Electron spin resonance analysis reveals that the encapsulated helium atom has a small but detectable influence on the electronic properties of the highly reactive nitrogen atom coexisting inside the fullerene, suggesting the potential usage of helium for controlling electronic properties of reactive species.