The nature of C−Li bonding in CH3Li and CLi6 was reconsidered using two recently proposed newmethodologies, namely the AIM generalized population analysis and Fermi hole analysis. The calculationswere performed at HF level of the theory using 6-311G** basis sets. The main issue was the realistic estimationof the polarity of C−Li bonds. The analysis confirms that C−Li bonds in CH3Li are predominantly ionic butsome slight modifications of the contemporary picture of bonding in CLi6 is proposed.
