High-resolution X-ray diffraction data, in conjunction with DFT(B3LYP) quantum calculations, have been used in a QTAIM analysis of the charge density in the trimethylenemethane (TMM) complex Fe(eta(4)-C{CH2}(3))-(CO)(3). The agreement between the theoretical and experimental topological properties is excellent. Only one bond path is observed between the TMM ligand and the Fe atom, from the central C-alpha atom. However, much evidence, including from the delocalization indices and the source function, suggests that there is a strong chemical interaction between the Fe and C-beta atoms, despite the formal lack of chemical bonding according to QTAIM.