Unique lanthanide complexes with dibenzoylmethane (DBM) ligands, which are propellershaped molecules, have been studied both for their structural characteristics and for application-oriented synthesis. Compounds of lanthanides with +3 oxidation states are important for nuclear-fuel processing and magnetic resonance imaging. The structures of seven-coordinate lanthanide complexes with three DBM ligands and a water molecule, such as Ho(III) aqua-tris(dibenzoylmethane) (Ho-(DBM) 3 • H 2 O), were investigated by Zalkin et al. using single-crystal X-ray diffraction (SC-XRD) in the late 1960s. This examination revealed that, in their crystalline structure, six oxygens in the DBMs and one oxygen in water are coordinated to Ho with an R3 space group. The packing arrangement of seven-coordinate complexes is much less dense than that of those with fourto six-coordination because of the unstable bonding structure resulting from lower orbital symmetry. Nevertheless, seven-coordinate complexes can exist as molecular crystals or in a solvent. A systematic molecular-orbital analysis of seven-coordinate molecules has been conducted with regard to the electronic structures of various geometries. A seven-coordinate complex structure such as Ho-(DBM) 3 • H 2 O has three-fold symmetry capped with a water molecule, and it exhibits strong luminescence and a very large radiative rate constant. Although a considerable number of studies has been conducted regarding synthesis toward applications and single-crystal structural analysis, molecular dynamics (MD) simulations of crystalline lanthanide complexes cannot be routinely performed. A wide range of simulation studies has been carried out to understand the structure and dynamics of metal-organic compounds during recent decades (for instance, Refs. ). MD simulations of organometallic frameworks formed from highly symmetric bonds have been successfully used to understand the host structures and the dynamics of guest molecules.