Insight into the Structural and Emissive Behavior of a Three‐Dimensional Americium(III) Formate Coordination Polymer

We report the structural, vibrational, and optical properties of americium formate (Am(CHO2)3) crystals synthesized via the in situ hydrolysis of dimethylformamide (DMF). The coordination polymer features Am3+ ions linked by formate ligands into a three‐dimensional network that is isomorphous to several lanthanide analogs, (e. g., Eu3+, Nd3+, Tb3+). Structure determination revealed a nine‐coordinate Am3+ metal center that features a unique local C3v symmetry. The metal–ligand bonding interactions were investigated by vibrational spectroscopy, natural localized molecular orbital calculations, and the quantum theory of atoms in molecules. The results paint a predominantly ionic bond picture and suggest the metal‐oxygen bonds increase in strength from Nd−O