Multiconfigurational Ground State of a Diradicaloid Characterized at the Atomic Scale

Journal article, 2025

We report the tip-induced generation and scanning probe characterization of a singlet diradicaloid, consisting of two phenalenyl units connected by an sp-hybridized C4 chain on an ultrathin insulating NaCl surface. The bond-order contrast along the C4 chain measured by atomic force microscopy and mapping of charge-state transitions by scanning tunneling microscopy, in conjunction with multiconfigurational calculations, reveal that the molecule exhibits a many-body ground state. Our study experimentally demonstrates the manifestation of strong electronic correlations in the geometric and electronic structures of a single molecule.