2025/05/16 by Aman Ullah, Ullah, Aman, Sergey A. Varganov +3
Chemistry · Materials Science · #FOS: Physical sciences #Magnetism in coordination complexes #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Organic and Molecular Conductors Research #Synthesis and Properties of Aromatic Compounds
paper · pdf · doi:10.48550/arxiv.2505.10904
openalex publication_date 2025/05/16 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
In single molecular magnets, chiral vibrations carrying vibrational angular momentum (Lvib) emerge due to the splitting of a doubly degenerate vibrational mode. Here, we identify a new type of effective spin-vibrational coupling responsible for lifting this degeneracy, which can facilitate optically selective excitations. In the presence of an external Zeeman field, this coupling breaks both inversion (in-plane parity) P and time-reversal T symmetries, imparting distinct geometric phases to the resulting dressed spin-vibronic states. The wave function of the spin-vibronic state is characterized by a π-Berry phase, which results in magneto-optical circular dichroism. This framework is validated using density functional theory and multi-reference ab initio calculations on the Ce(trenovan) molecular magnet.