Electron-Phonon and Magnetoelastic Interactions in FerromagneticCo[N(CN)2]2

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We combined Raman and infrared vibrational spectroscopies with complementary lattice dynamics calculations and magnetization measurements to reveal the dynamic aspects of charge-lattice-spin coupling in Co[N(CN)2]2. Our work uncovers electron-phonon coupling as a magnetic field-driven avoided crossing of the low-lying Co2+ electronic excitation with two ligand phonons and a magnetoelastic effect that signals a flexible local CoN6 environment. Their simultaneous presence indicates the ease with which energy is transferred over multiple length and time scales in this system.