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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.

physical review letters

Electron-Phonon and Magnetoelastic Interactions in Ferromagnetic<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mi>Co</mml:mi><mml:mo mathvariant="bold" stretchy="false">[</mml:mo><mml:mi mathvariant="bold">N</mml:mi><mml:mo mathvariant="bold" stretchy="false">(</mml:mo><mml:mi>CN</mml:mi><mml:msub><mml:mo mathvariant="bold" stretchy="false">)</mml:mo><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mo mathvariant="bold" stretchy="false">]</mml:mo><mml:mn>2</mml:mn></…

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