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We theoretically investigate transient dimer charge and C=C vibration frequencies during the photoinduced charge-order melting in the quasi-two-dimensional metal complex, Et2Me2Sb[Pd(dmit)2]2, by solving the time-dependent Schrodinger equation for an extended PeielsHubbard model. During the melting, the C=C vibration frequencies are modulated and deviate from their equilibrium counterparts. The contributions from electron-hole excitations coupled with the C=C vibrations dominate over the frequency modulations, which are reproduced by an extension from the second-order perturbation theory.

proceedings of the 12th asia pacific physics conference (appc12)

Intramolecular Orbital Excitations and Frequency Modulation of Molecular Vibrations during Photoinduced Charge-Order Melting in Et2Me2Sb[Pd(dmit)2]2