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We theoretically study pump-photon-energy-dependent pathways of aphotoinduced dimer-Mott-insulator-to-metal transition, on the basis ofnumerical solutions to the time-dependent Schr\"odinger equation for the exactmany-body wave function of a two-dimensional three-quarter-filled extendedPeierls-Hubbard model. When molecular degrees of freedom inside a dimer areutilized, photoexcitation can weaken the effective interaction or increase thedensity of photocarriers. In the organic dimer Mott insulator, $ \kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br, the intradimer and the interdimercharge-transfer excitations have broad bands that overlap with each other. Evenin this disadvantageous situation, the photoinduced conductivity change dependslargely on the pump photon energy, confirming the two pathways recentlyobserved experimentally. The characteristic of each pathway is clarified bycalculating the modulation of the effective interaction and the number ofcarriers involved in low-energy optical excitations. Thepump-photon-energy-dependent pathways are confirmed to be realized from thefinding that, although the effective interaction is always and slowly weakened,the introduction of carriers is sensitive to the pump-photon energy andproceeds much faster.

Photoexcitation-Energy-Dependent Transition Pathways from a Dimer Mott Insulator to a Metal