From theory, we investigate charge localization induced by higher-frequency off-resonance lightpulse excitation in the metallic phase of α-(BEDT-TTF) 2 I 3 by numerically solving the timedependent Schrödinger equation in the quarter-filled extended Hubbard model for the material. Around eaA (max) = 1, where eaA (max) is the maximum amplitude of the dimensionless vector potential of the pump pulse, the charge distribution is significantly changed by photoexcitation, and the light-pulse-induced collective charge oscillations continue after photoexcitation. Furthermore, the charge dynamics depend strongly on the polarization direction of the pump pulse. These results are consistent with experiment. The magnitudes of the effective transfer integrals are reduced by strong photoexcitation, and this precursory phenomenon for dynamical localization is mainly driven by a photoinduced change in the ratio of the effective transfer integrals between the two strongest bonds. For eaA (max) 2, the photoinduced transition to the charge-ordered state, which can be regarded as a light-dressed state, occurs because of dynamical localization. Furthermore, the type of photo-generated charge-ordered state can be controlled by choosing eaA (max) and the polarization direction.
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