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Using time-resolved near-infrared reflectance spectroscopy and time-resolved mid-infrared vibrational spectroscopy, we studied photoinduced phase transition of the charge-ordered insulating phase in a charge-transfer complex (EDO-TTF) 2 PF 6 (EDO-TTF: ethylenedioxy-tetrathiafulvalene) in the hundred picosecond range after photoexcitation. The temporal profiles at 0.83−1.03 eV, which are a characteristic of the photoinduced charge-disproportionate phase immediately after photoexcitation, suggested the formation of a new metastable phase in the hundred picosecond range. Time-resolved vibrational spectra at 1300−1700 cm −1 , where charge-and structure-sensitive CC stretching vibrational modes are located, elucidated that the nature of the new phase is very close to that of the high-temperature metallic phase and it takes about 100 ps for the new phase to emerge accompanied with charge and structure fluctuation.

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