Abstract

Phonon modes which are strongly coupled to the lowest optical transition of the quasi-one-dimensional organic crystal of MePTCDI ( N- N′-dimethylperylene-3,4,9,10-dicarboximide) are directly time-resolved as they appear as coherent wavepackets in femtosecond pump–probe experiments. We observe both coherent oscillations of intramolecular vibrational wavepackets (internal phonons) and, for the first time in a quasi-one-dimensional organic crystal, lower-energetic modulations which are related to coherent lattice phonons (external phonons). The phononic wavepacket motion is attributed to the electronic ground-state potential surface. The coherence decay of all observed vibrations is in the range of some picoseconds.

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