The fundamental aspects of exciton dynamics in double‐wall cylindrical aggregates of cyanine dyes are studied by means of frequency resolved femtosecond pump‐probe spectroscopy. The collective excitations of the aggregates, resulting from intermolecular dipole‐dipole interactions have the characteristic property – the localization of the lowest lying exciton states. The experimentally observed outer‐to‐inner tubule excitonic energy transfer dynamics and the internal energy relaxation at low temperatures reveal a non‐equilibrium population of the excitonic subsystem. The analysis of measured dynamics reveals very fast picosecond timescale energy relaxation to the optically active energy states. (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
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