1204.5579 (Yun-an Yan et al.)
Yun-an Yan, Oliver Kühn
There are two types of two-photon transitions in molecular aggregates, that is, non-local excitations of two monomers and local double excitations to some higher excited intra-monomer electronic state. As a consequence of the inter-monomer Coulomb interaction these different excitation states can be converted into each other. Higher excited intra-monomer states are rather short-lived due to efficient internal conversion of electronic into vibrational energy. Combining both processes leads to the annihilation of an electronic excitation state, which is a major loss channel for establishing high excitation densities in molecular aggregates. Applying theoretical pulse optimization techniques to a Frenkel exciton model it is shown that the dynamics of two-exciton states in linear aggregates (dimer to tetramer) can be influenced by ultrafast shaped laser pulses. In particular, it is studied to what extent the decay of the two-exciton population by inter-band transitions can be transiently suppressed. Intra-band dynamics is described by a dissipative hierarchy equation approach, which takes into account strong exciton-vibrational coupling in the non-Markovian regime.
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http://arxiv.org/abs/1204.5579
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