Abstract
Abstract Excitonic transitions responsible for low energy absorption and fluorescence in dilute solutions and thin films of the organic molecule 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) have been investigated. Combining the results of concentration-dependent solution and thin film absorption and fluorescence with results on thin film exciton diffusion lengths (presented in the following paper, Paper II), we proposed a comprehensive model for the low energy excitonic states in this archetype molecular crystal. We unambiguously identify an extended free charge transfer state at E F CT = 2.23±0.03 eV which has previously been observed to exhibit effects of quantum confinement in ultrathin layers grown under ultrahigh vacuum. This state self-traps at an energy of E ST CT = 2.11±0.04 eV due to the strong exciton-phonon coupling characteristic of this closely packed organic crystal.
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