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Mesoscopic order and the dimentionality of long-range resonance energy transfer in supramolecular semiconductors

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 Added by Carlos Silva
 Publication date 2008
  fields Physics
and research's language is English




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We present time-resolved photoluminescence measurements on two series of oligo-p-phenylenevinylene materials that self-assemble into supramolecular nanostructures with thermotropic reversibility in dodecane. One set of derivatives form chiral, helical stacks while the second set form less organised, frustrated stacks. Here we study the effects of supramolecular organisation on the resonance energy transfer rates. We measure these rates in nanoassemblies formed with mixed blends of oligomers and compare them with the rates predicted by Foerster theory. Our results and analysis show that control of supramolecular order in the nanometre lengthscale has a dominant effect on the efficiency and dimentionality of resonance energy transfer.



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Electronic and optical properties of doped organic semiconductors are dominated by local interactions between donor and acceptor molecules. However, when such systems are in crystalline form, long-range order competes against short-range couplings. In a first-principles study on three experimentally resolved bulk structures of quaterthiophene doped by (fluorinated) tetracyanoquinodimethane, we demonstrate the crucial role of long-range interactions in donor/acceptor co-crystals. The band structures of the investigated materials exhibit direct band-gaps decreasing in size with increasing amount of F atoms in the acceptors. The valence-band maximum and conduction-band minimum are found at the Brillouin zone boundary and the corresponding wave-functions are segregated on donor and acceptor molecules, respectively. With the aid of a tight-binding model, we rationalize that the mechanisms responsible for these behaviors, which are ubiquitous in donor/acceptor co-crystals, are driven by long-range interactions. The optical response of the analyzed co-crystals is highly anisotropic. The absorption onset is dominated by an intense resonance corresponding to a charge-transfer excitation. Long-range interactions are again responsible for this behavior, which enhances the efficiency of the co-crystals for photo-induced charge separation and transport. In addition to this result, which has important implications in the rational design of organic materials for opto-electronics, our study clarifies that cluster models, accounting only for local interactions, cannot capture the relevant impact of long-range order in donor/acceptor co-crystals.
We propose a method for nano-scale characterization of long range magnetic order in diluted magnetic systems to clarify the origins of the room temperature ferromagnetism. The GaN:Mn thin films are grown by metal-organic chemical vapor deposition with the concentration of Ga-substitutional Mn up to 3.8%. Atomic force microscope (AFM) and magnetic force microscope (MFM) characterizations are performed on etched artificial microstructures and natural dislocation pits. Numerical simulations and theoretical analysis on the AFM and MFM data have confirmed the formation of long range magnetic order and ruled out the possibility that nano-clusters contributed to the ferromagnetism. We suggest that delocalized electrons might play a role in the establishment of this long range magnetic order.
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