TY - JOUR
T1 - Long-range energy transport in single supramolecular nanofibres at room temperature
AU - Haedler, Andreas T.
AU - Kreger, Klaus
AU - Issac, Abey
AU - Wittmann, Bernd
AU - Kivala, Milan
AU - Hammer, Natalie
AU - Köhler, Jürgen
AU - Schmidt, Hans Werner
AU - Hildner, Richard
N1 - Funding Information:
support transport of excitons over macroscopic distances4,5. Hence, the efficient long-range transport must be occurring along the ordered nanofibre core, promoted by substantial electronic coupling between the H-aggregated CBT units. The electronic coupling gives rise to the formation of vibronic singlet excitons with a small transition dipole moment for the lowest-energy transition (Supplementary Information section 4). This strongly reduces the rate of the main loss mechanism for electronic excitations from the CBT units of compound 1, that is, energy transfer to the NIBT periphery10; this energy transfer to NIBT can thus no longer compete with transport along the core. However, excitation energy can be trapped at small defects within the core. Energy transfer to the periphery then becomes more likely and photoluminescence from NIBT is observed. In this sense, the NIBT emission reports on both the transport distance along the nanofibres and the structural order of the core. This interpretation is supported by
Publisher Copyright:
© 2015 Macmillan Publishers Limited. All rights reserved.
PY - 2015/7/9
Y1 - 2015/7/9
N2 - Efficient transport of excitation energy over long distances is a key process in light-harvesting systems, as well as in molecular electronics. However, in synthetic disordered organic materials, the exciton diffusion length is typically only around 10 nanometres (refs 4, 5), or about 50 nanometres in exceptional cases, a distance that is largely determined by the probability laws of incoherent exciton hopping. Only for highly ordered organic systems has the transport of excitation energy over macroscopic distances been reported - for example, for triplet excitons in anthracene single crystals at room temperature, as well as along single polydiacetylene chains embedded in their monomer crystalline matrix at cryogenic temperatures (at 10 kelvin, or -263 degrees Celsius). For supramolecular nanostructures, uniaxial long-range transport has not been demonstrated at room temperature. Here we show that individual self-assembled nanofibres with molecular-scale diameter efficiently transport singlet excitons at ambient conditions over more than four micrometres, a distance that is limited only by the fibre length. Our data suggest that this remarkable long-range transport is predominantly coherent. Such coherent long-range transport is achieved by one-dimensional self-assembly of supramolecular building blocks, based on carbonyl-bridged triarylamines, into well defined H-type aggregates (in which individual monomers are aligned cofacially) with substantial electronic interactions. These findings may facilitate the development of organic nanophotonic devices and quantum information technology.
AB - Efficient transport of excitation energy over long distances is a key process in light-harvesting systems, as well as in molecular electronics. However, in synthetic disordered organic materials, the exciton diffusion length is typically only around 10 nanometres (refs 4, 5), or about 50 nanometres in exceptional cases, a distance that is largely determined by the probability laws of incoherent exciton hopping. Only for highly ordered organic systems has the transport of excitation energy over macroscopic distances been reported - for example, for triplet excitons in anthracene single crystals at room temperature, as well as along single polydiacetylene chains embedded in their monomer crystalline matrix at cryogenic temperatures (at 10 kelvin, or -263 degrees Celsius). For supramolecular nanostructures, uniaxial long-range transport has not been demonstrated at room temperature. Here we show that individual self-assembled nanofibres with molecular-scale diameter efficiently transport singlet excitons at ambient conditions over more than four micrometres, a distance that is limited only by the fibre length. Our data suggest that this remarkable long-range transport is predominantly coherent. Such coherent long-range transport is achieved by one-dimensional self-assembly of supramolecular building blocks, based on carbonyl-bridged triarylamines, into well defined H-type aggregates (in which individual monomers are aligned cofacially) with substantial electronic interactions. These findings may facilitate the development of organic nanophotonic devices and quantum information technology.
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U2 - 10.1038/nature14570
DO - 10.1038/nature14570
M3 - Article
AN - SCOPUS:84936947439
SN - 0028-0836
VL - 523
SP - 196
EP - 199
JO - Nature
JF - Nature
IS - 7559
ER -